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Identifying the dynamic behaviors in complete reconstruction of Co-based complex precatalysts during electrocatalytic oxygen evolution

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Journal of Energy Chemistry 2025年第1期100卷 226-233页

作者： Jingfang Zhang Danyang Wu Linke Cai Youluan Lu Fanpeng Cheng Lijuan Shi Qun Yi Yao Liu Yi Huang Key Laboratory of Green chemical Engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education Hubei Key Laboratory of Novel Reactor and Green Chemical Technology School of Chemical Engineering & Pharmacy Wuhan Institute of Technology Key Laboratory of Pesticide & chemical biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education College of Chemistry Central China Normal University College of Materials Science and Engineering Fuzhou University

Transition metal-based nanomaterials have emerged as promising electrocatalysts for oxygen evolution reaction（OER）. Considerable research efforts have shown that self-reconstruction occurs on these nanomaterials under operating conditions of OER process. However, most of them undergo incomplete reconstruction with limited thickness of reconstruction layer, leading to low component utilization and arduous exploration of real catalytic mechanism. Herein, we identify the dynamic behaviors in complete reconstruction of Co-based complexes during OER. The hollow phytic acid（PA） cross-linked CoFe-based complex nanoboxes with porous nanowalls are designed because of their good electrolyte penetration and mass transport ability, in favor of the fast and complete reconstruction. A series of experiment characterizations demonstrate that the reconstruction process includes the fast substitution of PA by OH-to form Co（Fe）(OH)xand subsequent potential-driven oxidation to Co（Fe）OOH. The obtained CoFeOOH delivers a low overpotential of 290 mV at a current density of 10 mA cm-2and a long-term *** experiment results together with theory calculations reveal that the Fe incorporation can result in the electron rearrangement of reconstructed CoFeOOH and optimization of their electronic structure,accounting for the enhanced OER activity. The work provides new insights into complete reconstruction of metal-based complexes during OER and offers guidelines for rational design of high-performance electrocatalysts.

关键词： Complete reconstruction Co-based complex Precatalysts Oxygen evolution reaction

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Deciphering fungal metabolon coupling tandem inverse-electrondemand Diels-Alder reaction and semipinacol rearrangement for the biosynthesis of spiro polycyclic alkaloids

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Science China Chemistry 2025年第01期 288-296页

作者： Shuai Liu Wen-Qiang Xu Ying-Tong Di Man-Cheng Tang Ding-Kang Chen Ming-Ming Cao Yao-Wen Chang Hong-Yu Tang Chun-Mao Yuan Jun-Bo Yang Zhi-Li Zuo Han Guo Zi-Fei Xu Ying Zeng Yun-Dong Wu Xiao-Jiang Hao Key Laboratory of Phytochemistry and Natural Medicines (Chinese Academy of Sciences) Kunming Institute of Botany Chinese Academy of Sciences University of Chinese Academy of Sciences Lab of Computational Chemistry and Drug design State Key Laboratory of Chemical Oncogenomics Peking University Shenzhen Graduate School Shenzhen Bay Laboratory State Key Laboratory of Microbial Metabolism School of Life Sciences & Biotechnology Shanghai Jiao Tong University State Key Laboratory of Functions and Applications of Medicinal Plants Guizhou Medical University molecular biology Experimental Center Germplasm Bank of Wild Species in Southwest China Kunming Institute of Botany Chinese Academy of Sciences Yunnan Key Laboratory for Wild Plant Resources Kunming Institute of Botany Chinese Academy of Sciences Research Unit of chemical biology of Natural Anti-Virus Products Chinese Academy of Medical Sciences

In the intricate process of natural product biosynthesis, a metabolon can enhance metabolic flux by associating sequential enzymes. A fungal metabolon, comprising of flavin-dependent monooxygenase Spe F and P450 monooxygenase Spe G, is identified in the biosynthesis of spiro polycyclic alkaloids(+)-notoamide B and its diastereomer(+)-versicolamide B. Using notoamide E as a substance, Spe F/Spe G metabolon can control the stereoselectivity of its 2,3-epoxidation, followed by hydrogen atom ion at C-17 to generate reactive epoxide tau-m A with dienyl iminium unit. Subsequently,(+)-notoamide B and(+)-versicolamide B are produced via tandem nonenzymatic inverse-electron-demand Diels-Alder reaction and semipinacol rearrangement. This provides the first example of metabolon in the biosynthesis of spiro-prenylated indole alkaloids.

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Electrochemical conversion of methane to bridge the gap in the artificial carbon cycle

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Journal of Energy Chemistry 2025年第1期100卷 286-308页

作者： Yuhao Peng Yuefeng Song Ihar Razanau Juanxiu Xiao Wei Xiao Di Hu Guoxiong Wang College of Chemistry and molecular Sciences Hubei Key Laboratory of Electrochemical Power Sources Wuhan University State Key Laboratory of Catalysis Dalian National Laboratory for Clean Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics Chinese Academy of Sciences Laboratory of Physical-chemical Technologies SSPA Scientific and Practical Materials Research Centre of NAS of Belarus State Key Laboratory of Marine Resources Utilization in South China Sea Collaborative Innovation Center of Marine Science and Technology School of Marine Science and Engineering Hainan University Department of chemical and Environmental Engineering University of Nottingham Ningbo China

Methane, an abundant one-carbon（C1） resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO2emissions and coke deposition. Electrochemical conversion of methane（ECM） using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO2emission.

关键词： Methane Electrochemical conversion Reaction mechanism Catalyst design Electrode Electrocatalysis

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molecular modeling on Zn(II) binding modes of Alzheimer's amyloid β-peptide in insoluble aggregates and soluble complexes

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Science China Chemistry 2004年第2期47卷 126-133页

作者： HAN Daxiong YANG Pin Institute of molecular Science Chemical Biology and Molecular Engineering Laboratory of Ministry of Education Shanxi University Taiyuan 030006 China Institute of Molecular Science Chemical Biology and Molecular Engineering Laboratory of Ministry of Education Shanxi University Taiyuan 030006 China

Aggregation of the amyloid b-peptide (A b) into insoluble fibrils is a key pathologi-cal event in Alzheimers disease. Zn(II) ion induces significant Ab aggregation at nearly physio-logical concentrations in vitro. In order to explore the induce mechanism, the possible binding modes of Zn(II) in Ab peptide are studied by molecular modeling method. First, the Ab species containing 1,2,4 and 12 peptides are established respectively. And next a Zn(II) ion is manually hold the different sits of the Ab species based on the experimental data and subsequently the coordinate atom and number are assigned. Finally, the optimum binding site is found by the system energy minimization. Modeling results show that in soluble Zn(II) complex, Nt of imidazole ring of His14, O of carbonyl of main-chain, and two O of water occupy the four ligand positions of the tetrahedral complex; in the aggregation of Ab, the His13(Nt)-Zn(II)-His14(Nt) bridges are formed by Zn(II) cross-linking action. Therefore, the possible Zn(II) binding mode obtained by the studies will be helpful to reveal the form mechanism of pathogenic aggregates in brain.

关键词： molecular modeling amyloid b-peptide Zn(II) binding mode Alzheimers disease.

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Interaction of Ethylene-N,N'-dianthranilate to Ni(Ⅱ):Binding Properties and Coordination Mode Studies

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Chinese Journal of Structural Chemistry 2013年第12期32卷 1787-1792页

作者： FENG Jiao WANG Jing-Lin LIU Bin YANG Bin-Sheng Key Laboratory of chemical biology and molecular Engineering of Ministry of Education Institute of Molecular ScienceShanxi University

The binding properties of ethylene-N,N＇-dianthranilate （EDA） and Ni（II） were studied by difference UV-Vis in 0.05 M Tris-HCl buffer （pH 7.4）. The stoichiometric ratio of EDA to nickel （1：1） was confirmed and the conditional binding constant （IogKNi-EDA = 12.33 ± 0.06） was obtained. In addition, an interesting tetranuclear complex [Nin（EDA）4]·2CH3CH2OH-9H2O was obtained unexpectedly in alcohol-water solution and characterized by X-ray crystallography and electrospray ionization mass spectra （ESI-MS）. It is found that EDA acts as a pentadentate ligand and performs a chelating-bridging coordination mode.

关键词： ethylene-N,N'-dianthranilate Ni(Ⅱ) spectrum crystal structure

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Study of the interaction of unaggregated and aggregated amyloid β protein (10-21) with outward potassium channel

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Science China Chemistry 2007年第5期50卷 683-691页

作者： ZHANG ChaoFeng FAN Li YANG Pin Key Laboratory of chemical biology and molecular Engineering of Ministry of Education Institute of Molecular Science Shanxi University Taiyuan 030006 China Key Laboratory of Chemical Biology and Molecular Engineering of Ministry of Education Institute of Molecular Science Shanxi University Taiyuan 030006 China Key Laboratory of Chemical Biology and Molecular Engineering of Ministry of Education Institute of Molecular Science Shanxi University Taiyuan 030006 China

Metal ion-induced aggregation of A beta into insoluble plaques is a centralfactor in Alzheimer's ***^(2+) is the only physiologically available transition metal ionresponsible for aggregating A beta at pH *** make it clear that the neurotoxicity ofZn^(2+)-induced aggregation of A beta on neurons is the key to understand A beta mechanism of *** this paper,we choose A/?(10-21) as the model fragment to research hippocampal CA1pyramidal *** the first time,we adopt the combination of spectral analysis with patch-clamptechnique for the preliminary study of the mutual relations of Zn^(2+),A beta and ion channel fromthe cell *** following expounds upon the effects and mode of action of two forms (unaggregatedand aggregated) of A beta(10-21) on hippocampus outward potassium channel three processes(activation,inactivation and reactivation).It also shows the molecular mechanics of AD from thechannel *** results are significant for the further study of A beta nosogenesis and thedevelopment of new types of target drugs for the treatment of AD.

关键词： potassium channel amyloid beta protein (10-21) Zn^(2+) alzheimer's disease

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molecular modeling on the recognition of DNA sequence and conformational repair of sheared DNA by novel chiral metal complex D, L-[Co(phen)_(2)hpip]^(3+)

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Science China Chemistry 2006年第2期49卷 177-185页

作者： WU Yanbo ZHANG Cuiping YANG Pin Institute of molecular Science Key Laboratory of Chemical Biology of Molecular Engineering of Ministry of Education Shanxi University Taiyuan 030006 China Institute of Molecular Science Key Laboratory of Chemical Biology of Molecular Engineering of Ministry of Education Shanxi University Taiyuan 030006 China Institute of Molecular Science Key Laboratory of Chemical Biology of Molecular Engineering of Ministry of Education Shanxi University Taiyuan 030006 China

A study on the recognition of DNA sequence and conformational repair of sheared DNA by Novel Chiral Metal complex D,L-[Co(phen)2hpip]3+ (phen=1,10 phenanthroline, hpip=2-[2-hydroxyphenyl] imidazole [4,5-f][1,10] phenanthroline) is carried out with molecular simula-tions. The results reveal that two isomers of the complex could both recognize the normal DNA in the minor groove orientation, while recognize the sheared DNA in the major groove orientation and both isomers could convert the conformation of mismatched bases from sheared form to parallel form. Further analysis shows that the steric details of complex’s intercalation to base stack determine the results of recognition, which is induced by the steric collision among ancillary ligand phen, bases and DNA backbone, and by the steric crowding occurring in the process of structural expansion of bases and DNA backbone. Detailed analysis reveals that the conformational repair of mismatched bases relates not only to the steric interactions, but also to the π-π stack among normal bases, mismatched bases and hpip ligand.

关键词： mismatched DNA, metal complex, molecular modeling, docking.

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The selective recognition of mismatched d(GCGAGC)_2 by the cobalt(III) complex

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Science China Chemistry 2005年第1期48卷 58-66页

作者： CHEN Huili YANG Pin Key Laboratory of chemical biology and molecular Engineering of Ministry of Education Institute of Molecular Science Shanxi University Taiyuan 030006 China Key Laboratory of Chemical Biology and Molecular Engineering of Ministry of Education Institute of Molecular Science Shanxi University Taiyuan 030006 China

We studied the binding of [Co(phen)2(HPIP)]Cl3 to mismatched d(GCGAGC)2 con- taining two sheared G:A mispairs by NMR. The result shows that the complex was intercalated into G:A region from the minor groove and extended to the major groove, and could selectively recognize the mispairs. 31P NMR indicates that the complex binding induced the change of the phosphate backbone in the mismatched base pairs region.

关键词： cobalt complex, mismatched DNA, mispairing recognition.

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Theoretical Investigation on the Geometries and Properties of Guanine-BX_3 (X = F, Cl) Complex

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Chinese Journal of Structural Chemistry 2007年第7期26卷 783-792页

作者：张士国李红杨频 Department of Chemistry and chemical Engineering Institute of Material Chemistry Binzhou University Key Laboratory of chemical biology and molecular Engineering of Ministry of Education Institute of Molecular Science Shanxi University

Geometries and binding energies were predicted at the B3LYP/6-311＋G＊ level for the guanine-BX3 （X = F, Cl） systems and four isomers with no imaginary frequencies have been obtained for both guanine-BF3 and guanine-BCl3, respectively. Single energy calculations using much larger basis sets （6-311＋G（2df, p） and aug-cc-pVDZ were carded out as well. It was found that the most stable isomer of guanine-BF3 is BF3 connected to N3 of guanine with the stabilization energy of-19.93 kcal/mol （BSSE corrected）, while that of guanine-BC13 is BC13 connected to O10 of guanine having stabilization energy of -15.02 kcal/mol at the same level. The analyses for the combining interaction between BX3 and guanine with the atom-in-molecules theory （AIM） and natural bond orbital （NBO） methods have been performed. The results indicated that all the isomers are formed with σ-p type interactions between guanine and BX3, in which pyridine-type nitrogen or carbonyl oxygen or nitrogen atom of amino group offers its lone pair electrons to the empty p orbital of boron atom and the concomitance of charge transfer from guanine to BX3 has occurred. Still, one or two hydrogen bonds exist in some isomers of guanine-BX3 system and contribute to the stability of complex systems. Frequency analysis suggested that the stretching vibration of BX3 undergoes a red shift in complexes. Guanine-BF3 complex is more stable than guanine-BC13 although the B-Y （Y=N, O） bond distance in the latter is shorter.

关键词： density functional theory intermolecular interaction guanine-BF3 complex guanine-BCl3 complex

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Effects of La^(3+) on inward K^+ channels at plasma membr in guard cells

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Science China Chemistry 2005年第2期48卷 143-147页

作者： XUE Shaowu YANG Pin Institute of molecular Science Chemical Biology and Molecular Engineering Laboratory of Ministry of Education Shanxi University Taiyuan 030006 China Institute of Molecular Science Chemical Biology and Molecular Engineering Laboratory of Ministry of Education Shanxi University Taiyuan 030006 China

The effects of La3+ on inward K+ channels at plasma membrane in vicia guard cells are investigated using the whole-cell patch-clamp recording mode. It is shown that La3+ on both sides of plasma membrane blocks inward K+ currents in a concentration- dependent manner, indicating that La3+ binding sites may exist on both sides of plasma membrane in guard cells in vicia. The dose response is fitted by the Michaelis-Menten relation characterized by an inhibitor constant Ki of 2.56±0.25 μmol·L?1 (outside membrane) and (1.18±0.11)×10?15 mol·L?1 (inside membrane). Intracellular La3+ has much stronger inhibitory effect on inward K+ currents than ex- tracellular La3+ does, suggesting there may exist stronger binding sites inside membrane than outside membrane. Since ion channel activities of guard cells directly affect plant stomatal movement and water status, our results imply that rare earth elements might have potential practical values in regulating plant water status and strengthening plant drought endurance.

关键词： whole-cell patch-clamp, guard cell, stomatal movements, inward K+ channels, La3+.

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