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Accelerating Oxygen Electrocatalysis Kinetics on Metal-Organic Frameworks via Bond Length Optimization

Nano-Micro Letters 2024年第9期16卷 279-290页

作者： Fan He Yingnan Liu Xiaoxuan Yang Yaqi Chen Cheng‑Chieh Yang Chung‑Li Dong Qinggang He Bin Yang Zhongjian Li yongbo kuang Lecheng Lei Liming Dai Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China Institute of Zhejiang University-Quzhou Quzhou 324000People’s Republic of China Ningbo Institute of Materials Technology and Engineering Chinese Academy of SciencesNingbo 315201People’s Republic of China School of Biological and Chemical Engineering NingboTech UniversityNingbo 315100People’s Republic of China Department of Physics Tamkang UniversityNew Taipei 25137TaiwanPeople’s Republic of China Australian Carbon Materials Centre(A‑CMC) School of Chemical EngineeringUniversity of New South WalesSydneyNSW 2051Australia

Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hampered their practical use in water splitting.Herein,we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs(donated as AE-CoNDA)to serve as efficient catalyst for water splitting.AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm^(−2)and a small Tafel slope of 62 mV dec^(−1)with excellent stability over 100 h.After integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 V.Experimental investigations demonstrate that the stretched Co-O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p,which accounts for the fast kinetics and high activity.Theoretical calculations reveal that the stretched Co-O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.

关键词： Metal-organic frameworks Bond length adjustment Spin state transition Orbitals hybridization Water splitting

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Molecular understanding of cation effects on double layers and their significance to CO-CO dimerization

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National Science Review 2023年第9期10卷 125-135页

作者： Jia-Bo Le Ao Chen yongbo kuang Jun Cheng Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology of Zhejiang Province Ningbo Institute of Materials Technology and EngineeringChinese Academy of Sciences State Key Laboratory of Physical Chemistry of Solid Surfaces iChEM College of Chemistry and Chemical EngineeringXiamen University Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM)

Cation effects have been shown in numerous experiments to play a significant role in electro catalysis.To understand these effects at the molecular level,we systematically investigate the structures and capacitances of electric double layers with a variety of cations as counter charges at Pt(111)-COad/water interfaces with ab initio molecular dynamics.It is encouraging to find that the computed Helmholtz capacitances for different cations are in quantitative agreement with experiments,and that the trend of cation effects on capacitances shows clear correlation with the structures of interface cations of differing sizes and hydration energies.More importantly,we demonstrate the Helmholtz capacitance as the key descriptor for measuring the activity of CO-CO dimerization,the rate-determining step for C2+formation in electroreduction of CO and CO2.Our work provides atomistic insights into cation effects on electric double layers and electrocatalysis that are crucial for optimizing electrode and electrolyte materials.

关键词： cation effect electrocatalysis electric double layer CO-CO dimerization ab initio molecular dynamics

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High-performance bulk heterojunction-based photocathode with facile architecture for photoelectrochemical water splitting

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Chinese Chemical Letters 2023年第1期34卷 182-186页

作者： Yanling Wu Deyu Liu Huanglong Zhuang Jiabo Le yongbo kuang Ningbo Institute of Materials Technology and Engineering Chinese Academy of SciencesNingbo 315201China University of Chinese Academy of Sciences Beijing 100049China Fujian Provincial Key Laboratory of Featured Biochemical and Chemical Materials Ningde Normal UniversityNingde 352100China

Organic semiconductors are promising candidates as photoactive layers for photoelectrodes used in photoelectrochemical(PEC)cells due to their excellent light absorption and efficient charge transport properties with the help of interfacial materials.However,the use of multilayers will make the charge transfer mechanism more complicated and decrease the PEC performance of the photoelectrode caused by the increased contact resistance.In this work,a PM6:Y6 bulk heterojunction(BHJ)-based photocathode is fabricated for efficient PEC hydrogen evolution reaction(HER)in an acidic aqueous solution.With RuO_(2)as an interfacial modification layer,the photocathode with a simple structure(fluorine-doped tin oxide(FTO)/PM6:Y6/RuO_(2))generates a maximum photocurrent density up to-15 m A/cm^(2)at 0 V vs.reference hydrogen electrode(RHE),outperforming all previously reported BHJ-based photocathodes in terms of PEC performance.The highest ratiometric power-saved efficiency of 3.7%is achieved at 0.4 V vs.RHE.

关键词： Photocathodes Ruthenium oxide Bulk heterojunctions Hydrogen evolution Photoelectrochemical cells

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Instant formation of excellent oxygen evolution catalyst film via controlled spray pyrolysis for electrocatalytic and photoelectrochemical water splitting

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Journal of Energy Chemistry 2022年第3期31卷 657-665,I0018页

作者： Na An Hengzheng Tian Yang Zhou Yalong Zou Hao Xiu Yufeng Cao Ying Wang Jianming Li Deyu Liu yongbo kuang School of Materials Science and Chemical Engineering Ningbo UniversityNingbo 315211ZhejiangChina Ningbo Institute of Materials Technology and Engineering Chinese Academy of SciencesNingbo 315201ZhejiangChina Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100000China Petroleum Geology Research and Laboratory Center Research Institute of Petroleum Exploration&Development(RIPED)PetroChinaBeijing 100083China

The retarded kinetics of oxygen evolution on electrodes is a bottleneck for electrochemical energy conversion and storage systems.NiFe-based electrocatalysts provide a cost-effective choice to confront this challenge.However,there is a lack of facile techniques for depositing compact catalytic films of high coverage and possessing a state-of-the-art performance,which is especially desired in photoelectrochemical(PEC)systems.Herein,we demonstrate a spray pyrolysis(SP)route to address this issue,featuring the kinetic selective preparation towards the desired catalytic-active material.Differing from reported SP protocols which only produce inactive oxides,this approach directly generates a unique composite film consisting of NiFe layered oxyhydroxides and amorphous oxides,exhibiting an overpotential as small as 255 mV(10 mA cm^(−2))and a turnover frequency of∼0.4 s^(−1)per metal atom.By using such a facile protocol,the surface rate-limiting issue of BiVO_(4)photoanodes can be effectively resolved,resulting in a charge injection efficiency of over 90%.Considering this deposition directly start from simple nitrates but only takes several seconds to complete,we believe it can be developed as a widely applicable and welcomed functionalization technique for diverse electrochemical devices.

关键词： Spray pyrolysis Oxygen evolution catalysts Layered oxyhydroxide Heterogeneous structure Thin film

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Structural limiting factors of mixed-valent tin oxides in photoelectrochemical application:A comparative exploration

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Journal of Energy Chemistry 2021年第5期30卷 504-511页

作者： Yalong Zou Deyu Liu Xiangrui Meng Qitao Liu Yang Zhou Jianming Li Zhiying Zhao Ding Chen yongbo kuang School of Materials Science and Engineering Hunan UniversityChangsha 410082HunanChina Ningbo Institute of MaterialsTechnology and Engineering Chinese Academy of SciencesNingbo 315201ZhejiangChina University of Chinese Academy of Sciences Beijing 100000China Petroleum Geology Research and Laboratory Center Research Institute of Petroleum Exploration&Development(RIPED)PetroChinaBeijing 100083China Department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina

Photoelectrocatalytic(PEC)materials for harvesting solar energy can be discovered from existing photocatalytic semiconductors.Nonetheless,mixed valence tin oxides,a group of widely reported visible light active photocatalysts,can hardly be developed into efficient PEC photoelectrodes.To overcome this difficulty by clarifying its origin,two typical mixed valence tin oxides,Sn^(2+):SnO_(2) microrods and porous Sn_(3)O_(4) particles were deliberately prepared as the models.Sn^(2+):SnO_(2) microrods of less porosity exhibited a photocurrent over ten times higher than Sn_(3)O_(4) particles.Photo-electrochemical impedance spectroscopy revealed this was due to their charge kinetics difference,specifically the internal transport/-transfer responding to the morphology.Moreover,hydroxyl residuals from synthesis were found to be very inhibitive for the PEC efficiency as well,which was in coherence with our TGA and Raman spectroscopic study.These finding experimentally proved the necessity of reconsidering the surface area,crystallinity,and defects when developing photocatalysts into efficient PEC structures.

关键词： Mixed-valence tin oxide Photoelectrochemical water splitting Nanostructure

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Structural covariance network of the hippocampus–amygdala complex in medication-nale patients with first-episode major depressive disorder

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Psychoradiology 2022年第4期2卷 190-198页

作者： Lianqing Zhang Xinyue Hu yongbo Hu Mengyue Tang Hui Qiu Ziyu Zhu Yingxue Gao Hailong Li Weihong kuang Weidong Ji Functional and molecular imaging Key Laboratory of Sichuan Province West China HospitalSichuan UniversityChengdu 610041PR China Department of Radiology West China Hospital of Sichuan UniversityChengdu 610041PR China Department of Psychiatry West China Hospital of Sichuan UniversityChengdu 610041PR China Shanghai Key Laboratory of Mental Health and Psychological Crisis Intervention School of Psychology and Cognitive Science and Affiliated Mental Health CenterEast China Normal UniversityShanghai 200335China Child Psychiatry Shanghai Changning Mental Health CenterShanghai 200335China

Background The hippocampus and amygdala are densely interconnected structures that work together in multiple affective and cognitive processes that are important to the etiology of major depressive disorder(MDD).Each of these structures consists of several heterogeneous subfields.We aim to explore the topologic properties of the volume-based intrinsic network within the hippocampus–amygdala complex in medication-nale patients with first-episode MDD.Methods High-resolution T1-weighted magnetic resonance imaging scans were acquired from 123 first-episode,medication-nale,and noncomorbid MDD patients and 81 age-,sex-,and education level-matched healthy control participants(HCs).The structural covariance network(SCN)was constructed for each group using the volumes of the hippocampal subfields and amygdala subregions;the weights of the edges were defined by the partial correlation coefficients between each pair of subfields/subregions,controlled for age,sex,education level,and intracranial volume.The global and nodal graphmetrics were calculated and compared between groups.Results Compared with HCs,the SCN within the hippocampus–amygdala complex in patients with MDD showed a shortened mean characteristic path length,reduced modularity,and reduced small-worldness index.At the nodal level,the left hippocampal tail showed increased measures of centrality,segregation,and integration,while nodes in the left amygdala showed decreased measures of centrality,segregation,and integration in patients with MDD compared with HCs.Conclusion Our results provide the first evidence of atypical topologic characteristics within the hippocampus–amygdala complex in patients with MDD using structure network analysis.It provides more delineate mechanism of those two structures that underlying neuropathologic process in MDD.

关键词： Major depressive disorder hippocampus-amygdala complex structural covariance network global network metrics local network metrics

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Carbon Alloy Catalyst Catalyzed Selective Oxidation of Benzilic Alcohols： A Metal -Free, Aerobic Catalytic System

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华东理工大学学报（自然科学版） 2009年第6期35卷 917-917页

作者： yongbo kuang HAYAKA WA Teruaki KAKIMOTO Masa-aki Department of Organic and Polymeric Materials Tokyo Institute of Technology 2-12-10-okayama Meguro-ku Tokyo 152-8552 Japan

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光电化学水分解中铁酸盐光阴极的制备与改性

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化学进展 2020年第10期32卷 1515-1534页

作者：倪鑫周扬谭瑞琴况永波宁波大学信息科学与工程学院宁波315211 中国科学院宁波材料技术与工程研究所宁波315201

由n型半导体光阳极和p型半导体光阴极组成的无偏压光电化学电池通过太阳能可以将水直接转化为高能量密度的氢气,为解决太阳能利用过程中存在的间歇性和储存问题提供了一种潜在的经济有效的解决途径。金属氧化物具有低成本和易制备等优势... 详细信息

由n型半导体光阳极和p型半导体光阴极组成的无偏压光电化学电池通过太阳能可以将水直接转化为高能量密度的氢气,为解决太阳能利用过程中存在的间歇性和储存问题提供了一种潜在的经济有效的解决途径。金属氧化物具有低成本和易制备等优势,相比于发展较成熟的n型光阳极金属氧化物材料,传统的p型光阴极金属氧化物材料由于金属离子易受到光电腐蚀的影响,光电极寿命的提升是个很大的挑战。作为新型的金属氧化物光阴极材料,铁酸盐具有合适的带隙、较好的光稳定性、较正的起始电位以及较低的制备成本,正在成为光电化学电池实际应用中的有力竞争者。本文阐述了光电化学水分解的基本原理与提升光电极性能的一般方法,总结了近年来颇受关注的代表性铁酸盐光阴极材料CuFeO_2、CaFeO_4与LaFeO_3在制备方法、元素掺杂以及表面修饰等方面取得的重要进展,并对铁酸盐光阴极的未来发展趋势做了展望。

关键词：光电化学铁酸盐光阴极水分解制备改性

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Artificial intelligence for the development and implementation guidelines for traditional Chinese medicine and integrated traditional Chinese and western medicine

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TMR Modern Herbal Medicine 2021年第2期4卷 15-28页

作者： Yinghui Jin Xiangying Ren Lina Yu yongbo Wang Qiao Huang Xuhui Li Xiangge Ren Jiaao Lou kuang Gao Mukun Chen Wenbin Hu Xiantao Zeng Hongcai Shang Center for Evidence-Based and Translational Medicine Zhongnan Hospital of Wuhan UniversityWuhanChina College of Nursing and Health Henan UniversityKaifengHenanChina Department of Urology Zhongnan Hospital of Wuhan UniversityWuhanChina Henan University of Chinese Medicine ZhengzhouHenanChina College of Medicine Wuhan University of Science and TechnologyWuhanChina School of Computer Science Wuhan UniversityWuhanChina Key Laboratory of Chinese Internal Medicine of Ministry of Education and Beijing Dongzhimen HospitalBeijing University of Chinese MedicineBeijingChina.

The translation and implementation of clinical practice guidelines(CPGs)for Traditional Chinese Medicine(TCM)and Integrated Traditional Chinese and Western medicine is crucial to the adoption of medical science and technology,but the low operability and slow update of integrated traditional Chinese and Western Medicine guidelines,and the lack of integration between guidelines and clinical practice,result in the guidelines not having the desired clinical effects in practice.The application of Artificial Intelligence(AI)to the field of CPGs development aims to shorten the development time,optimize and accelerate the whole process of CPG’s development.This article summarized the current research and application status of AI in development and implementation CPGs for TCM and Integrated Traditional Chinese and Western medicine and proposed the method of Combining real world data and AI technology to enrich for TCM and Integrated Traditional Chinese and Western medicine.

关键词： Artificial Intelligence Traditional Chinese Medicine Clinical practice guidelines

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盾构隧道下穿水库引起的导水裂隙带发育规律研究

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低温建筑技术 2022年第5期44卷 93-96页

作者：彭斌张琳周永波郑雯邝利军谭芝文李平中国建筑五局华南公司广州510304 青岛理工大学山东青岛266033 山东华宇工学院山东德州253034 中建隧道建设有限公司重庆401320

为探究盾构隧道施工扰动所引起的导水裂隙带发育高度变化情况,依托深圳13号线留仙洞站-白芒站区间工程,提出一种导水裂隙带发育高度预测计算方法,确定留白区间导水裂隙带发育高度为22m,盾构施工引起的导水裂隙带高度不会波及上覆水体底... 详细信息

为探究盾构隧道施工扰动所引起的导水裂隙带发育高度变化情况,依托深圳13号线留仙洞站-白芒站区间工程,提出一种导水裂隙带发育高度预测计算方法,确定留白区间导水裂隙带发育高度为22m,盾构施工引起的导水裂隙带高度不会波及上覆水体底部,对引水隧道的结构安全和盾构施工进度影响较小。

关键词：盾构隧道水库导水裂隙带发育规律

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