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Mechanism regulation over dual-atom catalyst enables high-performance oxidative alcohol esterification

Science Bulletin 2025年第1期70卷 78-89页

作者： Ce Liu Teng Li Xingchao Dai Jian Zhao Liping Zhang Xinjiang Cui State key laboratory of low carbon Catalysis and carbon Dioxide Utilization State Key Laboratory for Oxo Synthesis and Selective OxidationLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China University of Chinese Academy of Sciences Beijing 100049China

The development of heterogeneous catalysts with well-defined uniform isolated or multiple active sites is of great importance for understanding catalytic performances and studying reaction ***,we present a CoCu dual-atom catalyst(CoCu-DAC)where bonded Co-Cu dual-atom sites are embedded in N-doped carbon matrix with a well-defined Co(OH)CuN_(6)*** CoCu-DAC exhibits higher catalytic activity and selectivity than the Co single-atom catalyst(Co-SAC)and Cu single-atom catalyst(CuSAC)counterparts in the catalytic oxidative esterification of alcohols and a variety of methyl and alkyl esters have been successfully *** studies reveal that the activation energy(29.7 kJ mol^(-1))over CoCu-DAC is much lower than that over Co-SAC(38.4 kJ mol^(-1))and density functional theory(DFT)studies disclose that two different mechanisms are regulated over CoCu-DAC and Co-SAC/Cu-SAC in three-step esterification of *** bonded Co-Cu and adjacent N species efficiently catalyze the elementary reactions of alcohol dehydrogenation,O2activation and ester formation,*** stepwise alkoxy pathway(O-H and C-H scissions)is preferred for both alcohol dehydrogenation and ester formation over CoCu-DAC,while the progressive hydroxylalkyl pathway(C-H and O-H scissions)for alcohol dehydrogenation and simultaneous hemiacetal dehydrogenation are favored over Co-SAC and *** peaks in the Fourier transform infrared spectroscopy analysis may confirm the formation of the metal-C intermediate and the hydroxylalkyl pathway over Co-SAC.

关键词： Dual-atom catalysts Oxidative esterification Mechanism regulation Alcohol

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Interfacial amine-assisted electrodeposition of superhydrophilic/superaerophobic metal hydroxides for robust oxygen evolution catalysis

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Science China Chemistry 2025年

作者： Qing Chen keyu Wang Shiyi Li Yixing Wang Linfeng Lei Minghui Zhu Linzhou Zhuang Zhi Xu State key laboratory of chemical engineering School of Chemical Engineering East China University of Science and Technology Suzhou laboratory

The oxygen evolution reaction（OER） is crucial for the electrocatalytic water electrolysis into oxygen and hydrogen, but the fourelectron transfer process hinders the OER dynamics. To realize the highly efficient water splitting, the nonprecious metal-based electrodes that can optimize the adsorption energy of intermediates and generate H2with low overpotential and robust stability are essential. Herein, we report a surface modification strategy to grow the trimetallic FeCoNi hydroxide on the amine linkersgrafted carbon cloth（CC-NH2@FeCoNi） by electro-deposition. CC-NH2@FeCoNi possesses a superhydrophilic/superaerophobic surface, which could significantly enhance the mass transfer, and meanwhile promote the in situ generation of MOOH active species. Meanwhile, the superhydrophilic surface could facilitate the adsorption of abundant OH-ions, and repel the Cl-ions via electrostatic repulsive force during seawater oxidation. Consequently, compared with the CC@FeCoNi that grown on the pure CC（320 mV）, the CC-NH2@FeCoNi needs an obviously smaller overpotential of 270 mV to achieve a current density of 100 mA cm-2, and meanwhile it exhibits a superior durability for 100 h at a current density of 200 mA cm-2in both alkaline water and seawater. This strategy could be even applied universally in the preparation of other nonprecious metal hydroxides for efficient OER catalysis.

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Meteorological effects on sources and future projection of nitrogen deposition to lakes in China

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Journal of Environmental Sciences 2025年第5期151卷 100-112页

作者： Cheng Shi Hao Guo Xue Qiao Jingsi Gao Ying Chen Hongliang Zhang Department of Biological and Ecological engineering Oregon State UniversityCorvallisOR 97331USA State key laboratory of Organic Geochemistry Guangzhou Institute of GeochemistryChinese Academy of SciencesGuangzhou 510640China Institute of New energy and low-carbon Technology Sichuan UniversityChengdu 610065China engineering Technology Development Center of Urban Water Recycling Shenzhen PolytechnicShenzhen 518055China Shanghai key laboratory of Atmospheric Particle Pollution and Prevention Department of Environmental Science and EngineeringFudan UniversityShanghai 200438China IRDR ICoE on Risk Interconnectivity and Governance on Weather/Climate Extremes Impact and Public Health Fudan UniversityShanghai 200438China

Lake ecosystems are extremely sensitive to nitrogen growth,which leads to water quality degradation and ecosystem health *** depositions,as one of the main sources of nitrogen in water,are expected to change under future climate change ***,it remains not clear how nitrogen deposition to lakes respond to future meteorological *** this study,a source-oriented version of Community Multiscale Air Quality(CMAQ)Model was used to estimate nitrogen deposition to 263 lakes in 2013 and under three RCP scenarios(4.5,6.0 and 8.5)in *** total deposition of 58.2 Gg nitrogen was predicted for all lakes,with 23.3 Gg N by wet deposition and 34.9 Gg N by dry *** and ammonium in aerosol phase are the major forms of wet deposition,while NH3 and HNO_(3)in gas phase are the major forms of dry *** emissions contribute to 57%of wet deposition and 44%of dry *** future meteorological conditions,wet deposition is predicted to increase by 5.5%to 16.4%,while dry deposition would decrease by 0.3%to 13.0%.Changes in wind speed,temperature,relative humidity(RH),and precipitation rates are correlated with dry and wet deposition *** predicted changes in deposition to lakes driven by meteorological changes can lead to significant changes in aquatic chemistry and ecosystem *** from future emission scenarios,different climate scenarios should be considered in future ecosystem health evaluation in response to nitrogen deposition.

关键词： Deposition Nitrogen Lakes CMAQ Meteorological variations

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Bandgap characteristics analysis and graded design of a novel metamaterial for flexural wave suppression

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Applied Mathematics and Mechanics(English Edition) 2025年第1期46卷 1-24页

作者： Fan YANG Zhaoyang MA Xingming GUO Shanghai key laboratory of Mechanics in energy engineering Shanghai Institute of Applied Mathematics and Mechanics School of Mechanics and Engineering ScienceShanghai University Shanghai Institute of Aircraft Mechanics and Control

A novel elastic metamaterial is proposed with the aim of achieving lowfrequency broad bandgaps and bandgap regulation. The band structure of the proposed metamaterial is calculated based on the Floquet-Bloch theorem, and the boundary modes of each bandgap are analyzed to understand the effects of each component of the unit cell on the bandgap formation. It is found that the metamaterials with a low elastic modulus of ligaments can generate flexural wave bandgaps below 300 Hz. Multi-frequency vibrations can be suppressed through the selective manipulation of bandgaps. The dual-graded design of metamaterials that can significantly improve the bandgap width is proposed based on parametric studies. A new way that can regulate the bandgap is revealed by studying the graded elastic modulus in the substrate. The results demonstrate that the nonlinear gradient of the elastic modulus in the substrate offers better bandgap performance. Based on these analyses, the proposed elastic metamaterials can pave the way for multi-frequency vibration control, low-frequency bandgap broadening, and bandgap tuning.

关键词： flexural wave bandgap graded design local resonance metamaterial O421+.5

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Flexible molecules dedicate to release strain of inverted inorganic perovskite solar cell

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Journal of energy Chemistry 2025年第1期100卷 87-93页

作者： Hongrui Sun Sanlong Wang Pengyang Wang Yali Liu Shanshan Qi Biao Shi Ying Zhao Xiaodan Zhang Institute of Photoelectronic Thin Film Devices and Technology Renewable Energy Conversion and Storage CenterState Key Laboratory of Photovoltaic Materials and CellsNankai UniversityTianjin 300350China key laboratory of Photoelectronic Thin Film Devices and Technology of Tianjin Tianjin 300350China Haihe laboratory of Sustainable chemical Transformations Tianjin 300192China engineering Research Center of Thin Film Photoelectronic Technology of Ministry of Education Tianjin 300350China Collaborative Innovation Center of chemical Science and engineering(Tianjin) Tianjin 300072China

The tensile strain in inorganic perovskite films induced by thermal annealing is one of the primary factors contributing to the inefficiency and instability of inorganic perovskite solar cells(IPSCs),which reduces the defect formation ***,a flexible molecule 5-maleimidovaleric acid(5-MVA)was introduced as a strain buffer to release the residual strain of CsPbI_(2.85)Br_(0.15)*** anhydride and carboxyl groups in 5-MVA interact strongly with the uncoordinated Pb^(2+)through Lewis acid-base reaction,thus tightly“pull”the perovskite *** in-between soft carbon chain increased the structural flexibility of CsPbI_(2.85)Br_(0.15)perovskite materials,which effectively relieved the intrinsic internal strain of CsPbI_(2.85)Br_(0.15),resisted the corrosion of external strain,and also reduced the formation of defects such as VIand *** addition,the introduction of 5-MVA improved crystal quality,passivated residual defects,and narrowed energy level ***,power conversion efficiency(PCE)of NiOxbased inverted IPSCs increased from 19.25%to 20.82%with the open-circuit voltage enhanced from 1.164 V to 1.230 *** release of strain also improved the stability of CsPbI_(2.85)Br_(0.15)perovskite films and devices.

关键词： Inverted inorganic perovskite solar cells Flexible molecules Strain release Crystallization energy barrier High PCE

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Gas-Solid Flow,Combustion Characteristics,and Gas Emissions in a 75 t/h CFB Boiler Based on the CPFD Method

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Journal of Thermal Science 2025年第1期34卷 323-336页

作者： HUANG Xiankun BAI Zhang ZHU Xiaoli WANG Shuoshuo MU Lin GONG Liang College of New energy China University of Petroleum(East China)Qingdao 266580China key laboratory of Ocean energy Utilization and energy Conservation of Ministry of Education School of Energy and Power EngineeringDalian University of TechnologyDalian 116024China

A 3D simulation using Computational Particle Fluid Dynamics(CPFD)methods was used to calculate coal combustion in a 75 t/h industrial-scale circulating fluidized bed(CFB)*** characteristics,gas-solid flow characteristics,and gaseous pollutant emissions of CFB boilers from combustion ignition to stable operation were systematically evaluated in this *** show that the temperature distribution is relatively uniform throughout the *** the combustion process unfolds within the boiler,the gas composition curve strikingly portrays the inverse correlation between CO_(2)and O_(2)*** the combustion reaction progresses,it becomes evident that the concentration of CO_(2)progressively increases,while the concentration of O_(2)concurrently *** inverse relationship underscores the fundamental combustion reaction,where carbon-based fuels react with oxygen to produce carbon dioxide and release ***,a comprehensive analysis has revealed that,from ignition to stable combustion,both nitric oxide(NO)and sulfur dioxide(SO_(2))emissions exhibit a declining *** reduction in pollutant generation is attributed to the improvement in combustion *** complete combustion leads to lower levels of unburned hydrocarbons,which are prone to NO ***,the sulfur content in the fuel is more efficiently oxidized to sulfur trioxide(SO_(3))or bound in sulfates,reducing SO_(2)*** steady state in the simulation,the SO_(2)mass flow rate varies significantly with the furnace height,gradually increasing from 0.07 kg·s^(-1)at 4 m at the bottom of the furnace to a peak of 0.078 kg·s^(-1)at 8 m in the center,and then decreasing to 0.06 kg·s^(-1)at 20m at the top of the furnace.

关键词： circulating fluidized bed particle flow combustion CPFD modeling

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Interfacial Zn^(2+)-solvation regulator towards reversible and stable Zn anode

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Journal of energy Chemistry 2025年第1期100卷 684-692页

作者： Miao Zhou Xiongbin Luo Hang Li Shan Guo Zhuang Tong Xiaotao Zhou Xu Li Zhaohui Hou Shuquan Liang Guozhao Fang College of Mechanical engineering Key Laboratory of Hunan Province for Advanced Carbon-based Functional MaterialsHunan Institute of Science and TechnologyYueyang 414006HunanChina School of Materials Science and engineering Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan ProvinceCentral South UniversityChangsha 410083HunanChina College of Materials and Metallurgy Guizhou UniversityGuiyang 550000GuizhouChina National energy Metal Resources and New Materials key laboratory Central South UniversityChangsha 410083HunanChina

Aqueous zinc-ion batteries (AZIBs) are fundamentally challenged by the instability of the electrode/electrolyte interface,predominantly due to irreversible zinc (Zn) deposition and hydrogen ***,the intricate mechanisms behind the electrochemical discrepancies induced by interfacial Zn^(2+)-solvation and deposition behavior demand comprehensive *** molecules endowed with special functional groups (such as hydroxyl,carboxyl,etc.) have the potential to significantly optimize the solvation structure of Zn^(2+)and regulate the interfacial electric double layer (EDL).By increasing nucleation overpotential and decreasing interfacial free energy,these functional groups facilitate a lower critical nucleation radius,thereby forming an asymptotic nucleation model to promote uniform Zn ***,this study presents a pioneering approach by introducing trace amounts of n-butanol as solvation regulators to engineer the homogenized Zn (H-Zn) anode with a uniform and dense *** interfacial reaction and structure evolution are explored by in/ex-situ experimental techniques,indicating that the H-Zn anode exhibits dendrite-free growth,no by-products,and weak hydrogen evolution,in sharp contrast to the bare ***,the H-Zn anode achieves a remarkable Zn utilization rate of approximately 20% and simultaneously sustains a prolonged cycle life exceeding 500 ***,the H-Zn//NH_(4)V_(4)O^(10)(NVO) full battery showcases exceptional cycle stability,retaining 95.04%capacity retention after 400 cycles at a large current density of 5 A g^(-1).This study enlightens solvation-regulated additives to develop Zn anode with superior utilization efficiency and extended operational lifespan.

关键词： Aqueous zinc-ion batteries Zn^(2+)-solvation structure Interfacial reaction Asymptotic nucleation model Reversible and stable Zn anode

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Development of ESIPT-based specific fluorescent probes for bioactive species based on the protection-deprotection of the hydroxyl

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Chinese chemical Letters 2025年第2期36卷 49-56页

作者： Haixian Ren Yuting Du Xiaojing Yang Fangjun Huo Le Zhang Caixia Yin Department of Chemistry Xinzhou Normal University Research Institute of Applied Chemistry Shanxi University Department of Chemistry The University of Texas at Austin key laboratory of chemical Biology and Molecular engineering of Ministry of Education Key Laboratory of Materials for Energy Conversion and Storage of Shanxi Province Institute of Molecular ScienceShanxi University

Excited-state intramolecular proton-transfer (ESIPT) based fluorescence probes are particularly attractive due to their unique properties including environmental sensitivity, a large Stokes shift, and potential for ratiometric sensing. In general, ESIPT-based fluorophore incorporates an intramolecular hydrogen bonding interaction between a hydrogen bond donor (–OH and NH2are common) and a hydrogen bond acceptor(C=N and C=O). More, protection–deprotection of hydroxyl group as hydrogen bond donor could induce an off-on switch of ESIPT-based emission. Therefore, protection–deprotection of hydroxyl group has been the widely used strategy to design fluorescent probes, where the potential key issue is selecting a protective group that can specifically leave in the presence of the target analyte. In this review, we mainly summarize the specific protecting groups (sites) and deprotection mechanisms for biologically important species (including reactive sulfur species (RSS), reactive oxygen species (ROS), enzymes, etc.), and analyze the advantages and disadvantages of different protection mechanisms from some aspects including probe stability, selectivity, response rate and assay system, etc. Based on the aforementioned, we further point out the current challenges and the potential future direction for developing ESIPT-based probes.

关键词： Bioimaging ESIPT Fluorescence probe Protection-deprotection Specificity

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CO hydrogenation conversion driven by micro-environments of active sites over iron carbide catalysts

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Green energy & Environment 2025年第2期10卷 367-373页

作者： Nan Song Xingxing Li Ebtihal Abograin Wenyao Chen Junbo Cao Jing Zhang De Chen Xuezhi Duan Xinggui Zhou State key laboratory of chemical engineering East China University of Science and Technology130 Meilong RoadShanghai200237China Department of chemical engineering Norwegian University of Science and TechnologyTrondheim7491Norway

Essentially clearing the structure-activity relationship between iron carbide catalysts involving multiple active centers to understand the reaction mechanism of CO hydrogenation conversion process is still a great ***,two main micro-environment factors,namely electronic properties and geometrical effects were found to have an integrated effect on the mechanism of CO hydrogenation conversion,involving active sites on multiple crystal *** Bader charge of the surface Fe atoms on the active sites had a guiding effect on the CO activation pathway,while the spatial configuration of the active sites greatly affected the energy barriers of CO *** the defective surfaces were more conducive to CO activation,the defective sites were not the only sites to dissociate CO,as CO always tended to dissociate in a wider *** synergistic effect of the micro-environment also occurred during the CO conversion *** C atoms on relatively flat configurations were more likely to form methane,while the electronic properties of the active sites could effectively describe the C-C coupling process,as well as distinguish the coupling mechanisms.

关键词： Micro-environment CO hydrogenation conversion Electronic property Local environment Synergistic effect

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Sulfur atom occupying surface oxygen vacancy to boost the charge transfer and stability for aqueous Bi2O3 electrode

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Journal of energy Chemistry 2025年第2期101卷 751-759页

作者： Guangmin Yang Jianyan Lin Guanwu Li Tian Li Dong Wang Weitao Zheng College of Physics Changchun Normal University School of Materials Science and engineering Northwestern Polytechnical University key laboratory of Automobile Materials of MOE School of Materials Science and Engineering and Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials Jilin University

Oxygen vacancies（Ov） within metal oxide electrodes can enhance mass/charge transfer dynamics in energy storage ***,construction of surface Ovoften leads to instability in electrode structure and irreversible electrochemical reactions,posing a significant *** overcome these challenges,atomic heterostructures are employed to address the structural instability and enhance the mass/charge transfer dynamics associated with phase conversion mechanism in aqueous electrodes,Herein,we introduce an atomic S-Bi2O3heterostructure(sulfur（S） anchoring on the surface Ovof Bi2O3).The integration of S within Bi2O3lattice matrix triggers a charge imbala nce at the heterointerfaces,ultimately resulting in the creation of a built-in electric field（BEF）.Thus,the BEF attracts OH-ions to be adsorbed onto Bi within the regions of high electron cloud overlap in S-Bi2O3,facilitating highly efficient charge ***,the anchored S plays a pivotal role in preserving structural integrity,thus effectively stabilizing the phase conversion reaction of *** a result,the S-Bi2O3electrode achieves72.3 mA h g-1at 10 A g-1as well as high-capacity retention of 81.9% after 1600 *** innovative SBi2O3design presents a groundbreaking approach for fabricating electrodes that exhibit efficient and stable mass and charge transfer ***,it enhances our understanding of the underlying reaction mechanism within energy storage electrodes.

关键词： Anchoring effect Atomic heterostructure Charge/mass transfer Oxygen vavancy Structural integrity

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