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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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Rational modulation of fluorophosphate cathode by anionic groups to reduce the polarization behavior for fast-charging sodium-ion batteries

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Journal of Energy chemistry 2025年第1期100卷 509-521页

作者： Xinyuan Wang Fan Zhang Xingyu Zhou Qian Wang Changyu Liu Yangyang Liu Hui Wang Xiaojie Liu key laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education College of Chemistry & Materials Science Northwest University

Na3V2（PO4）2O2F （VP） is recognized as a promising cathode material for sodium-ion batteries due to its stable structural framework and high specific *** functional theory （DFT） and finite element simulations show that incorporating SO42-into VP decreases its band gap,lowers the migration energy barrier,and ensures a uniform Na+concentration gradient and stress distribution during charge and discharge ***,the average Na+diffusion coefficient of Na3V2（PO4）1.95（SO4）0.05O2F（VPS-1） is roughly double that of VP,leading to enhanced rate capability (80 C,75.5 mAh g-1) and cycling stability (111.0 mAh g-1capacity after 1000 cycles at 10 C current density) for ***-1 exhibits outstanding fast-charging capabilities,achieving an 80%state of charge in just 8.1 *** assembled VPS-1//SbSn/NPC full cell demonstrated stable cycling over 200 cycles at a high 5 C current,maintaining an average coulombic efficiency of 95.35%.

关键词： Anionic group modulation Polarization behavior Fast-charging Sodium-ion battery Fluorophosphate Cathode

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Visible-light-responsive homologous heterostructure of oxynitrides constructed to boost charge separation and water splitting

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Science China chemistry 2025年第01期 186-191页

作者： Hai Zou Yunfeng Bao Xueshang Xin Yu Qi Tengfeng Xie Fuxiang Zhang state key laboratory of Catalysis Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences School of chemistry and Chemical Engineering Liaoning Normal University College of chemistry Jilin University

Constructing type II heterostructures represents a widely recognized strategy for enhancing charge separation and photocatalytic efficiency,but it remains challenging to fabricate homologous heterostructures based on visible-light-responsive semiconductors,especially for popularly investigated （oxy）nitrides with low thermal ***,we synthesized a homologous heterostructure （denoted as YTON＿H） based on the oxynitrides of YTaO4-xNyand YTa *** heterostructure exhibits type II band structure alignment and intimate interface achieved through a magnesium （Mg） powder-assisted nitridation *** with widely reported heterologous heterostructures,the as-obtained YTON＿H homologous heterostructure could similarly exhibit enhanced charge separation as well as photocatalytic water splitting performance with respect to its counterparts(YTaO4-xNyand YTaON2).Meanwhile,detailed structural characterizations and spectroscopy analysis have been made to confirm the formation of heterostructure and promotion of spatial charge separation.

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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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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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Role of iron ore in enhancing gasification of iron coke:structural evolution,influence mechanism and kinetic analysis

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International Journal of Minerals,Metallurgy and Materials 2025年第1期32卷 58-69页

作者： Jie Wang Wei Wang Xuheng Chen Junfang Bao Qiuyue Hao Heng Zheng Runsheng Xu School of chemistry and Materials Science Hubei Engineering UniversityXiaogan 432000China key laboratory for Ferrous Metallurgy and Resources Utilization of Ministry of Education Wuhan University of Science and TechnologyWuhan 430081China Institue of Ironmaking Technology Baosteel Central Research InstituteShanghai 201999China state key laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China

The utilization of iron coke provides a green pathway for low-carbon *** uncover the influence mechanism of iron ore on the behavior and kinetics of iron coke gasification,the effect of iron ore on the microstructure of iron coke was ***,a comparative study of the gasification reactions between iron coke and coke was conducted through non-isothermal thermogravimetric *** findings indicate that compared to coke,iron coke exhibits an augmentation in micropores and specific surface area,and the micropores further extend and *** provides more adsorption sites for CO_(2) molecules during the gasification process,resulting in a reduction in the initial gasification temperature of iron *** the heating rate in non-isothermal gasification can enhance the reactivity of iron *** metallic iron reduced from iron ore is embedded in the carbon matrix,reducing the orderliness of the carbon structure,which is primarily responsible for the heightened reactivity of the carbon *** kinetic study indicates that the random pore model can effectively represent the gasification process of iron coke due to its rich pore ***,as the proportion of iron ore increases,the activation energy for the carbon gasification gradually decreases,from 246.2 kJ/mol for coke to 192.5 kJ/mol for iron coke 15wt%.

关键词： low-carbon ironmaking iron coke gasification structural evolution kinetic model

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Insights into support effects on Ce-Zr-O mixed oxide-supported gold catalysts in CO oxidation

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Journal of Energy chemistry 2013年第1期22卷 98-106页

作者： Hongpeng Zhang Haichao Liu Beijing National laboratory for Molecular Sciences State Key Laboratory for Structural Chemistry of Stable and Unstable Species College of Chemistry and Molecular Engineering Peking University

Au]Cel_xZrxO2 catalysts （x = 0-0.8） were prepared by a deposition-precipitation method using Cel_xZrxO2 nanoparticles as supports with variable Ce and Zr contents. Their structures were characterized by complimentary means such as X-ray diffraction, Raman, scanning trans- mission electron microscopy and X-ray photoelectron spectroscopy （XPS）. These Au catalysts possessed similar sizes and crystalline phases of Cel_xZrzO2 supports as well as similar sizes and oxidation states of Au nanoparticles. The oxidation state of Au nanoparticles was dominated by Au~ especially in CO oxidation. Their activities were examined in CO oxidation at different temperatures in the range of 303-333 K. The CO oxidation rates normalized per Au atoms increased with the increasing Ce contents, and reached the maximum value over Au/CeO2. Such change was in parallel with the change in the oxygen storage capacity values, i.e. the amounts of active oxygen species on Au/Cel_zZrzO2 catalysts. The excellent correlation between the two properties of the catalysts suggests that the intrinsic support effects on the CO oxidation rates is related to the effects on the adsorption and activation of O2 on Au/Cel_xZrxO2 catalysts. Such understanding on the support effects may be useful for designing more active Au catalysts, for example, by tuning the redox properties of oxide supports.

关键词： gold catalyst ceria-zirconia support CO oxidation oxygen storage capacity support effect

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Functional molecular electronic devices through environmental control

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Science China Materials 2019年第1期62卷 1-7页

作者： Dingkai Su Chunhui Gu Xuefeng Guo Beijing National laboratory for Molecular Sciences State Key Laboratory for Structural Chemistry of Unstable and Stable Species College of Chemistry and Molecular Engineering Peking University

Motivated by Moore's law,molecular electronic devices are considered as a promising alternative of traditional silicon-based electronic devices due to their extreme miniaturization,low-cost manufacturing and versatility [1].The initial model of molecular electronics was a molecular diode theoretically proposed by Aviram and Ratner in 1974[2],where they utilized a single organic molecule to control the electric current flow in one-way direction.

关键词：分子电子器件环境调控化学反应动力学分子聚集体单个分子分子工程材料工程界面工程

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Promoting effect of chloride ions on selective oxidation of methanol to methyl formate over zirconia-supported ruthenium oxide catalysts

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Journal of Energy chemistry 2013年第3期22卷 512-516页

作者： Weizhen Li Hongpeng Zhang Xiaohui He Haichao Liu Beijing National laboratory for Molecular Sciences State Key Laboratory for Structural Chemistry of Stable and Unstable SpeciesCollege of Chemistry and Molecular EngineeringPeking University

The effect of chloride ions on a monoclinic ZrO2-supported RuOx （RuOx/m-ZrO2） catalyst with a Ru surface density of 0.3 Ru/nm2 was studied in the selective oxidation of methanol to methyl formate （MF） at a low temperature of 373 K. The m-ZrO2 support was Cl-free, and Cl- ions were introduced into the RuOx/m-ZrO2 catalyst by impregnation with zirconium oxychloride or ammonium chloride and subsequent thermal treatment in air at 673 K. The structures of these catalysts were characterized by X-ray diffraction, Raman and X-ray photoelectron spectroscopies. Their reducibility was probed by temperature-programmed reduction in H2. The RuOx domains were present as highly dispersed Rut42- structure on m-ZrO2 with similar reducibility for the RuOx/m-ZrO2 samples irrespective of modification with or without Cl ions. Introduction of appropriate amounts of zirconium oxychloride into RuOx/m-ZrO2 led to a remarkable increase in the methanol oxidation rate and MF selectivity, whereas introduction of ammonium chloride or zirconyl nitrate significantly inhibited the catalytic performance of RuOx/m-ZrO2. The promoting effect of Cl- ions derived from zirconium oxychloride can be tentatively attributed to their roles in facilitating the adsorption of methanol and desorption of MF product or its intermediates. This finding provides novel insights into the promoting effect of Cl- ions on oxides-based catalysts for selective oxidation reactions.

关键词： methanol oxidation ruthenium oxide monoclinic zirconia chloride promoting effect methyl formate

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Base-free aerobic oxidation of glycerol on TiO_2-supported bimetallic Au–Pt catalysts

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Journal of Energy chemistry 2015年第5期24卷 669-673页

作者： Yihong Shen Yuming Li Haichao Liu Beijing National laboratory for Molecular Sciences State Key Laboratory for Structural Chemistry of Stable and Unstable Species College of Chemistry and Molecular Engineering Peking University

The aerobic oxidation of glycerol provides an economically viable route to glyceraldehyde, dihydroxyacetone and glyceric acid with versatile applications, for which monometallic Pt, Au and Pd and bimetallic Au-Pt, Au- Pd and Pt-Pd catalysts on TiO2 were examined under base-free conditions. Pt exhibited a superior activity relative to Pd, and Au-Pd and Pt-Pd while Au was essentially inactive. The presence of Au on the Au-Pt/TiO2 catalysts led to their higher activities （normalized per Pt atom） in a wide range of Au/Pt atomic ratios （i.e. 1/3-7/1 ）, and the one with the Au/Pt ratio of 3/1 exhibited the highest activity. Such promoting effect is ascribed to the increased electron density on Pt via the electron transfer from Au to Pt, as characterized by the temperature-programmed desorption of CO and infra-red spectroscopy for CO adsorption. Meanwhile, the presence of Au on Au-Pt/TiO2, most like due to the observed electron transfer, changed the product selectivity, and facilitated the oxidation of the secondary hydroxyl groups in glycerol, leading to the favorable formation of dihydroxyacetone over glyceraldehyde and glyceric acid that were derived from the oxidation of the primary hydroxyl groups. The synergetic effect between Au and Pt demonstrates the feasibility in the efficient oxidation of glycerol to the targeted products, for example, by rational tuning of the electronic properties of metal catalysts.

关键词： Glycerol aerobic oxidation Glyceraldehyde Dihydroxyacetone Bimetallic Au-Pt catalyst Synergetic effect

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