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Immobilizing Triphenylamine with Photoredox Inert Sr^(2+)Forming Sr-MOF with Controlled Electron Migration for Photocatalytic Oxidation of Thiols to Disulfides

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Chinese Journal of Chemistry 2024年第10期42卷 1093-1099页

作者： Ying-Xia Wang Fang Zheng Dong-Xia Song Bao-Yue Niu Lu-Qian Deng Xian-Ming Zhang key laboratory of magnetic molecules and magnetic information materials(ministry of education) Schoolof Chemistry and Materials ScienceShanxi Normal UniversityTaiyuanShanxi 030006China key laboratory of Interface Science and Engineering in Advanced Material(ministry of education) College of ChemistryTaiyuan University of TechnologyTaiyuanShanxi 030024China

The photocatalytic oxidative coupling of thiols is one of the most popular methods to synthesize the disulfides.Triphenylamine and its derivatives(TPAs)are promising for the above reaction,but suffer from the easy polymerization and difficult separation.To overcome these obstacles while controlling the photogenerated electrons transfer directly to target substrates,herein,we constructed one TPA-based metal-organic framework(MOF),(Me_(2)NH_(2))[Sr(TCBPA)]·DMA·3H_(2)O(1),by direct self-assembly of tris(4′-carboxybiphenyl)amine(H_(3)TCBPA)and photoredox inert strontium ion(Sr^(2+)).DFT calculations revealed that the valence band maximum(VBM)and the conduction band minimum(CBM)are mainly located on TCBPA^(3-),successfully inhibiting the undesirable electron migration to metal nodes.Experimental results indicated that 1 displays superior performance than homogeneous H_(3)TCBPA,which may result from the abundant π…π and C—H…π interactions between the well-arranged TCBPA^(3-)and the build-in electric field between the anionic framework and the Me_(2)NH^(2+).This work highlights that immobilizing TPAs into MOFs is one promising approach to designing heterogeneous photocatalysts for the synthesis of disulfides by oxidative coupling of thiols.

关键词： Triphenylamine Metal-organic frameworks Strontium Photooxidation Thiols Disulfides

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Palladium Complexes with N,O-Bidentate Ligands Based on N-Oxide Units from Cyclic Secondary Amines:Synthesis and Catalytic Application in Mizoroki-Heck Reaction

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Chinese Journal of Chemistry 2024年第3期42卷 294-300页

作者： Xuefeng Jia Yanyan Wen Changhui He Xianqiang Huang key laboratory of magnetic molecules and magnetic information materials of ministry of education School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuanShanxi030032 China Shandong Provincial key laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry & Chemical EngineeringLiaocheng UniversityLiaochengShandong252059 China

Palladium-catalyzed Mizoroki-Heck reaction is a powerful and efficient method for construction of Csp2–Csp2 bonds.Herein,four palladium complexes(I—IV)with N,O-bidentate ligands(L1—L4)based on N-oxide units from cyclic secondary amines were easily synthesized and successfully applied in Mizoroki-Heck reaction of aryl bromides with electron-deficient olefins.X-ray diffraction analyses indicated the palladium(II)atom of II took the distorted square planar geometry and was four-coordinated by nitrogen and oxygen atoms from two ligands(L2).Two free chloride ions were presented as counter anions in complex II.But the palladium(II)center of IV was coordinated by nitrogen and oxygen atoms from one ligand(L4)as well as two chlorine atoms,which exhibited the nearly square-planar geometry.The study on catalytic properties of palladium complexes revealed that complex II exhibited high activity superior to the other complexes.The coupling reactions of a series of aryl bromides and olefin derivatives proceeded in the presence of 2—5 mol%palladium complex II,giving the desired products in good to excellent yields.The advantages of this method such as good compatibility of functional groups,high yields,and short reaction times made it more attractive for constructing Csp2–Csp2 bonds in the synthesis of functional molecules and materials.

关键词： Palladium complexes N,O-Bidentate ligands N-Oxide units Mizoroki-Heck reaction Aryl bromide Electron-deficient olefins C—C coupling Homogeneous catalysis Substituent effects

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Phase-engineering modulation of Mn-based oxide cathode for constructing super-stable sodium storage

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Journal of Energy Chemistry 2024年第1期88卷 421-427,I0010页

作者： Quanqing Zhao Ruru Wang Ming Gao Bolin Liu Jianfeng Jia Haishun Wu Youqi Zhu Chuanbao Cao key laboratory of magnetic molecules and magnetic information materials of ministry of education School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032ShanxiChina Metals and Chemistry Research Institute China Academy of Railway Sciences Corporation LimitedBeijing 100081China Research Center of materials Science Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green ApplicationsBeijing Institute of TechnologyBeijing 100081China

The Mn-based oxide cathode with enriched crystal phase structure and component diversity can provide the excellent chemistry structure for Na-ion batteries.Nevertheless,the broad application prospect is obstructed by the sluggish Na^(+)kinetics and the phase transitions upon cycling.Herein,we establish the thermodynamically stable phase diagram of various Mn-based oxide composites precisely controlled by sodium content tailoring strategy coupling with co-doping and solid-state reaction.The chemical environment of the P2/P'3 and P2/P3 biphasic composites indicate that the charge compensation mechanism stems from the cooperative contribution of anions and cations.Benefiting from the no phase transition to scavenge the structure strain,P2/P'3 electrode can deliver long cycling stability(capacity retention of 73.8%after 1000 cycles at 10 C)and outstanding rate properties(the discharge capacity of 84.08 mA h g^(-1)at 20 C)than P2/P3 electrode.Furthermore,the DFT calculation demonstrates that the introducing novel P'3 phase can significantly regulate the Na^(+)reaction dynamics and modify the local electron configuration of Mn.The effective phase engineering can provide a reference for designing other high-performance electrode materials for Na-ion batteries.

关键词： Sodium ion battery Oxide cathode Phase engineering Phase diagram Na~+kinetic

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Selective oxygen electroreduction to hydrogen peroxide in acidic media:The superiority of single-atom catalysts

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Nano Research 2024年第6期17卷 4668-4681页

作者： Ergui Luo Tongtong Yang Jingyi Liang Yuhong Chang Junming Zhang Tianjun Hu Junjie Ge Jianfeng Jia key laboratory of magnetic molecules and magnetic information materials of ministry of education School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032China School of Chemistry and materials Science University of Science and Technology of ChinaHefei 230026China State key laboratory of Electroanalytic Chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Two-electron oxygen reduction reaction(2e-ORR)provides an environmentally friendly direction for the on-site production of hydrogen peroxide(H_(2)O_(2)).Central to this technology is the exploitation of efficient,economical,and safe 2e-ORR electrocatalysts.This overview starts with the fundamental chemistry of ORR to highlight the decisive role of adsorbing intermediates on the reaction pathway and activity,followed by a comprehensive survey of the tuning strategies to favor 2e-ORR on traditional precious metals.The latest achievements in designing efficient and selective precious-metal-based single-atom catalysts(SACs)and metal-nitrogen-carbon(M-Nx/C)catalysts,from the aspects of material synthesis,theoretical calculations,and mass transport promotion,are systematically summarized.Brief introductions on the evaluation metrics for 2e-ORR catalysts and the primary reactor designs for cathodic H_(2)O_(2)synthesis are also included.We conclude this review with an outlook on the challenges and direction of efforts to advance electrocatalytic 2e-ORR into realistic H_(2)O_(2)production.

关键词： oxygen reduction reaction H_(2)O_(2)production single-atom catalysts selectivity

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Interfacial engineering of the layered oxide cathode materials for sodium-ion battery

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Nano Research 2024年第3期17卷 1441-1464页

作者： Quanqing Zhao Ruru Wang Ming Gao Faheem KButt Jianfeng Jia Haishun Wu Youqi Zhu key laboratory of magnetic molecules and magnetic information materials of ministry of education School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032China Metals and Chemistry Research Institute China Academy of Railway Sciences Corporation LimitedBeijing 100081China Department of Physics Division of Science and TechnologyUniversity of EducationLahore 54770Pakistan Research Center of materials Science Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green ApplicationsBeijing Institute of TechnologyBeijing 100081China

The layered metal oxides are reviewed as the hopeful cathode materials for high-performance sodium-ion batteries(SIBs)due to their large theoretical capacity,favorable two-dimensional(2D)ion diffusion channel,and simple manipuility.However,their cycling stability,rate capability,and thermal stability are still significantly concerned and highlighted before further practical application.The chemical,mechanical and electrochemical stability of the cathode–electrolyte interfaces upon cycling is of great significance.Herein,the unique structural and electrochemical properties of the layered oxide cathode materials for SIB are reviewed.The mechanism of bulk/surface degradation induced by oxygen evolution,phase transition,microcrack,and electrolyte decomposition is thoroughly understood.Furthermore,the interfacial engineering to construct stable interface through various effective methods is fully discussed.The future outlook and challenges for interfacial engineering in this filed are also summarized.This review should shed light on the rational design and construct of robust interface for applications of superior layered oxide cathodes in SIB and may suggest future research directions.

关键词： interfacial engineering sodium-ion battery layered oxide electrolyte interface

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Biomimetic design of highly flexible metal oxide nanofibrous membranes with exceptional mechanical performance for superior phosphopeptide enrichment

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Nano Research 2024年第5期17卷 4270-4278页

作者： Xue Mao Zhen-Zhen Li Dong-Lian Hao Wei-Dong Han Gao-Peng Li Yao-Yu Wang Kun Zhang School of Textile Science and Engineering Key Laboratory of Functional Textile Material and Product(Ministry of Education)Xi’an Polytechnic UniversityXi’an 710048China key laboratory of magnetic molecules&magnetic information materials of the ministry of education School of Chemistry&Material ScienceShanxi Normal UniversityTaiyuan 030031China Department of Clinical laboratory The Second Affiliated Hospital of Xi’an Jiaotong UniversityXi’an 710004China Shanghai iProteome Biotechnology Co. LtdShanghai 201210China College of Chemistry&materials Science Northwest UniversityXi'an 710127China

Developing free-standing and mechanical robust membrane materials capable of superior enrichment of phosphopeptides for analyzing and identifying the specific phosphoproteome of cancer cells is significant in understanding the molecular mechanisms of cancer development and exploring new therapeutic approaches,but still a significant challenge in materials design.To this end,we firstly constructed highly flexible ZrTiO_(4) nanofibrous membranes(NFMs)with excellent mechanical stability through a cost-effective and scalable electrospinning and subsequent calcination technique.Then,to further increase the enrichment capacity of the phosphopeptide,the biomimetic TiO_(2)@ZrTiO_(4) NFMs with root hair or leaf like branch microstructure are developed by the hydrothermal post-synthetic modification of ZrTiO_(4) NFMs through growing unfurling TiO_(2) nanosheets onto the ZrTiO_(4) nanofibers.Importantly,remarkable flexibility and mechanical stability enable the resulting TiO_(2)@ZrTiO_(4) NFMs excellent practicability,while the biomimetic microstructure allows it outstanding enrichment ability of the phosphopeptide and identification ability of the specific phosphoproteins in the digest of cervical cancer cells.Specifically,6770 phosphopeptides can be enriched by TiO_(2)@ZrTiO_(4) NFMs(2205 corresponding phosphoproteins can be identified),and the value is much higher than that of ZrTiO_(4) NFMs(6399 phosphopeptides and 2132 identified phosphoproteins)and commercial high-performance TiO_(2) particles(4525 phosphopeptides and 1811 identified phosphoproteins).These results demonstrate the super ability of TiO_(2)@ZrTiO_(4) NFMs in phosphopeptide enrichment and great potential for exploring the pathogenesis of cancer.

关键词： inorganic nanofibers flexible ceramic nanofibrous membranes biomimetic materials exceptional mechanical performance flexibility

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Room-temperature phonon-coupled single-photon emission in hexagonal boron nitride

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Science China(Physics,Mechanics & Astronomy) 2024年第5期67卷 109-114页

作者： Jia-Min Lai Qing-Hai Tan Feilong Song Haonan Chang Yanpei Lv Xue-Lu Liu Jinghua Teng Weibo Gao Ping-Heng Tan Jun Zhang State key laboratory of Superlattices and Microstructures Institute of SemiconductorsChinese Academy of SciencesBeijing100083China key laboratory of magnetic molecules and magnetic information materials of ministry of education&Research Institute of materials Science Shanxi Normal UniversityTaiyuan 030000China Center of materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Division of Physics and Applied Physics School of Physical and Mathematical SciencesNanyang Technological UniversitySingapore 637371Singapore Institute of materials Research and Engineering(IMRE) Agency for ScienceTechnology and Research(A*STAR)Singapore 138634Singapore

Photon-lattice(phonon)coupling is fundamental to light-matter interaction,particularly when it reaches the quantum limit of the phonon-coupled single-photon emission,which holds great potential for quantum manipulation and quantum information transduction.Here,we report single defect state-phonon coupling in hexagonal boron nitride(h BN)at room temperature.An ultrabroad spectrum of single-photon emissions can be achieved by selecting the excitation energies.Using photoluminescence excitation spectroscopy,we observe single-phonon-assisted resonance-enhanced single-photon emission,along with multiple phonon replicas that herald the creation of phonon Fock state.We also develop a transition model to gain insight into the physical process behind the single defect state-phonon coupling.Our work sets the stage for manipulating electron-phonon coupling state with single quantum-level precision at room temperature.

关键词： temperature phonon hexagonal

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Recent progress on valley polarization and valley-polarized topological states in two-dimensional materials

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Chinese Physics B 2024年第1期33卷 16-31页

作者：王斐张亚玲杨文佳张会生许小红 key laboratory of magnetic molecules and magnetic information materials of the ministry of education and Research Institute of Materials ScienceShanxi Normal UniversityTaiyuan 030006China College of Physics and Electronic information Shanxi Normal UniversityTaiyuan 030006China

Valleytronics, using valley degree of freedom to encode, process, and store information, may find practical applications in low-power-consumption devices. Recent theoretical and experimental studies have demonstrated that twodimensional(2D) honeycomb lattice systems with inversion symmetry breaking, such as transition-metal dichalcogenides(TMDs), are ideal candidates for realizing valley polarization. In addition to the optical field, lifting the valley degeneracy of TMDs by introducing magnetism is an efficient way to manipulate the valley degree of freedom. In this paper, we first review the recent progress on valley polarization in various TMD-based systems, including magnetically doped TMDs,intrinsic TMDs with both inversion and time-reversal symmetry broken, and magnetic TMD heterostructures. When topologically nontrivial bands are empowered into valley-polarized systems, valley-polarized topological states, namely valleypolarized quantum anomalous Hall effect can be realized. Therefore, we have also reviewed the theoretical proposals for realizing valley-polarized topological states in 2D honeycomb lattices. Our paper can help readers quickly grasp the latest research developments in this field.

关键词： valley polarization valley-polarized topological states two-dimensional material

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Pushing the high-k scalability limit with a superparaelectric gate layer

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Journal of Advanced Ceramics 2024年第4期13卷 539-547页

作者： Kun Wang Chao Liu Yuan Zhang Fuyu Lv Jun Ouyang Houbing Huang Rui-Long Yang Yu-Yao Zhao Hongbo Cheng Hanfei Zhu Xiaoming Shi Yun Tian Institute of Advanced Energy materials and Chemistry Jinan Engineering Laboratory for Multi-scale Functional MaterialsSchool of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan 250353China key laboratory for Liquid-Solid Structure Evolution and Processing of materials(ministry of education) School of Materials Science and EngineeringShandong UniversityJinan 250061China China Tobacco Shandong Industrial Co. Ltd.Jinan 250104China Department of materials Science and Engineering Southern University of Science and TechnologyShenzhen 518055China key laboratory of key Film materials&Application for Equipments(Hunan Province) School of Material Sciences and EngineeringXiangtan UniversityXiangtan 411105China Advanced Research Institute of Multidisciplinary Science and School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China key laboratory of magnetic molecules and magnetic information materials of ministry of education School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032China

To meet the expectation set by Moore’s law on transistors,the search for thickness-scalable high dielectric constant(k)gate layers has become an emergent research frontier.Previous investigations have failed to solve the“polarizability–scalability–insulation robustness”trilemma.In this work,we show that this trilemma can be solved by using a gate layer of a high k ferroelectric oxide in its superparaelectric(SPE)state.In the SPE,its polar order becomes local and is dispersed in an amorphous matrix with a crystalline size down to a few nanometers,leading to an excellent dimensional scalability and a good field-stability of the k value.As an example,a stable high k value(37±3)is shown in ultrathin SPE films of(Ba_(0.95),Sr_(0.05))(Zr_(0.2),Ti_(0.8))O_(3)deposited on LaNiO_(3)-buffered Pt/Ti/SiO_(2)/(100)Si down to a 4 nm thickness,leading to a small equivalent oxide thickness of~0.46 nm.The aforementioned characteristic microstructure endows the SPE film a high breakdown strength(~10.5 MV·cm^(−1)for the 4 nm film),and hence ensures a low leakage current for the operation of the complementary metal oxide semiconductor(CMOS)gate.Lastly,a high electrical fatigue resistance is displayed by the SPE films.These results reveal a great potential of superparaelectric materials as gate dielectrics in the next-generation microelectronics.

关键词： high-k transistors Moore's law superparaelectric insulation robustness

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General synthesis of transition metal nitride arrays by ultrafast flash Joule heating within 500 ms

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Science China Chemistry 2024年第6期67卷 1976-1982页

作者： Peiqi Shen Jiahui Zhao Yanan Gao Yunxiang Lin Yuchen Han Kun Xu School of Chemistry and Chemical Engineering Key Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationAnhui UniversityHefei230601China Institutes of Physical Science and information Technology Center of Free Electron Laser&High Magnetic FieldLeibniz International Joint Research Center of Materials Sciences of Anhui ProvinceAnhui UniversityHefei230601China

Transition metal nitrides(TMNs)are considered as viable alternatives to noble metal catalysts owing to their versatile electronic structure and favorable catalytic performance.However,the conventional synthetic processes for TMNs suffer from high energy consumption and low production yield.In this study,a range of TMNs and their hetero-composite arrays were successfully synthesized via an ultrafast flash Joule heating technology within 0.5 s.As a proof concept,the nitrides and hetero-composites were applied for the electrocatalytic hydrazine oxidation reaction(HzOR),in which the Co_(4)N/Mo_(16)N_(7)arrays shows the best performance with a geometric current density of 100 mA cm^(-2)at 23 mV(vs.reversible hydrogen electrode(RHE)).This work paves a new way for the ultrafast synthesis of TMNs which could meet the ever-increased energy crisis.

关键词： flash Joule heating rapid synthesis transition metal nitrides hydrazine oxidation reaction electrocatalysts

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