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Surface reconstruction and structural transformation of twodimensional Ni-Fe MOFs for oxygen evolution in seawater media

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Nano Research 2024年第4期17卷 2429-2437页

作者： Liyuan Xiao Xue Bai Jingyi Han Tianmi Tang Siyu Chen Hui Qi Changmin Hou Fuquan Bai Zhenlu Wang Jingqi Guan Institute of Physical chemistry College of ChemistryJilin UniversityChangchun 130021China The Second Hospital of Jilin University Changchun 130021China state key laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China laboratory of theoretical and Computational chemistry Institute of Theoretical ChemistryCollege of ChemistryChangchun 130023China

As a four-electron transfer reaction,oxygen evolution reaction(OER)is limited by large overpotential and slow ***,we in-situ synthesized two-dimensional(2D)Ni-Fe metal-organic framework nanosheets on nickel foam(NixFe-TPA/NF,TPA=terephthalic acid)for oxygen evolution in alkaline and alkaline seawater *** 1 M KOH,Ni3Fe-TPA/NF shows a low overpotential(η10)of 189 mV at 10 mA·cm^(-2) and an ultra-low overpotential of only 260 mV at 500 mA·cm^(-2).In alkaline seawater,Ni3Fe-TPA/NF still provides impressive OER performance,with anη10 of 265 ***-situ Raman characterization results show that the phase transition occurs during the OER,and Ni3FeOOH with more oxygen vacancies is in-situ formed,reducing the OER energy *** functional theory(DFT)reveals that the synergy between Ni and Fe reduces the energy barrier and accelerates the rate-determining *** addition,the ultra-thin 2D sheet structure and the close combination of Ni3FeOOH and highly conductive NF support ensure the high catalytic OER ***,the surface reconstruction and structural modification strategy can be used to design and prepare high-performance OER electrocatalysts for energy-related applications.

关键词： density functional theory(DFT)calculation Ni3FeOOH oxygen evolution reaction seawater electrolysis surface reconstruction

Switching on/off phosphorescent or non-radiative channels by aggregation-induced quantum interference

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Aggregate

Aggregate 2024年第1期5卷 175-184页

作者： Yi Kong Yu-Chen Wang Xunkun Huang WanZhen Liang Yi Zhao Department of chemistry State Key Laboratory of Physical Chemistry of Solid SurfacesiChEMFujian Provincial Key Laboratory of Theoretical and Computational Chemistryand College of Chemistry and Chemical EngineeringXiamen UniversityXiamenPeople’s Republic of China

Pure organic materials with persistent and efficient room-temperature phosphorescence have recently aroused great research interest due to their vast potential in *** crucial design principle for such materials is to suppress as much as possible the non-radiative decay of the triplet exciton while maintaining a moderate phosphorescent radiative ***,molecular engineering often exhibits similar regulation trends for the two ***,we propose that the quantum interference caused by aggregation can be utilized to control the phosphorescent and non-radiative decay *** systematically analyze various constructive and destructive transition pathways in aggregates with different molecular packing types and establish clear relationships between the luminescence characters and the signs of the singlet and triplet excitonic *** is shown that the decay channels can be flexibly switched on or off by regulating the packing type and excitonic *** importantly,an enhanced phosphorescent decay and a completely suppressed non-radiative decay can be simultaneously realized in the aggregate packed with inversion *** work lays the theoretical foundation for future experimental realization of quantum interference effects in phosphorescence.

关键词： excitonic coupling intersystem crossing organic aggregates organic room temperature phosphorescence quantum interference

Copper-catalyzed enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides via α-imino copper carbenes

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Science China chemistry 2024年第9期67卷 2982-2988页

作者： En-He Huang Li-Gao Liu You-Wei Yin Hao-Xuan Dong Ji-Jia Zhou Xin Lu 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 state key laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

α-Imino metal carbenes are versatile intermediates in organic synthesis,and have broad applications in the assembly of divergent ***,the catalytic enantioselective desymmetrization based onα-imino metal carbenes has not been developed to ***,we disclose an enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides viaα-imino copper carbenes,leading to the efficient assembly of divergent chiral indoloazepines in generally moderate to excellent yields with high ***,this reaction represents the first enantioselective desymmetrization based onα-imino metal *** synthetic transformations and biological tests show the potential utility of this ***,computational studies are employed to elucidate the reaction mechanism and the origin of enantioselectivity.

关键词： enantioselective desymmetrization metal carbenes copper catalysis nitrene transfer alkynes

维普期刊数据库

Rapid and controllable in-situ self-assembly of main-group metal nanofilms for highly efficient CO_(2)electroreduction to liquid fuel in flow cells

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Nano Research 2024年第6期17卷 5718-5725页

作者： Miao Wang Huaizhu Wang Yaoda Wang Junchuan Liang Mengfei Zhu Jiarui Li Zuoxiu Tie Zhong Jin state key laboratory of Coordination chemistry MOE Key Laboratory of Mesoscopic ChemistryMOE Key Laboratory of High Performance Polymer Materials and TechnologyJiangsu Key Laboratory of Advanced Organic MaterialsTianchang New Materials and Energy Technology Researc

The electrocatalytic reduction of CO_(2)is a promising pathway to generate renewable fuels and ***,its advancement is impeded by the absence of electrocatalysts with both high selectivity and ***,we present a scalable in-situ thermal evaporation technique for synthesizing series of Bi,In,and Sn nanofilms on carbon felt(CF)substrates with a high-aspect-ratio *** resulting main-group metal nanofilms exhibit a homogeneously distributed and highly exposed catalyst surface with ample active sites,thereby promoting mass transport and ad-/desorption of reaction *** from the unique fractal morphology,the Bi nanofilms deposited on CF exhibit optimal catalytic activities for CO_(2)electroreduction among the designed metal nanofilms electrodes,with the highest Faradaic efficiency of 96.9%for formate production at−1.3 V *** hydrogen electrode(RHE)in *** an industrially relevant current density of 221.4 mA·cm−2 in flow cells,the Bi nanofilms retain a high Faradaic efficiency of 81.7%at−1.1 V(***)and a good long-term stability for formate ***,a techno-economic analysis(TEA)model shows the potential commercial viability of electrocatalytic CO_(2)conversion into formate using the Bi nanofilms *** results offer a green and convenient approach for in-situ fabrication of stable and inexpensive thin-film catalysts with a fractal structure applicable to various industrial settings.

关键词： CO_(2)electroreduction non-noble metal nanofilms flow cells efficiency and selectivity techno-economic analysis

Cucurbit[8]uril-based non-covalent heterodimer realized NIR cell imaging through topological transformation from nanowire to nanorod

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Chinese Chemical Letters 2024年第10期35卷 288-294页

作者： Jianqiu Li Yi Zhang Songen Liu Jie Niu Rong Zhang Yong Chen Yu Liu College of chemistry State Key Laboratory of Elemento-Organic Chemistry Nankai University

In recent years,multicolor cascade supramolecular assemblies with controllable topological morphology have become a research hotspot due to their wide application in light-emitting materials,cell imaging and other ***,several kinds of macrocycles including cucurbiturils,calixarene and cyclodextrins are used as building blocks to construct fluorescent assemblies with anthryl-conjugated phenylpyridine（G）,wherein cucurbit[8]uril （CB[8]） and G can form nanowires at a stoichiometric ratio of n:n through host-guest encapsulation to form a non-covalent ***,the macrocycle confinement effect drastically enhances the fluorescence emission of G and emission peak generated bathochromic shift from 500 nm to 600 *** the supramolecular polymer is further assembled with amphiphilic calix[4]arene （SC4A8）,the fluorescence emission of G?CB[8]further increases to 1.4 times,accompanied by the morphological transformation from linear structure to nanorod ***,a very small amount of dye Cy5 is added to the assembly solution as an energy receptor,and the negatively charged G?CB[8]@SC4A8 system is regarded as an energy *** efficient energy transfer process enables near-infrared （NIR） emission at 675 nm with 71%energy transfer efficiency (ΦET) at a donor/receptor ratio of 100:***,the cascade supramolecular assembly has been successfully applied to targeted imaging in the nucleus of HeLa and A549 cancer cells.

关键词： Cucurbituril Morphological transformation Multivalent assemblies Targeted imaging

Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage

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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li Department of chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University state key laboratory of Surface Physics and Department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable ***,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as *** key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon *** mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion *** method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

Performance enhancement and active sites identification of Cu-Cd bimetallic oxide derived catalysts for electrochemical CO_(2) reduction

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Journal of Energy chemistry 2024年第4期91卷 50-58页

作者： Cai Wang Xin Hu Bairong Chen Houan Ren Xiaoyu Wang Yilin Zhang Xinyu Chen Yuping Liu Qingxin Guan Wei Li state key laboratory of Elemento-Organic chemistry Key Laboratory of Adv.Energy Mater.Chemistry(Ministry of Education)College of ChemistryNankai UniversityTianjin 300071China

The development of earth-abundant electrocatalysts with high performance for electrochemical CO_(2)reduction(ECR)is of great ***-based catalysts have been widely investigated for ECR due to their unique ability to generate various carbonaceous products,but directing selectivity toward one certain product and identifying the real active sites during ECR are still full of ***,after the incorporation of CdO into CuO,the Cu_(0.5)Cd_(0.5)-O catalyst achieves a 10.3-fold enhancement for CO selectivity in comparison with CuO,and a CO faradic efficiency nearly 90%with a current density around20 mA cm^(-2)could maintain at least 60 ***,a wide CO/H_(2)ratio(0.07-10)is reached on Cu_(x)Cd_(1-x)-O catalysts by varying the Cu/Cd ratio,demonstrating the potential of syngas production using such *** results of ex situ XRD,XPS,and in situ Raman reveal that the real active sites of Cu_(0.5)Cd_(0.5)-O catalysts for CO production during ECR reaction are the reconstructed mixed phases of CuCd alloy and CdCO_(3).In situ FTIR and theoretical calculations further implicate the presence of Cd related species promotes the CO desorption and inhibits the H_(2)evolution,thus leading to an enhanced CO generation.

关键词： CO_(2)reduction Cu-Cd bimetallic Real active sites CO production

维普期刊数据库

Dimensional regulation in gigantic molybdenum blue wheels featuring{(W)Mo_(5)}motifs for enhanced proton conductivity

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Nano Research 2024年第9期17卷 8261-8268页

作者： Yu-Lun Wu Jing Du Hai-Ying Zhang Ming-Jun Hou Qiao-Yue Li Wei-Chao Chen Kui-Zhan Shao Bo Zhu Chao Qin Xin-Long Wang Zhong-Min Su key laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China Hebei key laboratory of Organic Functional Molecules National Demonstration Center for Experimental Chemistry EducationTesting and Analysis CenterCollege of Chemistry and Materials ScienceHebei Normal UniversityShijiazhuang 050024China state key laboratory of Supramolecular Structure and Materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Dimensional regulation in polyoxometalates is an effective strategy during the design and synthesis of polyoxometalates-based high proton conductors,but it is not available to ***,the precise regulation of dimensionality has been realized in an unprecedented gigantic molybdenum blue wheel family featuring pentagonal{(W)Mo5}motifs through optimizing the molar ratio of Mo/W,including[Gd_(2)Mo_(124)W_(14)O_(422)(H_(2)O)62]38-(0D-{Mo_(124)W_(14)},1),[Mo_(126)W_(14)O441(H_(2)O)51]^(70-)(1D-{Mo_(126)W_(14)}n,2),and[Mo_(124)W_(14)O_(430)(H_(2)O)50]60-(2D-{Mo_(124)W_(14)}n,3).Such important{(W)Mo5}structural motif brings new reactivity into gigantic Mo blue *** are different numbers and sites of{Mo2}defects in each wheel-shaped monomer in 1-3,which leads to the monomers of 2 and 3 to form 1D and 2D architectures via Mo-O-Mo covalent bonds driven by{Mo2}-mediated H_(2)O ligands substitution process,respectively,thus achieving the controllable dimensional *** expected,the proton conductivity of 3 is 10 times higher than that of 1 and 1.7 times higher than that of *** continuous proton hopping sites in 2D network are responsible for the enhanced proton conductivity with lower activation *** study highlights that this dimensional regulation approach remains great potential in preparing polyoxometalates-based high proton conductive materials.

关键词： polyoxometalate molybdenum blue wheels Mo/W mixed-addenda polyoxometalates dimensional regulation proton conduction

Vibronic coupling effect on intersystem crossing rates of TADF emitters

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Chinese Journal of Structural chemistry 2024年第6期43卷 22-24页

作者： Xin Huang Yi Zhao Wanzhen Liang state key laboratory of Physical chemistry of Solid Surfaces iChEMFujian Provincial Key Lab of Theoretical and Computational ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China

To take advantage of all the singlet and triplet excitons and then achieve 100%internal quantum efficiency in OLED devices,the scientists have proposed the thermally activated delayed fluorescence(TADF)strategy which tries to achieve"delayed"fluorescence by converting triplet excitons to singlet excitons through a reverse intersystem crossing(ISC/RISC)process with the help of thermal activation[1].In the early days,the efficient RISC processes were facilitated by a negligible energy gap(△E_(ST))and a large spin-orbit coupling(SOC)matrix element(SOCME)between the first singlet(S_(1))and triplet(T_(1))excited states.

关键词： coupling system emitter