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Highly efficient pH-universal hydrogen evolution reaction catalyzed by rapidly reconstructed bimetallic cobalt-molybdenum alloy cuboids arrays

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Nano Research 2024年第8期17卷 6977-6983页

作者： Daolian liu Zihao Wang Yan Zhang Haiqing zhou Yong Zhang Dongyang Li fang Yu Key Laboratory of Low-Dimensional Quantum Structures and Quantum Control of Ministry of Education Key Laboratory for Matter Microstructure and Function of Hunan ProvinceDepartment of Physics and Synergetic Innovation Center for Quantum Effects and ApplicationsHunan Normal UniversityChangsha 410081China State Key Laboratory of Marine Resource Utilization in South China Sea and Department of Materials Science and EngineeringHainan UniversityHaikou 570228China Institute of Interdisciplinary Studies Hunan Normal UniversityChangsha 410081China

Given the inherent potential of seawater,industrial wastewater,and residential water as inherent feedstocks for hydrogen production through water electrolysis,there is a critical demand for the exploration of robust and stable hydrogen-evolving catalysts that can operate effectively across a diverse range of pH ***,the pursuit of hydrogen-evolving electrocatalysts that demonstrate both good stability and high efficiency over a wide pH range remains a formidable *** we report the rational design and synthesis of an outstanding nanoporous hybrid electrocatalyst consisting of intermetallic cobalt-molybdenum alloy particles anchoring on MoO2 cuboid arrays,which demands very low overpotentials of 72,123 and 134 mV to deliver a current density of−100 mA·cm^(−2)for hydrogen evolution reaction under alkaline,neutral and acidic conditions,*** catalytic activities are superior to most non-precious-metal-based catalysts documented in the literatures,and are even comparable to noble metal *** particular,this alloy electrocatalyst exhibits excellent stability at 50 or 300 mA·cm^(−2)without obvious activity degradation,which is further supported by the undetectable changes in the surface chemical valence states on the basis of in-situ X-ray photoelectron spectroscopic *** study provides an innovative strategy for the design and synthesis of effective non-noble intermetallic catalysts for pH-universal hydrogen evolution over a wide pH range.

关键词： electrocatalyst hydrogen evolution reaction pH-universal non-noble water splitting

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Removal of Cr(Ⅵ)by glutaraldehyde-crosslinked chitosan encapsulating microscale zero-valent iron:Synthesis,mechanism,and longevity

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Journal of Environmental Sciences 2024年第8期142卷 115-128页

作者： Yijun Duan fang liu Xiang liu Miao Li School of Environment Tsinghua UniversityBeijing 100084China Transportation Institute of Inner Mongolia University Hohhot 010070China

Microscale zero-valent iron(mZVI)has shown great potential for groundwater Cr(Ⅵ)***,low Cr(Ⅵ)removal capacity caused by passivation restricted the wide use of *** prepared mZVI/GCS by encapsulating mZVI in a porous glutaraldehydecrosslinked chitosan matrix,and the formation of the passivation layer was alleviated by reducing the contact between zero-valent iron *** average pore diameter of mZVI/GCS was 8.775 nm,which confirmed the mesoporous characteristic of this *** of batch experiments demonstrated that mZVI/GCS exhibited high Cr(Ⅵ)removal efficiency in a wide range of pH(2-10)and temperature(5-35℃).Common groundwater coexisting ions slightly affected m ZVI/*** material showed great reusability,and the average Cr(Ⅵ)removal efficiency was 90.41%during eight *** this study,we also conducted kinetics and isotherms ***-second-order model was the most matched kinetics *** Cr(Ⅵ)adsorption process was fitted by both Langmuir and Freundlich isotherms models,and the maximum Langmuir adsorption capacity of m ZVI/GCS reached243.63 mg/g,which is higher than the adsorption capacities of materials reported in most of the previous ***,the column capacity for Cr(Ⅵ)removal of a mZVI/GCS-packed column was 6.4 times higher than that of a mZVI-packed column in a 50-day ***,mZVI/GCS with a porous structure effectively relieved passivation problems of mZVI and showed practical application prospects as groundwater Cr(Ⅵ)remediation material with practical application prospects.

关键词： Chitosan Glutaraldehyde mZVI Cr(Ⅵ) Groundwater

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The role and applications of extracellular vesicles in osteoporosis

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Bone Research 2024年第1期12卷 62-77页

作者： Fei fang Jie Yang Jiahe Wang Tiantian Li Erxiang Wang Demao Zhang Xiaoheng liu Chenchen zhou Institute of Biomedical Engineering West China School of Basic Medical Sciences&Forensic MedicineSichuan UniversityChengdu 610041China State Key Laboratory of Oral Diseases National Clinical Research Center for Oral DiseasesWest China Hospital of StomatologySichuan UniversityChengdu 610041China

Osteoporosis is a widely observed condition characterized by the systemic deterioration of bone mass and microarchitecture,which increases patient susceptibility to fragile *** intricate mechanisms governing bone homeostasis are substantially impacted by extracellular vesicles(EVs),which play crucial roles in both pathological and physiological *** derived from various sources exert distinct effects on ***,EVs released by osteoblasts,endothelial cells,myocytes,and mesenchymal stem cells contribute to bone formation due to their unique cargo of proteins,miRNAs,and ***,EVs secreted by osteoclasts and immune cells promote bone resorption and inhibit bone ***,the use of EVs as therapeutic modalities or biomaterials for diagnosing and managing osteoporosis is ***,we review the current understanding of the impact of EVs on bone homeostasis,including the classification and biogenesis of EVs and the intricate regulatory mechanisms of EVs in ***,we present an overview of the latest research progress on diagnosing and treating osteoporosis by using ***,we discuss the challenges and prospects of translational research on the use of EVs in osteoporosis.

关键词： osteoporosis homeostasis biomaterials

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Skill enhancement learning with knowledge distillation

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Science China(Information Sciences) 2024年第8期67卷 206-220页

作者： Naijun liu Fuchun SUN Bin fang Huaping liu Department of Computer Science and Technology Tsinghua University

Skill learning through reinforcement learning has significantly progressed in recent years. However, it often struggles to efficiently find optimal or near-optimal policies due to the inherent trial-and-error exploration in reinforcement learning. Although algorithms have been proposed to enhance skill learning efficacy, there is still much room for improvement in terms of skill learning performance and training stability. In this paper, we propose an algorithm called skill enhancement learning with knowledge distillation(SELKD), which integrates multiple actors and multiple critics for skill learning. SELKD employs knowledge distillation to establish a mutual learning mechanism among actors. To mitigate critic overestimation bias,we introduce a novel target value calculation method. We also perform theoretical analysis to ensure the convergence of SELKD. Finally, experiments are conducted on several continuous control tasks, illustrating the effectiveness of the proposed algorithm.

关键词： skill learning enhancement learning reinforcement learning knowledge distillation

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Four New Terpyridine Complexes Based Polyoxometalates with[W_(10)O_(32)]^(4-) Anions as High-Efficiency Dual-Site Catalysis for Thioether Oxidation Reaction

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Chinese Journal of Chemistry 2024年第6期42卷 592-598页

作者： Yin Zhang Wei-Dong Yu fang-Qian Wang Xiangnan Wang Jiawan zhou Chao liu Jun Yan Junior Education Department Changsha Normal UniversityChangshaHunan410100 China School of Science Hunan University of Technology and BusinessChangshaHunan410000 China College of Chemistry and Chemical Engineering Central South UniversityChangshaHunan410000 China

Polyoxometalates modified with complex cations have attracted increasing attention because of the fascinating properties and the controllable *** adjusting the synthesis conditions,four new terpyridine complexes based hybrid POMs,[(TPY-H)CuCl]_(4)[W_(10)O_(32)]·2DMF·2H_(2)O(1),[(TPY-H)Cu(DMSO)(H_(2)O)]_(2)[W_(10)O_(32)]·2H_(2)O(2),[(TPY-H)_(2)Cu]_(2)[W_(10)O_(32)]·6DMSO·8H_(2)O(3) and[(TPY-Br)CuCl(DMSO)(H_(2)O)]_(2)[(TPY-Br)CuCl]_(2)[W_(10)O_(32)]·2DMSO·4H_(2)O(4),were prepared by using‘one-pot’***-crystal X-ray diffraction analyses,infrared radiation,etc.,revealed the structural composition of compounds 1—4,which indicates that synthesis conditions have a directional regulatory effect on the compounds *** oxidation catalytic reactions show 1—4 have good catalytic activities,and powder X-ray diffraction and thermogravimetry analysis show 1—4 have superduper catalytic ***,4 has better catalytic activity because of the different structure of terpyridine ***,a possible mechanism of dual-site catalysis by both cations and anions is proposed.

关键词： Polyoxometalates Terpyridine complexes Thioether oxidation Dual-site catalysis Clusters

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Exploring battery material failure mechanisms through synchrotron X-ray characterization techniques

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Journal of Energy Chemistry 2024年第7期94卷 128-135页

作者： Lingzhe fang Xiaozhao liu Tao Li Department of Chemistry and Biochemistry Northern Illinois UniversityDeKalbIL 60115USA X-ray Science Division and Joint Center forEnergy Storage Research Argonne National LaboratoryLemontIL6439UA

Rechargeable battery cycling performance and related safety have been persistent *** is crucial to decipher the capacity fading induced by electrode material failure via a range of *** these,synchrotron-based X-ray techniques with high flux and brightness play a key role in understanding degradation *** this comprehensive review,we summarize recent advancements in degra-dation modes and mechanisms that were revealed by synchrotron X-ray ***,an overview of X-ray absorption spectroscopy and X-ray scattering techniques is introduced for charac-terizing failure phenomena at local coordination atomic environment and long-range order crystal struc-ture scale,*** last,we envision the future of exploring material failure mechanism.

关键词： Battery failure Synchrotron-based techniques X-ray scattering X-ray absorption spectroscopy

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Evolutionary mechanisms and practical significance of reproductive success and clonal diversity in unisexual vertebrate polyploids

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Science China(Life Sciences) 2024年第3期67卷 449-459页

作者： Meng Lu Li zhou Jian-fang Gui State Key Laboratory of Freshwater Ecology and Biotechnology Hubei Hongshan Laboratorythe Innovation Academy of Seed DesignInstitute of HydrobiologyChinese Academy of SciencesWuhan 430072China University of Chinese Academy of Sciences Beijing 100049China

Unisexual reproduction is generally relevant to polyploidy, and unisexual vertebrates are often considered an evolutionary “dead end” due to the accumulation of deleterious mutations and absence of genetic diversity. However, some unisexual polyploids have developed strategies to avoid genomic decay, and thus provide ideal models to unveil unexplored evolutionary mechanisms, from the reproductive success to clonal diversity creation. This article reviews the evolutionary mechanisms for overcoming meiotic barrier and generating genetic diversity in unisexual vertebrates, and summarizes recent research advancements in the polyploid Carassius complex. Gynogenetic gibel carp(Carassius gibelio) is a unique amphitriploid that has undergone a recurrent autotriploidy and has overcome the bottleneck of triploid sterility via gynogenesis. Recently, an efficient strategy in which ploidy changes, including from amphitriploid to amphitetraploid, then from amphitetraploid to novel amphitriploid, drive unisexual-sexual-unisexual reproduction transition and clonal diversity has been *** on this new discovery, multigenomic reconstruction biotechnology has been used to breed a novel strain with superior growth and stronger disease resistance. Moreover, a unique reproduction mode that combines both abilities of ameiotic oogenesis and sperm-egg fusion,termed as ameio-fusiongensis, has been discovered, and it provides an efficient approach to synthesize sterile allopolyploids. In order to avoid ecological risks upon escape and protect the sustainable property rights of the aquaculture seed industry, a controllable fertility biotechnology approach for precise breeding is being developed by integrating sterile allopolyploid synthesis and gene-editing *** review provides novel insights into the origin and evolution of unisexual vertebrates and into the attempts being made to exploit new breeding biotechnologies in aquaculture.

关键词： unisexual vertebrates polyploidy reproduction transition clonal diversity precise breeding genomic reconstruction controllable fertility

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Southern Hemisphere Volcanism Triggered Multi-year La Niñas during the Last Millennium

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Advances in Atmospheric Sciences 2024年第4期41卷 587-592页

作者： Shangrong zhou Fei liu School of Atmospheric Sciences Sun Yat-Sen University Key Laboratory of Tropical Atmosphere-Ocean System Ministry of Educationand Southern Marine Science and Engineering Guangdong LaboratoryZhuhai 519082China Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters(CIC-FEMD) Nanjing University of Information Science and TechnologyNanjing 210044China

To explain the recent three-year La Niña event from 2020 to 2022,which has caused catastrophic weather events worldwide,Fasullo et al.(2023)demonstrated that the increase in biomass aerosol resulting from the 2019-20 Australian wildfire season could have triggered this multi-year La Niñ***,we present compelling evidence from paleo-proxies,utilizing a substantial sample size of 26 volcanic eruptions in the Southern Hemisphere(SH),to support the hypothesis that ocean cooling in the SH can lead to a multi-year La Niña *** research highlights the importance of focusing on the Southern Ocean,as current climate models struggle to accurately simulate the Pacific response driven by the Southern Ocean.

关键词： volcanic eruptions multi-year La Niñas Australian wildfire southern ocean cooling

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Modelling analysis embodies drastic transition among global potential natural vegetations in face of changing climate

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Forest Ecosystems 2024年第2期11卷 184-192页

作者： Zhengchao Ren Lei liu fang Yin Xiaoni liu School of Earth Science and Resources Chang’an UniversityXi’an710054China Research Center of Ecological Construction and Environmental Conservation in Gansu Province Gansu Agricultural UniversityLanzhou730070China State Key Laboratory of Tibetan Plateau Earth System Environment and Resources(TPESER)Institute of Tibetan Plateau ResearchChinese Academy of SciencesBeijing100101China School of Land Engineering Chang’an UniversityXi’an710054China College of Pratacultural Science Gansu Agricultural UniversityLanzhou730070China

Potential natural vegetation(PNV)is a valuable reference for ecosystem renovation and has garnered increasing attention ***,there is limited knowledge on the spatio-temporal distributions,transitional processes,and underlying mechanisms of global natural vegetation,particularly in the case of ongoing climate *** this study,we visualize the spatio-temporal pattern and inter-transition procedure of global PNV,analyse the shifting distances and directions of global PNV under the influence of climatic disturbance,and explore the mechanisms of global PNV in response to temperature and precipitation *** achieve this,we utilize meteorological data,mainly temperature and precipitation,from six phases:the Last Inter-Glacial(LIG),the Last Glacial Maximum(LGM),the Mid Holocene(MH),the Present Day(PD),2030(20212040)and 2090(2081–2100),and employ a widely-accepted comprehensive and sequential classification sy–stem(CSCS)for global PNV *** find that the spatial patterns of five PNV groups(forest,shrubland,savanna,grassland and tundra)generally align with their respective ecotopes,although their distributions have shifted due to fluctuating temperature and ***,we observe an unexpected transition between tundra and savanna despite their geographical *** shifts in distance and direction of five PNV groups are mainly driven by temperature and precipitation,although there is heterogeneity among these shifts for each ***,the heterogeneity observed among different global PNV groups suggests that they may possess varying capacities to adjust to and withstand the impacts of changing *** spatio-temporal distributions,mutual transitions and shift tendencies of global PNV and its underlying mechanism in face of changing climate,as revealed in this study,can significantly contribute to the development of strategies for mitigating warming and promoting re-vegetation in degraded regions worldwide.

关键词： Potential natural vegetation Global warming Vegetation classification Predicted model CSCS

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Design and synthesis of thiol-terminated imidothioether oligomer as thermally latent hardener and modifier for high-performance epoxy/thiol thermosets

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Science China Chemistry 2024年第2期67卷 632-641页

作者： Xing liu Jianjun zhou Shumei liu Jianqing Zhao School of Materials Science and Engineering South China University of TechnologyGuangzhou510640China Key Lab Guangdong High Property&Functional Polymer Materials Key Laboratory of Polymer Processing EngineeringMinistry of EducationGuangzhou510640China

Conventional base-catalyzed epoxy/aliphatic thiol systems have a poor storage stability,and are impossible to be one-pot systems.A widely accepted solution is to use the latent catalysts,which are usually insoluble anionic initiators sensitive to impurities and moisture,and have many limitations in practical *** this work,a soluble thiol-terminated imidothioether oligomer(TPI) was synthesized and used as a latent hardener and modifier to prepare one-pot epoxy/thiol systems without the latent *** latent behavior and curing mechanism of epoxy systems(EP/TPI series),consisted of bisphenol A diglycidyl ether(DGEBA),pentaerythritol tetrakis(mercaptoacetate)(PETMP) and TPI,were *** thiol exchange reaction between TPI and PETMP preceded the curing reaction of DGEBA,and produced aromatic thiols,which were unreactive at ambient conditions and reacted with DGEBA to form the thermosets at temperatures above 130 ℃.At the loading of 24.4 wt%TPI,the epoxy system(EP/TPI-3) had a shelf life of 13 days and was completely cured within 20 min at 180 ℃.Meanwhile,the catalyst-free curing process of EP/TPI-3 system was insensitive to impurities and ***,the thermal and mechanical properties of EP/TPI-3 thermoset were simultaneously improved,thereinto,the glass transition temperature,Young's modulus and ultimate tensile strength were increased by 16.7 ℃,12.9%,and 13.6%,respectively,compared with those of the commercial DGEBA/PETMP *** work shows that TPI has the potential to be a powerful alternative to commercial latent catalysts,and EP/TPI thermosets with high performance have broad application prospects.

关键词： thiol-terminated imidothioether oligomer epoxy systems thiol exchange reaction thermal latency high performance

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