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Science China chemistry 2025年第2期68卷 601-609页

作者： Fan Guo Zong-Zheng He Peng Wang Xiao-Yu Zhang Hongjian Yu Qin-Chao Wang Wei-Yin Sun School of chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China coordination chemistry Institute State Key Laboratory of Coordination ChemistrySchool of Chemistry and Chemical EngineeringNanjing National Laboratory of MicrostructuresCollaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210023China

Engineering nonmetallic atom-doped metal-organic framework(MOF)catalyst to promote C−C coupling and realize conversion of CO_(2) into C_(2 )multi-carbon hydrocarbon products is still ***,with 2-methylimidazole as a dopant of N element,an N-doped NH_(2)-CuBDC catalyst was obtained via a facile and simple stirring *** illumination,compared with catalytic CO_(2) reduction to C1 product of CO by original MOF,N-doped NH_(2)-CuBDC can motivate generation of C_(2)H_(4),which is difficult to achieve in photocatalytic system by MOF-based *** transfer rates of photo-generated charges have been expedited due to the high electron density around Cu catalytic sites after *** importantly,C–C coupling intermediate CO–CHO*was identified by in situ Fourier transform infrared spectroscopy during the catalytic CO_(2) reduction reaction process,which further indicates the presence of Cu–N sites in the NH_(2)-CuBDC can facilitate the formation of C2H_(4) *** work uncovers a new paradigm to design photocatalysts for enhancing the reduction of CO_(2) to C_(2) products.

关键词： metal-organic frameworks C-C coupling doping photocatalytic CO_(2) reduction Cu-based catalysts

Tetraphenylethylene-derived organic cages with persistent photogenic radicaloids and efficient photothermal conversion

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Science China chemistry 2025年第2期68卷 661-669页

作者： Suqiong Yan Bo Yang Fanda Feng Yuan Zhang Shirong Ban Hui Ma Wei Huang State Key laboratory of coordination chemistry School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210093China Shenzhen Research Institute of Nanjing University Shenzhen 518057China

Transformation of the electronic spin states has received significant interest in recent years because of its applications in the magnetic information storage materials and optical response ***,it can be formidably challenging to use ultraviolet(UV)light as a contactless stimulus to alter the electronic spin states of the supramolecular *** by the approach on the radical cation mechanism of the Scholl reaction and the photocyclization reactivity of tetraphenylethylene(TPE)derivatives,we report two photochromic cages(cage-TPE-1 and cage-TPE-2)that can be photochemically transformed from electron paramagnetic resonance(EPR)-silent to EPR-active form via UV irradiation due to the photo-induced electron transfer process at the TPE *** provided a strong single-electron signal with a g value of 2.003 in cage-TPE-1 and cage-TPE-2 but no signal was detected for the pristine samples without the *** transformation can be monitored by ultraviolet–visible–near-infrared(UV–vis–NIR)and photoluminescence(PL)*** photogenic radical cage intermediate was unstable in solution resulting in the degradation and intramolecular cyclization of the reactive species,while the radicals were found to be stable and persistent in the solid state due to the spin delocalization,the steric protection of confined cavities,and the oxygen *** theoretical calculations and spectral measurements suggest that the photogenic radical cage-TPE-2(•+)experiences photocyclization on the TPE *** with the close-shell cage,the radical cage-TPE-1(•+)and cage-TPE-2(•+)exhibit better photothermal conversion performance due to the incubated infrared absorption from open-shell electron feature and reduced band gap.

关键词： supramolecular cage photogenic radical photocyclization photothermal conversion

Trinuclear gold-catalyzed site-selective alkylation of peptides

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Science China chemistry 2025年第1期68卷 249-256页

作者： Qing-Yun Fang Chengyihan Gu Yinghan Chen Wencheng Yan Yong Liang Weipeng Li Chengjian Zhu Jie Han Jin Xie State Key laboratory of coordination chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsChemistry and Biomedicine Innovation Center(ChemBIC)School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Green Catalysis Center College of ChemistryZhengzhou UniversityZhengzhou 450001China State Key laboratory of Natural Medicines China Pharmaceutical UniversityNanjing 211198China

Selective modification of peptides has always been a challenging *** selective alkylation of peptides can alter the biological activity and physical properties of molecules,and it has gained significant research *** herein disclose an intriguing gold-catalyzed alkylation of peptides using bench-stable unactivated alkyl bromides under photoredox catalysis.A wide range of structurally diverse primary,secondary and tertiary alkyl bromides serve as effective coupling partners to precisely connect with theα-C(sp^(3))–H in glycine residue of *** protocol demonstrates an exceptionally broad scope for alkyl halides and excellent tolerance for a wide range of useful functional groups.A series of relay transformations to construct cyclic peptides,to proceed click reaction and to realize peptide fluorescence labeling further enhance its synthetic *** addition,mechanistic studies and density functional theory(DFT)calculations reveal an inner-sphere and subsequent outersphere single electron transfer(SET)mechanism.

关键词： gold catalysis peptide alkylation C-C coupling radical

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Deciphering the mechanism of structural transformation between Pd3L6 and Pd4L8 metal-organic cages

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Science China chemistry 2025年

作者： Xian-Chao Zhou Yong-Zhen Tan Ying-Ying Ge Ya-Liang Lai Dong Luo Xiao-Ping Zhou Dan Li College of chemistry and Materials Science Guangdong Provincial Key Laboratory of Supramolecular Coordination ChemistryJinan University

Metal-organic cages can undergo structural transformations due to the dynamic nature of dative bonds,however,the mechanism of transformation processes is often *** we report four metal-organic cages featuring Pd3L6-type and Pd4L8-type tubular structures by self-assembly of Pd（II） and two types of bidentate *** Pd3L6-type MOCs were synthesized in H2O while the Pd4L8-type cages were formed in dimethyl sulfoxide （DMSO）,indicating the solvent is critical for the *** structure transformation between Pd3L6and Pd4L8metal-organic cages can be interconverted when switching the DMSO and H2O in a relatively high *** cages partly disassemble into the metalloligands and Pd2+ions due to the competitive coordination of DMSO/H2O at low concentrations,achieving a concentration-controlled transformation ***,the structure transformation was monitored by ESI-MS,and the species of intermediate were detected,which provided direct clues for deciphering the mechanism of structural transformation.

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Robust free-base and metalated corrole radicals with reduction-induced emission

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Chinese Chemical Letters 2025年第2期36卷 426-431页

作者： Pengfei Li Chulin Qu Fan Wu Hu Gao Chengyan Zhao Yue Zhao Zhen Shen State Key laboratory of coordination chemistry Collaborative Innovation Center of Advanced MicrostructuresSchool of Chemistry and Chemical EngineeringNanjing University School of chemistry and Materials Science Nanjing Normal University College of Materials Science and Engineering Nanjing Forestry University

Preparing free-base porphyrinoid radicals that can function as coordination ligands is a challenging task. Here we report the synthesis of a stable, free-base benzocorrole(BC) radical containing only two inner NH protons via a retro-Diels-Alder conversion. The radical character of BC was fully supported by crystallographic analysis, spectroscopic evidence, and theoretical calculations. This neutral radical ligand allowed easy insertion of Zn(Ⅱ), Ga(Ⅲ), and Pd(Ⅱ) ions to produce radical complexes. All these radicals exhibited luminescence-on responses under weak reducing atmosphere, corresponding to the conversion to their aromatic anions. The red fluorescence was observed for BC and its Zn(Ⅱ) and Ga(Ⅲ) complexes,and the near-infrared phosphorescence(>900 nm) was detected for Pd(Ⅱ) complex at room ***, Ga(Ⅲ) corrole exhibited a variation in fluorescence in response to axial coordination. Our findings provide a promising radical platform for coordination and developing novel functional materials with switchable spin and emission.

关键词： Luminescence Macrocyclic ligands Porphyrinoids Radicals Redox chemistry

Plasmonic tandem heterojunctions enable high-efficiency charge transfer for broad spectrum photocatalytic hydrogen production

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Journal of Energy chemistry 2025年第1期100卷 710-720页

作者： Wenxuan Chen Xiu-Qing Qiao Guo Hui Bojing Sun Dongfang Hou Meidi Wang Xueqian Wu Tao Wu Dong-Sheng Li College of Materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion MaterialsChina Three Gorges UniversityYichang 443002HubeiChina Hubei Three Gorges laboratory Yichang 443007HubeiChina College of chemistry and Materials Science and Guangdong Provincial Key Laboratory of Supramolecular Coordination ChemistryJinan UniversityGuangzhou 510632GuangdongChina

Rational engineering of semiconductor photocatalysts for efficient hydrogen production is of great significance but still challenging,primarily due to the limitations in charge transfer ***,a fascinating plasmonic tandem heterojunction with the hc-CdS/Mo_(2)C@C heterostructure is aimfully prepared for effectively promoting the charge separation kinetics of the CdS photocatalyst via the synergistic strategy of phase junction,Schottky junction,and photothermal *** difference in atomic configuration between cubic-CdS (c-CdS) and hexagonal-CdS (h-CdS) leads to effective charge separation through a typical Ⅱ charge transfer mechanism,and plasmonic Schottky junction further extracts the electrons in the hc-CdS phase junction to realize gradient charge ***,the photothermal effect of Mo_(2)C@C helps to expand the light absorption,accelerate charge transfer kinetics,and reduce the hydrogen evolution energy *** carbon layer provides a fast channel for charge transfer and protects the photocatalyst from *** a result,the optimized hc-CMC photocatalyst exhibits a significantly high photocatalytic H_(2)production activity of 28.63 mmol/g/h and apparent quantum efficiency of 61.8%,surpassing most of the reported *** study provides a feasible strategy to enhance the charge transfer kinetics and photocatalytic activity of CdS by constructing plasmonic tandem heterogeneous junctions.

关键词： Heterojunctions Mo_(2)C LSPR Photocatalyst Phase junction Schottkyjunction Photothermal effect

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Modifying metabolic and immune hallmarks of cancer by a copper complex

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Science China chemistry 2025年第3期 1051-1066页

作者： Chengyan Chu Yunhua Zhang Chengyuan Qian Xiu-Zhi Yang Yicun Shang Zijian Guo Xiaoyong Wang State Key laboratory of Pharmaceutical Biotechnology School of Life SciencesNanjing University State Key laboratory of coordination chemistry School of Chemistry and Chemical EngineeringNanjing University

Metabolic adaptation of cancer cells is a key tactic for maintaining their tumorigenicity and viability in the tumor immune microenvironment（TIME）.Concurrent modulation on the metabolic pathway and immune system could change the living condition of cancer cells and potentiate the efficacy of anticancer drugs.A copper complex（DDCu） was designed to influence the energy metabolism of cancer cells and reshape the *** restrained the production and transportation of lactate by inhibiting the expression of lactate dehydrogenase and monocarboxylate transporter 4,thereby altering the metabolic pathway of cancer cells and improving the acidic tumor ***,DDCu was reduced to Cu+by cellular glutathione to react with lipoylated proteins of the tricarboxylic acid cycle and destabilize the Fe–S cluster proteins,leading to the aggregation of dihydrolipoamide S-acetyltransferase and cuproptosis in cancer ***,DDCu promoted the polarization of macrophages from the M2 to M1 phenotype,activated CD4+and CD8+T cells,and reversed the *** a result,DDCu inhibited the tumor growth through a synergy between metabolic regulation and immunomodulation.

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Palladium installed copper-organic framework for C–C coupling reactions

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Science China chemistry 2025年

作者： Yu-Mei Wang Mei-Xia Tao Kai-Ming Mo Xu Chen Shu-Hua Zhong Elena S Shubina Guo-Hong Ning Dan Li College of chemistry and Materials Science Guangdong Provincial Key Laboratory of Supramolecular Coordination ChemistryJinan University A.N.Nesmeyanov Institute of Organoelement Compounds Russian Academy of Sciences

The formation of C–C bonds is a crucial aspect of organic synthesis. Synthesists' long-term objective is to identify novel catalysts to optimize reaction systems based on traditional transition metal catalysis. This study explores the synthesis and catalytic potential of palladium-installed covalent metal-organic frameworks(CMOFs) based on copper cyclic trinuclear units(Cu-CTUs). By incorporating palladium ions into the imine-based framework JNM-7 through a straightforward immersion method, we achieved a notable enhancement in catalytic activity for critical C–C coupling reactions, including C–H arylation and Sonogashira cross-coupling. The resulting JNM-7-Pd demonstrated remarkable stability and recyclability, maintaining its efficiency over at least three cycles without any decline in efficiency.

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Research progress in metal-organic frameworks and their derivatives in electrochemistry

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Science China chemistry 2025年

作者： Lingling Chen Yuxin Liu Yichun Su Wenchen Zhu Guangyu Du Huan Pang School of chemistry and Chemical Engineering Yangzhou University Department of Applied Physics The Hong Kong Polytechnic University Interdisciplinary Materials Research Center Institute for Advanced Study Chengdu University State Key laboratory of coordination chemistry Nanjing University

Metal-organic frameworks (MOFs) are distinguished by their unique porosity and meticulously ordered framework structures,setting them apart from conventional complexes. These materials are defined by their highly organized crystalline and pore structures, extensive surface areas, robust porosity, and superior adsorption capabilities. Owing to their exceptional structural and functional attributes, MOFs and their derivatives are leveraged across a broad spectrum of applications, demonstrating significant potential across diverse sectors. In recent times, the scientific community has increasingly focused on MOFs, underscoring their growing importance in research. Despite the promising array of applications for MOFs and their derivatives,challenges persist in practical deployments, and the pathway to research advancement remains daunting. This document delves into the synthesis and various applications of MOFs and their derivatives, particularly in the domains of energy storage, catalysis,sensing, and water treatment. It also highlights the ongoing research progress in the field of electrochemistry, including developments in lithium ion batteries (LIBs), lithium-sulfur batteries (LSBs), zinc-ion batteries (ZIBs), aqueous nickel-zinc batteries (NZBs), and supercapacitors. Finally, it provides an outlook on the future prospects and potential hurdles facing the development of MOF materials.

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Microdynamic modulation through Pt–O–Ni proton and electron “superhighway” for pH-universal hydrogen evolution

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Journal of Energy chemistry 2025年第2期101卷 808-815页

作者： Dewen Wang Yuting Chen Bohan Yao Tian Meng Yanchao Xu Dongxu Jiao Zhicai Xing Xiurong Yang State Key laboratory of Electroanalytical chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences University of Science and Technology of China Department of chemistry Shenzhen Grubbs Institute and Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Southern University of Science and Technology State Key laboratory of Automotive Simulation and Control School of Materials Science and Engineering Jilin University

Optimizing the microdynamics in alkaline and neutral conditions is a significant but challenging task in developing pH-universal hydrogen evolution（HER） ***,a unique Pt-O-Ni bridge has been constructed to alter the coordination and electronic environment between Pt nanoparticles（Pt_n）and nickel metaphosphate（NPO） substrate（Pt-NPO）.Sufficient electron transfer from NPO to Pt_n to maintain an electron-rich environment and a low valence state of Pt_***,H*is produced from the H2O dissociation on Ni site and then spillover toward Pt sites to bind into H2,which makes up for the insufficient H2O dissociation ability of Pt in Volmer ***-NPO exhibits long-term stability and only need the overpotentials of 22.3,33.0 and 30.5 mV to attain 10 mA cm-2in alkaline,neutral and acidic media,*** anion-exchange membrane（AEM） water electrolyzer catalyzed by Pt-NPO shows high water electrolysis performance that a cell voltage of 1.73 V is needed to obtain the current density of500 mA cm-2in 1 M KOH at 80℃,at the same time maintains good stability for 350 *** regulation strategy proposed in this work is helpful for the design and synthesis of highly efficient pH-universal HER electrocatalysts.

关键词： Atomic and electronic regulation Hydrogen evolution reactions Metal-support interactions Microdynamics pH-universal HER electrocatalysts