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Metal-Organic Frameworks Offering Tunable Binary Active Sites toward HighlyEfficient Urea Oxidation Electrolysis

Research 2022年第4期2022卷 309-320页

作者： Xuefei Xu Qingming Deng hsiao-chien chen Muhammad Humayun Delong Duan Xia Zhang Huachuan Sun Xiang Ao Xinying Xue Anton Nikiforov Kaifu Huo Chundong Wang Yujie Xiong School of Optical and Electronic Information Wuhan National Laboratory for OptoelectronicsOptics Valley LaboratoryHuazhong University of Science and TechnologyWuhan 430074China Physics Department and Jiangsu Key Laboratory for Chemistry of Low-Dimensional Materials Huaiyin Normal UniversityHuaian 223300China Center for Reliability Science and Technologies Chang Gung UniversityTaoyuan33302 TaiwanChina School of Chemistry and Materials Science University of Science and Technology of ChinaHefei230026 AnhuiChina Department of Physics College of ScienceShihezi UniversityXinjang 832003China Department of Applied Physics Ghent UniversityGent 9000Belgium

Electrocatalytic urea oxidation reaction(UOR)is regarded as an effective yet challenging approach for the degradation of urea in wastewater into harmless N2 and CO_(2).To overcome the sluggish kinetics,catalytically active sites should be rationally designed to maneuver the multiple key steps of intermediate adsorption and ***,we demonstrate that metal-organic frameworks(MOFs)can provide an ideal platform for tailoring binary active sites to facilitate the rate-determining steps,achieving remarkable electrocatalytic activity toward ***,the MOF(namely,NiMn_(0.14)-BDC)based on Ni/Mn sites and terephthalic acid(BDC)ligands exhibits a low voltage of 1.317 V to deliver a current density of 10 mA cm^(-2).As a result,a high turnover frequency(TOF)of 0.15 s^(-1) is achieved at a voltage of 1.4 V,which enables a urea degradation rate of 81.87%in 0.33 M urea *** combination of experimental characterization with theoretical calculation reveals that the Ni and Mn sites play synergistic roles in maneuvering the evolution of urea molecules and key reaction intermediates during the UOR,while the binary Ni/Mn sites in MOF offer the tunability for electronic structure and d-band center impacting on the intermediate *** work provides important insights into active site design by leveraging MOF platform and represents a solid step toward highly efficient UOR with MOF-based electrocatalysts.

关键词： solution steps Highly

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Activation of the microstructures in nickel-based bimetallic complexes for aqueous batteries

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Science China Chemistry 2024年

作者： Yichun Su Yanfei Zhang Guoqiang Yuan Yijian Tang Guangxun Zhang Mohsen Shakouri hsiao-chien chen Huijie Zhou Zheng Liu Huan Pang School of Chemistry and Chemical Engineering Yangzhou University Canadian Light Source Inc. University of Saskatchewan Center for Reliability Science and Technologies Chang Gung University Kidney Research Center Department of Nephrology Chang Gung Memorial Hospital Institute of Technology for Carbon Neutralization Yangzhou University State Key Laboratory of Coordination Chemistry Nanjing University

The full utilization of active metal sites is meaningful for enhancing the application of materials in the energy storage field. In this study, a nickel-based nanosphere（NiSA-SSA-Co） precursor was obtained via effective doping based on a dual-ligand complex. With thermal activation, the pore microstructure of the precursor was modulated, and a transition state complex（NiSASSA-Co-350） was fabricated. NiSA-SSA-Co-350 not only retains part of the framework structure, but also fully exposes the metal nodes and enhances the efficiency of the active sites. NiSA-SSA-Co-350 exhibits optimal conductivity and intrinsic reactivity when applied as an electrode material for nickel-zinc batteries（NZBs）. In contrast to the precursor, NiSA-SSA-Co-350with large specific surface area shows a higher specific capacity(0.30 mAh cm-2at 3 mA cm-2). This work hopefully provides a new perspective on the study of nanomaterial porosity in energy storage applications.

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Highly efficient overall urea electrolysis via single-atomically active centers on layered double hydroxide

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Science Bulletin 2022年第17期67卷 1763-1775页

作者： Huachuan Sun Linfeng Li hsiao-chien chen Delong Duan Muhammad Humayun Yang Qiu Xia Zhang Xiang Ao Ying Wu Yuanjie Pang Kaifu Huo Chundong Wang Yujie Xiong School of Optical and Electronic Information Wuhan National Laboratory for OptoelectronicsOptics Valley LaboratoryHuazhong University of Science and TechnologyWuhan 430074China Center for Reliability Science and Technologies Chang Gung UniversityTaoyuan 33302China Kidney Research Center Department of NephrologyChang Gung Memorial HospitalLinkouTaoyuan 33305China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China Pico Center SUSTech Core Research FacilitiesSouthern University of Science and TechnologyShenzhen 518055China College of Chemistry and Chemical Engineering Tarim UniversityAlaer 843300China

Anodic urea oxidation reaction(UOR)is an intriguing half reaction that can replace oxygen evolution reaction(OER)and work together with hydrogen evolution reaction(HER)toward simultaneous hydrogen fuel generation and urea-rich wastewater purification;however,it remains a challenge to achieve overall urea electrolysis with high ***,we report a multifunctional electrocatalyst termed as Rh/Ni V-LDH,through integration of nickel-vanadium layered double hydroxide(LDH)with rhodium single-atom catalyst(SAC),to achieve this *** electrocatalyst delivers high HER mass activity of0.262 A mg^(-1) and exceptionally high turnover frequency(TOF)of 2.125 s^(-1) at an overpotential of100 m ***,exceptional activity toward urea oxidation is addressed,which requires a potential of 1.33 V to yield 10 mA cm^(-2),endorsing the potential to surmount the sluggish *** splendid catalytic activity is enabled by the synergy of the Ni V-LDH support and the atomically dispersed Rh sites(located on the Ni-V hollow sites)as evidenced both experimentally and *** selfsupported Rh/Ni V-LDH catalyst serving as the anode and cathode for overall urea electrolysis(1 mol L^(-1) KOH with 0.33 mol L^(-1) urea as electrolyte)only requires a small voltage of 1.47 V to deliver 100 mA cm^(-2) with excellent *** work provides important insights into multifunctional SAC design from the perspective of support sites toward overall electrolysis applications.

关键词： Single-atomically active centers Layer double hydroxide Hydrogen evolution reaction Overall urea electrolysis High turnover frequency

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Halogen composition and heterogeneity in the continental lithospheric mantle

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Science China Earth Sciences 2025年第1期68卷 310-314页

作者： Chunfei chen State Key Laboratory of Geological Processes and Mineral Resources School of Earth Sciences China University of Geosciences

1. Introduction Halogens, including fluorine(F), chlorine(Cl), bromine(Br), and iodine(I), are highly mobile and water-soluble elements that can become significantly enriched in melts and fluids. In fluids and melts, halogens react with nearly all metals and readily form complexes with metal cations, significantly influencing the distribution of metal elements between different phases. Therefore, halogens play a crucial role in the migration, enrichment, and mineralization of key metals in the lithosphere(Weis et al., 2012; Liu et al., 2024).

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Cyano migration-mediated radical-polar crossover cyclopropanation

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Science China Chemistry 2025年第1期68卷 241-248页

作者： Ziqiang Wang Yasu chen Jie Li chen Zhu Key Laboratory of Organic Synthesis of Jiangsu Province College of Chemistry Chemical Engineering and Materials ScienceSoochow University Frontiers Science Center for Transformative Molecules Zhangjiang Institute for Advanced Study and Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Shanghai Jiao Tong University

We report a novel cyano migration-mediated radical-polar crossover process, whereby both the sulfonylcyanation of aliphatic alkenes and the formation of cyclopropanes are concurrently achieved. This transformation yields a diverse array of multisubstituted cyclopropanes under mild photocatalytic conditions. Mechanistic studies elucidate that the reaction proceeds via intramolecular nucleophilic substitution, leading to the formation of the cyclopropane derivatives.

关键词： cyclopropanation cyano migration radical-polar crossover radical reactions

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Two paths, one goal: mechanism of calcium homeostasis to balance plant growth and immunity

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Science China Life Sciences 2025年第1期68卷 306-308页

作者： Aziz Ul Ikram Yanping Jing Huan chen Jian chen International Genome Center Jiangsu University Joint Center for Single Cell Biology School of Agriculture and BiologyShanghai Jiao Tong University

Calcium(Ca2+) is an essential nutrient and a cellular signal in plants. The level of free Ca2+in the apoplast is ～10,000-fold higher than that in the cytoplasm at the resting state. This large Ca2+level gradient across the membrane between the interior and exterior can cause Ca2+overload and toxicity. Plants have evolved mechanisms to export Ca2+out of the cytoplasm or store it in intracellular organelles, such as endoplasmic reticulum（ER）, mitochondria, and vacuole.

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Efficient photocatalytic reduction of CO2 to formate by a molecular noble metal-free system

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Science China Chemistry 2025年第1期68卷 152-156页

作者： Lihua Zhang Lingjing chen Huatian Shi Yue Wei Gui chen Tai-Chu Lau School of Environment and Civil Engineering Research Center for Eco-environmental Engineering Dongguan University of Technology Department of Chemistry and Institute of Molecular Functional Materials City University of Hong Kong

Reducing CO2to carbon-neutral solar fuels can not only alleviate the energy demand but also mitigate the greenhouse *** present,developing an efficient non-noble metal photo/electrocatalytic system for converting CO2to a specific product beyond CO is still a big ***,we report a new cobalt complex bearing 2,2′-bi-1,10-phenanthroline ligand that can photocatalytically reduce CO2to formate （HCOO-）.Turnover number （TON） for HCOO-up to 677 with 99%selectivity can be achieved using organic dyes purpurin as photosensitizer and 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole （BIH） as sacrificial reductant in a CO2-saturated NMP/TEA （v/v,3:1） solution under visible light *** potential electrolysis at-1.41 V （***/Ag Cl） in the presence of 12 m M Et3NHBF4also produced HCOO-with Faradaic efficiency of 39%.Spectroscopic and electrochemical studies suggest that a[CoI-H]species is the key intermediate for CO2reduction.

关键词： photocatalysis noble metal-free CO2 reduction formate cobalt hydride

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Toward understanding the role of genomic repeat elements in neurodegenerative diseases

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Neural Regeneration Research 2025年第3期20卷 646-659页

作者： Zhengyu An Aidi Jiang Jingqi chen Institute of Science and Technology for Brain-Inspired Intelligence Fudan UniversityShanghaiChina MOE Frontiers Center for Brain Science Fudan UniversityShanghaiChina MOE Key Laboratory of Computational Neuroscience and Brain-Inspired Intelligence Fudan UniversityShanghaiChina Zhangjiang Fudan International Innovation Center ShanghaiChina

Neurodegenerative diseases cause great medical and economic burdens for both patients and society;however, the complex molecular mechanisms thereof are not yet well understood. With the development of high-coverage sequencing technology, researchers have started to notice that genomic repeat regions, previously neglected in search of disease culprits, are active contributors to multiple neurodegenerative diseases. In this review, we describe the association between repeat element variants and multiple degenerative diseases through genome-wide association studies and targeted sequencing. We discuss the identification of disease-relevant repeat element variants, further powered by the advancement of long-read sequencing technologies and their related tools, and summarize recent findings in the molecular mechanisms of repeat element variants in brain degeneration, such as those causing transcriptional silencing or RNA-mediated gain of toxic function. Furthermore, we describe how in silico predictions using innovative computational models, such as deep learning language models, could enhance and accelerate our understanding of the functional impact of repeat element variants. Finally, we discuss future directions to advance current findings for a better understanding of neurodegenerative diseases and the clinical applications of genomic repeat elements.

关键词： Alzheimer's disease ataxia deep learning long-read sequencing neurodegeneration neurodegenerative diseases Parkinson's disease repeat element structural variant

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Fabrication and Mechano-sensing Characteristics of Bending Polypyrrole Actuator

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Journal of Wuhan University of Technology(Materials Science) 2025年第1期40卷 240-245页

作者： chen Jinyou HU Wei School of Automotive Engineering Hunan Financial&Industrial Vocational-technical CollegeHengyang 421002China College of Mechanical and Electrical Engineering Hunan Agricultural UniversityChangsha 410128China

To prepare a conductive polymer actuator with decent performance,a self-built experimental platform for the preparation of polypyrrole film is *** of the essential goals is to examine the mechanical characteristics of the actuator in the presence of various combinations of process parameters,combined with the orthogonal test method of"four factors and three levels".The bending and sensing characteristics of actuators of various sizes are methodically examined using a self-made bending polypyrrole *** functional relationship between the bending displacement and the output voltage signal is established by studying the characteristics of the actuator sensor subjected to various degrees of *** experimental results reveal that the bending displacement of the actuator tip almost exhibits a linear variation as a function of length and *** the voltage reaches 0.8 V,the bending speed of the actuator tends to be ***,the mechanical properties of the self-assembled polypyrrole actuator are verified by the design and fabrication of the microgripper.

关键词： conductive polymer polypyrrole mechanical characteristics actuators sensing characteristics

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Miyaoka-type inequalities for terminal threefolds with nef anti-canonical divisors

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Science China Mathematics 2025年第1期68卷 1-18页

作者： Masataka Iwai chen Jiang Haidong Liu Department of Mathematics Graduate School of ScienceOsaka University Shanghai Center for Mathematical Sciences & School of Mathematical Sciences Fudan University Department of mathematics Sun Yat-sen University

In this paper,we study Miyaoka-type inequalities on Chern classes of terminal projective 3-folds with nef anti-canonical *** X be a terminal projective 3-fold such that-KXis *** show that if c1（X） · c2（X）≠0,then c1（X） · c2（X） ≥ 1/252;if further X is not rationally connected,then c1（X） · c2（X） ≥ 4/5 and this inequality is *** order to prove this,we give a partial classification of such varieties along with many *** also study the nonvanishing of c1（X）dim X-2· c2（X） for terminal weak Fano varieties and prove a Miyaoka-Kawamata-type inequality.

关键词： terminal threefolds Miyaoka-type inequality boundedness

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