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energy & Environmental materials 2024年第4期7卷 74-82页

作者： Manying Cui Hongyang Zhao Yanyang Qin Shishi Zhang Ruxin Zhao Miao Zhang Wei Yu Guoxin Gao Xiaofei Hu Yaqiong Su Kai Xi Shujiang Ding school of chemistry Engineering Research Center of Energy Storage Materials and Devices Ministry of Education State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University Department of materials and Environmental chemistry Stockholm University

Inhomogeneous lithium-ion （Li+） deposition is one of the most crucial problems,which severely deteriorates the performance of solid'State lithium metal batteries （LMBs）.Herein,we discovered that covalent organic framework （COF-1） with periodically arranged boron-oxygen dipole lithiophilic sites could directionally guide Li+even deposition in asymmetric solid polymer electrolytes.

关键词： covalent organic framework ion transport regulation lithium metal battery solid polymer electrolyte

Photoredox catalytic alkylarylation of alkynes with arylsulfonylacetate as bifunctional reagent

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Science China chemistry 2024年第6期67卷 2022-2028页

作者： Chonglong He Min Wang Yulong Wang Lirong Zhao Youkang Zhou Keyuan Zhang Shenyu Shen Yaqiong Su Xin-Hua Duan Le Liu school of chemistry Engineering Research Center of Energy Storage Materials and DevicesMinistry of EducationXi’an Key Laboratory of Sustainable Energy Material ChemistryXi’an Jiaotong UniversityXi’an710049China

Difunctionalization of alkynes represents a powerful and straightforward approach to the synthesis of complex ***,the radical difunctionalization of alkynes mediated by bifunctional reagents remains challenging and underexplored,despite significant progress having been made in alkene ***,we report a novel arylsulfonylacetate skeleton in which aryl rings are attached to acetates through SO_(2),serving as a powerful bifunctional reagent for the alkylarylation of alkynes via vinyl-radical intermediate under photoredox *** modular bifunctional reagent enables the simultaneous incorporation of a wide range of functional groups,including(hetero)aryl ring and alkyl carboxylate into alkynes,resulting in synthetically valuable all-carbon tetrasubstituted alkene *** transformation is distinguished by its redox-neutral nature,readily accessible starting materials,compatibility with diverse functional groups and its capacity to facilitate convergent *** utility of this approach was further demonstrated by the late-stage functionalization of complex molecules and the preparation of fluorescent molecules and anti-cancer drugs.

关键词： bifunctional reagent photoredox catalysis Smiles rearrangement alkylarylation tetrasubstituted acyclic all-carbon olefins

Progress in processing of porous titanium:a review

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Rare Metals 2024年第5期43卷 1932-1955页

作者： Xiao-Li Yang Xian-Feng Du Zhi-Lin Xu Zhong-Shuai Liang Li-Long Xiong Engineering Research center of energy Storage materials and Devices Ministry of EducationSchool of ChemistryXi'an Jiaotong UniversityXi'an 710049China

As a novel structural and functional material,porous titanium and its alloys have been widely used in the aerospace,marine engineering and biomedical fields due to their high corrosion resistance,low density,good biocompatibility and excellent mechanical ***,in this paper,a comprehensive review of powder metallurgy(PM)(including additive manufacturing(AM)processes)for fabricating porous titanium is firstly covered in terms of their working principles,capabilities,shortcomings and ***,the influencing factors of various methods on final pore structure of porous Ti are ***,a summary of the chemical methods(CM)to obtain the porous Ti is also provided,such as dealloying method and reduction ***,the tendency and direction of preparation technology as well as application of porous titanium were prospected.

关键词： Porous titanium Powder metallurgy Chemical method Pore structure Processing process

The New Methods for Characterization of Molecular Weight of Supramolecular Polymers

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Chinese Journal of Polymer Science 2024年第10期42卷 1403-1413页

作者： Hui Liu Rui Hu Zi-Qing Hu Xiao-Fan Ji Key Laboratory of materials chemistry for energy Conversion and Storage Ministry of Education Hubei Key Laboratory of Materials Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective Materials School of Chemistry and Chemical Engineering Huazhong University of Science and Technology

Supramolecular polymers, as a type of dynamic polymers, are subordinate to the interdisciplinary field of polymer chemistry and supramolecular chemistry, whose development has greatly promoted the prosperity of new materials. Notably, molecular weight is one of the most important parameters of supramolecular polymers, which affects the physical/chemical properties and processing applications of *** new methods for characterizing the molecular weight of supramolecular polymers is crucial for advancing the development of supramolecular polymers. In this review, we elaborate and summarize three strategies for characterizing the molecular weight of supramolecular polymers that recently reported by our research group according to the characteristics of supramolecular polymers, including (1) the molecular weight distinction corresponding to variable fluorescence colors,(2) matching different molecular weights with different fluorescence lifetime,(3) transforming supramolecular polymers into mechanically interlocked polymers or covalent polymers. Besides, we also discuss the limitations of current methods for characterizing supramolecular polymers. We hope that this review can promote the development of supramolecular polymers and significantly inspire to exploit new methods to characterizing molecular weight of supramolecular polymers.

关键词： Dynamic polymers Mechanically interlocked polymers Molecular weight Self-assembly Supramolecular polymers

Selective Hydrodeoxygenation of Lignin-Derived Vanillin via Hetero-Structured High-Entropy Alloy/Oxide Catalysts

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energy & Environmental materials 2024年第3期7卷 206-214页

作者： Yan Sun Kaili Liang Ren Tu Xudong Fan Charles Q.Jia Zhiwen Jia Yingnan Li Hui Yang Enchen Jiang Hanwen Liu Yonggang Yao Xiwei Xu Key Laboratory for Biobased materials and energy of Ministry of Education College of Materials and EnergySouth China Agricultural University Department of Chemical Engineering and applied chemistry University of Toronto State Key Laboratory of materials Processing and Die & Mould Technology School of Materials Science and EngineeringHuazhong University of Science and Technology

The chemoselective hydrodeoxygenation of natural lignocellulosic materials plays a crucial role in converting biomass into value-added *** their complex molecular structures often require multiple active sites synergy for effective activation and achieving high ***,it is reported that a high-entropy alloy (HEA) on high-entropy oxide (HEO)hetero-structured catalyst for highly active,chemoselective,and robust vanillin *** heterogenous HEA/HEO catalysts were prepared by thermal reduction of senary HEOs (NiZnCuFeAIZrOx),where exsolvable metals (e.g.,Ni,Zn,Cu) in situ emerged and formed randomly dispersed HEA nanoparticles anchoring on the HEO *** catalyst exhibits excellent catalytic performance:100%conversion of vanillin and 95%selectivity toward high-value 2-methyl-4 methoxy phenol at low temperature of 120℃,which were attributed to the synergistic effect among HEO matrix(with abundant oxygen vacancies),anchored HEA nanoparticles (having excellent hydrogenolysis capability),and their intimate hetero-interfaces(showing strong electron transferring effect).Therefore,our work reported the successful construction of HEA/HEO heterogeneous catalysts and their superior multifunctionality in biomass conversion,which could shed light on catalyst design for many important reactions that are complex and require multifunctional active sites.

关键词： biomass conversion heterogeneous catalysts high-entropy oxide high-entropy alloys lignin pyrolysis

Polypyride intercalation boosting the kinetics and stability of V3O7·H2O cathodes for aqueous zinc-ion batteries

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Journal of energy chemistry 2024年第10期97卷 361-370页

作者： Qingqing He Jie Bai Mengda Xue Yanxin Liao Huayu Wang Mujun Long Lingyun Chen Department of applied chemistry School of Chemistry and Chemical Engineering Chongqing University Laboratory of materials and Metallurgy College of Materials Science and Engineering Chongqing University

V3O7·H2O（VO） is a high capacity cathode material in the field of aqueous zinc ion batteries（AZIBs）,but it is limited by slow ion migration and low electrical *** this paper,polypyridine（PPyd） intercalated VO with nanoribbon structure was prepared by a simple in-situ pre-intercalation,which is noted *** total density of states（TDOS） shows that after the pre-intercalation of PPyd,an intermediate energy level appears between the valence band and conduction band,which provides a step that can effectively reduce the band gap and enhance the electron ***,the density functional theory（DFT） results found that Zn2+is more easily de-intercalated from the V-O skeleton,which proves that the embeddedness of PPyd improves the diffusion kinetics of Zn2+.Electrochemical studies have shown that VO-PPyd cathode materials exhibit excellent rate performance(high specific capacity of 465 and 192 mA h g-1at 0.2 and 10 A g-1,respectively) and long-term cycling performance（92.7%capacity retention rate after 5300 cycles）,due to their advantages in structure and *** importantly,the energy density of VO-PPyd//Zn at 581 and 5806 W kg-1is 375 and 247 W h kg-1,***-PPyd exhibits excellent electrochemical properties compared to previously reported vanadium based cathodes,which makes it highly competitive in the field of high-performance cathode materials of AZIBs.

关键词： Aqueous zinc ion batteries DFT calculation Electrical conductivity Ion migration Polypyridine V3O7·H2O

Nickel-catalyzed carbonylative four-component 1,4-dicarbofunctionalization of 1,3-enynes

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Science China chemistry 2024年第6期67卷 2029-2038页

作者： Yan Zhao Qi-Chao Shan Hong Xin Pin Gao Xu Yang Xin-Hua Duan Li-Na Guo Department of chemistry School of ChemistryXi’an Key Laboratory of Sustainable Energy Material Chemistry and Engineering Research Center of Energy StorageMaterials and DevicesMinistry of EducationXi’an Jiaotong UniversityXi’an710049China school of Electrical Engineering Xi’an Jiaotong UniversityXi’an710049China

An efficient Ni-catalyzed four-component 1,4-carbocarbonylation of 1,3-enynes with activated alkyl halides and arylboronic acids under atmospheric pressure of CO is *** tuning the electronic and steric effects of alkyl radicals,both electronrich and electron-deficient 1,3-enynes were compatible with this *** protocol features mild conditions,broad substrate scope,excellent functional group compatibility and facile gram-scale synthesis,providing a practical approach to the quaternary carbon center-containing allenyl *** study revealed that the acyl-NiIIspecies plays an important role in both the coupling and the alkyl radical generation processes.

关键词： Ni catalysis four-component 1 4-carbocarbonylation 1 3-enynes

Molecule aging induced by electron attacking

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Journal of energy chemistry 2024年第6期93卷 519-525,I0013页

作者： Ping Song Yining Dong Xue Gong Mingbo Ruan Baoxin Ni Xuanhao Mei Kun Jiang Weilin Xu State Key Laboratory of Electroanalytical chemistry and Jilin Province Key Laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina school of applied chemistry and Engineering University of Science and Technology of Chin1Hefei 230026AnhuiChina Shanghai Key Laboratory of Molecular Catalysis and Innovative materials Collaborative Innovation Center of Chemistry for Energy MaterialsDepartment of ChemistryFudan UniversityShanghai 200438China

Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed *** further confirm such"molecule aging"via a long-term electron attacking to age water(H_(2)O)*** IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water *** facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule *** exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water molecule is lower than the fresh water on the same Pt/C *** density functional theory calculations indicate that the shortened O-H bond in H_(2)O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water *** results indicate significantly that the molecule aging can produce materials with new functions for new possible applications.

关键词： Aging of molecules Electron attacking Full width at half maxima Hydrogen evolution reaction

Binding SnO2 Nanoparticles with MoS2 Nanosheets Toward Highly Reversible and Cycle-Stable Lithium/Sodium Storage

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energy & Environmental materials 2024年第4期7卷 135-142页

作者： Deliang Cheng Wenbiao Zhang Yi Tang Qingsheng Gao Renzong Hu Lichun Yang Min Zhu Institute of Advanced materials Jiangxi Normal University school of materials Science and Engineering Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials South China University of Technology College of chemistry and materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications Jinan University Department of chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Laboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials Fudan University

SnO2,with its high theoretical capacity,abundant resources,and environmental friendliness,is widely regarded as a potential anode material for lithium-ion batteries （LIBs）.Nevertheless,the coarsening of the Sn nanop... 详细信息

关键词： 1 T-MoS2 heterostructure lithium-ion batteries Sn coarsening SnO2

Simultaneous integration of Fe clusters and NiFe dual single atoms in nitrogen-doped carbon for oxygen reduction reaction

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Nano Research 2024年第4期17卷 2291-2297页

作者： Jirong Bai Yuebin Lian Yaoyao Deng Mei Xiang Peng Xu Quanfa Zhou Yawen Tang Yaqiong Su Research center of Secondary Resources and Environment School of Chemical Engineering and MaterialsChangzhou Institute of TechnologyChangzhou 213022China Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China school of chemistry Engineering Research Center of Energy Storage Materials and Devices of Ministry of EducationNational Innovation Platform(Center)for Industry-Education Integration of Energy Storage TechnologyXi’an Jiaotong UniversityXi’an 710049China

Atomically-dispersed iron-based electrocatalysts are promising substitutes for noble metal electrocatalysts because of excellent performance in oxygen reduction reaction(ORR).Rationally modulating the local coordination environment of the Fe site and optimizing the binding energy of oxygen reduction intermediates are effective strategies to optimize ORR ***,we report a new method in which Ni is introduced to construct NiFe dual single atoms and iron nanoclusters loaded on the nitrogen-doped carbon with a highly porous *** design plays a synergistic role of dual single atoms and clusters,optimizes the 3d orbital and Fermi level of Fe,breaks the symmetrical structure of Fe-N_(4),and effectively improves the adsorption/desorption behavior of the oxygen-containing *** tests show FeNCs/NiFeSAs-NC has an excellent intrinsic *** calculations show the oxygen-containing species on the Ni active site will move to the middle of NiFe(bridge site connection)after optimization and that the key step is OH desorption,with a reaction energy of 0.27 *** electron exchange between NiFe-N6 and Fe-cluster is very strong,further indicating the introduction of Ni species and Fe clusters has a regulatory effect on the electronic structure of Fe-N_(4).

关键词： NiFe dual single atoms Fe clusters OH*adsorption energy oxygen reduction reaction