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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 *** controllable synthesis and manipulation of these materials are crucial for tailoring their properties and unlocking their full potential in various *** this context,the atomic substitution method has emerged as a favorable *** 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 *** 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 *** effects of substituting elements,substitution ratios,and substitution positions on the structures and morphologies of resulting material are *** enhanced electrocatalytic performance and photovoltaic properties of the obtained materials are also provided,emphasizing the role of atomic substitution in achieving these ***,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

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Electric-Induced Cycloelimination for Simulating Structural Plasticity in organic Nociceptors

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CCS Chemistry 2024年第6期6卷 1466-1476页

作者： Zhiheng Zhu Kai Liu Haojie Huang Yangshuang Bian Mingcong Qin Chengyu Wang Wei Wen Mingliang Zhu Wenkang Shi Yanwei Liu Zhiyuan Zhao Huijuan Yan Hanlin Wang Yunqi Liu Yunlong Guo Beijing National laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190 University of Chinese Academy of Sciences Beijing 100190

Continuous lifelong acquisition,updating,and finetuning of knowledge and skills is of crucial significance for the survival of ***,current neuromorphic devices exhibit obvious catastrophic forgetting when restimulated by new *** remains a challenge for neuromorphic devices and artificial intelligence to achieve continuous ***,we propose an electric-induced cycloelimination strategy to realize an organic transistor nociceptor that can simulate synaptic and structural *** system benefits from the ring-opening characteristics of cross-linked poly(vinyl cinnamate)under a strong pulse voltage,during which new energy-level trap states are *** prepared organic transistor nociceptors exhibit both structural and synaptic *** simulate the characteristics of human nociceptors,including threshold,relaxation,sensitization,and maladaptation *** the first time,we have simulated and explored the structural plasticity behavior in organisms based on electronic *** remarkably,the transistor nociceptors realize the reinput of information without forgetting the initial informa *** strategy developed for the preparation of organic transistor nociceptors provides insights for addressing the catastrophic forgetting in the lifelong learning of intelligent neuromorphic devices.

关键词： electric-induced cycloelimination structural plasticity organic nociceptors organic transistors metaplasticity

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 *** 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 ***,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 *** 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 *** 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

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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 ***,we report a biocompatible palladium-deposited graphdiyne nanocatalyst(Pd@GDY/DSPE-PEG)that can catalyze reductive denitration of nitroarenes under ambient physiological *** studies support this transformation via the oxidative addition of nitroarenes with Pd(0)and subsequent ligand exchange to form arylpalladium *** 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 ***,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 *** 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

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 ***,it still faces many challenges in searching for high activity,stability,and selectivity catalysts and ascertaining the catalytic mechanism with complete ***,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 *** 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,***,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 *** 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

Synthetic Strategies of Carbon Nanobelts and Beyond

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Chemical Research in Chinese Universities 2024年第4期40卷 627-631页

作者： LI Yanbang SHANG Wansong REN Yu ZHANG Xi-Sha LI Cheng ZHANG Guanxin ZHANG Deqing Beijing National laboratory for Molecular Science CAS Key Laboratory for Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing100190P.R.China University of Chinese Academy of Sciences Beijing100049P.R.China

Carbon nanobelts(CNBs)with aesthetically appealing molecular structures and outstanding physical properties have attracted more and more attentions from the scientific community due to their potential applications in synthetic materials,host-guest chemistry,optoelectronics,and so *** synthesis of CNBs at different stages was overviewed and some representative breakthroughs and advances in synthetic strategies were highlighted and *** key issue for the synthesis of CNBs is how to construct curved structures with high strain *** not only proposed a few unconventional CNBs as the promising target molecules,but also pointed out the bottom-up synthesis of conjugated tubular segments of carbon nanotubes sharing similar properties as carbon nanotubes is the next focus in this emerging area.

关键词： Carbon nanobelt Strain energy Carbon nanoring Single-walled carbon nanotube Bottom-up synthesis

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 ***-cell shows 94.2% capacity retention after 100 cycles at 3.0-4.6 V（***/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 *** 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 *** 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 *** 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 *** 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

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 ***,constructing a highly bionic and efficient catalytic hybrid system is a major ***,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 *** assembled hybrid nanofibrils achieve efficient H2 generation with a turnover number of 2.3×103,outperforming previously reported diiron catalyst-protein hybrid ***,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

Alkyl chain modulation of asymmetric hexacyclic fused acceptor synergistically with wide bandgap third component for high efficiency ternary organic solar cells

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International Journal of Minerals,Metallurgy and Materials 2024年第7期31卷 1713-1719页

作者： Shufang Li Huilan Guan Can Zhu Chaoyuan Sun Qingya Wei Jun Yuan Yingping Zou College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083China Beijing National laboratory for Molecular Sciences CAS Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China Institute of Carbon Neutrality and New Energy School of Electronics and InformationHangzhou Dianzi UniversityHangzhou 310018China

Herein,two asymmetric hexacyclic fused small molecule acceptors(SMAs),namely BP4F-HU and BP4F-UU,were *** elongated outside chains in the BP4F-UU molecule played a crucial role in optimizing the morphology of blend film,thereby improving charge mobility and reducing energy loss within the corresponding ***,the PM6:BP4F-UU device exhibited a higher open-circuit voltage(V_(oc))of 0.878 V compared to the PM6:BP4F-HU device with a V_(oc)of 0.863 ***,a new wide bandgap SMA named BTP-TA was designed and synthesized as the third component to the PM6:BP4F-UU host binary devices,which showed an ideal complementary absorption spectrum in PM6:BP4F-UU *** addition,BTP-TA can achieve efficient intermolecular energy transfer to BP4F-UU by fluorescence resonance energy transfer(FRET)pathway,due to the good overlap between the photoluminescence(PL)spectrum of BTP-TA and the absorption region of ***,ternary devices with 15wt%BTP-TA exhibits broader photon utilization,optimal blend morphology,and reduced charge recombination compared to the corresponding binary ***,PM6:BP4F-UU:BTP-TA ternary device achieved an optimal power conversion efficiency(PCE)of 17.83%with simultaneously increased V_(oc)of 0.905 V,short-circuit current density(J_(sc))of 26.14 mA/cm^(2),and fill factor(FF)of 75.38%.

关键词： asymmetric hexacyclic acceptor outside chain wide bandgap acceptor ternary organic solar cells

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