Article
Chemistry, Inorganic & Nuclear
Debashis Basu, Danielle L. Gray, Toby J. Woods, Thomas B. Rauchfuss, Federica Arrigoni, Giuseppe Zampella
Summary: In the field of bioorganometallic chemistry, progress has been made in studying mimics of the active sites of [NiFe]-hydrogenases, with challenges arising in the conversion and misassignment when using Ni(N2S2) derivatives.
Article
Chemistry, Inorganic & Nuclear
Ahmad Hobballah, Federica Arrigoni, Catherine Elleouet, Claudio Greco, Maxime Laurans, Francois Y. Petillon, Philippe Schollhammer
Summary: The synthesis, structural characterization, and electrochemical properties of triiron clusters with different dithiolate bridges were studied, focusing on their protonation and redox behaviors. The impact of the dithiolate bridges on the complexes' electrochemical properties was investigated using cyclic voltammetry and DFT calculations.
INORGANIC CHEMISTRY FRONTIERS
(2021)
Article
Chemistry, Multidisciplinary
Spencer A. Kerns, Junhyeok Seo, Vincent M. Lynch, Jason Shearer, Sean T. Goralski, Eileen R. Sullivan, Michael J. Rose
Summary: The research focuses on the synthesis and reactivity of a model of [Fe]-hydrogenase derived from an anthracene-based scaffold. It demonstrates the maintenance of well-defined chemistry upon addition of exogenous base, and the formation of a dimeric motif containing a new Fe-C(methine) bond through deprotonation of the acyl(methylene) C-H bond with a phenolate base.This study provides mechanistic insight into the lack of functional biomimetic behavior in acyl(methylene)pyridine based mimics of [Fe]-hydrogenase, shedding light on the reasons behind this phenomenon.
Article
Chemistry, Multidisciplinary
Sebastian Schaupp, Francisco J. Arriaza-Gallardo, Hui-jie Pan, Joerg Kahnt, Georgia Angelidou, Nicole Paczia, Kyle Costa, Xile Hu, Seigo Shima
Summary: In this study, an in vitro biosynthesis assay of the FeGP cofactor was conducted using cell extract of a specific bacterium, revealing that pyridinol derivatives 1, 2, and 3 are precursors of the FeGP cofactor, with the carboxy group of 3 being converted to the acyl ligand.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Inorganic & Nuclear
Li-Cheng Song, Shuai Chen, Xiao-Feng Han, Zhen-Qing Zhang, Yin-Peng Wang, Yi-Xiong Dong
Summary: This study focuses on the synthesis, structural characterization and reactivity of a new series of [NiFe]-H(2)ase model complexes, and discusses their possible formation pathways.
Article
Chemistry, Inorganic & Nuclear
Irene R. A. M. Ogutu, Richard C. Holz, Brian Bennett
Summary: Research has shown that an eight amino acid peptide based on the metal binding motif of Co-type nitrile hydratase from Pseudonocardia thermophilia can coordinate Fe(II) under anaerobic conditions. Exposure to air results in the formation of a low-spin Fe(III)-peptide complex, similar to the nitrile hydratase from Rhodococcus equi TG328-2.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Qian-Yu Liu, Cheng Shang, Zhi-Pan Liu
Summary: In this study, machine learning simulation was used to explore FeCx structures under FTS conditions, leading to the identification of the active site for CO activation. This understanding of atomic-level processes can help in correlating structure and activity, ultimately aiding in the design of improved FT catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Biochemistry & Molecular Biology
Giorgio Caserta, Sven Hartmann, Casey Van Stappen, Chara Karafoulidi-Retsou, Christian Lorent, Stefan Yelin, Matthias Keck, Janna Schoknecht, Ilya Sergueev, Yoshitaka Yoda, Peter Hildebrandt, Christian Limberg, Serena DeBeer, Ingo Zebger, Stefan Frielingsdorf, Oliver Lenz
Summary: In this study, the maturation process of [NiFe]-hydrogenase was investigated using biochemical analysis and various spectroscopic techniques, providing detailed insights into its complex maturation mechanism.
NATURE CHEMICAL BIOLOGY
(2023)
Article
Chemistry, Inorganic & Nuclear
Alejandro Torres, Alba Collado, Mar Gomez-Gallego, Carmen Ramirez de Arellano, Miguel A. Sierra
Summary: In this study, tetranuclear [Fe2S2] hydrogenase mimic complexes containing Pt(II), Ni(II), and Ru(II) complexes were synthesized and their electrochemical properties were investigated. The incorporation of metal complexes in the structure modulated the electronic communication between the redox-active [Fe2S2] centers. Specifically, the structure of the phosphine ligand in the Pt compounds played a crucial role in facilitating or hindering the electronic communication, while the addition of a Ru-bis(bipyridine) complex promoted the communication. These experimental and computational findings provide insights into the electronic interaction between redox-active centers in hydrogenase.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Chandan Kr Barik, Rakesh Ganguly, Jian Ming Kwan, Zhiyong Lam, Si Yuan Wong, Weng Kee Leong
Summary: The ruthenacyclic carbamoyl complexes with derivatized 4-position of the pyridinyl ring have been synthesized, serving as structural mimics of the metal cofactor of [Fe]-hydrogenase. The derivative with R = H reacts with phosphine to form a disubstituted product.
Article
Chemistry, Multidisciplinary
Anna L. Poptic, Ying-Pin Chen, Tieyan Chang, Yu-Sheng Chen, Curtis E. Moore, Shiyu Zhang
Summary: Class Ic ribonucleotide reductases (RNRIc) and R2-like ligand-binding oxidases (R2lox) assemble heterobimetallic (MnFeII)-Fe-II cofactors through carefully constructed protein structures. This study demonstrates the selective formation of (MnFeII)-Fe-II complex in the absence of a protein scaffold. The successful assembly of (MnFeII)-Fe-II is attributed to Fe-deficient conditions, site differentiation, and the inability of the ligand to accommodate a dimanganese complex.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Anna L. Poptic, Ying-Pin Chen, Tieyan Chang, Yu-Sheng Chen, Curtis E. Moore, Shiyu Zhang
Summary: This study investigates the assembly of MnIIFeII cofactors in class Ic ribonucleotide reductases (RNRIc) and R2 like ligand-binding oxidases (R2lox). The authors report the selective formation of MnIIFeII complex even in the absence of a protein scaffold. X-ray diffraction reveals that MnIIFeII exhibits the same site selectivity as RNRIc and R2lox. The assembly mechanism of MnIIFeII is elucidated.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Inorganic & Nuclear
Shu-Fen Bai, Xiu-Mei Du, Wen-Jing Tian, Hang Xu, Ru-Fen Zhang, Chun-Lin Ma, Yan-Lan Wang, Shuang Lu, Qian-Li Li, Yu-Long Li
Summary: In this study, a series of tertiary phosphine substituted Fe/Se carbonyls were successfully prepared and their synthesis and properties were extensively studied. Some of the compounds showed catalytic activity for the H2 evolution reaction under electrochemical conditions.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
Monika Tokmina-Lukaszewska, Qi Huang, Luke Berry, Hayden Kallas, John W. Peters, Lance C. Seefeldt, Simone Raugei, Brian Bothner
Summary: This study investigates protein motion during the catalysis of nitrogenase using time-resolved mass spectrometry and normal mode analysis. The results reveal the conformational changes induced by protein docking and their impact on the activity of metal cofactor, providing insights into the signal transduction pathways involved in this reaction.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Chemistry, Physical
Xin-Pu Fu, Wen-Zhu Yu, Chao Ma, Jun Lin, Shi-Qi Sun, Shan-Qing Li, Pu-Ning Ren, Feng-Yan Jia, Meng-Yuan Li, Wei-Wei Wang, Xu Wang, Chun-Jiang Jia, Ke Wu, Rui Si, Chun-Hua Yan
Summary: The study successfully synthesized phase-pure Fe2N nanoparticles on Al2O3, achieving effective phase transformation to Fe2C and demonstrating high catalytic activity and selectivity.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Multidisciplinary
Xingyu Wu, Nanjun Chen, Harm-Anton Klok, Young Moo Lee, Xile Hu
Summary: The research team has successfully prepared high-molecular-weight branched poly(aryl piperidinium) AEMs, which exhibit high OH- conductivity and dimensional stability. The optimized membrane b-PTP-2.5 performs well at 80 degrees Celsius, with high mechanical strength and alkaline stability, as well as achieving good peak power densities in both H-2-O-2 and H-2-air.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Seunghwa Lee, Aliki Moysiadou, You-Chiuan Chu, Hao Ming Chen, Xile Hu
Summary: By conducting operando UV-Vis, X-ray absorption, and Raman spectroscopy, it has been revealed that the concentration of Fe4+ species at the surface, rather than Co4+ in the bulk, scales with the catalytic activity of CoFeOxHy during the oxygen evolution reaction (OER). These results suggest the presence of an Fe4+-containing active site in CoFeOxHy.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Review
Chemistry, Multidisciplinary
Suzhe Liang, Xiaoyan Wang, Ruoxuan Qi, Ya-Jun Cheng, Yonggao Xia, Peter Mueller-Buschbaum, Xile Hu
Summary: This review discusses the potential and challenges of using titanium dioxide of bronze phase (TiO2(B)) as an anode material in lithium/sodium-ion batteries. It provides insights into the evolution of research on TiO2(B) anodes and suggests future directions for their practical application.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Lei Zhang, Bjorn Pfund, Oliver S. Wenger, Xile Hu
Summary: This study reports an isoquinoline-derived diaryl ketone-type photocatalyst that has enhanced absorption of blue and visible light compared to conventional diaryl ketones. It enables dehydrogenative cross-coupling of heteroarenes with unactivated and activated alkanes as well as aldehydes using air as the oxidant.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Sebastian Schaupp, Francisco J. Arriaza-Gallardo, Hui-jie Pan, Joerg Kahnt, Georgia Angelidou, Nicole Paczia, Kyle Costa, Xile Hu, Seigo Shima
Summary: In this study, an in vitro biosynthesis assay of the FeGP cofactor was conducted using cell extract of a specific bacterium, revealing that pyridinol derivatives 1, 2, and 3 are precursors of the FeGP cofactor, with the carboxy group of 3 being converted to the acyl ligand.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Wenhao Ren, Xin Tan, Chen Jia, Anna Krammer, Qian Sun, Jiangtao Qu, Sean C. Smith, Andreas Schueler, Xile Hu, Chuan Zhao
Summary: The researchers prepared a nickel single-atom/nanoparticle catalyst through direct solid-state pyrolysis, which exhibited high CO current density in an alkaline flow cell. Coupled with a nickel-iron anode in a zero-gap membrane electrolyzer, the catalyst achieved industrially relevant CO current density and low cell voltage, demonstrating a high overall energy efficiency.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Wenhao Ren, Aoni Xu, Karen Chan, Xile Hu
Summary: A cation concentration gradient strategy is employed to enhance the activity and adjust the selectivity of CO2 electroreduction, breaking the linear scaling relationship of intermediate binding energies.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Xingyu Wu, Nanjun Chen, Chuan Hu, Harm-Anton Klok, Young Moo Lee, Xile Hu
Summary: A fluorination strategy is reported to create a phase-separated morphological structure in poly(aryl piperidinium) anion-exchange membranes (AEMs). The fluorinated AEMs possess high conductivity and dimensional stability, as well as excellent mechanical and chemical stability. AEMFCs using these fluorinated AEMs achieve outstanding peak power density and remain stable over extended operation.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Miyeon Chang, Wenhao Ren, Weiyan Ni, Seunghwa Lee, Xile Hu
Summary: In this study, the effects of three different ionomers (Nafion, Sustainion-type XA-9, and poly(terphenyl piperidinium) (PTP)) on the electrochemical reduction of CO2 using Cu-based electrocatalysts were investigated. It was found that Nafion had little influence on the performance, XA-9 promoted CO formation, and PTP favored hydrogen and formate production. The observed effects were attributed to charge transfer and hydrophilicity/hydrophobicity of the ionomers. This study highlights the structure-sensitive nature of the ionomer-catalyst interaction in CO2RR.
Article
Chemistry, Physical
Srikrishna Bera, Chao Fan, Xile Hu
Summary: In drug discovery, the presence of aliphatic and chiral carbons in organic molecules increases their chances of clinical success. However, current methods for synthesizing chiral carbon-rich molecules have limitations and are not suitable for stereoselective synthesis using racemic reagents. This study presents a nickel-catalyzed hydroalkylation reaction that selectively forms one of the four possible stereoisomers, offering a promising approach for the stereoselective synthesis of carbon-rich molecules.
Article
Chemistry, Multidisciplinary
Weijin Wang, Ryo Tachibana, Zhi Zou, Dongping Chen, Xiang Zhang, Kelvin Lau, Florence Pojer, Thomas R. Ward, Xile Hu
Summary: In this study, manganese transfer hydrogenases based on the biotin-streptavidin technology were designed and developed for organic synthesis. These artificial enzymes exhibit high catalytic activity and enantioselectivity, and can be utilized for a wide range of substrates and functional groups.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Lara Lavrencic, Uttam Dhawa, Arthur Blumenstein, Xile Hu
Summary: Significant research efforts have been focused on the development of catalytic methods for lignocellulose depolymerization in the field of lignin biorefining. However, the conversion of obtained monomers into higher value-added products remains a key challenge in lignin valorization. In this study, copper-catalyzed reactions were utilized for benzylic functionalization of lignin-derived phenolics via the formation of hexafluoroisopropoxy-masked para-quinone methides (p-QMs). By controlling the rates of copper catalyst turnover and p-QM release, various unsaturated fragments suitable for further synthetic applications were successfully installed onto lignin-derived monomers.
Article
Chemistry, Physical
Weiyan Ni, Josephine Lederballe Meibom, Noor Ul Hassan, Miyeon Chang, You-Chiuan Chu, Anna Krammer, Songlan Sun, Yiwei Zheng, Lichen Bai, Wenchao Ma, Seunghwa Lee, Seongmin Jin, Jeremy S. Luterbacher, Andreas Schuler, Hao Ming Chen, William E. Mustain, Xile Hu
Summary: Hydroxide exchange membrane fuel cells (HEMFCs) are promising devices for energy conversion. Now, a porous nitrogen-doped carbon-supported PtRu catalyst for the hydrogen oxidation reaction is presented, consisting of Pt single atoms and PtRu nanoparticles that work synergistically. The catalyst enables a fuel cell that exceeds the US Department of Energy 2022 performance target.
Article
Chemistry, Physical
Wenhao Ren, Wenchao Ma, Xile Hu
Summary: Electrochemical CO reduction can be used to efficiently convert CO2 to chemical fuels. However, current membrane electrode assembly (MEA) CO electrolyzers suffer from low energy efficiency. This study shows that the transport of water and hydroxide ions at the quasi-two-phase interface of the cathode limits the performance of MEA electrolyzers at high current densities. By improving interfacial mass transport, the researchers achieved a lower cell voltage, higher stability, and higher Faradaic yield.
Article
Chemistry, Inorganic & Nuclear
Albert Claude Jean-Pierre Daubry, Zhuijun Xu, Ming Yang, Ya-Jun Cheng, Yonggao Xia, Xile Hu
Summary: This paper introduces a new concept to enhance the rate capability of lithium-ion batteries by incorporating a small amount of metal species into the electron conductive agent. Experimental results show that the Si/C composite anode with oxidized Ketjen black (KJB) incorporated with cobalt (Co-ox-KJB) exhibits improved capabilities at high current densities. The improved electrochemical performance is attributed to enhanced electron conductivity, improved affinity towards the electrolyte, and an enhanced desolvation process.
INORGANIC CHEMISTRY FRONTIERS
(2022)
