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Insight into the mechanism of 5-hydroxymethylfurfural electroreduction to 2,5-bis(hydroxymethyl)furan over Cu anchored N-doped carbon nanosheets

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Nano Research 2024年第9期17卷 7991-7999页

作者： Haoran Wu Xinwei Chen Haishan Xu Runlu Yang Xin Wang Junying Chen Zhenbing Xie Liang Wu yiyong mai School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Key Laboratory of Electrical Insulation and Thermal AgeingShanghai Jiao Tong UniversityShanghai 200240China Department of Chemistry Tangshan Normal UniversityTangshan 063000China

Design of non-noble metal electrocatalysts for biomass conversion to high-value chemicals and understanding the related catalytic mechanisms are of profound significance but have remained a major ***,we developed a novel biomass-derived electrocatalyst(denoted as Cu/NC),featuring with electron-deficient copper nanoparticles anchored on N-doped carbon nanosheets,for the electrochemical reduction of 5-hydroxymethylfurfural(HMF)to 2,5-bis(hydroxymethyl)furan(BHMF,a vital precursor of functional polymers).The optimized Cu/NC electrocatalyst exhibited an excellent performance with high Faradaic efficiency(89.5%)and selectivity(90.8%)of BHMF at a low concentration of HMF(18.1 mM).Even at a very high HMF concentration(108.6 mM),the Faraday efficiency and selectivity of BHMF could still reach 74.8%and 81.1%,*** performance approached those of the reported noble metal-based *** study revealed that the N doping in the Cu/NC catalyst could regulate the electronic structure of Cu,strengthening the adsorption of the HMF carbonyl group,and thus boosting the selectivity of ***,strong electronic metal-support interactions of Cu and the N-doped carbon support optimized the charge transfer rate,thus promoting the dissociation of water to the active hydrogen(H^(*))species and boosting the reaction kinetic rate of H^(*)and HMF.

关键词： biomass 5-hydroxymethylfurfural electrochemical reduction N-doped carbon materials 2,5-bis(hydroxymethyl)furan

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What Can Topology Bring to Chemistry?

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CCS Chemistry 2024年第9期6卷 2084-2109页

作者： Wei Wang Songtao Zhou Xiujun Yu Qing-Hui Guo Yanhang Ma Jie Song Liang Zhang Xuzhou Yan Lu Han Qing Liao Xiaopeng Li Wen-Bin Zhang yiyong mai Shaodong Zhang Shunai Che Hai-Bo Yang Xuefeng Fu Mei-Xiang Wang School of Chemistry and Molecular Engineering East China Normal UniversityShanghai 200062 Hangzhou Institute of Medicine Chinese Academy of SciencesHangzhou 310022Zhejiang College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060Guangdong MOE Key Laboratory of Bioorganic Phosphorous and Chemical Biology Department of ChemistryTsinghua UniversityBeijing 100084 School of Physical Science and Technology and Shanghai Key Laboratory of High-Resolution Electron Microscopy ShanghaiTech UniversityShanghai 201210 School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesState Key Laboratory of Composite MaterialsShanghai Key Laboratory for Molecular Engineering of Chiral DrugsShanghai Jiao Tong UniversityShanghai 200240 School of Chemical Science and Engineering Tongji UniversityShanghai 200092 Beijing Key Laboratory for Optical Materials and Photonic Devices Department of ChemistryCapital Normal UniversityBeijing 100048 Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationCenter for Soft Matter Science and EngineeringCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871 Department of Chemical Sciences National Natural Science Foundation of ChinaBeijing 10085

The unique mathematical perspectives and principal concepts of topology have not only promoted the development of other branches of mathematics but have also deeply influenced other subjects,particularly physics and *** minireview aims to elucidate the substantial influence of topology on chemistry by critically examining both the contributions of topology to current chemical science and its potential future *** will discuss the topology of molecular structures and assemblies across various scales—from small molecules and mechanically interlocked molecules to polymers,biomacromolecules,and supramolecular *** discussion will include an exploration of cutting-edge techniques for characterizing topological features,underscoring the role of topology as a novel paradigm for the design and synthesis of new molecular ***,a critical analysis of topology’s role in the development of functional materials—such as photonic materials,polymers,biomacromolecules,and chiral materials—will demonstrate its emerging significance as a crucial parameter in unveiling novel properties and *** topology’s formidable potential,it is anticipated to be used increasingly to address pivotal challenges within chemistry and adjacent disciplines.

关键词： chemical topology topological invariants molecular graphs links and knots structureproperty relationship

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Double diamond structured bicontinuous mesoporous titania templated by a block copolymer for anode material of lithium-ion battery

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Nano Research 2021年第4期14卷 992-997页

作者： Qingqing Sheng Qian Li Luoxing Xiang Tao Huang yiyong mai Lu Han School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Key Laboratory of Electrical Insulation and Thermal AgeingShanghai Jiao Tong Universityy 800 Dongchuan RoadShanghai 200240China School of Chemical Science and Engineering Tongji UniversityShanghai 200092China

Titania has received considerable attention as a promising anode material of Li-ion battery(LIB).Controlling the structure and morphology of titania nanostructures is crucial to govern their ***,we report a mesoporous titania scaffold with a bicontinuous shifted double diamond(SDD)structure for anode material of *** titania scaffold was synthesized by the cooperative self-assembly of a block copolymer poly(ethylene oxide)-block-polystyrene template and titanium diisopropoxide bis(acetylacetonate)as the inorganic precursor in a mixture solvent of tetrahydrofuran and HCl/*** structure shows tetragonal symmetry(space group I4_(1)/amd)comprising two sets of diamond networks adjoining each other with the unit cell parameter of a=90 nm and c=127 nm,which affords the porous titania a specific surface area(SSA)of 42 m^(2)·g^(-1)with a mean pore diameter of 38 *** as an anode material of LIB,the bicontinuous titania scaffold exhibits a high specific capacity of 254 mAh·g^(-1)at the current density of 1 A·g^(-1)and an alluring self-improving feature upon charge/discharge over 1,000 *** study overcomes the difficulty in building up ordered bicontinuous functional materials and demonstrates their potential in energy storage application.

关键词： bicontinuous structure block copolymer lithium-ion battery mesoporous titania self-assembly

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High-loading single cobalt atoms on ultrathin MOF nanosheets for efficient photocatalytic CO_(2) reduction

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Science China Chemistry 2023年第2期66卷 570-577页

作者： Quan Zuo Rui Cui Lei Wang Yuling Wang Chunyang Yu Liang Wu yiyong mai Yongfeng Zhou School of Packaging and Materials Engineering Hunan University of TechnologyZhuzhou412007China School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesState Key Laboratory of Metal Matrix CompositesShanghai Key Laboratory of Electrical Insulation and Thermal AgeingShanghai Jiao Tong UniversityShanghai200240China

Based on suitable scaffolds,constructing high-loading single-atom catalysts is a promising strategy to achieve highly efficient ***,using ultrathin metal-organic framework(MOF)nanosheets(2.4±0.5 nm)as the support,single-atom catalysts with high cobalt loading(6.0 wt%)were constructed(denoted as Co-MNSs)by a simple bottom-up synthetic *** catalytic system of Co-MNSs exhibited an outstanding photocatalytic CO_(2)-to-CO evolution rate of 7,041μmol g^(-1)h^(-1)and a selectivity of 86%in aqueous media under visible-light irradiation,which has reached the top level of the reported MOF-based *** control experiments and theoretical calculation revealed that the Co-N_(4)moiety in the MOF nanosheets acted as the active site for the photocatalytic CO_(2)-to-CO *** boosted photocatalytic performance could be ascribed to the high aspect-ratio of layered Co-MNSs providing abundant accessible active sites on their surfaces,which reduced the energy barrier,improved the charge separation efficiency,and also facilitated the adsorption of CO_(2)to form the reactive radicals of**** study provides an appealing strategy for constructing high-loading single-atom catalysts and demonstrates the significance of 2D ultrathin MOF nanosheets as the support in boosting CO_(2)photoreduction efficiency.

关键词： two-dimensional material single-atom catalyst metal-organic framework photocatalysis CO_(2)reduction

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Single-Metal-Atom Polymeric Unimolecular Micelles for Switchable Photocatalytic H_(2) Evolution

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CCS Chemistry 2021年第7期3卷 1963-1971页

作者： Quan Zuo Kun Feng Jun Zhong yiyong mai Yongfeng Zhou School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesState Key Laboratory of Metal Matrix CompositesShanghai Key Laboratory of Electrical Insulation and Thermal AgeingShanghai Jiao Tong UniversityShanghai 200240 Institute of Functional Nano and Soft Materials Laboratory(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123

Developing“green”catalytic systems with desirable performance such as good water solubility,recyclability,and switchability is a great ***,to address this challenge,we extend the concept of polymeric unimolecular micelles(a typical selfassembled structure)to the construction of a stimuli-responsive and recoverable molecular catalyst with single-metal atoms that exhibits switchable photocatalytic activity for water splitting.

关键词： polymer self-assembly unimolecular micelle stimuli-responsiveness photocatalyst water splitting

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Core-shell nanostructure of single-wall carbon nanotubes and covalent organic frameworks for supercapacitors

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Chinese Chemical Letters 2017年第12期28卷 2269-2273页

作者： Yang Han Qin Zhang Nantao Hu Xue Zhang yiyong mai Jiaqiang Liu Xiaolin Hua Hao Wei Key Laboratorty for Thin Film and Microfabrication Technology of Ministry of Education School of Electronic Information and Electrical Engineering School of Chemistry and Chemical Engineering Shanghai Jiao Tong University Department of Oral and Cranio-Maxillofacial Ninth People’s Hospital Xinhua Hospital Shanghai Jiao Tong University School of Medicine

Covalent organic frameworks （COFs） were nano-coated onto single-walled carbon nanotubes （SWCNTs） by in situ polymerization of TpPa-COFs together with SWCNTs under solvotherma] conditions. At the molecular level, the COF/SWCNT interface can be efficiently controlled. Thus, the TpPa-COF-SWCNTs nano-hybrid wire, which combines the excellent conductivity of SWCNTs and the high porosity and good redox activity of TpPa-COFs, was employed as active electrode materials for supercapacitors. The strategy reported in this work can give guidance for the design of other similar COF-based electrodes, and hold a great potential in energy storages

关键词： Covalent organic frameworks Supercapacitor Porous materialsn Energy storages Nano-hybrid wire

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Controlled Synthesis of Porous Carbon Nanostructures with Tunable Closed Mesopores via a Silica-Assisted Coassembly Strategy

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CCS Chemistry 2021年第5期3卷 1410-1422页

作者： Binbin Guo Chen Li Haoran Wu Jiahang Chen Jiulin Wang Hao Wei yiyong mai School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Key Laboratory of Electrical Insulation and Thermal AgeingShanghai Jiao Tong UniversityShanghai 200240 School of Electronic Information and Electrical Engineering Shanghai Jiao Tong UniversityShanghai 200240

Controllable fabrication of mesoporous carbon nanoparticles(MCNs)with tunable pore structures is of great interest,due to the remarkable effect of pore structure on electrochemical performance of the ***,it has remained a major ***,we demonstrate the controlled synthesis of MCNs with tunable closed pore structures via a silica-assisted coassembly strategy,which employs polystyrene-block-poly(ethylene oxide)diblock copolymers as soft template,phenolic resol and tetraethyl orthosilicate as carbon and silica precursors,*** simply varying the sequential cross-linking of the silica and carbon precursors or the copolymer composition,novel MCNs with alluring spherical,hollow-hoop-structured,or yolk-shell-like closed mesopores are tunably *** particular,serving as cathode materials of lithium-sulfur batteries,the resultant silica-hybridized MCNs with the exceptional hollow-hoop mesopores and a moderate sulfur-loading content of 46 wt%exhibit top-level electrochemical *** study opens an avenue for tunable construction of mesoporous particles with closed pores and provides clues for the effect of pore geometry on the electrochemical performance of porous cathode materials for lithium-sulfur batteries.

关键词： block copolymer self-assembly mesoporous carbon nanoparticles pore structure lithium-sulfur battery

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Bowl-shaped NiCo2O4 nanosheet clusters as electrode materials for high-performance asymmetric supercapacitors

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Science China Materials 2020年第12期63卷 2456-2464页

作者： Ruiyi Liu Haoran Wu Zheng Wang Hao Wei yiyong mai School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Key Laboratory of Electrical Insulation and Thermal AgeingSchool of Electronic Information and Electrical EngineeringShanghai Jiao Tong UniversityShanghai 200240China

The development of transition metal oxidebased electrode materials with proper controlled structures is highly desirable for high-performance ***,it remains a major ***,we present the first synthesis of bowl-like Ni Co2O4nanosheet clusters through a simple soft template guided hydrothermal *** resulting bowl-like clusters consist of numerous Ni Co2O4nanosheets with an average thickness of 19 nm and possess a mean diameter of 1μm along with a specific surface area of40 m2g^-***,serving as an electrode material in a three-electrode system,the bowl-like Ni Co2O4nanosheet clusters exhibit a high specific capacity of 1068 F g^-1at a current density of 1 A g^-1and excellent cycling stability with90%capacitance retention after 5000 charge-discharge ***,an asymmetric supercapacitor(ASC)assembled with the Ni Co2O4clusters and activated carbon(AC)as the two electrodes exhibits a high specific capacitance of 129 F g^-1at 1 A g^-1,along with a high energy density of 33 W h kg^-1at a power density of 0.66 k W kg^-*** performance is superior to those of many commercial *** study opens a new avenue for the construction of ordered complex particles with controlled architectures for energy storage and conversion applications.

关键词： bowl-like structure NiCo2O4 nanosheet cluster soft template asymmetric supercapacitors

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Fabrication of sulfur-doped cove-edged graphene nanoribbons on Au(111)

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Chinese Physics B 2021年第7期30卷 484-488页

作者： Huan Yang Yixuan Gao Wenhui Niu Xiao Chang Li Huang Junzhi Liu yiyong mai Xinliang Feng Shixuan Du Hong-Jun Gao Institute of Physics and University of Chinese Academy of Sciences(CAS) Beijing 100190China Center for Advancing Electronics Dresden(cfaed)&Faculty of Chemistry and Food Chemistry Technische Universität Dresden01062 DresdenGermany School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Key Laboratory of Electrical Insulation and Thermal AgeingShanghai Jiao Tong UniversityShanghai 200240China Department of Chemistry and State Key Laboratory of Synthetic Chemistry The University of Hong KongHong KongChina CAS Center for Excellence in Topological Quantum Computation University of Chinese Academy of SciencesBeijing 100190China

The on-surface synthesis from predesigned organic precursors can yield graphene nanoribbons(GNRs)with atomically precise widths,edge terminations and dopants,which facilitate the tunning of their electronic ***,we report the synthesis of novel sulfur-doped cove-edged GNRs(S-CGNRs)on Au(111)from a specifically designed precursor containing thiophene *** tunneling microscopy and non-contact atomic force microscopy measurements elucidate the formation of S-CGNRs through subsequent polymerization and cyclodehydrogenation,which further result in crosslinked branched *** tunneling spectroscopy results reveal the conduction band minimum of the S-CGNR locates at 1.2 e ***-principles calculations show that the S-CGNR possesses an energy bandgap of 1.17 e V,which is evidently smaller than that of an undoped cove-edged GNR(1.7 e V),suggesting effective tuning of the bandgap by introducing sulfur *** increasing the coverage of precursors close to a monolayer results in the formation of linear-shaped *** fabrication of S-CGNRs provides one more candidate in the GNR toolbox and promotes the future applications of heteroatom-doped graphene nanostructures.

关键词： on-surface synthesis sulfur-doped cove-edged graphene nanoribbons scanning tunneling microscopy non-contact atomic force microscopy

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Positron Annihilation and Chemistry of Groups in Hyperbranched Polymers

Positron Annihilation and Chemistry of Groups in Hyperbranch...

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The 9th International Workshop on Positron and Positronium Chemistry

作者： Wei Gong~(*1) Ning Qi~2 Bo Wang~2 yiyong mai~3 Deyue Yan~3 1 School of Municipal and Environmental Engineering,Harbin Institute of Technology,Harbin 150090,PR China 2 Department of Physics,Wuhan University,430072,China 3 College of Chemistry and Chemical Engineering,Shanghai Jiao Tong University,Shanghai 200240,China

In this paper,both lifetime and intensity in hyperbranched polymers were measured by using positron annihilation lifetime spectroscopy (PALS) measurements. Ortho-positronium properties upon the degree of branching (DB) have been studied;o-Ps lifetimes maintain a constant while an increase in o-Ps intensities has been detected with DB *** is inconsistent with author’s prediction and indicate that interactions between positronium and the free-volumes are strongly depend on not only the free-volume size properties but also its chemistry environment,due to the variations in the distribution of the different ending groups:-OH and -CH,caused by DB changes in hyperbranched *** present works demonstrate that in the polar-polymeric application of PALS, effects of the distribution of polar groups should be properly taken into consideration.

关键词： degree of branching hyperbranched positron annihilation free-volume

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