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中国化学快报（英文版）
中国化学快报（英文版）

梁晓天

月刊

1001-8417

cclbj@imm.ac.cn

010-63165638

100050

北京市先农坛街1号

中国化学快报（英文版）/Journal Chinese Chemical LettersCSCDCSTPCD北大核心SCI
查看更多>>本刊是由中国科协主管、中国化学会主办、中国医学科学院药物所承办的学术期刊，是由著名化学家梁晓天院士主编。是中国化学界通向世界的窗口，内容覆盖化学全领域。本刊的办刊宗旨是“新、快、准”，我们将坚持这个宗旨，力求及时反映化学研究中各个相关领域内的最新进展及热点问题，主要读者群是科研人员、研究生、大学教师。现已被国内外多家数据库收录，如SCI　Search、Chemical Abstract、Research Alert、Chemistry Citation Index、《日本科技文献速报》、万方数据数字化期刊群、中国学术期刊过刊全文数据库、中国学术期刊（光盘版）、中国学术期刊文摘、中文期刊全文数据库、俄罗斯Рж期刊源等。
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    Relaxor antiferroelectric-relaxor ferroelectric crossover in NaNbO3-based lead-free ceramics for high-efficiency large-capacitive energy storage

    Shuangliang XieYuyue ChenQing HeLiang Chen...
    465-469页
    查看更多>>摘要：Relaxor ferroic dielectrics have garnered increasing attention in the past decade as promising materi-als for energy storage.Among them,relaxor antiferroelectrics(AFEs)and relaxor ferroelectrics(FEs)have shown great promise in term of high energy storage density and efficiency,respectively.In this study,a unique phase transition from relaxor AFE to relaxor FE was achieved for the first time by introducing strong-ferroelectricity BaTiO3 into NaNbO3-BiFeO3 system,leading to an evolution from AFE R hierarchi-cal nanodomains to FE polar nanoregions.A novel medium state,consisting of relaxor AFE and relaxor FE,was identified in the crossover of 0.88NaNbO3-0.07BiFeO3-0.05BaTiO3 ceramic,exhibiting a distinc-tive core-shell grain structure due to the composition segregation.By harnessing the advantages of high energy storage density from relaxor AFE and large efficiency from relaxor FE,the ceramic showcased ex-cellent overall energy storage properties.It achieved a substantial recoverable energy storage density Wrec∼ 13.1 J/cm3 and an ultrahigh efficiency η ∼ 88.9% .These remarkable values shattered the trade-off rela-tionship typically observed in most dielectric capacitors between Wrec and η.The findings of this study provide valuable insights for the design of ceramic capacitors with enhanced performance,specifically targeting the development of next generation pulse power devices.
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    Excellent energy storage properties in non-stoichiometric Bi0.5Na0.5TiO3-based relaxor ferroelectric ceramics

    Shunshun JiangJi ZhangJing WangShan-Tao Zhang...
    470-472页
    查看更多>>摘要：The rapid development of high-power and pulsed-power techniques inspires extensive investigates on high-performance ceramic-based capacitors.However,the low recoverable energy density(Wrec)hampers their wider applications.Herein,the non-stoichiometric Bi0.5Na0.5TiO3-based ceramics were designed and studied.The proper introduction of oxygen vacancies facilitated activating defect dipole,giving rise to reduced remanent polarization.Consequently,the optimal composition exhibited an exceptional high Wrec of 8.3 J/cm3,a high efficiency of 85%,and excellent anti-fatigue and thermal reliability.This work provides an efficient approach to explore ceramic capacitors with high capacitive energy storage performances.
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    Oxygen self-doping pyrolyzed polyacrylic acid as sulfur host with physical/chemical adsorption dual function for lithium-sulfur batteries

    Yan WangHuixin ChenFuda YuShanyue Wei...
    473-479页
    查看更多>>摘要：Lithium-sulfur(Li-S)batteries with high theoretical capacity and energy density need to solve problems such as the high decomposition energy barrier of Li2S and large volume change of sulfur in the charging process caused by the shuttle effect before practical application.Herein,a green synthesis method is used to prepare polyacrylic acid(PAA)superabsorbent material,and then the pyrolyzed PAA(P/PAA)material is obtained as the positive electrode of Li-S battery.Density functional calculation reveals that the oxygen self-doping pyrolyzed polyacrylic acid(P/PAA)delivered stronger binding energy toward Li2S species in carbonyl C=O than that of graphite powder(GP)which are-1.58eV and-1.02eV,respectively.Coupled with the distribution of relaxation time analysis and the in-situ electrochemical impedance approach,it is further demonstrated that the designed P/PAA as sulfur host plays a physical/chemical adsorption dual function in maintaining the stability and rate performance of batteries.With an initial discharge capacity of 1258 mAh/g at 0.1 C and a minimal capacity decline of 0.05% per cycle even after 800 cycles at 0.5 C,the produced cathode demonstrated outstanding electrochemical performance.The average Coulombic efficiency is nearly 100% .The P/PAA electrodes may typically retain 96% of their capacity while declining on average only 0.033% per cycle after 130 cycles at 3 C.This effort provides a new method for the future development of heteroatomic self-doping superabsorbent with promising adsorption properties for polysulfides as cathode materials of Li-S batteries.
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    High-efficiency PdNi single-atom alloy catalyst toward cross-coupling reaction

    Baokang GengXiang ChuLi LiuLingling Zhang...
    480-483页
    查看更多>>摘要：The preparation of Pd-based catalysts with rich electrons and a high atom dispersion rate is of great significance for improving the reactivity of cross-coupling reactions,which is a powerful tool for pharma-ceutical and fine chemical synthesis.Here,we report a PdNi single-atom alloy(SAA)catalyst in which iso-lated Pd single atoms are anchored onto the surface of Ni nanoparticles(NPs)applied for Suzuki coupling reactions and Heck coupling reactions.The 0.1% PdNi SAA exhibits extraordinary catalytic activity(reac-tion rate:17,032.25mmol h-1 gPd-1)toward the Suzuki cross-coupling reaction between 4-bromoanisole and phenylboronic acid at 80℃ for 1h.The excellent activity is supposed to attribute to the 100 percent utilization rate of Pd atoms and the highly stable surface zero-valance Pd atoms,which provides abun-dant sites and electrons for the adsorption and fracture of the C-X(X=Cl,Br,I)bond.Moreover,our work demonstrates the excellent application prospect of SAAs for cross-coupling reactions.
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    Computational design of bimetallic TM2@g-C9N4 electrocatalysts for enhanced CO reduction toward C2 products

    Jiajun WangGuolin YiShengling GuoJianing Wang...
    484-490页
    查看更多>>摘要：Electrochemical CO reduction(ECOR)as a potential strategy for producing valuable chemicals and fuels has captured substantial attention.However,the currently available electrocatalysts suffer from poor se-lectivity and low Faradaic efficiency,limiting their industrial application.Herein,we systematically inves-tigate the potential of homonuclear bimetallic electrocatalysts,TM2@C9N4(TM=Fe,Co,Ni,and Cu),for the ECOR through extensive density functional theory calculations.Our findings suggest that all four pro-posed monolayers exhibit exceptional stability,making them highly suitable for experimental synthesis and practical applications.Interestingly,these transition-metal dual atoms anchored on C9N4 monolay-ers show great potential in facilitating the production of high-value C2 products,such as C2H5OH and C2H4,due to the significantly low limiting potentials(-0.06∼-0.46 V)and small kinetic energy barriers(0.54-1.08 eV)for the CO coupling process.Moreover,with the exception of Ni2@C9N4,these bimetallic catalysts demonstrate the impressive suppression of the competitive hydrogen evolution reaction(HER),leading to a high selectivity for C2 products in ECOR.Our predictions would accelerate the development of high-performance C9N4-based dual-atom catalysts for the ECOR.
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    Nanophase separated,grafted alternate copolymer styrene-maleic anhydride as an efficient room temperature solid state lithium ion conductor

    Qian WangTing GaoXiwen LuHangchao Wang...
    491-496页
    查看更多>>摘要：All solid-state lithium metal batteries(ASSLMBs)based on polymer solid electrolyte and lithium metal anode have attracted much attention due to their high energy density and intrinsic safety.However,the low ionic conductivity at room temperature and poor mechanical properties of the solid polymer elec-trolyte result in increased polarization and poor cycling stability of the Li metal batteries.In order to improve the ionic conductivity at room temperature while maintaining mechanical strength,we com-bine the conductivity of short chain polyethylene oxide(PEO)and strength of styrene-maleic anhydride copolymer(SMA)to obtain a grafted block copolymer with nanophase separation structure,which has room temperature ionic conductivity up to 1.14×10-4 S/cm and tensile strength up to 1.4 MPa.Li||Li symmetric cell can work stably for more than 1500h under the condition of 0.1mA/cm2.Li||LiFePO4 full cells can deliver a high capacity of 151.4 mAh/g at 25℃ and 0.2 C/0.2 C charge/discharge condi-tions,showing 85.6% capacity retention after 400 cycles.Importantly,the all solid state Li||LiFePO4 pouch cell shows excellent safety performance under different abuse conditions.These results demonstrate that the nanophase separated,grafted alternate copolymer electrolyte has huge potential for application in Li metal batteries.
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    Synthesis,chemical bonding and reactivity of new medium-sized polyarsenides

    Xu-Hui YueXiang-Wen ZhangHui-Min HeLei Qiao...
    497-501页
    查看更多>>摘要：Gaining an understanding of the growth mechanism from single atoms to clusters and bulk materials continues to present a challenge.Thus,it is important to explore the evolving trends of clusters in the structure and properties during the size evolution.In this work,we report the synthesis and charac-terization of two medium-sized chain-like polyarsenic anions.[As21]3-represents a trimeric example of polyarsenic anion assembled through oxidative coupling of As73-anions.The anion As184-included in[As18Mo2(CO)8]4-is regarded as formed by two realgar-type As8 subunits connected by a dinuclear As-As dumbbell.The As18 cluster was previously predicted by theory,and this is the first time successfully synthesized using wet chemistry method.Besides,small-sized polyarsenides As22-and As102-were found in compound[K(18-crown-6)]3[As10]0.5[As4{Mo(CO)3}2]0.5·2en.Among these,the former exhibits coordi-nation with metal atoms.Single-crystal X-ray diffraction combined with quantum chemical calculations revealed the formation of double bonded As22-stabilized by metal carbonyl groups.This work demon-strates a novel synthetic approach for the preparation of new polyarsenides and highlights their intriguing bonding characteristics,laying the foundation for the synthesis of such compounds and paving the way for their potential applications.
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    In situ sulfur-doped mesoporous tungsten oxides for gas sensing toward benzene series

    Yu DengYan LiuYonghui DengJinsheng Cheng...
    502-507页
    查看更多>>摘要：Benzene series as highly toxic gases have inevitably entered human life and produce great threat to hu-man health and ecological environment,and thus it is distinctly meaningful to monitor benzene series with quickly,real-time and efficient technique.Herein,novel sulfur-doped mesoporous WO3 materials were synthesized via classical in-situ solvent evaporation induced co-assembly strategy combined with doping engineering,which possessed highly crystallized frameworks,high specific surface area(40.9-63.8 m2/g)and uniform pore size(∼18nm).Benefitting from abundant oxygen vacancy and defects via S-doping,the tailored mesoporous S/mWO3 exhibited excellent benzene sensing performance,including high sensitivity(50 ppm vs.48),low detection limit(ca.500 ppb),outstanding selectivity and favorable stability.In addition,the reduction of band gap resulted from S-doping promotes the carrier migration in the sensing materials and the reaction at the gas-solid sensing interfaces.It provides brand-new ap-proach to design sensitive materials with multiple reaction sites.
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    Carbon dots confined nanosheets assembled NiCo2S4@CDs cross-stacked architecture for enhanced sodium ion storage

    Binyang QinMengqi WangShimei WuYining Li...
    508-513页
    查看更多>>摘要：Na batteries(SIBs)have been emerging as the most promising candidate for the next generation of sec-ondary batteries.However,the development of high-performance and cost-effective anode materials is urgently needed for the large-scale applications of SIBs.In this study,carbon dots confined bimetallic sulfide(NiCo2S4)architecture(NiCo2S4@CDs)was proposed and synthesized from assembling nanosheets into cross-stacked superstructure and the subsequent confinement of carbon dots.This novel decussated structure assembly from nanosheets is greatly beneficial to the structure stability of electrode material during the successive charge/discharge processes.Besides,the CDs based carbon conductive network can enhance the electrical conductivity for facilitating the easy transport of electron/Na.Benefitting from these advantages,NiCo2S4@CDs exhibits high-rate performance and an ultralong cycling life in SIBs.Specifically,the specific capacity of NiCo2S4@CDs can reach the discharge specific capacity as high as 568.9 mAh/g at 0.5 A/g,which can also maintain 302.7 mAh/g after 750 cycles at 5.0 A/g.Additionally,ex-situ characterization techniques such as ex-situ XRD and ex-situ XPS were employed to further explore the sodium storage mechanism of the NiCo2S4@CDs anode.
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    Highly efficient electrosynthesis of H2O2 in acidic electrolyte on metal-free heteroatoms co-doped carbon nanosheets and simultaneously promoting Fenton process

    Xiaodan WangYingnan LiuZhibin LiuZhongjian Li...
    514-518页
    查看更多>>摘要：Recently electrochemical synthesis of H2O2 through oxygen reduction reaction(ORR)via 2e- pathway is considered as a green and on-site route.However,it still remains a big challenge for fabricating novel metal-free catalysts under acidic solutions,since it suffers from high overpotential due to the intrinsically week *OOH adsorption.Herein,a co-doped carbon nanosheet(O/N-C)catalyst toward regulating O and N content was synthesized for improving the selectivity and activity of H2O2 electrosynthesis process.The O/N-C exhibits outstanding 2e-ORR performance with low onset potential of 0.4 V(vs.RHE)and a se-lectivity of 92.4％ in 0.1 mol/L HClO4 solutions.The in situ electrochemical impedance spectroscopy(EIS)tests reveals that the N incorporation contributes to the fast ORR kinetics.The density functional theory(DFT)calculations demonstrate that the binding strength of *OOH was optimized by the co-doping of oxygen and nitrogen at certain content,and the O/N-C-COOH site exhibits a lower theoretical overpoten-tial for H2O2 formation than O-C-COOH site.Furthermore,the promoted kinetics for typical organic dye degradation in simultaneous electron-Fenton process on O/N-C catalyst was demonstrated particularly for broadening its environmental application.
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