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Efficient bifunctional catalysts of CoSe/N-doped carbon nanospheres supported Pt nanoparticles for methanol electrolysis of hydrogen generation

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Nano Research 2022年第10期15卷 8936-8945页

作者： Yang Zhou Qiaowei Wang Xinlong Tian Ligang Feng School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China State Key Laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikou 570228China

Methanol electrolysis is significant but challenging as an energy-saving technique for electrochemical hydrogen production.Herein,we demonstrated a novel and efficient bifunctional catalyst of CoSe/N-doped carbon nanospheres supported Pt nanoparticles for hydrogen generation via methanol electrolysis;high catalytic performance for both methanol oxidation(MOR)and hydrogen evolution(HER)was observed benefitting from the effective interaction of metal and support effect as well as the oxophilic characteristics of cobalt selenide.Theoretical calculation disclosed the increased charge density of Pt induced by the CoSe/NC support has a bifunctional ability for optimizing the H*adsorption energy for hydrogen evolution reaction and weakening the CO adsorption energy of methanol oxidation reaction.Specifically,the largely improved CO-tolerance ability was observed in the CO-stripping technique,where about 90 mV less of the peak potential for CO oxidation than that of Pt/C catalyst was observed,resulting from a strong electronic effect as indicated by the spectroscopic analysis.The peak current density of 84.2 mA·cm^(–2) was found for MOR,which was about 3.1 times higher than that of Pt/C;and a low overpotential of 32 mV was required to reach 10 mA·cm^(–2) for HER in 0.5 mol·L^(–1) H_(2)SO_(4) with 1.0 mol·L^(–1) CH3OH.When serviced as both anode and cathode catalyst in a methanol electrolyzer,a low cell potential of 0.67 V to offer 10 mA cm^(-2) was obtained,about 170 mV less than that of Pt/C catalyst;moreover,it was 1.1 V lower than that of water-splitting(1.77 V),indicating a promising energy-saving technique for hydrogen generation.They also showed very good catalytic stability and anti-poisoning ability during the catalysis process.This work would help understand the metal-support interaction for hydrogen generation vis methanol electrolysis.

关键词： bifunctional electrocatalyst methanol electrolysis hydrogen evolution reaction Pt-based catalysts metal-organic frameworks

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Electron-enriched Pt induced by CoSe_(2)promoted bifunctional catalytic ability for low carbon alcohol fuel electro-reforming of hydrogen evolution

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Journal of Energy Chemistry 2022年第12期75卷 46-54,I0002页

作者： Yang Zhou Qiaowei Wang Xinlong Tian Jinfa Chang Ligang Feng School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002JiangsuChina State Key Laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikou 570228HainanChina NanoScience Technology Center University of Central FloridaOrlandoFL 32826USA

Alcohol fuel electro-reforming is promising for green hydrogen generation while developing efficient bifunctional catalysts for alcohol fuel electrolysis is still very tricky.Herein,we for the first time proposed the electron-enriched Pt induced by CoSe_(2)has an efficient bi-functional catalytic ability for alcohol fuels electro-reforming of hydrogen in acid electrolytes.The theoretical calculation revealed the advantages of electron-enriched Pt surface for the adsorption of intermediate,which is well supported by spectroscopic analysis and CO-stripping techniques.Largely improved catalytic performances of activity,durability,and kinetics are demonstrated compared to the conventional alloy system and commercial Pt/C catalyst,due to the efficient synergism of Pt and CoSe_(2);the peak current density of Pt/CoSe_(2)for methanol(ethanol)oxidation is 87.61(48.27)m A cm^(-2),which is about 3.3(2.0)times higher than that of Pt/C catalyst and 2.0(1.5)times that of the traditional PtCo alloy catalysts.Impressively,about 80%of the initial current was found after 1000 cycles of stability test for alcohol fuel oxidation of Pt/CoSe_(2)catalyst,higher than that of Pt/C(ca.50%)and PtCo catalyst(65%).When Pt/CoSe_(2)catalyst serviced as bi-functional catalysts for electrolyzer,a low cell potential of 0.65(0.78)V for methanol(ethanol)electrolysis was required to reach 10 m A cm^(-2),which was about 1030(900)m V less than that of conventional water electrolysis using Pt/C as the catalyst.The current result is instructive for the design of novel bifunctional catalyst and the understanding of hydrogen generation via alcohol fuel electro-reforming.

关键词： Cobalt selenide Electrolysis Pt nanoparticles Alcohol oxidation reaction Hydrogen evolution reaction

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Ordered Arrangement of Different Metals in Discrete and Infinite Building Blocks for Heterometallic Metal-Organic Frameworks Construction

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Chemical Research in Chinese Universities 2023年第6期39卷 902-906页

作者： XU Huoshu YAN Yu WU Yichen wang Junyi TANG Yi LI qiaowei Department of Chemistry Collaborative Innovation Center of Chemistry for Energy MaterialsShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsFudan UniversityShanghai 200433P.R.China

Construction of sophisticated metal-organic frameworks(MOFs)with multiple kinds of metals is essential for further advancement of porous materials toward various applications.Order and arrangement of the metals in the secondary building units(SBUs)greatly influence the MOF structures outcome.While most of the previous heterometallic MOFs either have multiple kinds of discrete SBUs with different metals,or single kind of SBU with mixed metals inside,other forms of metal distribution still need further exploration.Herein,a bifunctional linker is applied to achieving differential coordination toward different metals.With Ce and Cu serving as the carboxylate-philic and pyrazole-philic metal ions,three heterometallic MOFs(FDM-121—FDM-123)are synthesized.In addition to the common metal arrangement modes,the new MOFs provide a joint reticulation of a discrete SBU and an infinite chain-like SBU featuring different metals in FDM-121,and an assembly from heterometallic infinite chain-like SBU in FDM-122.This study demonstrates the potential of bifunctional linkers for the design and synthesis of heterometallic MOFs and opens up the possibilities to create MOFs with tailored properties for specific applications.

关键词： Heterometallic Metal-organic framework Secondary building unit Bifunctional

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Functionality proportion and corresponding stability study of multivariate metal-organic frameworks

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Chinese Chemical Letters 2018年第6期29卷 837-841页

作者： Jie Li Yecheng wang Yan Yu qiaowei Li Department of Chemistry iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical Engineering Nanjing University School of Physical Science and Technology Shanghai Tech University

Multivariate metal-organic frameworks（MTV-MOFs） with different ratios of terephthalate（BDC） linker and amino-benzenedicarboxylate（BDC-NH2） linker were synthesized through both direct synthesis from linker mixture and linker exchange of activated single-linker MOFs. Functionality proportion was impacted by the thermodynamics during the one-pot MOF construction, resulting in preference of BDC over BDC-NH2 in the MTV-MOF, in agreement with the quantum mechanics calculations. The functionality difference also affects the thermodynamics in the linker exchange process, as indicated by the more effective linker exchange in BDC-NH2-based IRMOF-3 than in BDC-based MOF-5. Furthermore,the thermal decomposition temperatures and chemical integrity upon ambient air exposure of these MOFs with variate functionalities were investigated, and it reveals that higher proportion of BDC in the MTV-MOF crystals contribute to both higher thermal and higher chemical stabilities.

关键词： Multivariate metal-organic frameworks Direct synthesis Linker exchange Functionality proportion

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Effects of Bivalirudin and Unfractionated Heparin on Liver and Renal Function in Chinese Patients with Coronary Artery Disease Undergoing Coronary Angiography with/without Percutaneous Coronary Intervention

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Journal of Clinical and Translational Hepatology 2021年第4期9卷 477-483页

作者： qiaowei Jia Jia Hu Wenfeng Ji Liansheng wang Enzhi Jia Department of Cardiovascular Medicine First Affiliated Hospital of Nanjing Medical UniversityNanjingJiangsuChina Department of Cardiovascular Medicine Liyang People’s HospitalLiyangJiangsuChina

Background and Aims:Unfractionated heparin(UFH)and bivalirudin are widely used as anticoagulants in cardiovascular medicine,including for thrombosis prevention during coronary angiography(CAG)and percutaneous coronary intervention(PCI).Little is known of the effects of UFH and bivalirudin on liver and kidney function in patients subjected to these procedures.This study compared the effects of bivalirudin and UFH on liver/renal function in patients with coronary artery disease who underwent CAG,with or without PCI.Methods:The study comprised 134 consecutive patients(40–89 years-old),who underwent CAG(or CAG and PCI);among them,66 and 68 patients were subject to,respectively,bivalirudin or UFH.The following indicators of liver/renal function were measured before and after the procedures:plasma alanine aminotransferase(ALT),aspartate aminotransferase(AST),blood urea nitrogen,estimated glomerular filtration rate(eGFR),creatinine clearance,and serum creatinine.Patients were further stratified by severity of chronic kidney disease(CKD),based on original eGFR.Results:Relative to baseline,in the bivalirudin group,ALT and AST were higher after CAG(p=0.005,0.025),while blood urea nitrogen and serum creatinine were lower(p=0.049,<0.001).In the UFH group,ALT,AST,eGFR,and creatinine clearance were lower after CAG(p≤0.001,all).Patients given bivalirudin with moderate or severe CKD,but not those with mild CKD,gained significant improvement in kidney function.Conclusions:Relative to UFH,bivalirudin may better safeguard the renal function of patients with coronary artery disease who undergo CAG,especially patients with moderate-to-severe renal insufficiency.UFH may cause less liver damage than bivalirudin.

关键词： Bivalirudin Unfractionated heparin Coronary artery disease Coro-nary angiography Percutaneous coronary intervention Liver function

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In Situ Fabrication of Graphene Scaffold-ZrO2 Nanofilms from Metal-Organic Oligomers for Thin Film Transistors

In Situ Fabrication of Graphene Scaffold-ZrO2 Nanofilms from...

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中国化学会第八届全国配位化学会议

作者： Qingqing Pang Deyan wang qiaowei Li Department of Chemistry Fudan University

In situ fabrication of graphenescaffold-ZrOnanofilmson SiO substrates is achieved by spin coating and thermal annealing of Zr-based metal-organic oligomers[1].Zirconium asmetal source was oxidized to ZrO nanoparticles upon annealing,and the conjugatedmoieties of the aromatic ligands in the oligomers reorganized into interconnected graphene scaffolds onthe surface of ZrOnanoparticles.The structural similarities of the aromatic moieties in the ligand(phenyl-,naphthyl-,anthryl-,and pyrenyl-)compared to graphene play a major role in the ordering of the graphene scaffolds obtained.XPS depth profile of the nanofilmreveals ultrathin carbon-pure or carbon-rich surface,and most of the nanofilmis intergrowth of carbon and ZrO nanoparticles.The heterogeneous graphene scaffold-ZrOnanofilms show low sheet resistance of 17 kΩ/□,corresponding to electrical conductivity of 3197 S/m.The conductivegraphene scaffold forms directly on top of high-k dielectricZrOnanoparticles,thus can be directly integrated into the fabrication process of electronicdevices.We fabricated the bottom-gated thin-film transistors(TFTs)byusing the graphene scaffold-ZrOnanofilms on the highly doped Si substrates.Whenthe copper grid was used as template to deposit Cr/Au source and drain electrodes,the obtained electriccharacteristic of the device shows p-type channel property with the current on/off ratio of.2.

关键词： graphene scaffold-ZrO2nanofilms metal-organic oligomer high-k dielectric thin film transistors p-type channel

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Synthesis,structure and luminescence properties of metal-organic frameworks based on benzo-bis(imidazole)

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Science China Chemistry 2014年第1期57卷 135-140页

作者： YIN XinBo SONG YuNa wang Yang ZHANG LiJuan LI qiaowei Laboratory of Advanced Materials Fudan University School of Chemistry Beijing Institute of Technology Department of Chemistry Fudan University

Metal-organic frameworks(MOFs)constructed from conjugated organic ligands are candidates for hybrid photoactive materials with potential applications.Compared to that from the ligands only,the intensity and wavelength of the luminescence could be tuned after they were incorporated in extended framework.In this report,by using an organic ligand with azolate moiety,benzo-bis(imidazole)(H2BBI),we synthesized two new MOF structures.Framework 1([Co(H2BBI)(DMSO)2Cl2]n,DMSO=dimethyl sulfoxide),constructed from tetrahedral Co(II)and H2BBI,exhibits zigzag 1D structure.Meanwhile,framework 2([Cu2(H2BBI)3(DMSO)6(NO3)4]n),a layered structure with hcb topology,was assembled from tetragonal pyramidal Cu(II)and H2BBI.Furthermore,2 exhibits strong luminescence emission(ex=280 nm).A blue shift of 40 nm(from 359 nm to 319 nm)was observed in framework 2 compared to the free ligand,which could be explained by the ligand-to-metal charge transfer in the network.

关键词： metal-organic frameworks,luminescence,synthetic methodology,topological analysis

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A Novel Method for Rich Nitrogen-Doped Ordered Mesoporous Carbon

A Novel Method for Rich Nitrogen-Doped Ordered Mesoporous Ca...

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第十七届全国分子筛学术大会

作者： Qiaowei Wang Yijie Mu Weili Zhang Qingjun Chen Yan Meng Yuhan Sun CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research Institution Chinese Academy of Science Graduate University of Chinese Academy of Science

N-doped ordered mesoporous carbon with high nitrogen content was directly prepared on the basis of Mannich condensation for the first time in which the combination of resorcinol,terephthalaldehyde,5-a

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Structural and functional imaging of brains

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Science China Chemistry 2023年第2期66卷 324-366页

作者： Zhichao Liu Ying Zhu Liming Zhang Weiping Jiang Yawei Liu qiaowei Tang Xiaoqing Cai Jiang Li Lihua wang Changlu Tao Xianzhen Yin Xiaowei Li Shangguo Hou Dawei Jiang Kai Liu Xin Zhou Hongjie Zhang Maili Liu Chunhai Fan Yang Tian Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai200241China Interdisciplinary Research Center Shanghai Synchrotron Radiation FacilityZhangjiang LaboratoryShanghai Advanced Research InstituteChinese Academy of SciencesUniversity of Chinese Academy of SciencesShanghai201210China State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics Chinese Academy of SciencesWuhan National Laboratory for OptoelectronicsWuhan430071China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China Department of Chemistry Tsinghua UniversityBeijing100084China School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesInstitute of Translational MedicineShanghai Jiao Tong UniversityShanghai200240China Interdisciplinary Center for Brain Information Brain Cognition and Brain Disease InstituteShenzhen-Hong Kong Institute of Brain Science-Shenzhen Fundamental Research InstitutionsFaculty of Life and Health SciencesShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen518055China Lingang Laboratory Shanghai201602China School of Biomedical Engineering Shanghai Jiao Tong UniversityShanghai200240China Institute of Systems and Physical Biology Shenzhen Bay LaboratoryShenzhen518055China Department of Nuclear Medicine Union HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan430022China

Analyzing the complex structures and functions of brain is the key issue to understanding the physiological and pathological processes.Although neuronal morphology and local distribution of neurons/blood vessels in the brain have been known,the subcellular structures of cells remain challenging,especially in the live brain.In addition,the complicated brain functions involve numerous functional molecules,but the concentrations,distributions and interactions of these molecules in the brain are still poorly understood.In this review,frontier techniques available for multiscale structure imaging from organelles to the whole brain are first overviewed,including magnetic resonance imaging(MRI),computed tomography(CT),positron emission tomography(PET),serial-section electron microscopy(ss EM),light microscopy(LM)and synchrotron-based X-ray microscopy(XRM).Specially,XRM for three-dimensional(3D)imaging of large-scale brain tissue with high resolution and fast imaging speed is highlighted.Additionally,the development of elegant methods for acquisition of brain functions from electrical/chemical signals in the brain is outlined.In particular,the new electrophysiology technologies for neural recordings at the single-neuron level and in the brain are also summarized.We also focus on the construction of electrochemical probes based on dual-recognition strategy and surface/interface chemistry for determination of chemical species in the brain with high selectivity and long-term stability,as well as electrochemophysiological microarray for simultaneously recording of electrochemical and electrophysiological signals in the brain.Moreover,the recent development of brain MRI probes with high contrast-to-noise ratio(CNR)and sensitivity based on hyperpolarized techniques and multi-nuclear chemistry is introduced.Furthermore,multiple optical probes and instruments,especially the optophysiological Raman probes and fiber Raman photometry,for imaging and biosensing in live brain are emphasized.Finally,a brief perspective on existing cha

关键词： brain structure brain function brain chemistry chemical signal biosensing and bioimaging

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基于“多宜性—稀缺性—多样性”的粤港澳大湾区土地利用冲突识别

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农业工程学报 2023年第17期39卷 245-255页

作者：董光龙周俏薇孙传谆王珏柯钦华山东建筑大学管理工程学院济南250101 华南农业大学公共管理学院广州510642 自然资源部华南热带亚热带自然资源监测重点实验室广州510700

精准识别土地利用冲突是国土空间治理的重要前提。该研究引入一个基于土地利用多宜性、土地资源稀缺性和需求多样性的土地利用冲突识别新框架,系统评估粤港澳大湾区土地利用冲突。结果表明:1)粤港澳大湾区土地利用冲突以中等为主,占比高... 详细信息

精准识别土地利用冲突是国土空间治理的重要前提。该研究引入一个基于土地利用多宜性、土地资源稀缺性和需求多样性的土地利用冲突识别新框架,系统评估粤港澳大湾区土地利用冲突。结果表明:1)粤港澳大湾区土地利用冲突以中等为主,占比高达43.67%;其次为高冲突(29.80%),低冲突区域所占比例最小(26.53%)。2)粤港澳大湾区土地利用冲突呈现显著的城乡差异特征。高冲突区集中在城镇和城乡过渡地带,尤其是城镇化快速发展的惠州市、江门市以及肇庆市;中冲突地区广泛分布在乡镇生产生活区域;低冲突区分布在土地利用适宜性低的山地丘陵地区。3)土地利用高冲突区域耕地和生态用地适宜性高,并且土地资源稀缺性普遍较高;中冲突区主要由于土地资源稀缺性、人类需求多样性高导致。在国土空间利用及相关规划中,应充分考虑潜在的土地利用冲突,建立土地利用冲突预警机制,并纳入相关规划监督实施体系,为优化国土空间格局提供科学依据。

关键词：土地利用冲突土地利用多宜性土地资源稀缺性需求多样性粤港澳大湾区

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