Article
Chemistry, Inorganic & Nuclear
Shuang Lu, Cui-Rong Qin, Hui-Lin Ma, Ji-Min Ouyang, Qian-Li Li
Summary: Two electron-rich, PR3-disubstituted diiron bis(monothiolate) carbonyls were prepared as biomimetic models of the active site of [FeFe]-H(2)ases. Mu-hydride diiron compounds were also synthesized as structural and functional models for the protonated diiron subsite. Characterization and electrochemical property studies were conducted for all compounds, with one compound found to catalyze H-2 production in the presence of acetic acid.
INORGANICA CHIMICA ACTA
(2021)
Article
Chemistry, Physical
Juan Amaro-Gahete, Dolores Esquivel, Mariia Pavliuk, Cesar Jimenez-Sanchidrian, Haining Tian, Sascha Ott, Francisco J. Romero-Salguero
Summary: A biomimetic model complex for light-driven hydrogen production was synthesized and anchored on heterogeneous supports, showing promising catalytic activity. The molecular complex achieved a decent turnover number, while the heterogenized complexes had slightly lower activities.
Article
Chemistry, Multidisciplinary
Aurore Jacq-Bailly, Martino Benvenuti, Natalie Payne, Arlette Kpebe, Christina Felbek, Vincent Fourmond, Christophe Leger, Myriam Brugna, Carole Baffert
Summary: Hnd, a tetrameric enzyme from Desulfovibrio fructosovorans, is capable of flavin-based electron bifurcation. Despite its complexity, the enzyme can catalytically exchange electrons with an electrode and demonstrates unique high potential inactivation/reactivation kinetics. The catalytic properties of Hnd are comparable to standard hydrogenases, suggesting that the additional subunits necessary for electron bifurcation do not alter the enzyme's catalytic behavior at the active site.
FRONTIERS IN CHEMISTRY
(2021)
Review
Biochemistry & Molecular Biology
Jason W. Sidabras, Sven T. Stripp
Summary: This article reviews 25 years of scientific literature on [FeFe]-hydrogenase and provides a personal account on essential research papers and review articles regarding catalytic mechanism, O-2 sensitivity, and the in vivo synthesis of the active site cofactor. It also highlights future directions in structural biology and molecular biophysics and aims to inspire young investigators in the competitive field of [FeFe]-hydrogenase research.
JOURNAL OF BIOLOGICAL INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Hassan Abul-Futouh, Daniel Costabel, Konrad Hotzel, Phil Liebing, Helmar Goeris, Wolfgang Weigand, Kalina Peneva
Summary: This report presents the synthesis and characterization of a mimic of [FeFe]-hydrogenase, named [Fe-2(CO)(6){μ-bdtf}] (2, bdtf = 3,4-dimercaptobenzaldehyde), obtained from the reaction between 3,4-dimercaptobenzaldehyde and Fe-3(CO)(12). Different ligands, such as PPh3 and P(OMe)(3), were used to modify complex 2, resulting in mono- and disubstituted complexes [Fe-2(CO)(5)PPh3{μ-bdtf}] (3), [Fe-2(CO)(4)(PPh3)(2){μ-bdtf}] (4), and [Fe-2(CO)(4)(P(OMe)(3))(2){μ-bdtf}] (5). The structures of complexes 2-5 were determined by X-ray diffraction analysis. The electrochemistry and catalytic activity of these mimics towards proton reduction were evaluated by cyclic voltammetry, with all complexes showing potential for hydrogen formation in the presence of weak acid, such as acetic acid (AcOH).
INORGANICA CHIMICA ACTA
(2023)
Article
Chemistry, Physical
Shuang Lue, Shu-Fen Bai, Xin-Ping Gao, Yan-Lan Wang, Qian-Li Li
Summary: A convenient method for synthesizing aminediphosphine (PNP) substituted Fe/Se models with [Fe2(& mu;-Se2)(CO)4(& mu;-PNP)] as a new precursor was described. Various complexes were successfully prepared and characterized using spectral techniques and X-ray crystallography. The electrochemical and electrocatalytic properties of the synthesized complexes were compared.
JOURNAL OF MOLECULAR STRUCTURE
(2023)
Article
Chemistry, Inorganic & Nuclear
Shuang Lu, Sheng Gong, Cui-Rong Qin, Qian-Li Li
Summary: A series of monosubstituted and disubstituted diiron bis(monoselenolate) carbonyls were prepared to enrich the chemistry of diiron diselenolate compounds and synthesize new hydrogen evolution catalysts. The new compounds were characterized by various analytical techniques and their electrochemical properties were studied by cyclic voltammetry in MeCN.
Review
Chemistry, Inorganic & Nuclear
Juan Amaro-Gahete, Mariia Pavliuk, Haining Tian, Dolores Esquivel, Francisco J. Romero-Salguero, Sascha Ott
Summary: A global hydrogen economy can be achieved through environmentally sustainable, safe, and cost-efficient renewable energy, with solar hydrogen production through artificial photosynthesis as a key strategy. The [FeFe]-hydrogenase enzymes found in anaerobic bacteria and green algae are highly efficient biological catalysts for hydrogen evolution, inspiring the design of synthetic catalyst systems. Various synthetic models based on the [FeFe]-hydrogenase enzyme active site have been explored for the reduction of protons to molecular hydrogen, utilizing a combination of different photocatalysis systems and components like [2Fe2S] clusters, photosensitizers, and molecular triads. The review highlights the importance of rational design in creating biomimetic catalysts for efficient hydrogen production, and the design features shared by stable and efficient photosystems.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Chemistry, Multidisciplinary
Roman Rohac, Lydie Martin, Liang Liu, Debashis Basu, Lizhi Tao, R. David Britt, Thomas B. Rauchfuss, Yvain Nicolet
Summary: FeFe-hydrogenases use a unique H cluster to convert H-2 into protons and low-potential electrons. The [2Fe](H) center is where the reaction occurs and is built stepwise by maturating enzymes, with HydE performing complex modifications of complex-B to produce a precursor to the [2Fe](H) center.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Inorganic & Nuclear
Federica Arrigoni, Fabio Rizza, Luca Bertini, Luca De Gioia, Giuseppe Zampella
Summary: The feasibility of designing a stable inverted (or rotated) disposition of the two FeL3 pyramidal moieties in the dimetallic core of [FeFe]-hydrogenase cofactor was assessed through a DFT multi-functional study using the electron rich Fe-2(pdt)(RNC)(6) 1 as a starting point. The study found that combining coordination asymmetry, electron donor presence, and isocyanides R substituents capable of establishing intramolecular interactions effectively stabilizes the rotated isomer.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Georgia R. F. Orton, Shishir Ghosh, Lucy Alker, Jagodish C. Sarker, David Pugh, Michael G. Richmond, Frantisek Hartl, Graeme Hogarth
Summary: In this study, FeFe biomimics containing redox-active ferrocenyl diphosphine were prepared and their ability to reduce protons and oxidize H-2 was investigated. The complexes exhibited different chemical behavior in oxidation reactions in different solvents, providing valuable insights for studying their catalytic performances.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Physical
Shu-Fen Bai, Jun-Wei Ma, Ya-Nan Guo, Xiu-Mei Du, Yan-Lan Wang, Qian-Li Li, Shuang Lu
Summary: Researchers successfully prepared four types of aminophosphine substituted Fe/E (E = S, Se) carbonyls related to [FeFe]-hydrogenases. These compounds have interesting structures and can be used for electrocatalytic hydrogen production.
JOURNAL OF MOLECULAR STRUCTURE
(2023)
Article
Chemistry, Applied
Xu-Feng Liu, Yu-Long Li, Xing-Hai Liu
Summary: A series of diiron dithiolato analogues with a pyrazole moiety were synthesized as models for [FeFe]-hydrogenases active site, and their electrocatalytic properties for proton reduction to H2 and fungicidal activities were investigated.
APPLIED ORGANOMETALLIC CHEMISTRY
(2022)
Review
Chemistry, Multidisciplinary
Adrien Pagnier, Batuhan Balci, Eric M. Shepard, William E. Broderick, Joan B. Broderick
Summary: The assembly and installation of the [FeFe]-hydrogenase H-cluster is not fully understood, but in vitro approaches using semisynthetic and enzyme-based methods have provided new insights into the maturation process. These approaches have shed light on the roles of individual maturation enzymes, the nature of H-cluster assembly intermediates, the molecular precursors of H-cluster ligands, and the sequence of steps involved in [FeFe]-hydrogenase maturation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Princess R. Cabotaje, Kaija Walter, Afridi Zamader, Ping Huang, Felix Ho, Henrik Land, Moritz Senger, Gustav Berggren
Summary: [FeFe] hydrogenases, a type of metalloenzymes, have remarkable catalytic properties and (bio-)technological potential. This study focuses on the Group D hydrogenases, which exhibit relatively low catalytic activity and may have an alternative proton transfer pathway. By analyzing the amino acid residues in Group D hydrogenases, the study provides initial evidence for the existence of this alternative pathway.
Article
Business, Finance
Jiancheng Shen, John Griffith, Mohammad Najand, Licheng Sun
Summary: We examine the predictability of market emotions (fear, gloom, joy, optimism) on returns of S&P 500 Index and 10-year Treasury notes futures using VAR and TGARCH models. Our VAR models suggest that one of the four emotions (fear) has predictive power for stock index futures returns. Additionally, we find that joy and optimism measures of emotions influence Treasury futures market returns. Further analysis using a TGARCH model with an emotional sentiment measure (fear) reveals that fear significantly affects market returns and conditional volatility of futures markets.
JOURNAL OF BEHAVIORAL FINANCE
(2023)
Article
Chemistry, Multidisciplinary
Chen Wang, Panlong Zhai, Mingyue Xia, Wei Liu, Junfeng Gao, Licheng Sun, Jungang Hou
Summary: This study reports the reversible reconstruction behavior accompanied by copper dynamic evolution, leading to the formation of high-valent cobalt species in active sites during water-alkali electrolysis. The crucial roles of electronic structure evolution and oxygen-vacancy-site mechanism in catalyst activity are revealed through experimental and theoretical investigations.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Zhaozhong Fan, Ruichun Luo, Yanxue Zhang, Bo Zhang, Panlong Zhai, Yanting Zhang, Chen Wang, Junfeng Gao, Wu Zhou, Licheng Sun, Jungang Hou
Summary: Researchers have developed an indium-nickel dual-atom catalyst that exhibits high CO selectivity and achieves a high industrial CO partial current density. The synergistic effect of the dual-sites and oxygen bridge in the catalyst reduces the reaction barrier for *COOH formation and suppresses the undesired hydrogen evolution reaction.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Teng Shao, Yuan Chang, Zhuwei Li, Yurou Song, Dingfeng Jin, Junfeng Gao, Licheng Sun, Jungang Hou
Summary: Artificial photosynthesis is a promising solution for the efficient production of hydrogen peroxide. A chemically bonded and plasmonic Z-scheme junction of WO and CNs was developed for high-performance artificial photosynthesis. This Z-scheme catalyst exhibits a high H2O2 generation rate, even under broad-spectrum response irradiation.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Nanoscience & Nanotechnology
Sebastian Svanstrom, Alberto Garcia Fernandez, Tamara Sloboda, T. Jesper Jacobsson, Fuguo Zhang, Fredrik O. L. Johansson, Danilo Kuhn, Denis Ceolin, Jean -Pascal Rueff, Licheng Sun, Kerttu Aitola, Hakan Rensmo, Ute B. Cappel
Summary: In this study, the band alignment and interfacial electric field variations of a fully functional lead halide perovskite solar cell structure under operating conditions were measured directly using hard X-ray photoelectron spectroscopy (HAXPES). The results showed that 70% of the photovoltage was generated at the back contact, with equal contributions from the hole transport material/gold interface and the perovskite/hole transport material interface.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Tianqi Liu, Shaoqi Zhan, Nannan Shen, Linqin Wang, Zoltan Szabo, Hao Yang, Marten S. G. Ahlquist, Licheng Sun
Summary: Inspired by biological systems, a Ru-based molecular water oxidation catalyst was designed to mimic enzymatic framework, utilizing a configurationally labile ligand that acts as both an electron donor and a proton acceptor. Through various analysis and calculations, it was demonstrated that the self-adaptive ligand enables fast catalytic kinetics with a turnover frequency comparable to natural photosynthesis.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Yu Guo, Johannes Messinger, Lars Kloo, Licheng Sun
Summary: O2 formation in photosystem II (PSII) is still not well understood, but the prevailing theoretical model involves a Mn(IV)-oxyl unit in an open-cubane Mn4CaO6 cluster. However, it has been proposed that the S3 state of higher plants lacks an extra ligand, and instead features a penta-coordinate dangler Mn(V)=oxo covalently linked to a closed-cubane Mn3CaO4 cluster. In this study, the researchers explored various possible pathways and found that the nucleophilic oxo-oxo coupling (NOOC) between Mn(V)=oxo and mu 3-oxo is the only feasible mechanism. They described an energetically feasible process starting from the S4 state, involving the formation of peroxide and superoxide, followed by O2 release and a second water insertion.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Jian Du, Dexin Chen, Yunxuan Ding, Linqin Wang, Fei Li, Licheng Sun
Summary: Exploring highly active and durable electrocatalysts for oxygen evolution reaction (OER) is significant to achieve efficient anion exchange membrane (AEM) water electrolysis. In this study, hollow Co-based N-doped porous carbon spheres decorated with ultrafine Ru nanoclusters (HS-RuCo/NC) were developed as efficient OER electrocatalysts. The unique hollow structure with hierarchically porous characteristics contributed to fast mass transport and increased metal site exposure, while the in situ formed RuO2 and Co3O4 exhibited a synergistic effect on enhancing OER performance. The integration of HS-RuCo/NC into an AEM water electrolyzer resulted in improved cell voltage and long-term stability compared to commercial RuO2-based AEM water electrolyzer.
Article
Chemistry, Physical
Xiansheng Li, Mahdi Haghshenas, Linqin Wang, Jing Huang, Esmaeil Sheibani, Shichen Yuan, Xin Luo, Xuehan Chen, Changting Wei, Hengyang Xiang, Glib Baryshnikov, Licheng Sun, Haibo Zeng, Bo Xu
Summary: In this study, we designed a multifunctional small-molecule hole-transporting material (HTM) called X10 for use in perovskite quantum dot light-emitting diodes (Pe-QLEDs). X10 exhibited high hole mobility, good film-forming ability, strong solvent resistance, and defect passivation effect. Pe-QLEDs using X10 as the HTM achieved a promising external quantum efficiency (EQE) of 20.18%, which was 7-fold higher than that of reference HTM-TCTA-based ones (EQE approximately 2.88%). This is the first case where a small-molecule HTM has shown a high EQE over 20% in Pe-QLEDs. Our work provides important guidance for the rational design of multifunctional small-molecule HTMs for high-performance Pe-QLEDs.
ACS ENERGY LETTERS
(2023)
Article
Business, Finance
Zhaobo Zhu, Licheng Sun, Min Chen
Summary: When stocks are trading near their 52-week high, investors have low expectations for future returns. However, for firms with strong fundamentals, investors' expectations are too low, indicating the psychological anchor of the 52-week high. A trading strategy based on fundamental strength and the 52-week high outperforms the unconditional strategy by significantly increasing the average return. Interestingly, this effect is most evident when investor sentiment is high, but not observed among sophisticated institutions and short sellers.
REVIEW OF QUANTITATIVE FINANCE AND ACCOUNTING
(2023)
Article
Chemistry, Multidisciplinary
Zhuofeng Li, Linqin Wang, Tao Wang, Licheng Sun, Wenxing Yang
Summary: Developing alternative electrolysis techniques is crucial for advancing electrocatalysis. Recent studies have shown that pulse electrochemical CO2 reduction reaction (CO2RR) can improve the selectivity of CO2RR. This study reveals that pulse electrolysis improves the C(2+) selectivity of CO2RR through dynamic controls of the surface CuxO/Cu composition.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Materials Science, Multidisciplinary
Zi-Yang Xia, Wei Zhang, Cheng Chen, Hao-Xin Wang, Lin-Qin Wang, Ya-Wei Miao, Xing-Dong Ding, Li-Cheng Sun, Ming Cheng
Summary: In order to overcome the energy loss caused by the valence band offset between Cs2AgBiBr6 and the hole transport layer (HTL), a novel deep-level hole transport material (HTM) was designed and synthesized to optimize the energy level alignment. While the introduction of deep-level HTMs successfully reduced the valence band offset between Cs2AgBiBr6 and HTL, it also increased the valence band offset at the HTL/Au interface, limiting the improvement of the power conversion efficiency (PCE). To further improve the PCE, a gradient energy level arrangement combining the newly developed deep-level HTM with Spiro-OMeTAD was constructed. Through optimization, an impressive PCE of 3.50% with high open-circuit voltage and fill factor was achieved, making it one of the best Cs2AgBiBr6 perovskite solar cells.
Article
Multidisciplinary Sciences
Yilong Zhao, Yunxuan Ding, Wenlong Li, Chang Liu, Yingzheng Li, Ziqi Zhao, Yu Shan, Fei Li, Licheng Sun, Fusheng Li
Summary: Electrocatalytic urea synthesis is a promising alternative to traditional energy-intensive urea synthesis. By stabilizing intermediates of *NO2 and *CO, a CuWO4 catalyst achieves efficient co-reduction of CO2 and NO3- to urea via C-N coupling.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Yue Zhao, Lei Ran, Rui Chen, Yurou Song, Junfeng Gao, Licheng Sun, Jungang Hou
Summary: This study presents an integrated photoanode by grafting covalent triazine frameworks as conjugated molecules on the surface of ferroelectric BaTiO3-x nanorod array, and constructing oxyhydroxide oxygen evolution cocatalyst (OEC). The integrated OEC/CTF/BTO array achieves high photocurrent density and low onset potential, while also exhibiting outstanding stability. The enhanced PEC activity is attributed to the integration of CTF and OEC, which enhances light-harvesting capability, boosts charge carrier mediation, and promotes water oxidation kinetics.
Article
Green & Sustainable Science & Technology
Guoheng Ding, Husileng Lee, Zhiheng Li, Jian Du, Linqin Wang, Dexin Chen, Licheng Sun
Summary: Ni2Fe8/Ni3S2/NF catalyst is fabricated on nickel foam by a simple one-pot hydrothermal reaction, exhibiting high current densities at low overpotential and outperforming noble metal-based catalysts. Coupled with Ni4Mo/MoO2/NF, the AEM-WE device shows high performance and durability, making the catalyst highly efficient and robust.
ADVANCED ENERGY AND SUSTAINABILITY RESEARCH
(2023)
Article
Biochemistry & Molecular Biology
Michael Ramek, Jasmina Sabolovic
Summary: This paper investigates the geometries, energy landscapes, and magnetic parameters of copper(II) amino acid compounds using density functional theory calculations. The results show that certain conformers with histaminate-like and glycine-like modes have low Gibbs free energies and high metal-binding affinities. The predicted conformations reproduce the experimental electron paramagnetic resonance parameters.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2024)
Article
Biochemistry & Molecular Biology
Wei Tian, Wen Zhong, Zengyan Yang, Ling Chen, Shijie Lin, Yanping Li, Yuxing Wang, Peilin Yang, Xing Long
Summary: A series of novel dibutyltin complexes based on salen-like ligands were synthesized and characterized. Complex S03 showed excellent in vitro anticancer activity and induced cancer cell death through multiple mechanisms. This study reveals new mechanisms of organotin complexes and provides new insights into the development of organotin metal complexes as anticancer drugs.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2024)
Article
Biochemistry & Molecular Biology
Natalie C. Korkola, Martin J. Stillman
Summary: Many proteins require a metal cofactor for their function, and these metals play a role in protein folding. The study found that the metallation rates of different metal binding pathways are influenced by pH, with the less cooperative pathway being more affected by low pH conditions. Specific mixtures of structures are formed in the initial steps of metallation, and unfolding the disordered apo-MT structure hinders the formation of these preliminary structures. The compact conformation of the native apo-MT allows for rapid formation of metal-thiolate structures with high affinity, providing protection from oxidation.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2024)
Article
Biochemistry & Molecular Biology
Boxuan Yang, Xitong Song, Binju Wang
Summary: The diiron active site plays a crucial role in catalytic transformations in both biological and chemical systems. Recent advancements in the field include the synthesis of biomimetic diiron catalysts inspired by the active structure of soluble methane monooxygenase (sMMO), which have been successfully applied to the dehydrogenation of indolines.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2024)
Article
Biochemistry & Molecular Biology
Christina N. Banti, Angeliki A. Piperoudi, Catherine P. Raptopoulou, Vassilis Psycharis, Constantinos M. Athanassopoulos, Sotiris K. Hadjikakou
Summary: Two copper(I) polymorphs with mitochondria-targeting properties were successfully prepared via metal ion conjugation. These compounds showed promising activities in DNA binding, enzyme inhibition, and cancer cell inhibition. The molecular mechanisms of action were investigated.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2024)