@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}

}

@article{ISI:000557552100001,

title = {Water Oxidation at Neutral pH using a Highly Active Copper-Based  Electrocatalyst},

author = {Hussein A Younus and Yan Zhang and Matthias Vandichel and Nazir Ahmad and Kari Laasonen and Francis Verpoort and Ce Zhang and Shiguo Zhang},

doi = {10.1002/cssc.202001444},

issn = {1864-5631},

year  = {2020},

date = {2020-07-15},

journal = {CHEMSUSCHEM},

abstract = {The sluggish kinetics of the oxygen evolution reaction (OER) at the 

 anode severely limit hydrogen production at the cathode in water 

 splitting systems. Although electrocatalytic systems based on cheap and 

 earth-abundant copper catalysts have shown promise for water oxidation 

 under basic conditions, only very few examples with high overpotential 

 can be operated under acidic or neutral conditions, even though hydrogen 

 evolution in the latter case is much easier. This work presents an 

 efficient and robust Cu-based molecular catalyst, which self-assembles 

 as a periodic film from its precursors under aqueous conditions on the 

 surface of a glassy carbon electrode. This film catalyzes the OER under 

 neutral conditions with impressively low overpotential. In controlled 

 potential electrolysis, a stable catalytic current of 1.0 mA cm(-2)can 

 be achieved at only 2.0 V (vs. RHE) and no significant decrease in the 

 catalytic current is observed even after prolonged bulk electrolysis. 

 The catalyst displays first-order kinetics and a single site mechanism 

 for water oxidation with a TOF (k(cat)) of 0.6 s(-1). DFT calculations 

 on of the periodic Cu(TCA)(2)(HTCA=1-mesityl-1H-1,2,3-triazole-4-carboxylic acid) film 

 reveal that TCA defects within the film create Cu(I)active sites that 

 provide a low overpotential route for OER, which involves Cu-I, Cu-II-OH},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{ISI:000547455300015,

title = {Understanding Solid-Gas Reaction Mechanisms by Operando Soft X-Ray 

 Absorption Spectroscopy at Ambient Pressure},

author = {Luca Braglia and Martina Fracchia and Paolo Ghigna and Alessandro Minguzzi and Daniela Meroni and Raju Edla and Matthias Vandichel and Elisabet Ahlberg and Giuseppina Cerrato and Piero Torelli},

doi = {10.1021/acs.jpcc.0c02546},

issn = {1932-7447},

year  = {2020},

date = {2020-07-01},

journal = {JOURNAL OF PHYSICAL CHEMISTRY C},

volume = {124},

number = {26},

pages = {14202-14212},

abstract = {Ambient-pressure operando soft X-ray absorption spectroscopy (soft-XAS) 

 was applied to study the reactivity of hydroxylated SnO(2 )nanoparticles 

 toward reducing gases. H-2 was first used as a test case, showing that 

 the gas phase and surface states can be simultaneously probed: Soft-XAS 

 at the O K-edge gains sensitivity toward the gas phase, while at the Sn 

 M-4,M-5-edges, tin surface states are explicitly probed. Results 

 obtained by flowing hydrocarbons (CH4 and CH3CHCH2) unequivocally show 

 that these gases react with surface hydroxyl groups to produce water 

 without producing carbon oxides and release electrons that localize on 

 Sn to eventually form SnO. The partially reduced SnO2-x layer at the 

 surface of SnO2 is readily reoxidized to SnO2 by treating the sample 

 with O-2 at mild temperatures (>200 degrees C), revealing the nature of 

 ``electron sponge'' of tin oxide. The experiments, combined with DFT 

 calculations, allowed devising of a mechanism for dissociative 

 hydrocarbon adsorption on SnO2, involving direct reduction of Sn sites 

 at the surface via cleavage of C-H bonds and the formation of methoxy- 

 and/or methyl-tin species at the surface.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{ISI:000526300600012,

title = {Reversible Switching between Nonporous and Porous Phases of a New SIFSIX 

 Coordination Network Induced by a Flexible Linker Ligand},

author = {Bai-Qiao Song and Qing-Yuan Yang and Shi-Qiang Wang and Matthias Vandichel and Amrit Kumar and Clare Crowley and Naveen Kumar and Cheng-Hua Deng and Victoria GasconPerez and Matteo Lusi and Hui Wu and Wei Zhou and Michael J Zaworotko},

doi = {10.1021/jacs.0c01314},

issn = {0002-7863},

year  = {2020},

date = {2020-04-01},

journal = {JOURNAL OF THE AMERICAN CHEMICAL SOCIETY},

volume = {142},

number = {15},

pages = {6896-6901},

abstract = {Closed-to-open structural transformations in flexible coordination 

 networks are of potential utility in gas storage and separation. Herein, 

 we report the first example of a flexible SiF62--pillared square grid material, [Cu(SiF6)(L)(2)](n) (L = 1,4-bis(1-imidazolyl)benzene), 

 SIFSIX-23-Cu. SIFSIX-23-Cu exhibits reversible switching between 

 nonporous (beta 1) and several porous (alpha, gamma 1, gamma 2, and 

 gamma 3) phases triggered by exposure to N-2, CO2, or H2O. In addition, 

 heating beta 1 to 433 K resulted in irreversible transformation to a 

 closed polymorph, beta 2. Single-crystal X-ray diffraction studies 

 revealed that the phase transformations are enabled by rotation and 

 geometrical contortion of L. Density functional theory calculations 

 indicated that L exhibits a low barrier to rotation (as low as 8 

 kJmol(-1)) and a rather flat energy surface. In situ neutron powder 

 diffraction studies provided further insight into these sorbate-induced 

 phase changes. SIFSIX-23-Cu combines stability in water for over a year, 

 high CO2 uptake (ca. 216 cm(3)/g at 195 K), and good thermal stability.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{ISI:000505822700001,

title = {Oxygen Evolution on Metal-oxy-hydroxides: Beneficial Role of Mixing Fe,  Co, Ni Explained via Bifunctional Edge/acceptor Route},

author = {Matthias Vandichel and Michael Busch and Kari Laasonen},

doi = {10.1002/cctc.201901951},

issn = {1867-3880},

year  = {2020},

date = {2020-03-01},

journal = {CHEMCATCHEM},

volume = {12},

number = {5},

pages = {1436-1442},

abstract = {Oxygen evolution reaction (OER) via mixed metal oxy hydroxides 

 [M(O)(OH)] may take place on a large variety of possible active sites 

 on the actual catalyst. A single site computational description assumes 

 a 4-step electrochemical mechanism with coupled H+/e(-) transfers between 4 intermediates (M-*, M-OH},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{YOUNUS2020100437,

title = {Engineering of a highly stable metal-organic Co-film for efficient electrocatalytic water oxidation in acidic media},

author = {H A Younus and M Vandichel and N Ahmad and E Ahlberg and M Busch and F Verpoort},

url = {http://www.sciencedirect.com/science/article/pii/S2468606920300563},

doi = {10.1016/j.mtener.2020.100437},

issn = {2468-6069},

year  = {2020},

date = {2020-01-01},

journal = {Materials Today Energy},

volume = {17},

pages = {100437},

abstract = {Water oxidation is traditionally performed over IrO2 and RuO2 owing to their high stability at low pH compared to molecular O2 evolution catalysts. The low stability of molecular complexes in acids limits their industrial exploitation as anodes in water-splitting devices, where high current densities and proton conductivity are required. Herein, an existing Co(1,10-phenanthroline)2 complex film is engineered to improve its pH-stability via extra OH substituents on the ligand, i.e. 1,10-phenanthroline-4,7-diol. This novel Co(1,10-phenanthroline-4,7-diol)2 complex film is active for water oxidation at low overpotentials and stable at low pH. Since the calculated water oxidation overpotentials of both complexes are similar, the difference in water oxidation activity is attributed to a smaller charge transfer resistance, which originates from a different anchoring style to the electrode via the OH groups of the ligand. This result is supported by electrochemical impedance measurements. The high pH-stability of the Co(1,10-phenanthroline-4,7-diol)2 film is computationally rationalized by a high crystal formation energy observed in DFT calculations. In summary, an acid-stable and active cobalt-based metal-organic film is reported that competes well with most reported earth-abundant catalysts for water oxidation under similar conditions.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{https://doi.org/10.1002/cctc.202001284,

title = {Microwave-heated γ-Alumina Applied to the Reduction of Aldehydes to Alcohols},

author = {Bhausaheb Dhokale and Arturo Susarrey-Arce and Anna Pekkari and August Runemark and Kasper Moth-Poulsen and Christoph Langhammer and Hanna Härelind and Michael Busch and Matthias Vandichel and Henrik Sundén},

url = {https://chemistry-europe.onlinelibrary.wiley.com/doi/abs/10.1002/cctc.202001284},

doi = {https://doi.org/10.1002/cctc.202001284},

year  = {2020},

date = {2020-01-01},

journal = {ChemCatChem},

volume = {12},

number = {24},

pages = {6344-6355},

abstract = {Abstract The development of cheap and robust heterogeneous catalysts for the Meerwein-Ponndorf-Verley (MPV) reduction is desirable due to the difficulties in product isolation and catalyst recovery associated with the traditional use of homogeneous catalysts for MPV. Herein, we show that microwave heated γ-Al2O3 can be used for the reduction of aldehydes to alcohols. The reaction is efficient and has a broad substrates scope (19 entries). The products can be isolated by simple filtration, and the catalyst can be regenerated. With the use of microwave heating, we can direct the heating to the catalyst rather than to the whole reaction medium. Furthermore, DFT was used to study the reaction mechanism, and we can conclude that a dual-site mechanism is operative where the aldehyde and 2-propoxide are situated on two adjacent Al sites during the reduction. Additionally, volcano plots were used to rationalize the reactivity of Al2O3 in comparison to other metal oxides.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{https://doi.org/10.1002/smm2.1008,

title = {A square lattice topology coordination network that exhibits highly selective C2H2/CO2 separation performance},

author = {Naveen Kumar and Soumya Mukherjee and Andrey A Bezrukov and Matthias Vandichel and Mohana Shivanna and Debobroto Sensharma and Alankriti Bajpai and Victoria Gascón and Ken-ichi Otake and Susumu Kitagawa and Michael J Zaworotko},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/smm2.1008},

doi = {https://doi.org/10.1002/smm2.1008},

year  = {2020},

date = {2020-01-01},

journal = {SmartMat},

volume = {1},

number = {1},

pages = {e1008},

abstract = {Abstract C2H2/CO2 separation is an industrially important process that remains challenging because of the similar physicochemical properties of C2H2 and CO2. We herein report that the new square lattice (sql) coordination network [Cu(bipy-xylene)2(NO3)2]n, sql-16-Cu-NO3, 16 = bipy-xylene = 4,4′-(2,5-dimethyl-1,4-phenylene)dipyridine, exists in at least three forms, as-synthesised (α), activated (α′) and hydrated (β). The activated phase, sql-16-Cu-NO3-α′, is an ultramicroporous material that exhibits high selectivity towards C2H2 over CO2 as revealed by dynamic gas breakthrough experiments (1:1, C2H2/CO2) that afforded 99.87% pure CO2 in the effluent stream. The separation selectivity at 298 K and 1 bar, 78, is the third best value yet reported for C2H2 selective physisorbents whereas the mid-loading performance sets a new benchmark. The performance of sql-16-Cu-NO3-α′ is attributed to a new type of C2H2 binding site in which CH···ONO2 interactions enable moderately strong sorbent-sorbate binding (Qst (C2H2) = 38.6 kJ/mol) at low loading. Conversely, weak CO2 binding (Qst (CO2) = 25.6 kJ/mol) at low loading means that (ΔQst)AC [Qst (C2H2)–Qst (CO2)] is 13 kJ/mol at low coverage and 11.4 kJ/mol at mid-loading. Analysis of in situ powder X-ray diffraction and modelling experiments provide insight into the sorption properties and high C2H2/CO2 separation performance of sql-16-Cu-NO3-α′.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{ISI:000498288300001,

title = {Viewpoint: Atomic-Scale Design Protocols toward Energy, Electronic, 

 Catalysis, and Sensing Applications},

author = {Florian Belviso and Victor E P Claerbout and Aleix Comas-Vives and Naresh S Dalal and Feng-Ren Fan and Alessio Filippetti and Vincenzo Fiorentini and Lucas Foppa and Cesare Franchini and Benjamin Geisler and Luca M Ghiringhelli and Axel Gross and Shunbo Hu and Jorge Iniguez and Steven Kaai Kauwe and Janice L Musfeldt and Paolo Nicolini and Rossitza Pentcheva and Tomas Polcar and Wei Ren and Fabio Ricci and Francesco Ricci and Huseyin Sener Sen and Jonathan Michael Skelton and Taylor D Sparks and Alessandro Stroppa and Andrea Urru and Matthias Vandichel and Paolo Vavassori and Hua Wu and Ke Yang and Hong Jian Zhao and Danilo Puggioni and Remedios Cortese and Antonio Cammarata},

doi = {10.1021/acs.inorgchem.9b01785},

issn = {0020-1669},

year  = {2019},

date = {2019-11-01},

journal = {INORGANIC CHEMISTRY},

volume = {58},

number = {22},

pages = {14939-14980},

abstract = {Nanostructured materials are essential building blocks for the 

 fabrication of new devices for energy harvesting/storage, sensing, 

 catalysis, magnetic, and optoelectronic applications. However, because 

 of the increase of technological needs, it is essential to identify new 

 functional materials and improve the properties of existing ones. The 

 objective of this Viewpoint is to examine the state of the art of 

 atomic-scale simulative and experimental protocols aimed to the design 

 of novel functional nanostructured materials, and to present new 

 perspectives in the relative fields. This is the result of the debates 

 of Symposium I ``Atomic-scale design protocols towards energy, 

 electronic, catalysis, and sensing applications'', which took place 

 within the 2018 European Materials Research Society fall meeting.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{ISI:000474796600046,

title = {Initial Fe3O4(100) Formation on Fe(100)},

author = {Markus Soldemo and Matthias Vandichel and Henrik Gronbeck and Jonas Weissenrieder},

doi = {10.1021/acs.jpcc.9b04625},

issn = {1932-7447},

year  = {2019},

date = {2019-07-01},

journal = {JOURNAL OF PHYSICAL CHEMISTRY C},

volume = {123},

number = {26},

pages = {16317-16325},

abstract = {The initial oxidation of Fe(100) at 400 degrees C has been studied by 

 X-ray photoelectron spectroscopy (XPS), scanning tunneling microscopy 

 (STM), and low-energy electron diffraction, in combination with density 

 functional theory calculations. The first observed well-ordered surface 

 oxide is formed at a coverage of similar to 3 oxygen atoms per 

 unreconstructed surface Fe(100) atom. STM shows that this surface oxide 

 is terminated by straight atomic rows exhibiting a p(2 X 1) periodicity. 

 However, already for oxide films with a coverage of similar to 4 oxygen 

 atoms (corresponding to one Fe3O4 unit cell thickness), wiggly atomic 

 rows appear similar to the c(2 X 2) reconstructed Fe3O4 (100)-surface 

 with the Fe3O4 unit vectors rotated 45 degrees to Fe(100). The wiggly 

 rows are a consequence of subsurface cation iron vacancies, which 

 previously have been observed for bulk surfaces. The formation of 

 subsurface vacancies is supported by the XPS O is signature, which is 

 modeled by considering the core-level shifts for all oxygen atoms in the 

 film. Throughout the oxidation series, the microscopy results reveal a 

 layer-by-layer (Frank-van der Merwe) growth.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{ISI:000459731200013,

title = {A dimer path for CO dissociation on PtSn},

author = {Matthias Vandichel and Henrik Gronbeck},

doi = {10.1039/c8cy01989d},

issn = {2044-4753},

year  = {2019},

date = {2019-02-01},

journal = {CATALYSIS SCIENCE & TECHNOLOGY},

volume = {9},

number = {3},

pages = {695-701},

abstract = {Density functional theory calculations are used to investigate CO 

 adsorption, dissociation and SnOX formation on Pt3Sn. We find that 

 direct CO dissociation is prevented by high activation energies. An 

 energetically feasible path is instead CO dimer formation followed by 

 C-O bond cleavage. Dimers are formed in the presence of Sn adatoms which 

 effectively stabilize anionic OCCO- species. The presence of Sn adatoms 

 is crucial as dimers are unstable on Pt-only systems. The proposed 

 mechanism may explain recent experimental observations of SnOX and C-C 

 formation as PtxSn is exposed to CO.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}