@article{RN18,

title = {A Needle in a Haystack: Transient Porosity in a Closed Pore Square Lattice Coordination Network},

author = {K. Koupepidou and A. C. Eaby and D. Sensharma and S. J. Nikkhah and T. He and M. Lusi and M. Vandichel and L. J. Barbour and S. Mukherjee and M. J. Zaworotko},

url = {<Go to ISI>://WOS:001420558800001},

doi = {10.1002/anie.202423521},

year  = {2025},

date = {2025-01-01},

journal = {Angewandte Chemie-International Edition},

volume = {64},

number = {14},

abstract = {Guest transport through discrete voids (closed pores) in crystalline solids is poorly understood. Herein, we report the gas sorption properties of a nonporous coordination network, [Co(bib)2Cl2] & sdot; 2MeOHn (sql-bib-Co-Cl-alpha), featuring square lattice (sql) topology and the bent linker 1,3-bis(1H-imidazol-1-yl)benzene (bib). The as-synthesized sql-bib-Co-Cl-alpha has 11.3 % (313 & Aring;3) of its unit cell volume in closed pores occupied by methanol (MeOH). Upon desolvation and air exposure, sql-bib-Co-Cl-alpha underwent a single-crystal to single-crystal (SC-SC) phase transformation to sql-bib-Co-Cl-beta ', wherein MeOH was replaced by water. Activation (vacuum or N2 flow) resulted in dehydration and retention of the closed pores, affording sql-bib-Co-Cl-beta with 7.7 % (194 & Aring;3) guest-accessible space. sql-bib-Co-Cl-beta was found to preferentially adsorb C2H2 (at 265 K) over CO2 (at 195 K) through gate-opening mechanisms, at gate-opening pressures of 59.8 and 27.7 kPa, respectively, while other C2 gases were excluded. PXRD was used to monitor transformations between the three phases of sql-bib-Co-Cl, while in situ DSC, in situ SCXRD under CO2 pressure, and computational studies provided insight into the guest transport mechanism, which we attribute to the angular, flexible nature of the bib ligand. Further, the preferential adsorption of C2H2 over CO2 and other C2 gases suggests that transiently porous sorbents might have utility in separations.},

note = {0yd7s 

Times Cited:0 

Cited References Count:61},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{RN8,

title = {Hydride-Induced Reconstruction of Pd Electrode Surfaces: A Combined Computational and Experimental Study},

author = {A. Ngoipala and C. Schott and V. Briega-Martos and M. Qamar and M. Mrovec and S. J. Nikkhah and T. O. Schmidt and L. Deville and A. Capogrosso and L. Moumaneix and T. Kallio and A. Viola and F. Maillard and R. Drautz and A. S. Bandarenka and S. Cherevko and M. Vandichel and E. L. Gubanova},

url = {<Go to ISI>://WOS:001370021500001},

doi = {10.1002/adma.202410951},

issn = {0935-9648},

year  = {2025},

date = {2025-01-01},

journal = {Advanced Materials},

volume = {37},

number = {4},

abstract = {Designing electrocatalysts with optimal activity and selectivity relies on a thorough understanding of the surface structure under reaction conditions. In this study, experimental and computational approaches are combined to elucidate reconstruction processes on low-index Pd surfaces during H-insertion following proton electroreduction. While electrochemical scanning tunneling microscopy clearly reveals pronounced surface roughening and morphological changes on Pd(111), Pd(110), and Pd(100) surfaces during cyclic voltammetry, a complementary analysis using inductively coupled plasma mass spectrometry excludes Pd dissolution as the primary cause of the observed restructuring. Large-scale molecular dynamics simulations further show that these surface alterations are related to the creation and propagation of structural defects as well as phase transformations that take place during hydride formation.},

note = {U1u1v 

Times Cited:2 

Cited References Count:76},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{RN17,

title = {Dissipative Particle Dynamics Modeling in Polymer Science and Engineering},

author = {S. J. Nikkhah and M. Vandichel},

url = {<Go to ISI>://WOS:001466957800001},

doi = {ARTN e70018 

10.1002/wcms.70018},

issn = {1759-0876},

year  = {2025},

date = {2025-01-01},

journal = {Wiley Interdisciplinary Reviews-Computational Molecular Science},

volume = {15},

number = {2},

abstract = {Polymeric materials are intricate systems with unique properties across different length and time scales, presenting challenges in understanding the hierarchical features that govern their behavior. Advancing innovative polymeric systems requires a deep comprehension of these complexities. Dissipative particle dynamics (DPD), a mesoscale simulation technique, has proven instrumental in elucidating polymer behavior. Unlike molecular dynamics, which tracks individual molecules, DPD employs a coarse-graining approach, to describe molecular systems as particles interacting via soft potentials. Thanks to its computational efficiency, DPD has enabled researchers to numerically study several complex fluid applications in detail. Moreover, with the ever-increasing high-performance computing resources, it has become possible to tackle larger molecular systems beyond the nanoscale, typically micrometer-sized systems. An in-depth analysis of the theoretical foundations of DPD is presented, focusing on its methodology, mathematical formulations, and computational implementation. This review then explores various applications of DPD simulations for polymeric systems, demonstrating DPD's ability to accurately capture phenomena such as polymer self-assembly, polymer behavior in solutions and blends, charged polymers, polymer interfaces, polymer rheology, polymeric membranes, polymerization reactions, and polymeric composites. Overall, this review examines the adoption of DPD as a predictive modeling tool for polymeric materials, focusing on its key features and its integration with methods such as atomistic molecular dynamics to determine the interaction parameters. Building on these advancements, future directions for DPD include its potential applications in other systems like biological membranes, macromolecules, and shape-memory materials.},

note = {1ke1b 

Times Cited:0 

Cited References Count:398},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{RN15,

title = {An ionic ultramicroporous polymer with engineered nanopores enables enhanced acetylene/carbon dioxide separation},

author = {A. Raza and S. J. Nikkhah and L. Croitor and A. G. Attallah and E. Hirschmann and M. Vandichel and S. Mukherjee},

url = {<Go to ISI>://WOS:001460265600001},

doi = {10.1039/d5cc01092f},

issn = {1359-7345},

year  = {2025},

date = {2025-01-01},

journal = {Chemical Communications},

volume = {61},

number = {35},

abstract = {A nanopore engineering approach enhances acetylene (C2H2) over carbon dioxide (CO2) selectivity in ionic ultramicroporous polymers (IUPs), an understudied class of sorbents. Extending the cationic arm of a prototypical IUP nearly doubles its C2H2/CO2 selectivity from 4.9 to 8.5 (at 298 K, 1 bar), underpinned by further observations from dynamic separation experiments and bespoke computational insights.},

note = {1tt6j 

Times Cited:0 

Cited References Count:20},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{RN21,

title = {Improved low-temperature CO oxidation using heterogeneous nanofibrous structures decorated with Pd atoms and nanocrystals},

author = {M. A. Rodriguez-Olguin and D. Cazac and F. Ruiz-Zepeda and S. Bartling and M. Bosco and H. Atia and R. Eckelt and A. Manzo-Robledo and M. Vandichel and A. Aguirre and J. G. E. Gardeniers and A. Susarrey-Arce},

url = {https://www.sciencedirect.com/science/article/pii/S2949754X25000067},

doi = {https://doi.org/10.1016/j.mtcata.2025.100093},

issn = {2949-754X},

year  = {2025},

date = {2025-01-01},

journal = {Materials Today Catalysis},

volume = {9},

pages = {100093},

abstract = {Amorphous alumina shaped as nanofibers forming a non-woven network, functioning as a heterogeneous dispersion for palladium (Pd) atoms and nanocrystals, is unique yet unstudied for low-temperature CO oxidation. This work demonstrates that nanometric-size alumina fibers (ANFs) with a surface area of ⁓230 m2/g can host Pd species that remain nearly intact after CO oxidation. The ANFs contain various Pd (Pd-ANFs) loadings, ranging from 1 %wt. (Pd1-ANFs), 3 %wt. (Pd3-ANFs), to 5 %wt. (Pd5-ANFs). Among them, Pd3-ANFs show the highest CO chemisorption. Hence, the chemical environment of the Pd3-ANFs is assessed using NAP-XPS under various CO and O2 mixtures. NAP-XPS shows the presence of metallic and oxidized Pd species. The results are correlated with DRIFT spectroscopy, which unveils the CO species adsorbed over Pd. Furthermore, a computational-based kinetic model for CO oxidation shows that Pd single atoms start the CO-oxidation, followed by larger Pd crystals during light-off. Our results demonstrate that the Pd-ANFs have higher activity when compared with the Pd alumina nanoparticles (Pd-ANP) counterpart that lacks a fibrous structure, highlighting the benefits of the ANF's structural network in stabilizing atomic and nanometric scale metal catalysts for low-temperature CO oxidation.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{RN22,

title = {Multivariate modulation of Zr6 UiO-66 for enhanced cooperative CO2 adsorption through defect multi-functionalisation},

author = {Carmen Rosales-Martínez and Sousa Javan Nikkhah and Marcileia Zanatta and Juan Carlos Martínez and Matthias Vandichel and Isabel Abánades Lázaro},

url = {http://dx.doi.org/10.1039/D5MH00650C},

doi = {10.1039/D5MH00650C},

issn = {2051-6347},

year  = {2025},

date = {2025-01-01},

journal = {Materials Horizons},

abstract = {The multivariate modulation of MOFs allows for the simultaneous introduction of multiple functionalities at defect sites during synthesis, enhancing the MOF porosity. By the thoughtful choice of modulators’ functionalities targeted at CO2 adsorption, the designed dimodulated MOF, UiO-66-NH2/SO3, has a 6.6 mmol/g CO2 adsorption at 273K and 1 bar, a 2.15-fold increase compared to the pristine MOF and a 1.6-fold enhancement compared to the single-modulated MOFs. This enhancement is due to the cooperative effect of functional units, which is supported by Monte Carlo simulations.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{RN19,

title = {Palladium Nanocubes with 100 Facets for Hydrogen Evolution Reaction: Synthesis, Experiment and Theory},

author = {I. Saldan and L. Moumaneix and M. Umer and D. Pavlinak and M. Rihova and E. Kolibalova and J. Petrus and T. Kallio and M. Vandichel and J. M. Macak},

url = {<Go to ISI>://WOS:001413862400001},

doi = {10.1002/smll.202408788},

issn = {1613-6810},

year  = {2025},

date = {2025-01-01},

journal = {Small},

volume = {21},

number = {11},

abstract = {Spatially separated palladium nanocubes (Pd NCs) terminated by 100 facets are synthesized using direct micelles approach. The stepwise seed-mediated growth of Pd NCs is applied for the first time. The resulting Pd NCs are thoroughly characterized by HR-TEM, XPS, Raman, ATR-FTIR, TGA, and STEM-EDX spectroscopies. Some traces of residual stabilizer (polyvinylpyrrolidone, PVP) attached to the vertices of Pd NCs are identified after the necessary separation-washing procedure, however, it is vital to avoid aggregation of the NCs. Pd NCs are subsequently and uniformly loaded on Vulcan carbon (approximate to 20 wt.%) for the electrochemical hydrogen cycling. By post-mortem characterizations, it is revealed that their shape and size remained very stable after all electrochemical experiments. However, a strong effect of the NCs size on their hydrogen interaction is revealed. Hydrogen absorption capacity, measured as the H:Pd ratio, ranges from 0.28 to 0.48, while hydrogen evolution and oxidation reactions (HER and HOR) kinetics decrease from 15.5 to 4.6 mA.mg Pd-1 between approximate to 15 and 34 nm of Pd NCs, respectively. Theoretical calculations further reveal that adsorption of H atoms and their penetration into the Pd lattice tailors the NCs electronic structure, which in turn controls the kinetics of HER, experimentally observed by the electrochemical tests. This work may pave the way to the design of highly active electrocatalysts for efficient HER stable for a long reactive time. In particular, obtained results might be transferred to active Pd-alloy-based NCs terminated by 100 facets.},

note = {0hq6y 

Times Cited:1 

Cited References Count:68},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{RN20,

title = {One Step Further: A Flexible Metal-Organic Framework that Functions as a Dual-Purpose Water Vapor Sorbent},

author = {S. M. Shabangu and A. A. Bezrukov and A. C. Eaby and S. J. Nikkhah and S. Darwish and V. I. Nikolayenko and D. Sensharma and S. Q. Wang and M. Vandichel and M. J. Zaworotko},

url = {<Go to ISI>://WOS:001388634600001},

doi = {10.1021/acsmaterialslett.4c02019},

year  = {2025},

date = {2025-01-01},

journal = {Acs Materials Letters},

volume = {7},

number = {2},

pages = {433-441},

abstract = {We report a water induced phase transformation in a flexible MOF, [Zn3(OH)2(btca)2] (Hbtca = 1H-benzotriazole-5-carboxylic acid), that exhibits a two-step water vapor sorption isotherm associated with water-induced phase transformations. Variable temperature X-ray diffraction studies revealed that the dehydrated phase, LP-beta, is almost isostructural with the previously reported solvated phase, LP-alpha. LP-beta reversibly transformed to a partially hydrated phase, NP, at 5% RH, and a fully hydrated phase, LP-gamma, at 47% RH. Structural studies reveal that host-guest and guest-guest interactions are involved in the NP, LP-alpha, and LP-gamma phases. The LP-beta phase, however, is atypical; molecular modeling studies indicating that it is indeed energetically favorable as a LP structure. To our knowledge, [Zn3(OH)2(btca)2] is only the second sorbent that exhibits water induced LP-NP-LP transformations (after MIL-53) and represents the first regeneration optimized sorbent (ROS) with two steps at RH ranges relevant for both atmospheric water harvesting and dehumidification.},

note = {U5n0b 

Times Cited:1 

Cited References Count:79},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{RN14,

title = {A pcu topology metal-organic framework, Ni(1,4-bib)(inca) 

, that exhibits high CO 

/N 

 selectivity and low water vapour affinity},

author = {S. M. Shabangu and A. C. Eaby and S. J. Nikkhah and L. Croitor and T. He and A. A. Bezrukov and M. Vandichel and M. J. Zaworotko},

url = {<Go to ISI>://WOS:001485341600001},

doi = {10.1039/d5ta01995h},

issn = {2050-7488},

year  = {2025},

date = {2025-01-01},

journal = {Journal of Materials Chemistry A},

abstract = {Herein we report the synthesis of a new metal-organic framework, Ni(1,4-bib)(inca)2 or pcu-1-Ni, where 1},

note = {2lg7t 

Times Cited:0 

Cited References Count:58},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{RN16,

title = {Exploring a new silica-supported BrØnsted-Lewis ionic liquid catalyst for the cycloaddition of CO2 and propylene oxide: A combined experimental and computational study},

author = {H. D. Velázquez and K. V. Vega-Calleja and R. Lipin and M. Vandichel and L. E. Quintero-Mondragón and J. N. Castillo-Cervantes and J. G. Hernández-Cortez and R. Martínez-Palou},

url = {<Go to ISI>://WOS:001442572000001},

doi = {ARTN 103048 

10.1016/j.jcou.2025.103048},

issn = {2212-9820},

year  = {2025},

date = {2025-01-01},

journal = {Journal of Co2 Utilization},

volume = {94},

abstract = {The field of liquid phase catalysis has explored the replacement of traditional solvents with ionic liquids, as well as the use of ionic liquids as catalyst. Herein, a novel silica-supported Fe-based Br & Oslash;nsted-Lewis functionalized ionic liquid (BLsIL-Fe) was synthesized and used as a catalyst for the cycloaddition of CO2 to propylene oxide, yielding propylene carbonate. The catalyst was prepared by grafting a sulfonic acid-functionalized imidazole with a FeCl4- complex anion onto a commercial silica support (silica gel 60). The effects of temperature, pressure, catalyst loading, and reaction time on the catalytic activity of BLsILs were investigated. Our findings reveal that our catalyst remained active at a low catalyst loading of 0.18 mol% (active sites per mol of propylene oxide) at 120 degrees C, achieving up to 90.5 % conversion with a propylene carbonate selectivity above 97.0 % after four hours. The catalyst demonstrated reusability through a simple filtration and washing procedure, maintaining its catalytic activity over five cycles. Plausible catalytic reaction pathways for the CO2 valorization process using BLsILs were elucidated using density functional theory, revealing that the ring-closing step is the rate determining step. Overall, the work opens new avenues for designing dual-acid functionalized ILs, enhancing performance across a wide range of catalytic reactions.},

note = {0ag1n 

Times Cited:0 

Cited References Count:73},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{NGOIPALA2024829,

title = {Computational unravelling of cathodic hydride formation on palladium surfaces},

author = {Apinya Ngoipala and Raju Lipin and Ryan Lacdao Arevalo and Matthias Vandichel},

url = {https://www.sciencedirect.com/science/article/pii/S0360319923062456},

doi = {https://doi.org/10.1016/j.ijhydene.2023.12.019},

issn = {0360-3199},

year  = {2024},

date = {2024-01-01},

urldate = {2024-01-01},

journal = {International Journal of Hydrogen Energy},

volume = {53},

pages = {829-839},

abstract = {Palladium (Pd) is well-known for its role in catalyzing hydrogen-based reduction reactions, owing to its excellent catalytic activity and hydrogen storage ability. Its surface and subsurface structures under electrochemical conditions are vital in understanding the hydrogen evolution reaction (HER) mechanism at the Pd cathodes where the most active sites are located on ‘in situ’ formed Pd-hydride layers. In this work, we investigate the process of Pd-hydride formation as well as the step-by-step formation and stability of Pd-hydride/Pd interfaces under electrochemical conditions using first-principles calculations. Our results reveal that among the low-indexed surfaces (111), (110) and (100), the (111) surface is expected to be the most dominant surface in a Pd nanostructure in addition to being the most preferred surface for hydrogen adsorption. Based on calculated Pourbaix diagrams, we can identify the relevant regions close to the equilibrium electrode potential and pH for proton electroreduction and hydrogen evolution, where the Pd surfaces start to be covered by hydrogen adatoms, and when the electrode potential is decreased, there are clear thermodynamic indications for more and more subsurface hydride layers. Overall, the results provide insights into the stability and formation of hydrogen-containing Pd surfaces, forming PdH/Pd type interfaces. Our idealized model systems are a first step towards elucidation of relevant active sites on Pd.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/acsami.3c16634,

title = {Crystal Engineering of a New Hexafluorogermanate Pillared Hybrid Ultramicroporous Material Delivers Enhanced Acetylene Selectivity},

author = {Nathan C. Harvey-Reid and Debobroto Sensharma and Soumya Mukherjee and Komal M. Patil and Naveen Kumar and Sousa Javan Nikkhah and Matthias Vandichel and Michael J. Zaworotko and Paul E. Kruger},

url = {https://doi.org/10.1021/acsami.3c16634},

doi = {10.1021/acsami.3c16634},

year  = {2024},

date = {2024-01-01},

journal = {ACS Applied Materials & Interfaces},

volume = {16},

number = {4},

pages = {4803-4810},

note = {PMID: 38258417},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/acs.nanolett.3c02810,

title = {Resolving Multielement Semiconductor Nanocrystals at the Atomic Level: Complete Deciphering of Domains and Order in Complex CuαZnβSnγSeδ (CZTSe) Tetrapods},

author = {Huan Ren and Yuanwei Sun and Frank Hoffmann and Matthias Vandichel and Temilade E. Adegoke and Ning Liu and Conor McCarthy and Peng Gao and Kevin M. Ryan},

url = {https://doi.org/10.1021/acs.nanolett.3c02810},

doi = {10.1021/acs.nanolett.3c02810},

year  = {2024},

date = {2024-01-01},

journal = {Nano Letters},

volume = {24},

number = {7},

pages = {2125-2130},

note = {PMID: 38341872},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{LIPIN2024460,

title = {Computational surface Pourbaix diagrams to unravel cathodic hydride formation on defective palladium surfaces},

author = {Raju Lipin and Apinya Ngoipala and Ryan Lacdao Arevalo and Matthias Vandichel},

url = {https://www.sciencedirect.com/science/article/pii/S0360319924006724},

doi = {https://doi.org/10.1016/j.ijhydene.2024.02.248},

issn = {0360-3199},

year  = {2024},

date = {2024-01-01},

journal = {International Journal of Hydrogen Energy},

volume = {61},

pages = {460-472},

abstract = {Defects, both intrinsic and hydrogen-induced, are commonplace in electrochemical processes, particularly in catalysis where hydrogen can penetrate the catalysts and influence chemical reactions. Palladium (Pd), renowned for its high hydrogen permeability, forms defects upon exposure to hydrogen. Herein, we investigate various defective Pd-surfaces containing missing row, vacancy, and adatom defects, and their interplay with hydrogen atoms to enhance our understanding of Pd-based catalysts during hydrogenation reactions or with Pd as a cathode. Low-index defective surfaces and various hydrogen (H) coverages are explored to construct surface Pourbaix diagrams (SPD) and study their H-termination at specific pH and potential. The SPDs show increased hydrogen adsorption upon lowering the electrode potential. The stability of defective surfaces follows Pd’(110) > Pd’(100) > Pd’(111), in contrast to the stability trend observed for pristine surfaces, Pd(111) > Pd(100) > Pd(110). This reversal is attributed to the tendency of ‘less stable’ open surfaces, such as Pd(110), to reconstruct, or be stabilized by hydrogen. Our study emphasizes the importance of hydrogen sublayers in stabilizing H-covered defective surfaces, which facilitates the formation of Pd vacancies in the sublayers. Our work is essential to advance catalysis and surface science, as it provides valuable insights into material restructuring under electrocatalytic environments.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/acsami.4c03777,

title = {Effect of Polymorphism on the Sorption Properties of a Flexible Square-Lattice Topology Coordination Network},

author = {Aizhamal Subanbekova and Andrey A. Bezrukov and Volodymyr Bon and Varvara I. Nikolayenko and Kyriaki Koupepidou and Debobroto Sensharma and Sousa Javan Nikkhah and Shi-Qiang Wang and Stefan Kaskel and Matthias Vandichel and Michael J. Zaworotko},

url = {https://doi.org/10.1021/acsami.4c03777},

doi = {10.1021/acsami.4c03777},

year  = {2024},

date = {2024-01-01},

journal = {ACS Applied Materials & Interfaces},

volume = {16},

number = {18},

pages = {24132-24140},

note = {PMID: 38666365},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/acsmaterialslett.4c00511,

title = {Gate-opening Induced by C8 Aromatics in a Double Diamondoid Coordination Network},

author = {Kyriaki Koupepidou and Shi-Qiang Wang and Varvara I. Nikolayenko and Dominic C. Castell and Catiúcia R. M. O. Matos and Matthias Vandichel and Michael J. Zaworotko},

url = {https://doi.org/10.1021/acsmaterialslett.4c00511},

doi = {10.1021/acsmaterialslett.4c00511},

year  = {2024},

date = {2024-01-01},

journal = {ACS Materials Letters},

volume = {6},

number = {6},

pages = {2197-2204},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/jacs.4c03555,

title = {Reversible Phase Transformations in a Double-Walled Diamondoid Coordination Network with a Stepped Isotherm for Methane},

author = {Xia Li and Debobroto Sensharma and Leigh Loots and Shubo Geng and Sousa Javan Nikkhah and En Lin and Volodymyr Bon and Wansheng Liu and Zhifang Wang and Tao He and Soumya Mukherjee and Matthias Vandichel and Stefan Kaskel and Leonard J. Barbour and Zhenjie Zhang and Michael J. Zaworotko},

url = {https://doi.org/10.1021/jacs.4c03555},

doi = {10.1021/jacs.4c03555},

year  = {2024},

date = {2024-01-01},

journal = {Journal of the American Chemical Society},

volume = {146},

number = {27},

pages = {18387-18395},

note = {PMID: 38904843},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/acs.inorgchem.4c01933,

title = {Hemilabile Binding of Acetylene in an Amide-Rich Ultramicroporous MOF Enables Strong Acetylene Selectivity},

author = {Subhajit Dutta and Soumya Mukherjee and Sousa Javan Nikkhah and Omid T. Qazvini and Gourab K. Dam and Matthias Vandichel and Tarak Nath Mandal and Sujit K. Ghosh},

url = {https://doi.org/10.1021/acs.inorgchem.4c01933},

doi = {10.1021/acs.inorgchem.4c01933},

year  = {2024},

date = {2024-01-01},

journal = {Inorganic Chemistry},

volume = {63},

number = {27},

pages = {12404-12408},

note = {PMID: 38913858},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{https://doi.org/10.1002/advs.202402154,

title = {Structure-Property Correlations in CZTSe Domains within Semiconductor Nanocrystals as Photovoltaic Absorbers},

author = {Apinya Ngoipala and Huan Ren and Kevin M. Ryan and Matthias Vandichel},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/advs.202402154},

doi = {https://doi.org/10.1002/advs.202402154},

year  = {2024},

date = {2024-01-01},

journal = {Advanced Science},

volume = {11},

number = {31},

pages = {2402154},

abstract = {Abstract Semiconductor nanocrystals (NCs) are promising materials for various applications. Two of four recently identified CuαZnβSnγSeδ (CZTSe) domains demonstrate metallic character, while the other two exhibit semiconductor character. The presence of both metallic and semiconductor domains in one NC can hugely benefit future applications. In contrast to traditional band gap studies in the NC community, this study emphasizes that NC domain interfaces also affect the electronic properties. Specifically, the measured band gap of a tetrapod-shaped CZTSe NC is demonstrated to originate from two specific domains (tetragonal I4¯$bar 4$ and monoclinic P1c1 Cu2ZnSnSe4). The heterojunction between these two semiconductor domains exhibits a staggered type-II band alignment, facilitating the separation of photogenerated electron-hole pairs. Interestingly, tetrapod NCs have the potential to be efficient absorber materials with higher capacitance in photovoltaic applications due to the presence of both semiconductor/semiconductor interfaces and metal/semiconductor “Schottky”-junctions. For the two photo-absorbing domains, the calculated absorption spectra yield maximum photon-absorption coefficients of about 105 cm−1 in the visible and UV regions and a theoretical solar power conversion efficiency up to 20.8%. These insights into the structure-property relationships in CZTSe NCs will guide the design of more efficient advanced optical CZTSe materials for various applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{D4TA04116J,

title = {Temperature promotes selectivity during electrochemical CO2 reduction on NiO:SnO2 nanofibers},

author = {M. A. Rodriguez-Olguin and R. Lipin and M. Suominen and F. Ruiz-Zepeda and E. Castañeda-Morales and A. Manzo-Robledo and J. G. E. Gardeniers and C. Flox and T. Kallio and M. Vandichel and A. Susarrey-Arce},

url = {http://dx.doi.org/10.1039/D4TA04116J},

doi = {10.1039/D4TA04116J},

year  = {2024},

date = {2024-01-01},

journal = {J. Mater. Chem. A},

pages = {-},

publisher = {The Royal Society of Chemistry},

abstract = {Electrolyzers operate over a range of temperatures; hence, it is crucial to design electrocatalysts that do not compromise the product distribution unless temperature can promote selectivity. This work reports a synthetic approach based on electrospinning to produce NiO:SnO2 nanofibers (NFs) for selectively reducing CO2 to formate above room temperature. The NFs comprise compact but disjoined NiO and SnO2 nanocrystals identified with STEM. The results are attributed to the segregation of NiO and SnO2 confirmed with XRD. The NFs are evaluated for the CO2 reduction reaction (CO2RR) over various temperatures (25, 30, 35, and 40 °C). The highest faradaic efficiencies to formate (FEHCOO−) are reached by NiO:SnO2 NFs containing 50% of NiO and 50% SnO2 (NiOSnO50NF), and 25% of NiO and 75% SnO2 (NiOSnO75NF), at an electroreduction temperature of 40 °C. At 40 °C, product distribution is assessed with in situ differential electrochemical mass spectrometry (DEMS), recognizing methane and other species, like formate, hydrogen, and carbon monoxide, identified in an electrochemical flow cell. XPS and EELS unveiled the FEHCOO− variations due to a synergistic effect between Ni and Sn. DFT-based calculations reveal the superior thermodynamic stability of Ni-containing SnO2 systems towards CO2RR over the pure oxide systems. Furthermore, computational surface Pourbaix diagrams showed that the presence of Ni as a surface dopant increases the reduction of the SnO2 surface and enables the production of formate. Our results highlight the synergy between NiO and SnO2, which can promote the electroreduction of CO2 at temperatures above room temperature.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/jacs.3c07198,

title = {Highly Selective p-Xylene Separation from Mixtures of C8 Aromatics by a Nonporous Molecular Apohost},

author = {Maryam Rahmani and Catiúcia R. M. O. Matos and Shi-Qiang Wang and Andrey A. Bezrukov and Alan C. Eaby and Debobroto Sensharma and Yassin Hjiej-Andaloussi and Matthias Vandichel and Michael J. Zaworotko},

url = {https://doi.org/10.1021/jacs.3c07198},

doi = {10.1021/jacs.3c07198},

year  = {2023},

date = {2023-12-06},

urldate = {2023-01-01},

journal = {Journal of the American Chemical Society},

volume = {145},

number = {50},

pages = {27316-27324},

note = {PMID: 38055597},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/acsabm.3c00452,

title = {Anticancer Potential of Dendritic Poly(aryl ether)-Substituted Polypyridyl Ligand-Based Ruthenium(II) Coordination Entities},

author = {Liju Raju and Sousa Javan Nikkhah and MosaChristas K and Matthias Vandichel and Rajkumar Eswaran},

url = {https://doi.org/10.1021/acsabm.3c00452},

doi = {10.1021/acsabm.3c00452},

year  = {2023},

date = {2023-10-20},

urldate = {2023-01-01},

journal = {ACS Applied Bio Materials},

volume = {6},

number = {10},

pages = {4226-4239},

note = {PMID: 37782900},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{https://doi.org/10.1002/anie.202309985,

title = {Shape-Memory Effect Enabled by Ligand Substitution and CO2 Affinity in a Flexible SIFSIX Coordination Network},

author = {Bai-Qiao Song and Mohana Shivanna and Mei-Yan Gao and Shi-Qiang Wang and Cheng-Hua Deng and Qing-Yuan Yang and Sousa Javan Nikkhah and Matthias Vandichel and Susumu Kitagawa and Michael J. Zaworotko},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202309985},

doi = {https://doi.org/10.1002/anie.202309985},

year  = {2023},

date = {2023-09-28},

urldate = {2023-01-01},

journal = {Angewandte Chemie International Edition},

volume = {62},

number = {47},

pages = {e202309985},

abstract = {Abstract We report that linker ligand substitution involving just one atom induces a shape-memory effect in a flexible coordination network. Specifically, whereas SIFSIX-23-Cu, [Cu(SiF6)(L)2]n, (L=1,4-bis(1-imidazolyl)benzene, SiF62−=SIFSIX) has been previously reported to exhibit reversible switching between closed and open phases, the activated phase of SIFSIX-23-CuN, [Cu(SiF6)(LN)2]n (LN=2,5-bis(1-imidazolyl)pyridine), transformed to a kinetically stable porous phase with strong affinity for CO2. As-synthesized SIFSIX-23-CuN, α, transformed to less open, γ, and closed, β, phases during activation. β did not adsorb N2 (77 K), rather it reverted to α induced by CO2 at 195, 273 and 298 K. CO2 desorption resulted in α′, a shape-memory phase which subsequently exhibited type-I isotherms for N2 (77 K) and CO2 as well as strong performance for separation of CO2/N2 (15/85) at 298 K and 1 bar driven by strong binding (Qst=45–51 kJ/mol) and excellent CO2/N2 selectivity (up to 700). Interestingly, α′ reverted to β after re-solvation/desolvation. Molecular simulations and density functional theory (DFT) calculations provide insight into the properties of SIFSIX-23-CuN.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/acs.inorgchem.3c01777,

title = {Hf-Based MOF for Rapid and Selective Sensing of a Nerve Agent Simulant and an Aminophenol: Insights from Experiments and Theory},

author = {Subhrajyoti Ghosh and Raju Lipin and Apinya Ngoipala and Niklas Ruser and Diletta Morelli Venturi and Abhijeet Rana and Matthias Vandichel and Shyam Biswas},

url = {https://doi.org/10.1021/acs.inorgchem.3c01777},

doi = {10.1021/acs.inorgchem.3c01777},

year  = {2023},

date = {2023-08-28},

urldate = {2023-01-01},

journal = {Inorganic Chemistry},

volume = {62},

number = {36},

pages = {14632-14646},

note = {PMID: 37640009},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{zand_role_2023,

title = {Role of decomposition products in the oxidation of cyclohexene using a manganese(III) complex},

author = {Zahra Zand and Younes Mousazade and Ryan Lacdao Arevalo and Robabeh Bagheri and Mohammad Reza Mohammadi and Rahman Bikas and Petko Chernev and Pavlo Aleshkevych and Matthias Vandichel and Zhenlun Song and Holger Dau and Mohammad Mahdi Najafpour},

url = {https://doi.org/10.1038/s42004-023-00881-x},

doi = {10.1038/s42004-023-00881-x},

issn = {2399-3669},

year  = {2023},

date = {2023-05-01},

journal = {Communications Chemistry},

volume = {6},

number = {1},

pages = {94},

abstract = {Metal complexes are extensively explored as catalysts for oxidation reactions; molecular-based mechanisms are usually proposed for such reactions. However, the roles of the decomposition products of these materials in the catalytic process have yet to be considered for these reactions. Herein, the cyclohexene oxidation in the presence of manganese(III) 5,10,15,20-tetra(4-pyridyl)-21H,23H-porphine chloride tetrakis(methochloride) (1) in a heterogeneous system via loading the complex on an SBA-15 substrate is performed as a study case. A molecular-based mechanism is usually suggested for such a metal complex. Herein, 1 was selected and investigated under the oxidation reaction by iodosylbenzene or (diacetoxyiodo)benzene (PhI(OAc)2). In addition to 1, at least one of the decomposition products of 1 formed during the oxidation reaction could be considered a candidate to catalyze the reaction. First-principles calculations show that Mn dissolution is energetically feasible in the presence of iodosylbenzene and trace amounts of water.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{https://doi.org/10.1002/smll.202206945,

title = {A Robust Molecular Porous Material for C2H2/CO2 Separation},

author = {Mei-Yan Gao and Debobroto Sensharma and Andrey A. Bezrukov and Yassin H. Andaloussi and Shaza Darwish and Chenghua Deng and Matthias Vandichel and Jian Zhang and Michael J. Zaworotko},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/smll.202206945},

doi = {https://doi.org/10.1002/smll.202206945},

year  = {2023},

date = {2023-01-01},

urldate = {2022-12-22},

journal = {Small},

volume = {19},

number = {n/a},

issue = {11},

pages = {2206945},

abstract = {Abstract A molecular porous material, MPM-2, comprised of cationic [Ni2(AlF6)(pzH)8(H2O)2] and anionic [Ni2Al2F11(pzH)8(H2O)2] complexes that generate a charge-assisted hydrogen-bonded network with pcu topology is reported. The packing in MPM-2 is sustained by multiple interionic hydrogen bonding interactions that afford ultramicroporous channels between dense layers of anionic units. MPM-2 is found to exhibit excellent stability in water (>1 year). Unlike most hydrogen-bonded organic frameworks which typically show poor stability in organic solvents, MPM-2 exhibited excellent stability with respect to various organic solvents for at least two days. MPM-2 is found to be permanently porous with gas sorption isotherms at 298 K revealing a strong affinity for C2H2 over CO2 thanks to a high (ΔQst)AC [Qst (C2H2) − Qst (CO2)] of 13.7 kJ mol−1 at low coverage. Dynamic column breakthrough experiments on MPM-2 demonstrated the separation of C2H2 from a 1:1 C2H2/CO2 mixture at 298 K with effluent CO2 purity of 99.995% and C2H2 purity of >95% after temperature-programmed desorption. C-H···F interactions between C2H2 molecules and F atoms of AlF63− are found to enable high selectivity toward C2H2, as determined by density functional theory simulations.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{D3NJ00335C,

title = {Peripherally “tertiary butyl ester” functionalized bipyridine cored dendrons: from synthesis and characterization to molecular dynamic simulation study},

author = {Liju Raju and Sousa Javan Nikkhah and Matthias Vandichel and Eswaran Rajkumar},

url = {http://dx.doi.org/10.1039/D3NJ00335C},

doi = {10.1039/D3NJ00335C},

year  = {2023},

date = {2023-01-01},

journal = {New J. Chem.},

volume = {47},

issue = {18},

pages = {8913-8924},

publisher = {The Royal Society of Chemistry},

abstract = {In this research, we have designed and synthesized a series of novel bipyridine cored poly(benzyl-ether) dendrons containing tertiary butyl esters at their periphery. The molecular structures of the synthesized dendrons were characterized via NMR and mass spectrometry. We investigated the solvent dependent hydrodynamic size of the synthesized dendrons in dimethyl sulfoxide (DMSO) and water using dynamic light scattering (DLS) experiments and the water contact angle of the dendrons was also analyzed. To understand the structure and solvation behaviour of these novel dendrons at the atomistic level, we performed all-atom molecular dynamics (MD) simulations. The behaviour, configuration, and size of the dendrons in DMSO and water were studied through calculation of the radius of gyration (Rg), radial distribution function g(r), and solvent accessible surface area (SASA). The modelling results confirmed the experimental observations that DMSO is a better solvent than water for dendrons as it results in a more unfolded molecular structure. Based on the above experimental results, these dendritic polymers are an excellent candidate for multifunctional theranostics platforms.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/jacs.3c01113,

title = {One Atom Can Make All the Difference: Gas-Induced Phase Transformations in Bisimidazole-Linked Diamondoid Coordination Networks},

author = {Kyriaki Koupepidou and Varvara I. Nikolayenko and Debobroto Sensharma and Andrey A. Bezrukov and Matthias Vandichel and Sousa Javan Nikkhah and Dominic C. Castell and Kolade A. Oyekan and Naveen Kumar and Aizhamal Subanbekova and William G. Vandenberghe and Kui Tan and Leonard J. Barbour and Michael J. Zaworotko},

url = {https://doi.org/10.1021/jacs.3c01113},

doi = {10.1021/jacs.3c01113},

year  = {2023},

date = {2023-01-01},

journal = {Journal of the American Chemical Society},

volume = {145},

number = {18},

pages = {10197-10207},

note = {PMID: 37099724},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/jacs.3c03505,

title = {Highly Productive C3H4/C3H6 Trace Separation by a Packing Polymorph of a Layered Hybrid Ultramicroporous Material},

author = {Mei-Yan Gao and Andrey A. Bezrukov and Bai-Qiao Song and Meng He and Sousa Javan Nikkhah and Shi-Qiang Wang and Naveen Kumar and Shaza Darwish and Debobroto Sensharma and Chenghua Deng and Jiangnan Li and Lunjie Liu and Rajamani Krishna and Matthias Vandichel and Sihai Yang and Michael J. Zaworotko},

url = {https://doi.org/10.1021/jacs.3c03505},

doi = {10.1021/jacs.3c03505},

year  = {2023},

date = {2023-01-01},

journal = {Journal of the American Chemical Society},

volume = {145},

number = {21},

pages = {11837-11845},

note = {PMID: 37204941},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/acsami.2c02520,

title = {Enhanced Photocatalytic Hydrogen Evolution from Water Splitting on Ta2O5/SrZrO3 Heterostructures Decorated with CuxO/RuO2 Cocatalysts},

author = {Ali Margot Huerta-Flores and Francisco Ruiz-Zepeda and Cavit Eyovge and Jedrzej P. Winczewski and Matthias Vandichel and Miran Gaberšček and Nicolas D. Boscher and Han J. G. E. Gardeniers and Leticia M. Torres-Martínez and Arturo Susarrey-Arce},

url = {https://doi.org/10.1021/acsami.2c02520},

doi = {10.1021/acsami.2c02520},

year  = {2022},

date = {2022-07-12},

urldate = {2022-07-12},

journal = {ACS Applied Materials & Interfaces},

volume = {14},

issue = {28},

pages = {31767–31781},

note = {PMID: 35786845},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{https://doi.org/10.1002/smll.202202410,

title = {Elucidation of Structure–Activity Relations in Proton Electroreduction at Pd Surfaces: Theoretical and Experimental Study},

author = {Thorsten O. Schmidt and Apinya Ngoipala and Ryan L. Arevalo and Sebastian A. Watzele and Raju Lipin and Regina M. Kluge and Shujin Hou and Richard W. Haid and Anatoliy Senyshyn and Elena L. Gubanova and Aliaksandr S. Bandarenka and Matthias Vandichel},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/smll.202202410},

doi = {https://doi.org/10.1002/smll.202202410},

year  = {2022},

date = {2022-06-20},

urldate = {2022-06-20},

journal = {Small},

volume = {n/a},

number = {18},

pages = {2202410},

abstract = {Abstract The structure–activity relationship is a cornerstone topic in catalysis, which lays the foundation for the design and functionalization of catalytic materials. Of particular interest is the catalysis of the hydrogen evolution reaction (HER) by palladium (Pd), which is envisioned to play a major role in realizing a hydrogen-based economy. Interestingly, experimentalists observed excess heat generation in such systems, which became known as the debated “cold fusion” phenomenon. Despite the considerable attention on this report, more fundamental knowledge, such as the impact of the formation of bulk Pd hydrides on the nature of active sites and the HER activity, remains largely unexplored. In this work, classical electrochemical experiments performed on model Pd(hkl) surfaces, “noise” electrochemical scanning tunneling microscopy (n-EC-STM), and density functional theory are combined to elucidate the nature of active sites for the HER. Results reveal an activity trend following Pd(111) > Pd(110) > Pd(100) and that the formation of subsurface hydride layers causes morphological changes and strain, which affect the HER activity and the nature of active sites. These findings provide significant insights into the role of subsurface hydride formation on the structure–activity relations toward the design of efficient Pd-based nanocatalysts for the HER.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{RODRIGUEZOLGUIN2022101528,

title = {Chlorine in NiO promotes electroreduction of CO2 to formate},

author = {M. A. Rodriguez-Olguin and C. Flox and R. Ponce-Pérez and R. Lipin and F. Ruiz-Zepeda and J. P. Winczewski and T. Kallio and M. Vandichel and J. Guerrero-Sánchez and J. G. E. Gardeniers and N. Takeuchi and A. Susarrey-Arce},

url = {https://www.sciencedirect.com/science/article/pii/S2352940722001639},

doi = {https://doi.org/10.1016/j.apmt.2022.101528},

issn = {2352-9407},

year  = {2022},

date = {2022-05-23},

urldate = {2022-05-23},

journal = {Applied Materials Today},

volume = {28},

pages = {101528},

abstract = {We report the exceptional finding that NiO, a known electroactive catalyst for the reduction of CO2 to CO, can be tuned to become an active electrocatalyst for CO2 reduction to formate when chlorine is synthetically incorporated into NiO. The CO2 reduction reaction (CO2RR) is carried out on chlorine-containing NiO octahedral particles made by a solid-state synthesis method yielding a Faradaic efficiency (FE) of 70 % for formate production at -0.8 V vs. RHE with a partial current density of 14.7 mA/cm2. XPS confirms the presence of Ni3+ and Ni2+ species, indicating the existence of uncoordinated Ni. The Ni3+/Ni2+ ratio increases with the Cl concentrations on NiO. Cl concentrations are also confirmed with STEM-EDX. DFT modeling provides insights into the thermodynamic stability and CO2RR mechanism over the Cl-containing NiO surface. It is suggested that Cl can occupy the defective sites created by oxygen vacancies on the NiO model with Cl (O-alpha+Cl). The surface Pourbaix diagrams constructed from DFT indicate the preferred surface terminations favorable at the operating conditions for the CO2RR, which closely agrees with the experimental findings. The O-alpha+Cl has been found to promote CO2RR to formate. Our results create new possibilities in the development of earth-abundant electrocatalysts for selective CO2RR},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{ALI2022121541,

title = {Hydrogen Evolution in Alkaline Medium on Intratube and Surface Decorated PtRu Catalyst},

author = {Farhan S. M. Ali and Ryan Lacdao Arevalo and Matthias Vandichel and Florian Speck and Eeva-Leena Rautama and Hua Jiang and Olli Sorsa and Kimmo Mustonen and Serhiy Cherevko and Tanja Kallio},

url = {https://www.sciencedirect.com/science/article/pii/S0926337322004829},

doi = {https://doi.org/10.1016/j.apcatb.2022.121541},

issn = {0926-3373},

year  = {2022},

date = {2022-05-23},

urldate = {2022-05-23},

journal = {Applied Catalysis B: Environmental},

volume = {315},

pages = {121541},

abstract = {For anion exchange membrane (AEM) electrolysis, challenges include finding an optimal catalyst for hydrogen evolution reaction (HER), as the noble metals are scarce while non-noble metals are inferior. Here, the noble metal amount is reduced in a straightforward solution synthesis which produces Pt-Ru surface nanoparticles and unique intratube nanowires decorated on single walled carbon nanotubes (SWNT). In half-cell tests, 5 wtPtRu-% Pt-Ru SWNT demonstrates stable 10mAcm−2 HER current at 46mV overpotential and outperforms commercial electrocatalysts. When integrated in an AEM electrolyser, a high current density of 500mAcm−2 at a low voltage of 1.72V is achieved with 34µgcm−2 metal loading. First-principles calculations reveal that both the Pt-Ru alloy nanoparticle and intratube nanowires promote near optimal H* binding energy, thereby releasing the H2 faster. Thus, our approach yields an active low metal loading alkaline HER catalyst without sacrificing the performance in an AEM electrolyser.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Modeling Polyzwitterion-Based Drug Delivery Platforms: A Perspective of the Current State-of-the-Art and Beyond},

author = {Sousa Javan Nikkhah and Matthias Vandichel},

doi = {10.1021/acsengineeringau.2c00008},

year  = {2022},

date = {2022-05-03},

urldate = {2022-05-03},

journal = {ACS Engineering Au},

volume = {2},

pages = {274−294},

abstract = {Drug delivery platforms are anticipated to have biocompatible and bioinert surfaces. PEGylation of drug carriers is the most approved method since it improves water solubility and colloid stability and decreases the drug vehicles’ interactions with blood components. Although this approach extends their biocompatibility, biorecognition mechanisms prevent them from biodistribution and thus efficient drug transfer. Recent studies have shown (poly)zwitterions to be alternatives for PEG with superior biocompatibility. (Poly)zwitterions are super hydrophilic, mainly stimuli-responsive, easy to functionalize and they display an extremely low protein adsorption and long biodistribution time. These unique characteristics make them already promising candidates as drug delivery carriers. Furthermore, since they have highly dense charged groups with opposite signs, (poly)zwitterions are intensely hydrated under physiological conditions. This exceptional hydration potential makes them ideal for the design of therapeutic vehicles with antifouling capability, i.e., preventing undesired sorption of biologics from the human body in the drug delivery vehicle. Therefore, (poly)zwitterionic materials have been broadly applied in stimuli-responsive “intelligent” drug delivery systems as well as tumor-targeting carriers because of their excellent biocompatibility, low cytotoxicity, insignificant immunogenicity, high stability, and long circulation time. To tailor (poly)zwitterionic drug vehicles, an interpretation of the structural and stimuli-responsive behavior of this type of polymer is essential. To this end, a direct study of molecular-level interactions, orientations, configurations, and physicochemical properties of (poly)zwitterions is required, which can be achieved via molecular modeling, which has become an influential tool for discovering new materials and understanding diverse material phenomena. As the essential bridge between science and engineering, molecular simulations enable the fundamental understanding of the encapsulation and release behavior of intelligent drug-loaded (poly)zwitterion nanoparticles and can help us to systematically design their next generations. When combined with experiments, modeling can make quantitative predictions. This perspective article aims to illustrate key recent developments in (poly)zwitterion-based drug delivery systems. We summarize how to use predictive multiscale molecular modeling techniques to successfully boost the development of intelligent multifunctional (poly)zwitterions-based systems.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/acs.inorgchem.1c03665,

title = {Surprisingly Low Reactivity of Layered Manganese Oxide toward Water Oxidation in Fe/Ni-Free Electrolyte under Alkaline Conditions},

author = {Mahya Salmanion and Ivan Kondov and Matthias Vandichel and Pavlo Aleshkevych and Mohammad Mahdi Najafpour},

url = {https://doi.org/10.1021/acs.inorgchem.1c03665},

doi = {10.1021/acs.inorgchem.1c03665},

year  = {2022},

date = {2022-01-14},

urldate = {2022-01-14},

journal = {Inorganic Chemistry},

volume = {61},

number = {0},

issue = {4},

pages = {2292–2306},

abstract = {So far, many studies on the oxygen-evolution reaction (OER) by Mn oxides have been focused on activity; however, the identification of the best performing active site and corresponding catalytic cycles is also of critical importance. Herein, the real intrinsic activity of layered Mn oxide toward OER in Fe/Ni-free KOH is studied for the first time. At pH ≈ 14, the onset of OER for layered Mn oxide in the presence of Fe/Ni-free KOH happens at 1.72 V (vs reversible hydrogen electrode (RHE)). In the presence of Fe ions, a 190 mV decrease in the overpotential of OER was recorded for layered Mn oxide as well as a significant decrease (from 172.8 to 49 mV/decade) in the Tafel slope. Furthermore, we find that both Ni and Fe ions increase OER remarkably in the presence of layered Mn oxide, but that pure layered Mn oxide is not an efficient catalyst for OER without Ni and Fe under alkaline conditions. Thus, pure layered Mn oxide and electrolytes are critical factors in finding the real intrinsic activity of layered Mn oxide for OER. Our results call into question the high efficiency of layered Mn oxides toward OER under alkaline conditions and also elucidate the significant role of Ni and Fe impurities in the electrolyte in the presence of layered Mn oxide toward OER under alkaline conditions. Overall, a computational model supports the conclusions from the experimental structural and electrochemical characterizations. In particular, substitutional doping with Fe decreases the thermodynamic OER overpotential up to 310 mV. Besides, the thermodynamic OER onset potential calculated for the Fe-free structures is higher than 1.7 V (vs RHE) and, thus, not in the stability range of Mn oxides.},

note = {PMID: 35029976},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{https://doi.org/10.1002/anie.202116145,

title = {The First Sulfate-Pillared Hybrid Ultramicroporous Material, SOFOUR-1-Zn, and Its Acetylene Capture Properties},

author = {Debobroto Sensharma and Daniel J. O'Hearn and Amin Koochaki and Andrey A. Bezrukov and Naveen Kumar and Benjamin H. Wilson and Matthias Vandichel and Michael J. Zaworotko},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202116145},

doi = {https://doi.org/10.1002/anie.202116145},

year  = {2022},

date = {2022-01-02},

urldate = {2022-01-02},

journal = {Angewandte Chemie International Edition},

volume = {61},

pages = {e202116145},

abstract = {Abstract Hybrid ultramicroporous materials, HUMs, are comprised of metal cations linked by combinations of inorganic and organic ligands. Their modular nature makes them amenable to crystal engineering studies, which have thus far afforded four HUM platforms (as classified by the inorganic linkers). HUMs are of practical interest because of their benchmark gas separation performance for several industrial gas mixtures. We report herein design and gram-scale synthesis of the prototypal sulfate-linked HUM, the fsc topology coordination network ([Zn(tepb)(SO4)]n), SOFOUR-1-Zn},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{RODRIGUEZOLGUIN2021,

title = {Al2O3 Nanofibers Prepared from Aluminum Di(sec-butoxide)acetoacetic Ester Chelate Exhibits High Surface Area and Acidity},

author = {M. A. Rodriguez-Olguin and H. Atia and M. Bosco and A. Aguirre and R. Eckelt and E. D. Asuquo and M. Vandichel and J. G. E. Gardeniers and A. Susarrey-Arce},

url = {https://www.sciencedirect.com/science/article/pii/S0021951721004796},

doi = {https://doi.org/10.1016/j.jcat.2021.11.019},

issn = {0021-9517},

year  = {2022},

date = {2022-01-01},

urldate = {2021-11-22},

journal = {Journal of Catalysis},

volume = {405},

pages = {520-533},

abstract = {Alumina (Al2O3) is a widely used material for catalysis in the chemical industry. Besides a high specific surface area, acid sites on Al2O3 play a crucial role in the chemical transformation of adsorbed molecules, which ultimately react and desorb from the catalyst. This study introduces a synthetic method based on electrospinning to produce Al2O3 nanofibers (ANFs) with acidity and porosity tuned using different aluminum precursor formulations. After electrospinning and heat treatment, the nanofibers form a non-woven network with macropores (∼4 μm). Nanofibers produced from aluminum di(sec-butoxide)acetoacetic ester chelate (ASB) show the highest total acidity of ca. 0.70 µmol/m2 determined with temperature-programmed desorption of ammonia (NH3-TPD) and BET. The nature of the acid site in ASB ANFs is studied in detail with infrared (IR) spectroscopy. Pyridine is used as a molecular probe for the identification of acid sites in ASB. Pyridine showed the presence of Lewis acid sites prominently. Density-functional theory (DFT) is conducted to understand the desorption kinetics of the adsorbed chemical species, such as ammonia (NH3) on crystalline γ-Al2O3. For our analysis, we focused on a mobile approach for chemisorbed and physisorbed NH3. The computational results are compared with NH3-TPD experiments, ultimately utilized to estimate the desorption energy and kinetic desorption parameters. The experiments are found to pair up with our simulation results. We predict that these non-woven structures will find application as a dispersion medium of metallic particles in catalysis.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{KUMAR20213085,

title = {Breaking the trade-off between selectivity and adsorption capacity for gas separation},

author = {Naveen Kumar and Soumya Mukherjee and Nathan C. Harvey-Reid and Andrey A. Bezrukov and Kui Tan and Vinicius Martins and Matthias Vandichel and Tony Pham and Lisa M. Wyk and Kolade Oyekan and Amrit Kumar and Katherine A. Forrest and Komal M. Patil and Leonard J. Barbour and Brian Space and Yining Huang and Paul E. Kruger and Michael J. Zaworotko},

url = {https://www.sciencedirect.com/science/article/pii/S2451929421003636},

doi = {https://doi.org/10.1016/j.chempr.2021.07.007},

issn = {2451-9294},

year  = {2021},

date = {2021-11-11},

urldate = {2021-01-01},

journal = {Chem},

volume = {7},

number = {11},

pages = {3085-3098},

abstract = {Summary The trade-off between selectivity and adsorption capacity with porous materials is a major roadblock to reducing the energy footprint of gas separation technologies. To address this matter, we report herein a systematic crystal engineering study of C2H2 removal from CO2 in a family of hybrid ultramicroporous materials (HUMs). The HUMs are composed of the same organic linker ligand, 4-(3,5-dimethyl-1H-pyrazol-4-yl)pyridine, pypz, three inorganic pillar ligands, and two metal cations, thereby affording six isostructural pcu topology HUMs. All six HUMs exhibited strong binding sites for C2H2 and weaker affinity for CO2. The tuning of pore size and chemistry enabled by crystal engineering resulted in benchmark C2H2/CO2 separation performance. Fixed-bed dynamic column breakthrough experiments for an equimolar (v/v = 1:1) C2H2/CO2 binary gas mixture revealed that one sorbent, SIFSIX-21-Ni, was the first C2H2 selective sorbent that combines exceptional separation selectivity (27.7) with high adsorption capacity (4 mmol·g−1).},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{ABDI202137774,

title = {The importance of identifying the true catalyst when using Randles-Sevcik equation to calculate turnover frequency},

author = {Zahra Abdi and Matthias Vandichel and Alla S. Sologubenko and Marc-Georg Willinger and Jian-Ren Shen and Suleyman I. Allakhverdiev and Mohammad Mahdi Najafpour},

url = {https://www.sciencedirect.com/science/article/pii/S0360319921035199},

doi = {https://doi.org/10.1016/j.ijhydene.2021.09.039},

issn = {0360-3199},

year  = {2021},

date = {2021-09-29},

urldate = {2021-01-01},

journal = {International Journal of Hydrogen Energy},

volume = {46},

number = {76},

pages = {37774-37781},

abstract = {Water splitting will become important to store excess renewable electrical energy into hydrogen. Although the oxygen-evolution reaction (OER) by water oxidation is a critical reaction for water splitting, further investigations are needed to find the details of the OER mechanism for various electrocatalysts. More in particular for homogeneous electrocatalysts, the Randles-Sevcik equation has been extensively applied to determine the turnover frequency (TOF). Herein, using vitamin B12 as a case study, we show that the dynamical deposition/dissolution of the heterogeneous catalyst during OER makes the Randles-Sevcik equation too complicated to be used for calculating the TOF. Indeed, the conventionally applied post-characterization methods do not provide sufficient accuracy to prove the homogeneity of OER mechanisms; thus, using the Randles-Sevcik equation to calculate the TOF is not necessarily correct.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{D1FD90057A,

title = {Theory and modelling: general discussion},

author = {Dmytro Äntypov and Vonika Ka-Man Au and Isabel Cooley and François-Xavier Coudert and Deanna M. D’Alessandro and Qiaowei Li and Martin Schroder and Mikhail Suyetin and Matthias Vandichel and Sihai Yang and Michael Zaworotko and Elena" Besley},

url = {http://dx.doi.org/10.1039/D1FD90057A},

doi = {10.1039/D1FD90057A},

year  = {2021},

date = {2021-09-29},

urldate = {2021-01-01},

journal = {Faraday Discuss.},

volume = {231},

pages = {258-265},

publisher = {The Royal Society of Chemistry},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/acs.chemmater.1c01723,

title = {Efficient Capture of Trace Acetylene by an Ultramicroporous Metal–Organic Framework with Purine Binding Sites},

author = {Shivani Sharma and Soumya Mukherjee and Aamod V Desai and Matthias Vandichel and Gourab K Dam and Ashwini Jadhav and Gabriele Kociok-Köhn and Michael J Zaworotko and Sujit K Ghosh},

url = {https://doi.org/10.1021/acs.chemmater.1c01723},

doi = {10.1021/acs.chemmater.1c01723},

year  = {2021},

date = {2021-07-09},

urldate = {2021-07-09},

journal = {Chemistry of Materials},

volume = {33},

number = {14},

pages = {5800-5808},

abstract = {Efficient separation of acetylene (C2H2) from its byproducts, especially CO2, is difficult because of their similar physicochemical properties, including molecular dimensions and boiling point. Herein, we demonstrate trace C2H2 removal from C2H2/CO2 mixtures enabled by a new ultramicroporous metal–organic framework (MOF) adsorbent, IPM-101, which features an optimal pore size of 4 Å (close to the kinetic diameter of C2H2, 3.3 Å) and one-dimensional channels lined by Lewis basic purine groups. Single-component gas adsorption isotherms revealed a clear affinity toward C2H2 versus CO2 at low pressures with a substantial C2H2 uptake of 0.9 mmol g–1 at 3000 ppm and 298 K. Dynamic column breakthrough experiments revealed separation of C2H2 from 1:1 and 1:99 v/v C2H2/CO2 mixtures. IPM-101 exhibits one of the highest dynamic separation selectivity (αAC) values yet reported, 22.5 for 1:1 C2H2/CO2. Computational simulations indicated that the purine moiety was key to the strong C2H2 selectivity thanks to C2H2 selective N···HC≡CH interactions.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/acssuschemeng.1c03539,

title = {Understanding the Dynamics of Molecular Water Oxidation Catalysts with Liquid-Phase Transmission Electron Microscopy: The Case of Vitamin B12},

author = {Zahra Abdi and Esmael S Balaghi and Alla S Sologubenko and Marc-Georg Willinger and Matthias Vandichel and Jian-Ren Shen and Suleyman I Allakhverdiev and Greta R Patzke and Mohammad Mahdi Najafpour},

url = {https://doi.org/10.1021/acssuschemeng.1c03539},

doi = {10.1021/acssuschemeng.1c03539},

year  = {2021},

date = {2021-07-07},

journal = {ACS Sustainable Chemistry & Engineering},

volume = {9},

number = {28},

pages = {9494-9505},

abstract = {Cobalt compounds are intensely explored as efficient catalysts for the oxygen evolution reaction (OER). Since vitamin B12 is a soluble cobalt compound with high enzymatic activity, evaluating its OER activity is of relevance for biomimetic catalyst research. In this work, the temporal evolution of a homogenous vitamin B12 catalyst in the early stages of OER was investigated by an advanced combination of in situ electrochemical liquid transmission electron microscopy (EC-LTEM), in situ UV–vis spectroelectrochemistry, and extended X-ray absorption fine structure (EXAFS) methods. For the first time, we provided direct evidence of diffuse layer dynamics on the working electrode interface. The results suggested that the formation of cobalt oxyphosphate nanoparticles on the working electrode interface and in the presence of phosphate buffer is the initial stage of the catalytic pathway. Computational results confirmed that the ligand oxidation pathway could occur at potentials below the OER thermodynamic barrier (1.23 V vs reversible hydrogen electrode (RHE)), which leads to a Co ion leaching into the electrolyte. This study showed that investigation of the apparent molecular mechanisms of OER with metal complexes requires careful analyses. We illustrate the high precision and sensitivity of EC-LTEM under operational conditions to monitor heterogeneous catalysts generated during OER and to evaluate their actual roles in the catalytic process.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/acsami.1c06241,

title = {High Working Capacity Acetylene Storage at Ambient Temperature Enabled by a Switching Adsorbent Layered Material},

author = {Shi-Qiang Wang and Xiao-Qing Meng and Matthias Vandichel and Shaza Darwish and Ze Chang and Xian-He Bu and Michael J Zaworotko},

url = {https://doi.org/10.1021/acsami.1c06241},

doi = {10.1021/acsami.1c06241},

year  = {2021},

date = {2021-05-13},

journal = {ACS Applied Materials & Interfaces},

volume = {13},

number = {20},

pages = {23877-23883},

abstract = {Unlike most gases, acetylene storage is a challenge because of its inherent pressure sensitivity. Herein, a square lattice (sql) coordination network [Cu(4,4′-bipyridine)2(BF4)2]n (sql-1-Cu-BF4) is investigated with respect to its C2H2 sorption behavior from 189 to 298 K. The C2H2 sorption studies revealed that sql-1-Cu-BF4 exhibits multistep isotherms that are temperature-dependent and consistent with the transformation from “closed” (nonporous) to four “open” (porous) phases induced by the C2H2 uptake. The Clausius–Clapeyron equation was used to calculate the performance of sql-1-Cu-BF4 for C2H2 storage at pressures >1 bar, which revealed that its volumetric working capacity at 288 K is slightly superior to acetone (174 vs 170 cm3 cm–3) over a safer pressure range (1–3.5 vs 1–15 bar). Molecular simulations provided insights into the observed switching phenomena, revealing that the layer expansion of sql-1-Cu-BF4 occurs via intercalation and inclusion of C2H2. These results indicate that switching adsorbent layered materials offer promise for utility in the context of C2H2 storage and delivery.},

note = {PMID: 33983706},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{doi:10.1021/acs.inorgchem.0c03746b,

title = {Oxygen-Evolution Reaction by a Palladium Foil in the Presence of Iron},

author = {Nader Akbari and Ivan Kondov and Matthias Vandichel and Pavlo Aleshkevych and Mohammad Mahdi Najafpour},

url = {https://doi.org/10.1021/acs.inorgchem.0c03746},

doi = {10.1021/acs.inorgchem.0c03746},

year  = {2021},

date = {2021-04-07},

journal = {Inorganic Chemistry},

volume = {60},

number = {8},

pages = {5682–5693},

abstract = {Herein, we investigate the oxygen-evolution reaction (OER) and electrochemistry of a Pd foil in the presence of iron under alkaline conditions (pH ≈ 13). As a source of iron, K2FeO4 is employed, which is soluble under alkaline conditions in contrast to many other Fe salts. Immediately after reacting with the Pd foil, [FeO4]2– causes a significant increase in OER and changes in the electrochemistry of Pd. In the absence of this Fe source and under OER, Pd(IV) is stable, and hole accumulation occurs, while in the presence of Fe this accumulation of stored charges can be used for OER. A Density Functional Theory (DFT) based thermodynamic model suggests an oxygen bridge vacancy as an active site on the surface of PdO2 and an OER overpotential of 0.42 V. A substitution of Pd with Fe at this active site reduces the calculated OER overpotential to 0.35 V. The 70 mV decrease in overpotential is in good agreement with the experimentally measured decrease of 60 mV in the onset potential. In the presence of small amounts of Fe salt, our results point toward the Fe doping of PdO2 rather than extra framework FeOx (Fe(OH)3, FeO(OH), and KFeO2) species on top of PdO2 as the active OER sites.},

note = {PMID: 33826338},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{Zhou2021,

title = {Synthesis of Colloidal WSe2 Nanocrystals: Polymorphism Control by Precursor-Ligand Chemistry},

author = {Pengshang Zhou, Pieter Schiettecatte, Matthias Vandichel, Anastasia Rousaki, Peter Vandenabeele, Zeger Hens, and Shalini Singh},

doi = {https://doi.org/10.1021/acs.cgd.0c01036},

year  = {2021},

date = {2021-01-29},

journal = {Crystal Growth & Design},

volume = {21},

number = {3},

pages = {1451-1460},

abstract = {Syntheses of transition-metal dichalcogenides (TMDs) using colloidal-chemistry approaches are gaining significant interest in recent years, as these methods enable the morphology and properties of the nanocrystals to be tuned for targeted applications. In this work, by only varying the ligand used during synthesis, we synthesized nanoflowers with oleic acid (OA) and 1T′ phase dominated WSe2 nanosheets with oleylamine (OLA). WSe2 nanocrystals show slower rate of formation for the metastable 1T′ phase. Surface chemistry analyses of the synthesized nanocrystals by solution NMR establish that neither of the ligands bind strongly to the surface of nanocrystals but are in a dynamic coordination with the WSe2 surface. A further examination of the coordination of tungsten hexacarbonyl (W(CO)6) with the respective ligands confirms that W(CO)6 decomposes in OA, losing its octahedral symmetry, which leads to fast reactivity in the flask. In contrast to this, W(CO)6 reacts with OLA to form a new complex, which leads to slower reactivity and crystallization of the synthesized nanocrystals in the octahedral 1T′ phase. These insights into the influence of precursor-ligand chemistry on reaction outcome and the peculiar surface chemistry of colloidal TMD nanocrystals will be instrumental in developing future colloidal TMD nanocrystals.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{ISI:000553709000001,

title = {Oxygen Evolution and Reduction on Fe-doped NiOOH: Influence of Solvent,  Dopant Position and Reaction Mechanism},

author = {Matthias Vandichel and Kari Laasonen and Ivan Kondov},

url = {https://doi.org/10.1007/s11244-020-01334-8},

doi = {10.1007/s11244-020-01334-8},

issn = {1022-5528},

year  = {2020},

date = {2020-07-29},

journal = {TOPICS IN CATALYSIS},

abstract = {The oxygen evolution reaction (OER) is the limiting factor in an 

 electrolyzer and the oxygen reduction reaction (ORR) the limiting factor 

 in a fuel cell. In OER, water is converted to O(2)and H+/e(-)pairs, 

 while in ORR the reverse process happens to form water. Both reactions 

 and their efficiency are important enablers of a hydrogen economy where 

 hydrogen will act as a fuel or energy storage medium. OER and ORR can 

 both be described assuming a four-step electrochemical mechanism with coupled H+/e(-)transfers between four intermediates (M-*},

keywords = {},

pubstate = {published},

tppubtype = {article}

}