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中国化学会·第一届全国二氧化碳资源化利用学术会议

作者： Qing Huang ya-qian lan School of Chemistry and Materials Science Jiangsu Key Laboratory of Biofunctional Materials Nanjing Normal University

The activation of CO on the electrocatalyst surface is regarded as the rate determining step in electrocatalytic CO reduction(ECR), and therefore it is highly important to find out its adsorption and activation mechanism. Herein, we develop the OH–-coordinated MOF(NNU-15) to simulate the surface state of catalyst in alkaline environment of ECR and then further explore its activation mechanism to CO. NNU-15 shows high faradaic efficiency for CO(FECO) reaching up to 99.2% at-0.6 V vs. RHE along with a long-term stability(110 h) and surpassing 96% over a wide potential range from-0.6 to-0.9 V. In ECR process, single-crystal to single-crystal transformation between NNU-15 and NNU-15-CO demonstrates that coordinated OH– can activate the CO into HCO that will chelate to metal center. Theoretical calculations validate that both O-adsorbed and C-adsorbed initial geometries are inclined to result in the formation of HCO during ECR process.

关键词： electrocatalytic CO2 reduction high faradaic efficiency OH-–coordinated MOF CO2 adsorption and activation single-crystal to single-crystal transformation

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Multielectron transportation of polyoxometalate-grafted metalloporphyrin coordination frameworks for selective CO2-to-CH4 photoconversion

Multielectron transportation of polyoxometalate-grafted meta...

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中国化学会·第一届全国二氧化碳资源化利用学术会议

作者： Qing Huang ya-qian lan School of Chemistry and Materials Science Jiangsu Key Laboratory of Biofunctional Materials Nanjing Normal University

Photocatalytic CO reduction into energy carriers is of utmost importance due to the rising concentrations of carbon dioxide and the depleting energy resource. However, the highly selective generation of desirable hydrocarbon fuel, such as methane(CH), from CO remains extremely challenging. Herein, we present two stable polyoxometalate-grafted metalloporphyrin coordination frameworks(POMCFs), which are constructed with reductive Zn-ε-Keggin clusters and photosensitive TCPP linkers, exhibiting high selectivity(> 96%) for CH formation in photocatalytic CO reduction system. To our knowledge, the high CH selectivity of POMCFs has surpassed all of the reported coordiantion framework-based heterogeneous photocatalysts for CO-to-CH conversion. Significantly, the introduction of Zn-ε-keggin cluster with strong reducing ability is the important origin for POMCFs to obtain high photocatalytic selectivity for CH formation, considering that eight Mo atoms can theoretically donate eight electrons to fulfill the multi-electrons reduction process of CO to CH transformation.

关键词： reductive polyoxometalate coordination frameworks CO2 photoreduction high selectivity methane

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Covalent organic frameworks:a new platform for next-generation batteries of Na-,K-and Zn-ions

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Science Bulletin 2022年第16期67卷 1621-1624页

作者： Ying Zang Di-Qiu Lu ya-qian lan School of Chemistry South China Normal UniversityGuangzhou 510006China

With the rapid development of globalization and growing energy consumption,there is a huge demand for smart grids,electric vehicles,and large-scale energy *** of electrochemical energy storage devices with high efficiency have been developed and *** recent years,lithium-based batteries have been widely developed and achieved groundbreaking progress in practical applications,which are accepted as an effective way to realize high-energy-density electronic devices[1].However,it is undeniable that lithium-based batteries have entered a bottleneck period,and many technical problems need to be solved *** energy density can hardly be improved.

关键词：锌离子电池共价有机框架材料 lithium

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维普期刊数据库

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Self-assembly of single metal sites embedded covalent organic frameworks into multi-dimensional nanostructures for efficient CO_(2) electroreduction

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Chinese Chemical Letters 2022年第3期33卷 1439-1444页

作者： Yi-Lu yang Yi-Rong Wang Guang-Kuo Gao Ming Liu Chang Miao Le-yan Li Wei Cheng Zi-Yue Zhao Yifa Chen Zhifeng Xin Shun-Li Li Dong-Sheng Li ya-qian lan Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials Jiangsu Key Laboratory of New Power BatteriesSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China School of Chemistry South China Normal UniversityGuangzhou 510006China Institute of Molecular Engineering and Applied Chemistry Anhui University of TechnologyMa'anshan 243002China College of Materials and Chemical Engineering Hubei Provincial Collaborative Innovation Center for New Energy MicrogridKey Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion MaterialsChina Three Gorges UniversityYichang 443002China

Morphology-controlled electrocatalysts with the ability of CO_(2) adsorption/activation, mass transfer, high stability and porosity are much desired in electrochemical CO_(2) reduction reaction (CO_(2)RR). Here, three kinds of multi-dimensional nanostructures (i.e., hollow sphere, nanosheets and nanofibers) have been successfully produced through the modulation of porphyrin-based covalent organic frameworks (COFs) with various modulators. The obtained nanostructures with high-stability, large surface-area, and single metal sites enable efficient CO_(2)RR into CH_(4). Notably, they all exhibit higher FE (hollow sphere, 68.2%;nanosheet, 64.2% and nanofiber, 71.0%, -0.9 V) than COF-366-Cu (43.0%, -0.9 V) after morphology control. Noteworthy, the FE of COF-366-Cu (HS) keeps higher than 52.4% over a wide potential range from -0.9 V to -1.1 V and the achieved FECH_(4) + C_(2)H_(4) (82.8%, -0.9 V) is superior to most of reported COFs and copper-based electrocatalysts. This work paves a new way in the exploration of COF-based multi-dimensional nanostructures applicable in efficient CO_(2)RR to CH_(4).

关键词： CO_(2)electroreduction Covalent organic frameworks Hollow sphere Nanofiber Nanosheet

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维普期刊数据库

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Cobalt-Based Molecular Clusters for Photocatalytic CO2 Reduction

Cobalt-Based Molecular Clusters for Photocatalytic CO2 Reduc...

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中国化学会第八届全国配位化学会议

作者： Lei Zhang Jiang Liu ya-qian lan School of Chemistry and Materials Science Nanjing Normal University

With the exploitation and exhaustion of fossil fuel reserves,it has raised concerns on the problems of theglobal warming and future energy *** COinto value-added chemicals by solar energy as a greenand abundant resource could simultaneously deal with both of theproblems above,as well as provide a convenient meansfor energy ***,aSeries of Cobalt-Based Molecular Clusters[Co(L)Cl]({Co}),[Co(L)(L)(OMe)(HO)]({Co}),[Co(L)(L)(OC)(HO)]({Co})were successfully synthesized(L,Lare both polynitrogen heterocyclic ligands).All of these compounds have the leaving groups(Clin{Co}and HO in{Co},{Co})or cobalt ions in unsaturated coordination({Co}and{Co}),which result in good performance in photocatalytic CO ***’s noted that the production of CO can reach 22.5μmol,24.8μmol and 15.2μmol when using{Co},{Co}and{Co}as photocatalyst,respectively,showing high activity forvisible-light-induced CO reduction.

关键词： Molecular catalysis Photocatalytic CO2 reduction

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A High StablePolyoxometalate-Based Metal-Organic Frameworkwith ABW Zeolite-Like Structure

A High StablePolyoxometalate-Based Metal-Organic Frameworkwi...

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中国化学会第八届全国配位化学会议

作者： Xiao-Xin Li Jiang Liu ya-qian lan School of Chemistry and Materials Science Nanjing Normal University

Lithium-ion batteries(LIBs) as one kind of new-type power source,accounted strong commercial development potential in energy supply of portable electronics and new energy *** for a stable material possessing both high energy density and splendid rate performance has recently aroused widely concern from ***,asteady polyoxometalate-based metal-organic framework(POMOF) with ABW zeolite-like topology ,NENU-601,was successfully ***-601 can be not only stable in air for nearly 180 days,but also it’s obviously revealed that the crystalline integrity of NENU-601 can be kept in aqueous solution in different pH values(pH=1,3,9 and 12,adjust by HCl or NaOH) for 24 hours and electrolyte for 12 *** to its structural stability and potential redox ability,under a current density of100 mA g,NENU-601 delivered reversible capacity of 770 mA h g,indicating it is an excellent material for LIBs with high and stable ***,POMOFs with zeolite framework has great potential and wide application prospect in the energy storage,which is still a long way to go.

关键词： POMOFs Zeolite-like Lithium-ion batteries

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Superprotonic Conductivity of H2SO4@MIL-101-SO3H Affected by Multiple Proton Units at Subzero Temperatures

Superprotonic Conductivity of H2SO4@MIL-101-SO3H Affected by...

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中国化学会第七届全国结构化学学术会议

作者： Xiao-Min Li Jiang Liu ya-qian lan School of Chemistry and Materials Science Nanjing Normal University

A water stable MOF-based composite,HSO@MIL-101-SOH,configured with functionalized sulfonate groups bound to the polymeric backbone and nonvolatilestrong acid HSO encapsulated into pores,was demonstrated as a superior ...

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Modulation of Slow Magnetic Relaxation by Mono-/Di-atoms Bridged Dinuclear Dysprosium Cluster

Modulation of Slow Magnetic Relaxation by Mono-/Di-atoms Bri...

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中国化学会第七届全国结构化学学术会议

作者： Jiang Liu Ming-Liang Tong ya-qian lan School of Chemistry and Chemical Engineering Sun Yat-Sen University School of Chemistry and Materials Science Nanjing Normal University

Single molecule magnets(SMMs)with magnetic bistability in the field of molecular magnetism have received considerable attention owing to their potential utilities in high density information storage and molecular *** pursuit of such applications connects inevitably to the magnetic performance of the SMMs,which typically depends on the magnitude of spin-inversion

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Nickel-doped W2C/NRGO Composite as Active Electrocatalysts for Hydrogen Evolution Reaction

Nickel-doped W2C/NRGO Composite as Active Electrocatalysts f...

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中国化学会第七届全国结构化学学术会议

作者： Yu-Jia Tang Wei Huang ya-qian lan School of Chemistry and Materials Science Nanjing Normal University

Design and synthesize of highly active elelctrocatalysts for hydrogen evolution reaction(HER)is very desirable for the future sustainable clean-energy ***,we report a nickel-doped tungsten carbide and nitrogen-doped reduced graphene oxide composite(denote as Ni-WC/NRGO)by directly carbonizing polyoxometalates/conductive polymer/GO

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A High Stability imidazole-based covalent organic frameworks for Proton conduction

A High Stability imidazole-based covalent organic frameworks...

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中国化学会第八届全国配位化学会议

作者： Meng Lu Feng-Ming Zhang ya-qian lan School of Chemistry and Materials Science Nanjing Normal University

Proton-conduction materials are key components of fuel cells and transport protons from the anode to the cathode for the reduction of oxygen to produce an electrical *** organic frameworks(COFs)with ordered 1D nanochannels are a desirable platform for designing protonconduction ***,we desighed an imidazole-base COFs that exhibits intrinsic proton *** targeted COF was synthesized by condensation of 1,3,5-triformylphloroglucinol(TP)and 1,2,4,5-benzenentetramine tetrahydrochloride(TBA)using the Schiff base *** imidazole group are aligned on the two-dimensional(2D)layers at periodic intervals and promote the proton hopping inside the hexagonal one-dimensional *** proton conductivity of ImCOF was measured as 1.35×10 S cm with long-term stability at ambient temperature and 98%relative humidity(RH),the activation energy is 0.47 eV suggesting the Vehicular mechanism for proton *** study demonstrated that the high intrinsic proton conductivity of COFs shedding lights on their wide applications in proton-conduction materials.

关键词： Covalent organic frameworks(COFs) imidazole Proton-conduction

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