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Journal of Energy chemistry 2023年第5期80卷 58-67,I0003页

作者： Kai Zhang Zixiang Zhan Minzhi Zhu Haiwei Lai Xiangyang He Weiping Deng Qinghong Zhang Ye Wang state key laboratory of physical chemistry of solid surfaces Collaborative Innovation Center of Chemistry for Energy MaterialsInnovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM)College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina

Selective oxidation of biomass and its derivatives to dicarboxylic acids represents a promising route for biomass ***,the co-presence of multiple functional groups in biomass molecules makes the selective oxidation of particular functional a challenging ***,we demonstrate an efficient electrocatalytic system consisting of nickel oxide(NiO)and a nitroxyl radical,i.e.,2,2,6,6-tetrame thylpiperidine-1-oxyl(TEMPO)or 4-acetamido-TEMPO(ACT),for the selective oxidation of key bioplatform molecules including glucose,xylose and 5-hydroxymethylfurfural(HMF)into corresponding dicarboxylic acids,i.e.,glucaric acid,xylaric acid,and 2,5-furandicarboxylic acid(FDCA).NiO is clarified as the active catalyst for the oxidation of aldehyde in bio-platform molecules to carboxylic acid,while TEMPO or ACT is responsible for the oxidation of primary alcohol to *** combination of NiO and TEMPO or ACT significantly accelerated the tandem oxidation of aldehyde and hydroxyl groups in glucose,xylose and HMF,thus achieving excellent yields(83%-99%)of dicarboxylic ***,the combination catalyst enables the selective oxidation of glucose and xylose with high concentrations(e.g.,20 wt%),which offers a promising strategy for biomass valorization.

关键词： Biomass Electrocatalysis Nio Nitroxyl radical Dicarboxylic acid

Erratum to: Bimetallic clusters confined inside silicalite-1 for stable propane dehydrogenation

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Nano Research 2024年第4期17卷 3423-3423页

作者： Xueer Wei Jiawei Cheng Yubing Li Kang Cheng Fanfei Sun Qinghong Zhang Ye Wang state key laboratory of physical chemistry of solid surfaces Collaborative Innovation Center of Chemistry for Energy MaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Innovation laboratory for Sciences and Technologies of Energy Materials of fujian province(IKKEM) Xiamen 361005China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201800China Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201204China

Erratum to Nano Research,2023,16(8):10881–10889 https://***/10.1007/s12274-023-5953-y The equal contribution symbols were unfortunately *** of Xueer Wei1,Jiawei Cheng1,Yubing Li1,Kang Cheng1,2(✉),Fanfei Sun3,4(✉),Qinghong Zhang1(✉),and Ye Wang1,21 state key laboratory of physical chemistry of solid surfaces,Collaborative Innovation Center of chemistry for Energy Materials,College of chemistry and chemical Engineering,Xiamen University,Xiamen 361005,China 2 Innovation laboratory for Sciences and Technologies of Energy Materials of fujian province(IKKEM),Xiamen 361005,China 3 Shanghai Synchrotron Radiation Facility,Shanghai Advanced Research Institute,Chinese Academy of Sciences,Shanghai 201800,China 4 Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Shanghai 201204,China.

关键词： Xiamen confined China

Understanding reaction mechanisms of metal-free dinitrogen activation by methyleneboranes

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Chinese chemical Letters 2023年第2期34卷 210-213页

作者： Jie Zeng Jiaying Su Feiying You Jun Zhu state key laboratory of physical chemistry of solid surfaces and fujian Provincial key laboratory of Theoretical and Computational chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Dinitrogen activation under mild conditions is important but extremely challenging due to the inert nature of the N≡N triple bond evidenced by high bond dissociation energy(945 k J/mol) and large HOMOLUMO gap(10.8 e V). In comparison with largely developed transition metal systems, the reported main group species on dinitrogen activation are rare. Here, we carry out density functional theory calculations on methyleneboranes to understand the reaction mechanisms of their dinitrogen activation. It is found that the methyleneboranes without any substituent at the boron atom performs best on dinitrogen activation, which could be contributed to its small singlet-triplet gap. In addition, strong correlations are achieved on dinitrogen activation between the singlet-triplet energy gap and the reaction energies for the formation of the end-on products as well as the side-on ones. The principal interacting orbital analysis suggests that methyleneboranes can mimic transition metals to cleave the N≡N triple bond. Our findings could be helpful for experimental chemists aiming at dinitrogen activation by main group species.

关键词： Dinitrogen activation Methyleneborane NHC-stabilized borylene Reaction mechanism Singlet–triplet gap

Three-dimensional direct-writing via photopolymerization based on triplet-triplet annihilation

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Science China chemistry 2022年第11期65卷 2283-2289页

作者： Zhiye Wang Yusheng Zhang Yuming Su Cankun Zhang Cheng Wang state key laboratory for physical chemistry of solid surfaces iChEMCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China Innovation laboratory for Sciences and Technologies of Energy Materials of fujian province(IKKEM) Xiamen 361005China

3D direct-writing via photopolymerization based on two-photon absorption(TPA) can achieve excellent out-of-plane *** key to this technology is a quadratic intensity dependence in photoexciting the TPA photosensitizers. Triplet-triplet annihilation(TTA) also has similar nonlinear light-intensity dependence. As a result, TTA can also generate spatially confined excitation near the beam focus. Combining the photopolymerization reaction with the TTA system composed of palladium porphyrin and diphenylanthracene, 3D direct-writing micro-fabrication based on photopolymerization and the TTAwas *** out-of-plane resolution can reach 10 μm under continuous-wave laser excitation. TTA-based 3D direct-writing technology does not need an expensive femtosecond pulsed laser, showing the potential of a next-generation 3D printing technology.

关键词： triplet-triplet annihilation photopolymerization 3D printing energy transfer

Chiral Br?nsted acid-catalyzed asymmetric intermolecular[4+2]annulation of ynamides with para-quinone methides

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Science China chemistry 2023年第5期66卷 1467-1473页

作者： Hang-Hao Li Ya-Nan Meng Can-Ming Chen Yu-Qi Wang Zhi-Xin Zhang Zhou Xu Bo Zhou Long-Wu Ye key laboratory for chemical biology of fujian province and state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Jiangsu key laboratory of New Drug Research and Clinical Pharmacy School of PharmacyXuzhou Medical UniversityXuzhou 221004China state key laboratory of Elemento-Organic chemistry Nankai UniversityTianjin 300071China state key laboratory of Organometallic chemistry Chinese Academy of SciencesShanghai 200032China

Catalytic asymmetric transformations of ynamides have attracted considerable attention in recent ***,most of them were limited to intramolecular reactions or required metal ***,a chiral Br?nsted acid-catalyzed asymmetric intermolecular[4+2]annulation of ynamides with para-quinone methides(p-QMs)is disclosed,which not only represents the first metal-free protocol for catalytic asymmetric nucleophilic addition of ynamides to electrophiles,but also constitutes the first enantioselective annulation between p-QMs and *** methodology leads to the practical synthesis of biologically important chiral 4-aryl-3,4-dihydrocoumarins and *** control experiments indicate that the orthohydroxyphenyl substituted p-QMs could isomerize into ortho-quinone methides(o-QMs)in the presence of chiral catalyst,which further react with ynamides via enantioselective[4+2]annulation,to generate the chiral product.

关键词： stereoselective metal-free cyclization ynamides p-QMs

Spontaneous local redox reaction to passivate CNTs as lightweight current collector for high energy density lithium ion batteries

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Journal of Energy chemistry 2023年第5期80卷 553-561,I0013页

作者： Chao Lv Zhen Tong Shi-Yuan Zhou Si-Yu Pan Hong-Gang Liao Yao Zhou Jun-Tao Li College of Energy Xiamen UniversityXiamen 361005FujianChina state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina

Extensive usage of highly conductive carbon materials with large specific surface area(e.g.,carbon nanotubes,CNTs)in lithium ion batteries(LIBs),especially as current collector of anodes,suffers from low initial coulombic efficiency(ICE),large interfacial resistance,and severe embrittlement,as the large specific surface area often results in severe interfacial decomposition of the electrolyte and the formation of thick and fluffy solid electrolyte interphase(SEI)during cycling of ***,we demonstrate that when the CNT-based current collector and Na foil(which are being stacked intimately upon each other)are being placed in Na+-based organic electrolyte,local redox reaction between the Na foil and the electrolyte would occur spontaneously,generating a thin and homogeneous NaF-based passivating layer on the *** importantly,we found that owing to the weak solvation behaviors of Na+in the organic electrolyte,the resulting passivation layer,which is rich in NaF,is thin and dense;when used as the anode current collector in LIBs,the pre-existing passivating layer can function effectively in isolating the anode from the solvated Li+,thus suppressing the formation of bulky SEI and the destructive intercalation of solvated Li+.The relevant half-cell(graphite as anode)exhibits a high ICE of 92.1%;the relevant pouch cell with thus passivated CNT film as current collectors for both electrodes(LiCoO_(2)as cathode,graphite as anode)displays a high energy density of 255 Wh kg^(-1),spelling an increase of 50%compared with that using the conventional metal current collectors.

关键词： Lightweight current collector Passivating layer Initial coulombic efficiency High energy density storage

Promising Electrode and Electrolyte Materials for High-Energy-Density Thin-Film Lithium Batteries

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Energy & Environmental Materials 2022年第1期5卷 133-156页

作者： Jie Lin Liang Lin Shasha Qu Dongyuan Deng Yunfan Wu Xiaolin Yan Qingshui Xie Laisen Wang Dongliang Peng College of Materials State Key Laboratory for Physical Chemistry of Solid SurfacesFujian Key Laboratory of Materials GenomeCollaborative Innovation Center of Chemistry for Energy MaterialsXiamen UniversityXiamen 361005China

All-solid-state thin-film lithium batteries(TFLBs)are the ideal wireless power sources for on-chip micro/nanodevices due to the significant advantages of safety,portability,and *** the bottleneck for increasing the energy density of TFLBs,the key components of cathode,electrolyte,and anode are still underway to be *** this review,a brief history of TFLBs is first outlined by presenting several TFLB *** on the state-of-the-art materials developed for lithium-ion batteries(LIBs),the challenges and related strategies for the application of those potential electrode and electrolyte materials in TFLBs are *** the advanced manufacture and characterization techniques,the recent advances of TFLBs are reviewed for pursuing the high-energy-density and long-termdurability demands,which could guide the development of future TFLBs and analogous all-solid-state lithium batteries.

关键词： all-solid-state high-energy-density lithium battery physical vapor deposition thin film

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 *** 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 *** 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 *** 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 *** 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

Antiaromaticity-promoted radical anion stability in α-vinyl heterocyclics

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Organic chemistry Frontiers 2022年第5期9卷 1427-1436页

作者： Lu Lin Jun Zhu state key laboratory of physical chemistry of solid surfaces Fujian Provincial Key Laboratory of Theoretical and Computational ChemistryDepartment of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005People’s Republic of China

As an electron-rich species,radical anions have a wide range of applications in organic *** addition,aromaticity is an essential concept in chemistry that has attracted considerable attention from experimentalists and... 详细信息

关键词： synthesis radical heterocyclic

Electrochemistry enabled selective vicinal fluorosulfenylation and fluorosulfoxidation of alkenes

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Chinese chemical Letters 2022年第4期33卷 2009-2014页

作者： Yi Yu Yimin Jiang Shaofen Wu Zhaojiang Shi Jinnan Wu Yaofeng Yuan keyin Ye key laboratory of Molecule Synthesis and Function Discovery(fujian province University) College of ChemistryFuzhou UniversityFuzhou 350108china state key laboratory of physical chemistry of solid surfaces Xiamen UniversityXiamen 361005china

Both sulfur and fluorine play important roles in organic synthesis, the life science, and materials *** direct incorporation of these elements into organic scaffolds with precise control of the oxidation states of sulfur moieties is of great significance. Herein, we report the highly selective electrochemical vicinal fluorosulfenylation and fluorosulfoxidation reactions of alkenes, which were enabled by the unique ability of electrochemistry to dial in the potentials on demand. Preliminary mechanistic investigations revealed that the fluorosulfenylation reaction proceeded through a radical-polar crossover mechanism involving a key episulfonium ion intermediate. Subsequent electrochemical oxidation of fluorosulfides to fluorosulfoxides were readily achieved under a higher applied potential with the adventitious H;O in the reaction mixture.

关键词： Alkene Chemoselectivity Electrochemistry Fluorine Sulfur