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Science China Chemistry 2025年

作者： Jun-Qiang Chen Qiao-Hong Li Qin-Long Hong Ping Shao Hai-Xia Zhang Jian Zhang State Key laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences

Single-atom catalyst has garnered widespread attention to mimic mature enzymes due to its well-defined atomic structure and coordination environments. However, since the carbon–carbon（C–C） coupling reactions require synergistic catalysis of multiple sites, single-atom catalysts suffer from insufficient active sites and unclear reaction mechanisms. Controlling the reaction intermediates in a precisely targeted pocket through careful metal–organic cage design is therefore crucial. Here, we prepare a tetrahedral [Cu6L4]-type boron–imidazolate cage integrating highly active Cu sites and optimized cavity, which exhibits enzyme like specific catalytic performance in electrochemical CO2reduction reaction（CO2RR） to enhance the selectivity of *** analyses and computational calculations suggest that the single Cu site together with neighboring boron–imidazolate ligands provides suitably synergistic effects that enable the energetically favorable formation of an *COCHO intermediate, a key step determining selectivity. As a result, the [Cu6L4]-type cage of BIC-145 achieves a Faradaic efficiency of 28% for C2H4maintaining an average current density of -3.54 mA cm-2over a 5-hour electrolysis period. This work represents the first example for studying single-metal site catalysts with ultra-low coordination numbers through the rational design of metal–organic cages.

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High-energy-density lithium manganese iron phosphate for lithium-ion batteries: Progresses, challenges, and prospects

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Journal of Energy Chemistry 2025年第1期100卷 1-17页

作者： Bokun Zhang Xiaoyun Wang Shuai Wang Yan Li Libo Chen Handong Jiao Zhijing Yu Jiguo Tu State Key laboratory of Advanced Metallurgy University of Science and Technology Beijing Research Institute for Intelligent Wearable Systems The Hong Kong Polytechnic University Institute of Advanced structure Technology Beijing Institute of Technology

The soaring demand for smart portable electronics and electric vehicles is propelling the advancements in high-energy–density lithium-ion *** manganese iron phosphate (LiMnxFe1-xPO4) has garnered significant attention as a promising positive electrode material for lithium-ion batteries due to its advantages of low cost,high safety,long cycle life,high voltage,good high-temperature performance,and high energy *** LiMnxFe1-xPO4has made significant breakthroughs in the past few decades,there are still facing great challenges in poor electronic conductivity and Li-ion diffusion,manganese dissolution affecting battery cycling performance,as well as low tap *** review systematically summarizes the reaction mechanisms,various synthesis methods,and electrochemical properties of LiMnxFe1-xPO4to analyze reaction processes accurately and guide material ***,the main challenges currently faced are concluded,and the corresponding various modification strategies are discussed to enhance the reaction kinetics and electrochemical performance of LiMnxFe1-xPO4,including multi-scale particle regulation,heteroatom doping,surface coating,as well as microscopic morphology ***,in view of the current research challenges faced by intrinsic reaction processes,kinetics,and energy storage applications,the promising research directions are *** importantly,it is expected to provide key insights into the development of high-performance and stable LiMnxFe1-xPO4materials,to achieve practical energy storage requirements.

关键词： Semiconductor doping

Breaking the structural symmetry of active sites in zeolite imidazolate framework for enhanced CO2 photoreduction

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Science China Chemistry 2025年

作者： Yupeng Han Yayu Yan Qiaohong Li Xin Wu Fei Wang Jian Zhang State Key laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences University of Chinese Academy of Sciences College of Chemistry Fuzhou University

Adjusting the structure and composition of active sites is a highly effective method for activating linear ***, precise control of interfacial chemistry within molecular-scale environments presents a significant challenge in heterogeneous catalysis. In our study, we present symmetry-broken Mo-O-Co triple-atom active sites within the hybrid zeolite imidazole framework HZIF-CoMo. These sites disrupt the electronic balance and create a weak built-in electric field, thus promoting photocatalytic CO2reduction. The CO yield over HZIF-CoMo is improved to 3.1 mmol g-1h-1, which is over four times higher than the parent cobalt-imidazole framework MAF-6-Co. Both experimental and theoretical studies indicate that electronic modulation through the symmetry-breaking Mo-O-Co moiety acts as an organizing knob to accelerate charge separation and result in more carriers participating in the catalytic reaction. This work provides important insights into optimizing site-related electronic structures for targeted photocatalytic reactions.

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Reverse modulation of defect density of Ce-MOF-808 by solventassisted ligand exchange for dicyclopentadiene hydrogenation

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Science China Chemistry 2025年

作者： Danfeng Zhao Fajie Hu Rushuo Li Xinmeng Xu Zhaokun Wang Zuoshuai Xi Jun Tong Xiubing Huang Ge Wang Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule & Structure Construction School of Materials Science and Engineering University of Science and Technology Beijing

Defect engineering is a pivotal strategy for tailoring the electronic structure and physicochemical properties of catalysts, yet the straightforward manipulation of defect density in porous materials presents a current challenge. In this work, we achieved precise control over the coordination unsaturated site（CUS） content and pore architecture of Ce-MOF-808 by employing 2-fluorobenzoic acid（2-FBA） as a modifier. Leveraging the p Kadisparities among three ligands（1,3,5-tricarboxylic benzoic acid,formic acid, and 2-FBA）, we preserved the spn topology of Ce-MOF within an aqueous system, while realizing partial substitution of the auxiliary ligands and saturation of the CUS. The amount of 2-FBA was negatively correlated with the number of ligand defects, and the consequent decrease in Ce3+content and the increase in the number of ligand linkages also induced crystal structure transformation. The modulation of the defect structure was correlated with the catalytic performance of dicyclopentadiene（DCPD） hydrogenation reaction, in which Ce-MMF0.15, constructed by the modulation of 0.15 mol amount of 2-fluorobenzoic acid, exhibited an optimal ligand defect density and micro-mesoporous structure, enabling almost complete conversion of DCPD at 100 ℃ and 2 MPa. This article also elucidates the correlation between the regulation of defect density and the accessibility of frustrated Lewis pair（FLP） active sites, guiding the application of novel porous intrinsic FLP materials in hydrogenation catalysis.

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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： Oxygen evolution reaction

Dramatical enhancement of circular dichroism in chiral hybrid perovskites via carboxylic hydrogen bond engineering

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Science China Chemistry 2025年

作者： Hang Li Xinling Li Peng Wang Tingting Zhu Ruiqing Li Huang Ye Yaru Geng Hongliang Dai Junhua Luo State Key laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences University of Chinese Academy of Sciences Fujian College University of Chinese Academy of Sciences College of Chemistry Fuzhou University College of Chemistry and Materials Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationJiangxi Normal University

Chiral hybrid perovskites （CHPs） have been regarded as promising candidates for developing chiroptoelectronics ***,circular dichroism （CD）,as one of the most important characteristics to evaluate the chiroptical activity,remains at a comparatively low level in CHPs compared to other chiral materials,which hinders the successful applications of CHPs in stateof-the-art ***,exploring new methods for enhancing CD in CHPs is urgently needed and remains ***,enhanced CD response has been successfully realized via constructing carboxylic hydrogen bonding in chiralachiral mixed cations perovskites （R/S-PPA）2（ABA）PbBr5（2R/2S）(PPA=1-phenylpropylamine,ABA=4-aminobutyric acid).Compared with the prototype （R/S-PPA）PbBr3（1R/1S）,2R/2S provide intimate connections between organic units and inorganic parts via carboxylic hydrogen bonding N–H···O bridge,contributing new chirality transfer paths.A larger inorganic skeletons’helicity in 2R/2S predicts a high degree of chirality ***,2R/2S exhibit significantly enhanced CD response with an anisotropy factor amplified by an order of ***,bright blue circularly polarized luminescence applications are achieved in 2R/*** work systematically investigates the correlation between CD and hydrogen bonding interaction in CHPs,meanwhile providing a new avenue to develop the application potential of chiral materials in chiroptoelectronics.

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Recent progress on photoactive nonprecious transition-metal complexes

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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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Direct Photolithography of WO_(x)Nanoparticles for High‑Resolution Non‑Emissive Displays

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Nano-Micro Letters 2025年第3期17卷 297-309页

作者： Chang Gu Guojian Yang Wenxuan Wang Aiyan Shi Wenjuan Fang Lei Qian Xiaofei Hu Ting Zhang Chaoyu Xiang Yu‑Mo Zhang laboratory of Optoelectronic Information Technology and Devices Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201People’s Republic of China Hangzhou Bay laboratory of Advanced Nano‑Optoelectronic Materials and Devices Qianwan Institute of CNITECHNingbo 315336People’s Republic of China Smart Materials for Architecture Research Lab Innovation Center of Yangtze River DeltaZhejiang UniversityJiaxing 314100People’s Republic of China University of Science and Technology of China Hefei 230026People’s Republic of China State Key Lab of Supramolecular structure and Materials College of ChemistryJilin UniversityChangchun 130012People’s Republic of China

High-resolution non-emissive displays based on electrochromic tungsten oxides(WOx)are crucial for future near-eye virtual/augmented reality interactions,given their impressive attributes such as high environmental stability,ideal outdoor readability,and low energy ***,the limited intrinsic structure of inorganic materials has presented a significant challenge in achieving precise patterning/pixelation at the micron ***,we successfully developed the direct photolithography for WOx nanoparticles based on in situ photo-induced ligand *** strategy enabled us to achieve ultra-high resolution efficiently(line width3600 cycles),as well as promising applications in electronic logos,pixelated displays,flexible electronics,*** success and advancements presented here are expected to inspire and accelerate research and development(R&D)in high-resolution non-emissive displays and other ultra-fine micro-electronics.

关键词： Electrochromic Direct photolithography WOx nanoparticles In situ photo-induced ligand exchange High-resolution displays

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： Energy dispersive spectroscopy

Differential Hydrocarbon Accumulation Controlled by Structural Styles along the Southern and Northern Tianshan Thrust Belt

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Acta Geologica Sinica(English Edition) 2013年第4期87卷 1109-1119页

作者： SONG Yan ZHAO Mengjun FANG Shihu LI Benliang LIU Shaobo ZHUO Qingong Key laboratory of Basin structure and Hydrocarbon Accumulation CNPC State Key laboratory of Petroleum Resource and Prospecting Research Institute of Petroleum Exploration and development PetroChina

The Kuqa and the Southern Junggar foreland thrust belts, which lie to the southern and northern Tianshan, respectively, were formed under a strong compressional tectonic setting. Due to the differential propagation and deformation under the control of the décollement horizon, the structural deformation styles differ in the Kuqa and Southern Junggar thrust belts. Imbricated stacking is developed in the Kuqa thrust belt, forming a piggyback imbricated pattern of faulted anticline and fault-block structural assemblage dominated by salt structures. In contrast, wedge-shaped thrusts are developed in Southern Junggar, mainly forming vertical laminated patterns of multi-wedge-structure stacks strongly influenced by the décollement horizons. The different deformation patterns and structural styles of the north and south of Tian Shan control the contrasting characteristics of hydrocarbon accumulation in the foreland thrust belts of the Kuqa and the Southern Junggar thrust belts, including the variance in the hydrocarbon trap types, pathway systems and hydrocarbon-bearing horizons. Proven by the hydrocarbon accumulation research and exploration achievements, recent exploration targets should focus on sub-salt piggyback imbricated structural patterns in the Kuqa and the deep laminated patterns in the Southern Junggar thrust belt.

关键词： northern and southern TianShan structural style hydrocarbon accumulation,accumulation model

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