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Recent progress on photoactive nonprecious transition-metal complexes

Science China chemistry 2025年第1期 46-95页

作者： Zhong-Liang Gong Hong-Jie Zhang Yan Cheng Jianxun Liu Yuhan Ai Yaqin Li Zhihui Feng Qiong Zhang Shaolong Gong Yong Chen Chang-Jiang Yao Yuan-Yuan Zhu Liang-Jin Xu Yu-Wu Zhong CAS Key laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences State Key laboratory of Structural Cemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences School of chemistry and Chemical Engineering Anhui Key Laboratory of Advanced Catalytic Materials and Reaction EngineeringHefei University of Technology State Key laboratory of Explosion Science and Safety Protection School of Mechatronical Engineering Beijing Institute of Technology College of chemistry and Molecular Sciences Hubei Key Lab on Organic and Polymeric Optoelectronic Materials Wuhan University School of chemistry and Chemical Engineering Anhui University Key laboratory of Photochemical Conversion and Optoelectronic Materials & CAS-HKU Joint laboratory on New Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences

Photoactive complexes of nonprecious transition metals, mainly including those in the first-row and partially the second-row of the Periodic table of elements, have received increasing attention in view of their low cost and long-term sustainability. They are recognized as promising alternatives to noble transition metal complex congeners that have been extensively studied in optoelectronic devices, artificial photosynthesis, photocatalysis, biodiagnostics, and therapeutics, etc. This review is devoted to a comprehensive summary on the classical and recent advances on photoactive nonprecious transition metal complexes, including photoactive Zr, V, Cr, Mo, and W complexes, Mn complexes and hybrids, Fe, Co, Ni, and Cu complexes, and Zn and Cd complexes and hybrids. A particular focus is given on the molecular design, modulation of photophysical and photochemical properties, and applications of the representative and lately-developed nonprecious metal complexes. In addition, a perspective on the future development in this field is provided at the end of this review.

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Cyano migration-mediated radical-polar crossover cyclopropanation

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Science China chemistry 2025年第01期 241-248页

作者： Ziqiang Wang Yasu Chen Jie Li Chen Zhu Key laboratory of organic Synthesis of Jiangsu Province College of Chemistry Chemical Engineering and Materials ScienceSoochow University Frontiers Science Center for Transformative Molecules Zhangjiang Institute for Advanced Study and Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Shanghai Jiao Tong University

We report a novel cyano migration-mediated radical-polar crossover process, whereby both the sulfonylcyanation of aliphatic alkenes and the formation of cyclopropanes are concurrently achieved. This transformation yields a diverse array of multisubstituted cyclopropanes under mild photocatalytic conditions. Mechanistic studies elucidate that the reaction proceeds via intramolecular nucleophilic substitution, leading to the formation of the cyclopropane derivatives.

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Porous organic Cage‑Based Quasi‑Solid‑State Electrolyte with Cavity‑Induced Anion‑Trapping Effect for Long‑Life Lithium Metal Batteries

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Nano-Micro Letters 2025年第2期17卷 376-386页

作者： Wei-Min Qin Zhongliang Li Wen‑Xia Su Jia‑Min Hu Hanqin Zou Zhixuan Wu Zhiqin Ruan Yue‑Peng Cai Kang Li Qifeng Zheng School of chemistry South China Normal UniversityGuangzhou 510006People’s Republic of China Key laboratory of Functional Metal‑organic Compounds of Hunan Province College of Chemistry and Material ScienceHengyang Normal UniversityHengyang 421008People’s Republic of China Guangzhou Key laboratory of Energy Conversion and Energy Storage Materials Guangzhou 510006People’s Republic of China

Porous organic cages(POCs)with permanent porosity and excellent host–guest property hold great potentials in regulating ion transport behavior,yet their feasibility as solid-state electrolytes has never been testified in a practical ***,we design and fabricate a quasi-solid-state electrolyte(QSSE)based on a POC to enable the stable operation of Li-metal batteries(LMBs).Benefiting from the ordered channels and cavity-induced anion-trapping effect of POC,the resulting POC-based QSSE exhibits a high Li+transference number of 0.67 and a high ionic conductivity of 1.25×10^(−4) S cm^(−1) with a low activation energy of 0.17 *** allow for homogeneous Li deposition and highly reversible Li plating/stripping for over 2000 *** a proof of concept,the LMB assembled with POC-based QSSE demonstrates extremely stable cycling performance with 85%capacity retention after 1000 ***,our work demonstrates the practical applicability of POC as SSEs for LMBs and could be extended to other energy-storage systems,such as Na and K batteries.

关键词： Porous organic cage Cavity-induced anion-trapping Quasi-solid-state electrolyte Homogeneous Li+flux Lithium metal battery

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Cobalamin-dependent radical S-adenosyl-L-methionine protein functions with a partner to successively methylate tricyclic indole alkaloid for chuangxinmycin maturation and derivatization

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Science China chemistry 2025年第1期 308-316页

作者： Sili Wang Jiancheng Huang Yanan Du Wei Huang Yufeng Xue Xiaokun Xu Guannan Zhong Yuanyuan Shi Bin Hong Xiaoying Bian Wen Liu State Key laboratory of Chemical Biology Shanghai Institute of Organic Chemistry University of Chinese Academy of SciencesChinese Academy of Sciences State Key laboratory of Microbial Technology Shandong University National Health Commission (NHC) Key laboratory of Biotechnology for Microbial Drugs Institute of Medicinal BiotechnologyChinese Academy of Medical Science & Peking Union Medical College

Cobalamin(Cbl)-dependent radical S-adenosyl-L-methionine(SAM) proteins constitute the largest collection of the radical SAM superfamily that has hundreds of thousands of individual members. Many of these proteins are involved in the biosynthesis of pharmaceutically important natural products to catalyze chemically demanding reactions. In the biosynthetic pathway of chuangxinmycin(CXM), a unique indole alkaloid antibiotic with potent anti-infective activity, functionalization of the characteristic thiopyrano[4,3,2-cd]indole scaffold by regio-and stereoselective C3-methylation is believed to rely on a Cbl-dependent radical process, which, however, remained to be reconstituted biochemically. We here report the dissection of this enzymatic process, which requires the incorporation of Cxm8, a Cbl-dependent radical SAM protein, with Cxm9, a DUF5825family protein that shares no homology to any proteins of known functions. Cxm8 and Cxm9 function together by forming an unexpected heterodimeric complex that selectively catalyzes C3-methylation of the tricyclic indole-S-hetero ring system in a successive manner, achieving CXM and a recently identified, C3-dimethylated congener. Detailed biochemical characterization,isotope labeling, structural simulation and bioinformatics analysis rationalized the catalysis of the Cxm8/Cxm9 complex and particularly the necessity of the DUF5825 protein for C3-methylase activity. This is the first example that a Cbl-dependent protein acts with a partner to exhibit radical SAM activity.

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A low redox potential and long life organic anode material for sodium-ion batteries

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Journal of Energy chemistry 2025年第1期100卷 557-564页

作者： Zhi Li Yang Wei Kang Zhou Xin Huang Xing Zhou Jie Xu Taoyi Kong Junwei Lucas Bao Xiaoli Dong Yonggang Wang Department of chemistry and Shanghai Key laboratory of Molecular Catalysis and Innovative Materials Institute of New Energy Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) Fudan University Department of chemistry Boston College School of Materials Science and Engineering Anhui University of Technology

Sodium-ion batteries （SIBs） with organic electrodes are an emerging research direction due to the sustainability of organic materials based on elements like C,H,O,and sodium ***,organic electrode materials for SIBs are mainly used as cathodes because of their relatively high redox potentials（>1 V）.organic electrodes with low redox potential that can be used as anode are ***,a novel organic anode material （tetrasodium 1,4,5,8-naphthalenetetracarboxylate,Na4TDC） has been developed with low redox potential （<0.7 V） and excellent cyclic *** three-sodium storage mechanism was demonstrated with various in-situ/ex-situ spectroscopy and theoretical calculations,showing a high capacity of 208 mAh/g and an average decay rate of merely 0.022%per ***,the Na4TDC-hard carbon composite can further acquire improved capacity and cycling stability for 1200 cycles even with a high mass loading of up to 20 mg *** pairing with a thick Na3V2（PO4）3cathode (20.6 mg cm-2),the as-fabricated full cell exhibited high operating voltage （2.8 V）,excellent rate performance and cycling stability with a high capacity retention of 88.7% after 200 cycles,well highlighting the Na4TDC anode material for SIBs.

关键词： organic anode material Low redox potential Composite anode Sodium-ion batteries

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Metal nanoparticles decorated CoFe-(oxy)hydroxysulfides nanosheets fabricated by a general strategy for electrocatalytic water splitting

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Journal of Energy chemistry 2025年第1期100卷 26-38页

作者： Xiaodong Yang Haochen Shen Xiaoming Xiao Zhichao Li Qi Zhou Wei Yang Bin Jiang Yongli Sun Luhong Zhang Zhenhua Yan School of Chemical Engineering and Technology Tianjin University Key laboratory of Advanced Energy Materials chemistry (Ministry of Education) Nankai University

This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides （M/SLDH） through spontaneous redox and sulfurization *** developed Ag/SLDH and Pt/SLDH catalysts with abundant heterogeneous interfaces and hierarchical nanostructures demonstrated outstanding oxygen evolution reaction （OER） and hydrogen evolution reaction （HER） performance,achieving low overpotentials of 212 and 35 mV at 10 mA cm-2in 1 M KOH,*** both anode and cathode in water splitting,they required only 1.47 V to reach 10 mA cm-2and exhibited high structural robustness,maintaining stability at 1000 mA cm-2for 300 ***-situ Raman analysis revealed that the synergistic effects of metal nanoparticles and S doping significantly promote the transformation into the S-Co1-xFexOOH layer,which serves as the active phase for water ***,ultraviolet photoelectron spectroscopy （UPS） and density functional theory （DFT） analyses indicated that incorporating metal nanoparticles and S doping increase electron density near the Fermi level and reduce reaction energy barriers,thus enhancing intrinsic OER and HER *** study provides a scalable strategy for synthesizing high-performance electrocatalysts for water splitting,with promising potential for broader applications.

关键词： LDH Spontaneous reaction Metal nanoparticles Water splitting

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A Formal Synthesis of Betamethasone

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Chinese Journal of chemistry 2015年第6期33卷 637-642页

作者： Shasha Wang Yong Shi Weisheng Tian CAS Key laboratory of Synthetic chemistry of natural substances Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

A formal synthesis of betamethasone from 5α-pregnane-3β,16β,20S-triol is *** transformations are a bromination-acetylation of triol,an SN2 reaction of the resulting C16α-bromide with dimethylcopperlithium to get t... 详细信息

关键词： betamethasone pregnanetriol formal synthesis C16β-alkyl group double epoxidation

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Synthesis of C1-C9 Domain of the Nominal Didemnaketal A

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Chinese Journal of chemistry 2015年第6期33卷 663-668页

作者： Shunji Zhang Yong Shi Weisheng Tian CAS Key laboratory of Synthetic chemistry of natural substances Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Based on chiral pool strategy,a synthesis of the C1-C9 domain of the proposed structure of didemnaketal A,a natural product with potent HIV-1 protease inhibitory activity,has been *** transformations are a Shar-pless ... 详细信息

关键词： didemnaketal chiral pool chelation-controlled allylation natural products Sharpless AD

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Stereoselective Total Synthesis of Tubulysin V

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Chinese Journal of chemistry 2013年第1期31卷 40-48页

作者： Rui Wang Ping Tian Guoqiang Lin CAS Key laboratory of Synthetic chemistry of natural substances Shanghai Institute of Organic Chemistry Chinese Academy of Sciences Shanghai 200032 China

The total synthesis of tubulysin V was accomplished in 1.0% overall yield with linear 13 steps. Our synthetic strategy featured the following two reactions. One is zinc-mediated aza-Barbier reaction of （R）-N-tert-butane- sulfinyl imine 8 with β-ester group functionalized allylic bromide 9 to afford the chiral homo-allylic amine （7）; the other is to employ the methodology of aqueous indium-mediated aza-Barbier reaction previously developed by our group, giving the chiral homo-allylic amine 13 with high efficiency.

关键词： tubulysin V N-tert-butanesulfinyl imines zinc indium aza-Barbier reaction

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Unraveling post-growth mechanisms of monolayer CsPbBr3 nanocubes:Laser-enhanced transformations and cathodoluminescence-electron microscopy correlations

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Journal of Energy chemistry 2025年第1期100卷 146-156页

作者： Mingxing Li Xiaoge Wang Xiaofan Cao Zhiqun He Chunjun Liang Mingxing Chen Jing Ju Fangtian You Key laboratory of Luminescence and Optical Information Ministry of Education Institute of Optoelectronic Technology Beijing Jiaotong University Beijing National laboratory for Molecular Sciences (BNLMS) College of Chemistry and Molecular Engineering Peking University

Lead-halide perovskite nanoparticles（LHP NPs） are highly promising materials for next-generation displays and solid-state lighting due to their exceptional optical properties. However, their inherent instability presents a significant challenge. Recent advances have demonstrated that optoelectronic devices based on monolayer nanoparticle films exhibit both high luminescence efficiency and long-term *** research demonstrates that mobility limitations and anisotropic alignments in CsPbBr3nanocube monolayer films are key to their stabilization, hindering spontaneous growth through face-to-face fusion and resulting in the formation of connecting necks in a diagonal direction. Introducing laser irradiation confirmed this by significantly accelerating nanocubes growth, increasing mobility, and enhancing local structural ordering, leading to larger and more regularly shaped nanosheets. Fourier transform infrared spectroscopy and energy dispersive spectroscopy line-scan analyses indicated that laser irradiation did not disrupt the ligand structure. Transmission electron microscopy and correlative cathodoluminescence electron microscopy revealed the effects of post-growth and heterogeneous structures, including enhanced luminescence and inhomogeneous intensity in the nanosheets. These findings deepen the understanding of the post-growth mechanism of monolayer nanoparticles and the structure-emission correlation and highlight the unique role of laser irradiation in directing the formation of well-defined and regular nanostructures.

关键词： Post-growth mechanism Heterogeneous structure Single-particle spectroscopy Laser irradiation

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