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Synthesis and Modulation of Low-Dimensional Transition Metal Chalcogenide Materials via Atomic Substitution

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Nano-Micro Letters 2024年第9期16卷 49-94页

作者： Xuan Wang Akang Chen XinLei Wu Jiatao Zhang Jichen Dong Leining Zhang key laboratory of Cluster Science Ministry of Education of ChinaBeijing Key Laboratory of Photoelectronic and Electrophonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081People’s Republic of China Beijing National laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of Chemistry Chinese Academy of SciencesBeijing 100190People’s Republic of China

In recent years,low-dimensional transition metal chalcogenide(TMC)materials have garnered growing research attention due to their superior electronic,optical,and catalytic properties compared to their bulk counterparts.The controllable synthesis and manipulation of these materials are crucial for tailoring their properties and unlocking their full potential in various applications.In this context,the atomic substitution method has emerged as a favorable approach.It involves the replacement of specific atoms within TMC structures with other elements and possesses the capability to regulate the compositions finely,crystal structures,and inherent properties of the resulting materials.In this review,we present a comprehensive overview on various strategies of atomic substitution employed in the synthesis of zero-dimensional,one-dimensional and two-dimensional TMC materials.The effects of substituting elements,substitution ratios,and substitution positions on the structures and morphologies of resulting material are discussed.The enhanced electrocatalytic performance and photovoltaic properties of the obtained materials are also provided,emphasizing the role of atomic substitution in achieving these advancements.Finally,challenges and future prospects in the field of atomic substitution for fabricating low-dimensional TMC materials are summarized.

关键词： Transition metal chalcogenides Atomic substitution Ion exchange Low-dimensional materials Controllable synthesis

Denitration of Nitroarenes Under Ambient Physiological Conditions Catalyzed by Graphdiyne-Supported Palladium

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CCS Chemistry 2024年第3期6卷 641-651页

作者： Endong Zhang Yanyan Chen Fengting Lv Zicheng Zuo Feng He Yongjun Li Yiming Huang Yuliang Li Shu Wang Beijing National laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190 College of Chemistry University of Chinese Academy of SciencesBeijing 100049

The direct cleavage of C–NO_(2)bonds for reductive denitration of nitroarenes remains a challenging transformation in synthetic organic chemistry.Herein,we report a biocompatible palladium-deposited graphdiyne nanocatalyst(Pd@GDY/DSPE-PEG)that can catalyze reductive denitration of nitroarenes under ambient physiological conditions.Mechanistic studies support this transformation via the oxidative addition of nitroarenes with Pd(0)and subsequent ligand exchange to form arylpalladium hydride.This one-step reductive denitration via Pd@GDY/DSPE-PEG successfully facilitates the repair of the nitrated proteins arising from endogenic ONOO−and restores their physiological function,including blocking the apoptosis pathway in living cells.Moreover,Pd@GDY/DSPE-PEG was further successfully applied for catalytic denitration to reduce the level of 3-nitrotyrosine residues of proteins located in the mouse brain hippocampus in vivo.This study provides an ideal strategy for designing highly active enzymatic mimicking synthetic catalysts for the regulation of the nitrated protein level and the detoxification of nitrative damage of living cells and tissues.

关键词： 3-nitrotyrosine artificial nanaocatalysts reductive denitration palladium-deposited graphdiyne repairing nitrated protein

The design and synthesis of fused thiophenes and their applications in organic field-effect transistors

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Science China Chemistry 2010年第4期53卷 779-791页

作者： LIU Ying, YU Gui & LIU YunQi Beijing National laboratory for Molecular Sciences, key laboratory of organic solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China Beijing National laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing China

Fused thiophenes refer to oligothienoacenes in which several thiophenes are coupled together via twoor multi-positions and their derivatives. The synthesized organic semiconductors based on fused thiophenes exhibit excellent field effect properties due to their efficient intermolecular S…S interactions and π…π stacking. The performances of organic field-effect transistors (OFETs) depend not only on the materials but also on the devices. Such factors which influence the device performances as device structures, fabrication technologies and interface engineering are extensively investigated based on the fused thiophenes. Searching for new organic semiconductors and improving the device fabrication technologies are two major issues in the development of OFETs.

关键词： fused thiophenes oligothienoacenes organic field-effect transistors device performance

organic single crystals or crystalline micro/nanostructures: Preparation and field-effect transistor applications

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Science China Chemistry 2010年第6期53卷 1225-1234页

作者： FU XiaoLong,WANG ChengLiang,LI RongJin,DONG HuanLi & HU WenPing Beijing National laboratory for Molecular Sciences,key laboratory of organic solids,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190,China Beijing National laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing China

organic single crystals hold great promise for the development of organic semiconductor materials,because they could reveal the intrinsic electronic properties of these materials,providing high-performance electronic devices and probing the structureproperty relationships.This article reviews the preparation methods for organic single crystals or crystalline micro/nanostructures,including vapor phase growth methods and solution-processed methods,and summarizes a few methods employed in the fabrication of field-effect transistors along with dozens of examples concerning both small molecules and polymers with high field-effect performance.

关键词： organic single crystal physical vapor transport (PVT) solution-processed technique field-effect transistors (FETs) micro/nanostructures

Asymmetric side-chain engineering of organic semiconductor for ultrasensitive gas sensing

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Chinese Chemical Letters 2024年第3期35卷 428-433页

作者： Xiaoying Ma Xiaojuan Dai Lanyi Xiang Jiajun Chang Danfeng Zhi Haozhen Zhao Zhenjie Ni Ye Zou Xike Gao Fengjiao Zhang School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China laboratory of organic solids Institute of ChemistryChinese Academy of SciencesBeijing 100190China key laboratory of Synthetic and Self-Assembly Chemistry for organic Functional Molecules Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China Binzhou Institute of Technology Binzhou 256606China

Molecular structure of organic semiconductor plays a critical role in determining the performance and functionality of organic electronic devices,by optimizing the electrical,optical and physicochemical properties.Substituted alkyl chains are fundamental units in tailering the solubility and assemblability,among which the asymmetric properties have been reported as key element for controlling the packing motifs and intrinsic charge transport.Here,we expanded the scope of molecular asymmetry dependent sensing features based on a new series of naphthalene diimides(NDI)-based derivatives substituted with a same branching alkyl chain but various linear-shaped alkyl chains(Cn-).A clear molecular stacking change,from head-to-head bilayer to head-to-tail monolayer packing model,is observed based on the features of anisotropic molecular interactions with the change in the chain length.Most importantly,a unique LUMO level shift of 0.17 eV is validated for NDI-PhC4,providing a record sensitivity up to 150%to 0.01 ppb ammonia,due to the desired molecular reactivity and device amplification properties.These results indicate that asymmetric side-chain engineering opens a route for breath healthcare.

关键词： organic thin film transistor Asymmetric side chain Gas sensing Molecular stacking Energy level manipulating

Theoretical screening of cooperative N-bridged dual-atom sites for efficient electrocatalytic nitrogen reduction with remolding insight

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Nano Research 2024年第4期17卷 3413-3422页

作者： Huimei Chen Yan Yang Chi Jiao Zhiwen Zhuo Junjie Mao Yan Liu key laboratory of Functional Molecular solids Ministry of EducationCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China

The electrocatalytic nitrogen reduction reaction(e-NRR)is a promising alternative method for the Haber–Bosch process.However,it still faces many challenges in searching for high activity,stability,and selectivity catalysts and ascertaining the catalytic mechanism with complete insight.Here,a series of graphene-based N-bridged dual-atom catalysts(M1-N-M2/NC)are systematically investigated via first-principle calculation and a high-throughput screening strategy.The result unveils that N_(2) adsorption on M1-N-M2/NC in bridge-on adsorption mode can effectively break the scaling relationship on single-atom catalysts(SACs).Moreover,V-N-Ru/NC and V-N-Os/NC are systematically screened out as promising e-NRR catalysts,with extremely low limiting potentials of-0.20 and-0.18 V,respectively.Furthermore,the adsorption site competition between*N_(2) and*H,as well as the competitive twin reactions of hydrogen evolution reaction(HER)on intermediates(N_(n)H_(m))during the e-NRR process,is systematically evaluated to form a remodeling insight for the reactions in mechanism,and the e-NRR of new proposed dual-atom catalysts(DACs)is strategically optimized for its high-efficiency performance potential via our remolding insight in e-NRR mechanism.This work provides new ideas and insights for the design and mechanism of e-NRR catalysts and an effective strategy for rapidly screening highly efficient e-NRR catalysts.

关键词： nitrogen reduction dual-atom catalysts high-throughput screening hydrogen evolution reaction density functional theory calculations

Self-Assembled Protein Hybrid Nanofibrils for Photosynthetic Hydrogen Evolution

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CCS Chemistry 2024年第3期6卷 812-823页

作者： Weijian Chen Xiantao Hu Andi Hu Luyang Ji Yiming Huang Hao Heng Fude Feng Shu Wang Department of Polymer Science and Engineering School of Chemistry and Chemical EngineeringNanjing UniversityJiangsuNanjing 210023 Beijing National laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190

In artificial photosynthesis systems,synthetic diiron complexes are popular[FeFe]-hydrogenase mimics,which are attractive for the fabrication of photocatalyst-protein hybrid structures to amplify hydrogen(H2)generation capability.However,constructing a highly bionic and efficient catalytic hybrid system is a major challenge.Notably,we designed an ideal hybrid nanofibrils system that incorporates the crucial components:(1)a[FeFe]-H2ase mimic,which has a three-arm architecture(named triFeFe)for more interaction sites and higher catalytic activity and(2)uniform hybrid nanofibrils as the biological environment in which cysteine-catalyst coordination and the hydrogen-bonding network play a vital role in both catalyst binding and hydrogen evolution reaction activity.The assembled hybrid nanofibrils achieve efficient H2 generation with a turnover number of 2.3×103,outperforming previously reported diiron catalyst-protein hybrid systems.Additionally,the hybrid nanofibrils work with photosynthetic thylakoids to produce H2,without extra photosensitizers or electron shuttle proteins,which advances the bioengineering of living systems for solar-driven biofuel production.

关键词： hybrid photocatalyst in situ assembly amyloid fibrils photosynthetic hydrogen evolution thylakoid

Polaron interfacial entropy as a route to high thermoelectric performance in DAE-doped PEDOT:PSS films

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National Science Review 2024年第3期11卷 259-270页

作者： Jiajia Zhang Caichao Ye Genwang Wei Liang Guo Yuhang Cai Zhi Li Xinzhi Wu Fangyi Sun Qikai Li Yupeng Wang Huan Li Yuchen Li Shuaihua Wang Wei Xu Xuefeng Guo Wenqing Zhang Weishu Liu Department of Materials Science and Engineering Southern University of Science and Technology Academy for Advanced Interdisciplinary Studies and Guangdong Provincial key laboratory of Computational Science and Material Design Southern University of Science and Technology Department of Mechanical and Energy Engineering Southern University of Science and Technology Beijing National laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences College of Chemistry and Molecular Engineering National Biomedical Imaging Centre Peking University Guangdong Provincial key laboratory of Functional Oxide Materials and Devices Southern University of Science and Technology

Enhancing the thermoelectric transport properties of conductive polymer materials has been a long-term challenge, in spite of the success seen with molecular doping strategies. However, the strong coupling between the thermopower and the electrical conductivity limits thermoelectric performance. Here, we use polaron interfacial occupied entropy engineering to break through this intercoupling for a PEDOT:PSS(poly（3,4-ethylenedioxythiophene）-poly（4-styrenesulfonate）) thin film by using photochromic diarylethene（DAE） dopants coupled with UV-light modulation. With a 10-fold enhancement of the thermopower from 13.5 μV K-1to 135.4 μV K-1and almost unchanged electrical conductivity, the DAE-doped PEDOT:PSS thin film achieved an extremely high power factor of 521.28 μW m-1K-2from an original value of 6.78 μW m-1K-2. The thermopower was positively correlated with the UV-light intensity but decreased with increasing temperature, indicating resonant coupling between the planar closed DAE molecule and PEDOT. Both the experiments and theoretical calculations consistently confirmed the formation of an interface state due to this resonant coupling. Interfacial entropy engineering of polarons could play a critical role in enhancing the thermoelectric performance of the organic film.

关键词： thermoelectric PEDOT: PSS interfacial occupied entropy resonant coupling UV-light modulation

Selective core-shell doping enabling high performance 4.6 V-LiCoO2

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Journal of Energy Chemistry 2024年第8期95卷 684-693页

作者： Yueming Xia Jianrui Feng Jinhui Li Yan Li Zhengfeng Zhang Xiaoqi Wang Jianli Shao Manling Sui Pengfei Yan Beijing key laboratory of Microstructure and Property of solids College of Materials Science & Engineering Beijing University of Technology Petro China Research Institute of Petroleum Exploration & Development State key laboratory of Explosion Science and Technology Beijing Institute of Technology

Constructing robust surface and bulk structure is the prerequisite for realizing high performance high voltage LiCoO2（LCO）.Herein,we manage to synthesize a surface Mg-doping and bulk Al-doping coreshell structured LCO,which demonstrates excellent cycling performance.Half-cell shows 94.2% capacity retention after 100 cycles at 3.0-4.6 V（vs.Li/Li+） cycling,and no capacity decay after 300 cycles for fullcell test（3.0-4.55 V）.Based on comprehensive microanalysis and theoretical calculations,the degradation mechanisms and doping effects are systematically revealed.For the undoped LCO,high voltage cycling induces severe interfacial and bulk degradations,where cracks,stripe defects,fatigue H2 phase,and spinel phase are identified in grain bulk.For the doped LCO,Mg-doped surface shell can suppress the interfacial degradations,which not only stabilizes the surface structure by forming a thin rock-salt layer but also significantly improves the electronic conductivity,thus enabling superior rate performance.Bulk Al-doping can suppress the lattice "breathing" effect and the detrimental H3 to H1-3 phase transition,which minimizes the internal strain and defects growth,maintaining the layered structure after prolonged cycling.Combining theoretical calculations,this work deepens our understanding of the doping effects of Mg and Al,which is valuable in guiding the future material design of high voltage LCO.

关键词： Doping effect Electron microscopy Failure mechanism High-voltage LiCoO2 Lithium-ion battery