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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

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Controlled cationic ring-opening polymerization of L-lactide by organic ion pair: novel approach to isotactic-rich and crystalline polylactide

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science china Chemistry 2025年第1期68卷 394-402页

作者： Zhiqiang Ding Mingqian Wang Zijing Zhou Bin Wang Yuesheng Li Tianjin Key Laboratory of Composite & Functional Materials School of Materials Science and Engineering Tianjin University

Living/controlled cationic ring-opening polymerization （ROP） of L-lactide is a promising approach to isotactic-rich and crystalline poly（L-lactide）.In contrast with the unsubstituted lactones,L-LA can not be polymerized by organic Lewis acids or carbenium ions,and the state of the art in this field is the cationic ROP of L-LA catalyzed by Br?nsted acid/alcohol system via activated monomer ***,we reported the first example of controlled cationic ROP of L-LA by using Meerweintype ion pair[Me3O]+[B（C6F5）4]-as the catalyst.[Me3O]+[B（C6F5）4]-promoted rapid L-LA cationic polymerization in the absence of alcohol,producing isotactic-rich and crystalline PLLA without transesterification and epimerization side *** activated chain end mechanism,involving twice SN2 substitution and configuration-inversion （S→R→S） with the assistance of released Me2O,was proposed and further verified by density functional theory and control *** work expands the catalytic toolbox of isotactic-rich and crystalline polylactide *** represents a unique example of cationic-controlled polymerization of L-LA catalyzed by an organic ion pair.

关键词： organic ion pair controlled cationic ring-opening polymerization activated chain end mechanism isotactic-rich polylactide

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Direct and rapid detection of serum amino acid and monoamine neurotransmitters to assist the diagnosis of panic disorder

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science china Chemistry 2025年第1期68卷 377-384页

作者： Shiwen Liu Xuerui Wan Meng Zhao Jiaqi Wang Weilan Wu Linlin You Yonggui Yuan Qian Xu Rong Gao Key Laboratory of Environmental Medicine Engineering Ministry of Education School of Public Health Southeast University Key Laboratory of Modern Toxicology of Ministry of Education Department of Hygienic Analysis and Detection School of Public HealthNanjing Medical University Department of Psychosomatics and Psychiatry Zhongda Hospital School of Medicine Southeast University

The measurement of amino acid and monoamine neurotransmitters（NTs） in serum plays a central role in the identification and monitoring of clinical panic disorder（PD）. However, the strong polarity and chemical heterogeneity of NTs make direct extraction and rapid detection extremely challenging. Herein, we developed a strategy that integrated solid phase extraction based on magnetic Fe3O4coated with polydopamine（Fe3O4@PDA） and direct analysis of mass spectrometry in real time（DART-MS） for quantification of 10 NTs. We systematically investigated the optimal conditions of this strategy to achieve good accuracy and precision. Compared with existing magnetic solid phase extraction methods for NTs detection in biological samples, this strategy could adsorb more targets while having similar adsorption efficiencies, and the total process time was reduced by an average of 69.42%. We rapidly determined the metabolic abnormality of 6 types of NTs in the serum of PD patients and demonstrated their diagnostic accuracy. In addition, an outstanding feature of PD in which tryptophan was more metabolized by the KYN pathway and the 5-hydroxytryptamine pathway was inhibited could be elucidated by this strategy. Our results highlighted the potential ability of Fe3O4@PDA coupled with DART-MS to assist in the clinical diagnosis of PD.

关键词： neurotransmitters panic disorder magnetic solid phase extraction direct analysis of mass spectrometry in real time

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Potassium ions and cyano group modified g-C3N4 for effective generation of H2O2 through two-electron oxygen reduction

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science china Chemistry 2025年第1期68卷 192-200页

作者： Dongying Wang Shulan Pu Yongmin Chen Ke Lei Yujie Duan Linjiao Mao Xuhui Zeng Xi Luo Yuntao Zhang Yuqin Dong Jin Zhong Zhang Yan Sun School of Mechanical Engineering Chengdu University Department of Chemistry and Biochemistry University of California

Potassium ions （K+） doped graphitic carbon nitride （g-C3N4） was prepared by a thermal etching method using potassium hydroxide （KOH） as an ion *** transform infrared spectroscopy （FTIR） and X-ray photoelectron spectroscopy （XPS）results showed that the generation of the cyano group was detected while introducing K+.under simulated sunlight irradiation,the sample with a K+doping amount of 10%showed the highest hydrogen peroxide （H2O2） generation rate of2,140.2μmol *** apparent quantum yield （AQY） at 400 nm and the solar-to-chemical conversion （SCC） are 4.35%and1.23%,respectively.K+acted as a bridge between g-C3N4layers,which enhanced charge transfer ***,the cyano group enhanced the adsorption capacity of protons （H+） and promoted the yield of *** catalyst exhibited excellent photocatalytic stability based on four-cycle *** addition,a mechanism study showed that superoxide radicals （·O2-）were the most important active species in the reaction *** production of H2O2was achieved through consecutive single-electron *** study deepens the understanding of the oxygen reduction reaction process and opens up a new venue for improving H2O2generation.

关键词： photocatalysis hydrogen peroxide oxygen reduction reaction potassium doping cyano group

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Fine-tuning the spatial allocation of phytohormones for smart canopy, smart breeding, and smart agriculture

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science china Life sciences 2025年第1期68卷 309-310页

作者： Tao Zhou Lin Li national Key Laboratory of Crop Genetic Improvement Huazhong Agricultural University HuBei HongShan Laboratory

The dual challenges of global climate change and population growth have increased demand for higher crop yields per unit area. The innovative technology of smart agriculture aims to synergize breeding, cultivation, and production through the application of biological and informatics technologies. Historically, the “Green Revolution” introduced semidwarf varieties of certain key crops by utilizing mutations affecting gibberellin pathways, which significantly increased planting densities and yields.

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Targets capture by distributed active swarms via bio-inspired reinforcement learning

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science china(Physics,Mechanics & Astronomy) 2025年第1期Mechanics & Astronomy) .卷 210-221页

作者： Kun Xu Yue Li Jun Sun Shuyuan Du Xinpeng Di Yuguang Yang Bo Li Institute of Biomechanics and Medical Engineering Applied Mechanics Laboratory Department of Engineering MechanicsTsinghua University Institute of Nuclear and New Energy Technology Tsinghua University Shanghai Aerospace Control Technology Institute Shanghai Key Laboratory of Aerospace Intelligent Control Technology College of Automation Engineering Nanjing University of Aeronautics and Astronautics

natural swarms arranged from cells to herds are usually decentralized but display intriguing collective intelligence in coordinating individuals across large scales to efficiently achieve their common goals. Learning from nature may provide new strategies for controlling collective dynamics of synthetic swarms to accomplish specific functions. Here, we present a bioinspired computational framework that steers distributed active swarms to collectively capture and merge targets via reinforcement learning. We exploit collective milling structures of natural herds to cage the targets, and adopt a switching control policy inspired by sperms' chiral dynamics to optimize the trajectories of individuals, through which the active swarms can selforganize to enclose single or multiple distant targets in a dynamical, adaptive and scalable manner. There exists a critical swarm size, beyond which the excessive competition between agents would generate large mechanical forces, leading to capture instability but enabling the transition from short-distance to long-distance merging capture of multiple targets. This work provides physical insights into distributed active swarms and could offer a multilevel, decentralized strategy toward controlling swarm robotics in wide applications such as bio-medical devices, machine immunity, and target clearance.

关键词： swarm intelligence robotics multi-tasks artificial intelligence bionics

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Numerical Simulation of Radiation Transport to Improve Microalgae Cultivation in an Air-Lift Photobioreactor

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Journal of Thermal science 2025年第1期34卷 62-76页

作者： ZHANG Xianbin LI Mingjia HuNG Tzuchen ZHANG Zixun Key Laboratory of Thermo-Fluid science and Engineering of Ministry of Education School of Energy and Power EngineeringXi'an Jiaotong University School of Mechanical Engineering Beijing Institute of Technology Department of Mechanical Engineering Taipei University of Technology

A comprehensive numerical model is developed to simulate the growth of microalgae under light/dark cycling *** purpose of this study is to predict the growth rate of Chlorella vulgaris cultivated in photobioreactors(PBRs) in order to improve the light conditions for microalgae and enhance the photosynthetic *** fluid dynamics(CFD) is used to simulate its internal hydrodynamic *** Lagrangian method is employed to track the movement of microalgae *** radiative transfer equation(RTE)is used to obtain light intensity *** combination of light radiation field and microalgae cell motions is used to construct the light history and they are integrated into the model of the photosynthetic units(PSu) to calculate the microalgae growth *** numerical results demonstrate that enhanced light/dark cycling frequency with ordered mixing can promote efficient microalgae *** effect of the vortex flow field generated by the baffles in an air-lift PBR is analyzed for increasing microalgae growth *** using the 1:1 baffle spacing,the biomass production of microalgae is increased by 41.8% compared to the original PBR.

关键词： light distribution particle tracking photobioreactor structure optimization

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Separation of the ionospheric and thermospheric contributions in the data from the Triple Ionosophere Photo Meter onboard the Feng-Yun 3E satellite

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science china Earth sciences 2025年第1期68卷 172-184页

作者： Fang JIANG Tian MAO Jin-Song WANG Xiu-Qing Hu Xiao-Xin ZHANG Liping Fu Nan JIA Tianfang WANG national Space science Center Chinese Academy of Sciences Beijing Key Laboratory of Space Environment Exploration Key Laboratory of Environmental Space Situation Awareness Technology national Satellite Meteorological Center China Meteorological Administration

The Triple Ionosphere Photo Meter （TRIPM） is a far ultraviolet nadir-view photometer that is onboard the secondgeneration,polar-orbiting Chinese meteorological satellite Feng-Yun 3E （FY-3E）,which was launched on July 5,*** has three channels,and each is used to measure different types of emissions:（1） 135.6 nm airglow produced by the recombination of the O+ions and electrons in the absence of sunlight （nighttime channel）;（2） 135.6 nm airglow from the OI when sunlight is present （daytime/dusk-dawn 135.6 nm channel）;and （3） Airglow in the N2LBH of the TRIPM （daytime/dusk-dawn N2LBH channel）.FY-3E is a satellite operating in the early morning ***,the data are mostly distributed on the dawndusk side or at times when the solar zenith angle is relatively *** this study,combined with simulation calculations,the data are *** further explore the application value of the data products,a model is used to separate the ionospheric radiative recombination contribution from the thermosphere photoelectron impact excitation contribution in the data from the daytime/dusk-dawn 135.6 nm *** approach not only improves the accuracy of O/N2derived from the 135.6 nm channel and N2LBH channel but also provides the ionospheric 135.6 nm radiance at the same time as the *** results show that the 135.6 nm radiance originating from the combination of O+and electrons extracted from the measurement data exhibits similar equatorial anomaly peak structure characteristics and seasonal variations as the corresponding GPS total electron content （TEC） *** the other hand,the separated 135.6 nm radiance generated from the thermosphere photoelectron collision excitation does not contain radiative recombination contributions;thus,the ionosphere influence is greatly avoided when the O/N2is obtained.

关键词： Far ultraviolet 135.6 nm emission intensity Photoelectron impact excitation Radiative recombination excitation

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Electrocatalytic cleavage of a lignin β-O-4 model compound and coupling with nitrogen-containing aromatics using Prussian blue analogue-derived nickel–cobalt spinel

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Journal of Energy Chemistry 2025年第1期100卷 628-636页

作者： Yi Qi Xueying Chen Bowen Liu Xuliang Lin Xueqing Qiu Yanlin Qin Guangdong Provincial Key Laboratory of Plant Resources Biorefinery School of Chemical Engineering and Light Industry Guangdong University of Technology Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center Guangdong Basic Research Center of Excellence for Ecological Security and Green Development Guangdong University of Technology

Electrochemical conversion of lignin for the production of high-value heterocyclic aromatic compounds has great *** demonstrate the targeted synthesis and cation modulation of NiCo2O4spinel nanoboxes,synthesized via cation exchange and calcination *** catalysts exhibit excellent efficacy in the electrocatalytic conversion of lignin model compounds,specifically 2-phenoxy-1-phenylethanol,into nitrogen-containing aromatics,achieving high conversion rates and *** catalysts were synthesized via a cation exchange and calcination oxidation process,using Prussian blue nanocubes as *** porous architecture and polymetallic composition of the NiCo2O4spinel demonstrated superior performance in electrocatalytic oxidative coupling,achieving a 99.2 wt%conversion rate of the 2-phenoxy-1-phenylethanol with selectivities of 37.5 wt%for quinoline derivatives and 31.5 wt%for *** innovations include the development of a sustainable one-pot synthesis method for quinoline derivatives,the elucidation of a multistage reaction pathway involving CAO bond cleavage,hydroxyaldol condensation,and CAN bond formation,and a deeper mechanistic understanding derived from DFT *** work establishes a new strategy for lignin valorization,offering a sustainable route to produce high-value nitrogen-containing aromatics from renewable biomass under mild conditions,without the need for additional reagents.

关键词： Spinel Biomass valorization Electrocatalysis Lignin oxidation Coupling

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Effect of order–disorder transition on thermodynamic and electronic properties of σ and χ phases in W–Re alloy: the first-principles calculation

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Tungsten 2025年第1期7卷 195-213页

作者： Zhi-Peng Zhu Dian Jia William Yi Wang Jun-Lei Yin Xing-Yu Gao Shu-Feng Yang Hai-Feng Song Jin-Shan Li State Key Laboratory of Solidification Processing Northwestern Polytechnical University Laboratory of Computational Physics Institute of Applied Physics and Computational Mathematics School of Metallurgical and Ecological Engineering University of Science and Technology Beijing

The Tungsten-Rhenium(W-Re) alloys,celebrated for their high melting point,strength at elevated temperatures,electrical resistivity,and radiation resistance,have been widely utilized in high-temperature components,aerospace,electronics,and nuclear *** constituents of the topologically close-packed(TCP) phases,the sigma phase(σ) and chi phase(χ) formed within W-Re alloys wield considerable influence on the mechanical properties and the stability of the *** calculations were utilized in the present work to explore the structural,thermodynamic,and electronic properties of both ordered and disordered configurations within the σ and χ phases,culminating in a systematic elucidation of the higher phase stability exhibited by the ordered *** is found that the bulk modulus of these two phases is directly proportional to the concentration of Re in the alloy,while the equilibrium volume is inversely *** thermodynamic parameters of the σ and χ phases are calculated via the mean-field potential *** similar trends observed in the isobaric heat capacity,enthalpy increment,and entropy change curves for these two phases suggest they possess comparable thermodynamic *** is noteworthy that the contribution of ionic vibrations predominantly affects the isobaric heat capacity,while the contribution of thermal electronic excitations increases linearly with *** the structure and thermodynamic properties of TCP phases in W-Re alloys at low temperatures has profound significance for optimizing material performance,microstructures features,establishing theoretical foundations,and predicting material behavior.

关键词： First-principles calculations Phase stability TCP phases Thermodynamic properties W–Re alloy

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