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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 Materials China Three Gorges University Hubei Three Gorges laboratory College of chemistry and Materials Science and Guangdong Provincial Key Laboratory of Supramolecular Coordination Chemistry Jinan University

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/Mo2C@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 Mo2C@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 H2production 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： Cadmium sulfide

Modifying metabolic and immune hallmarks of cancer by a copper complex

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Science China chemistry 2025年

作者： Chengyan Chu Yunhua Zhang Chengyuan Qian Xiuzhi Yang Yicun Shang Zijian Guo Xiaoyong Wang State Key laboratory of Pharmaceutical Biotechnology School of Life Sciences Nanjing University State Key laboratory of coordination chemistry School of Chemistry and Chemical Engineering Nanjing 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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Boosting aqueous nickel-zinc battery stability with bimetallic ion-integrated 1D metal-organic nanowires

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Science China chemistry 2025年

作者： Yihao Chen Jin Liang Yichun Su Guoyin Zhu Hengyue Xu Hongye Ding Guangxun Zhang Dianheng Yu Zizhou Shen Yizhou Zhang Wei Huang Huan Pang School of chemistry and Chemical Engineering Yangzhou University Key laboratory of flexible Electronics (KLofE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Institute of Advanced Materials and flexible Electronics (IAMfE) School of Chemistry and Materials Science Nanjing University of Information Science & Technology Department of chemistry Tsinghua University State Key laboratory of coordination chemistry Nanjing University

Limited by low conductivity,designing cathode materials with excellent electron transfer efficiency for high-performance nickel-zinc batteries （NZBs） remains *** this study,a series of bimetallic metal-organic nanowires were fabricated by doping M ions in NiNTA,resulting in NiMNTA (M=Mg2+,Mn2+,Co2+,Zn2+,Ag+),and NixCo6-xNTA （x=1,2,3,4,5）.The proportions and types of metal ions can be modified without altering the initial coordination structure.X-ray absorption fine structure spectroscopy （XAfS） revealed that only M–O bonds,not metal bonds,were present in the *** performance of Ni2Co4NTA as the cathode for aqueous NZBs was significantly improved,achieving the maximum energy density of 279.17Wh kg-1with the high cycle stability （retention rate of 72.0%after 1,000 cycles）.The flexible Ni2Co4NTA//Zn@carbon cloth battery employing gel electrolyte also exhibits the excellent Coulombic efficiency of 96%after 350 *** approach shows considerable potential for designing one-dimensional materials with bimetallic modifications,providing new strategies for developing cathode materials for NZBs with high specific capacity and cycle stability.

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Electrochemical sensor for dopamine detection based on multiwalled carbon nanotube/molybdenum disulfide quantum dots with machine learning integration and anti-interference capability

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Tungsten 2025年第1期7卷 137-151页

作者： Geethukrishnan Onkar Apte Kiran Kumar Tadi Energy Electrodics and Electrocatalysis (EEE) Lab Department of Chemistry School of Advanced Sciences Vellore Institute of Technology School of Computer Science and Engineering Vellore Institute of Technology

The precise detection and measurement of dopamine（DA）,a crucial neurotransmitter in the human body,plays a significant role in diagnosing,preventing,and treating neurological diseases associated with its levels.A highly sensitive DA electrochemical sensor was constructed by combining molybdenum disulfide quantum dots（MSQDs） with multiwalled carbon nanotubes（MWCNTs）.The MSQDs were synthesized using the shear exfoliation *** sensors consist of MSQDs with Mo-S edge catalytic centers for the DA redox reaction,and MWCNTs amplify the sensor *** linearity of the sensor for the detection of DA was tested in the presence of ascorbic acid(AA,50 μmol·L-1) and uric acid(UA,200 μmol·L-1),and exhibited linearity from 2 to 966 μmol·L-1of DA with 0.097 μA(mol·L-1)-1sensitivity and a low limit of detection of0.6 μmol·L-1（the ratio between signal and noise,S/N=3）.Moreover,the sensitivity and selectivity of the sensor were also studied using *** is no increase in amperometric current after adding the most potentially interfering *** sensor was successfully applied to recover DA in human blood sera ***,machine learning algorithms were operated to aid in the near-precise detection of DA in the heterogeneous mixture containing AA and *** algorithms facilitate the identification and quantification of DA amidst coexisting interferents,including AA,that are commonly present in biological matrices.

关键词： Biosensor Complex mixture Dopamine Machine learning MoS2 Multiwalled carbon nanotubes

Surface-confined persistent luminescence with amplified fRET efficiency for cell-cell communication monitoring

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Science China chemistry 2025年

作者： Ziyun Miao Wenjing Dai Yubin Jin Bing Qi Jiayi Chen Lingling Qiu Yurong Wei Jie Wang The Key lab of Health chemistry&Molecular Diagnosis of Suzhou College of ChemistryChemical Engineering&Materials ScienceSoochow University

Microbial communication monitoring is vital for understanding the mechanisms beneath gut microbiota equilibrium, infections,and biomanufacturing. Herein, we reported monitoring bacterial communication by surface-confined persistent ***, we constructed core-shell structured Zn1.4Ga1.2Ge0.4O4@Zn1.4Ga1.2Ge0.4O4:Cr（ZGGO@ZGGO:Cr） persistent luminescence nanoparticles（PLNPs） with amplified fRET efficiency for the detection of azoreductase（AzoR） that participates in bacterial communication. ZGGO@ZGGO:Cr nanoparticles were functionalized with an azo black hole quencher（ZGGO@ZGGO:Cr-BHQ-3）. Due to the proximity of surface-confined persistent luminescence with the surface-bound BHQ-3,ZGGO@ZGGO:Cr-BHQ-3 exhibited a fRET efficiency up to 1.6 times that of traditional ZGGO:Cr-BHQ-3. further, the specific catalytic reduction of azo bonds in BHQ-3 by bacterial extracellular AzoR recovers the persistent luminescence of ZGGO@ZGGO:Cr. ZGGO@ZGGO:Cr-BHQ-3 displayed superior sensitivity and speed in detecting extracellular AzoR over ZGGO:Cr-BHQ-3, attributed to its surface-confined persistent luminescence. We found that the peak secretion of AzoR occurs during the exponential growth period of bacteria including S. aureus and E. coli based on the persistent luminescence recovery rate of ZGGO@ZGGO:Cr-BHQ-3. furthermore, ZGGO@ZGGO:Cr-BHQ-3 was used to probe the communication between different bacterial species. R. palustris is a kind of lycopene-production bacteria. We found that the cohabitation of R. palustris and S. putrefaciens boosted both AzoR secretion and lycopene production. Moreover, the secretion and activity of AzoR positively correlated with lycopene production, suggesting that AzoR may participate in the communication between R. palustris and S. putrefaciens to promote lycopene production. This study offers a robust method to enhance PLNP-based biosensing sensitivity and provides a promising strategy for microbial communication monitoring.

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Recent progress on photoactive nonprecious transition-metal complexes

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Science China chemistry 2025年第1期68卷 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.

关键词： photoactive metal complexes earth-abundant metals nonprecious metal complexes luminescence photochemistry

BODIPY-derived ratiometric fluorescent sensors: pH-regulated aggregation-induced emission and imaging application in cellular acidification triggered by crystalline silica exposure

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Science China chemistry 2018年第11期61卷 1413-1422页

作者： Yang Bai Danyang Liu Zhong Han Yuncong Chen Zhongyan Chen Yang Jiao Weijiang He Zijian Guo State Key laboratory of coordination chemistry Coordination Chemistry Institute School of Chemistry and Chemical EngineeringNanjing University

Modification of classic fluorophore to possess the emission transitions between aggregation-induced emission （ALE） and intrinsic emission offers reliable approach to the design of ratiometric fluorescent sensors. In this study, a proton acceptor benzimidazole was integrated with BODIPY to form three compounds, BBI-1/2/3, which demonstrated the AIE （-595 nm, Iagg） in neutral aqueous medium and intrinsic BODIPY emission （-510 nm,Iint） in acidic medium. All the three showed the ratiometric pH sensing behavior in a dual excitation/dual emission mode, yet BBI-3 displayed still the dual emission ratiometric pH sensing ability. The pH-dependent emission ratio/int/Iagg of the three were fully reversible, and no interference was observed from normal abundant chemical species in live cells. Their different pKa （BBI-1, pKa 4.4; BBI-2, pKa 2.7; BBI-3, pKa 3.6） suggested that the substituents on benzimidazole moiety were essential to govern their functioning pH range. The ratiometric imaging of BBI-1 in A549 cells provided an effective intracellular pH （pHi） calibration formula corresponding to emission ratio oflJ Iint/Iagg. Ratiometric pH imaging in A549 cells upon small particle exposure confirmed the particle-induced cellular acidification with this formula. Both particle size and the chemical nature of the particle contribute to the observed acidification effect. The synchronization of lysosome disruption to cellular acidification in A549 cells upon crystalline silica exposure was directly observed for the first time with BBI-1, showing the potential application of BBI-1 in the study of silicosis and other related diseases. This study de- monstrated that endowing fluorophore with AIE/intrinsic emission transition could be a promising strategy for ratiometric sensor design.

关键词： fluorescence imaging sensor cellular acidification aggregation-induced emission crystalline silica lysosome BODIPY

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