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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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    Synergic catalysis of W and Ni originating from substitution of trivacant phosphotungstate for the selective oxidation of aniline to azoxybenzene

    Sheng CaiXiao-Yuan WuWeiming WuSa-Sa Wang...
    558-563页
    查看更多>>摘要：Partial substitution of polyoxometalate(POM)is an efficient route to modulate the catalytic property of maternal POM.In this work,a new Keggin type POM involving {Ni6} cluster,{[Ni(H2O)2(Dach)2][Ni(Dach)2]2}{[Ni6Cl(μ-OH)3(H2O)(Dach)3(WO4)(PW9O34)][Ni6(μ-OH)3(H2O)2(Dach)3(WO4)(PW9O34)]}Cl-27H2O,(1,Dach=1,2-diaminocyclohexane)was synthesized.Compounds 1 shows excellent catalytic performance in the selective oxidation of aniline to azoxybenzene(AOB)in water.The apparently different results from that with the matrix {PW9O34}({PW9})suggest the successful regulation of the catalytic property of {PW9} by the introduction of the {Ni6} cluster into the skeleton.The experimental results indicate that the highlighted performance of 1 is contributed by the synergy of W and Ni sites,which are respectively responsible for the oxidation and condensation steps in the production of AOB.The good selectivity to AOB is essentially attributed to the effective modulation of the reaction rates of oxidation and condensation steps by W and Ni sites,respectively.
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    Enhancing the electrocatalytic performance of nitrate reduction to ammonia by in-situ nitrogen leaching

    Mimi FuYini MaoHua WangWei Luo...
    564-569页
    查看更多>>摘要：Electrochemical nitrate reduction reaction(NITRR)is regarded as a"two birds-one stone"method for the treatment of nitrate contaminant in polluted water and the synthesis of valuable ammonia,which is re-tarded by the lack of highly reactive and selective electrocatalysts.Herein,for the first time,nickel foam supported Co4N was designed as a high-performance NITRR catalyst by an in-situ nonmetal leaching-induced strategy.At the optimal potential,the Co4N/NF catalyst achieves ultra-high Faraday efficiency and NH3 selectivity of 95.4％and 99.4％,respectively.Ex situ X-ray absorption spectroscopy(XAS),together with other experiments powerfully reveal that the nitrogen vacancies produced by nitrogen leaching are stable and play a key role in boosting nitrate reduction to ammonia.Theoretical calculations confirm that Co4N with abundant nitrogen vacancies can optimize the adsorption energies of NO3-and intermediates,lower the free energy(ΔG)of the potential-determining step(*NH3 to NH3)and inhibit the formation of N-containing byproducts.In addition,we also conclude that the nitrogen vacancies can stabilize the adsorbed hydrogen,making H2 quite difficult to produce,and lowering ΔG from*NO to*NOH,which facilitates the selective reduction of nitrate.This study reveals significant insights about the in-situ non-metal leaching to enhance the NITRR activity.
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    Phosphorous-doped carbon nanotube/reduced graphene oxide aerogel cathode enabled by pseudocapacitance for high energy and power zinc-ion hybrid capacitors

    Junjun YaoFuzhi LiRuyi ZhouChenchen Guo...
    570-576页
    查看更多>>摘要：The design and development of energy storage device with high energy/power density has become a research hotspot.Zinc-ion hybrid capacitors(ZHCs)are considered as one of the most promising candi-dates.However,the application of ZHCs is hindered by their low energy density at high power density due to the unsatisfactory cathode material.In this study,a novel 3D phosphorus-doped carbon nan-otube/reduced graphene oxide(P-CNT/rGO)aerogel cathode is synthesized through a synergistic modi-fication strategy of CNT insertion and P doping modification combined with 3D porous design.The as-obtained P-CNT/rGO aerogel cathode manifests significantly increased surface aera,expanded interlayer spacing,and enhanced pseudocapacitance behavior,thus leading to significantly enhanced specific capac-itance and superb ions transport performance.The as-assembled ZHC based on P-CNT/rGO cathode deliv-ers a superior energy density of 42.2 Wh/kg at an extreme-high power density of 80 kW/kg and excellent cycle life.In-depth kinetic analyses are undertaken to prove the enhanced pseudocapacitance behavior and exceptional power output capability of ZHCs.Furthermore,the reaction mechanism of physical and chemical adsorption/desorption of electrolyte ions on the P-CNT/rGO cathode is revealed by systematic ex-situ characterizations.This work can provide a valuable reference for developing advanced graphene-based cathode for high energy/power density ZHCs.
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    Tuning the exciton binding energy of covalent organic frameworks for efficient photocatalysis

    Zhangjie GuZhen ShanYulan WangJinjian Wang...
    577-583页
    查看更多>>摘要：Owing to the large exciton binding energy(＞100 meV)of most organic materials,the process of exciton dissociation into free electrons and holes is seriously hindered,which plays a key role in the photocat-alytic system.In this study,a series of chalcogen(S,Se)-substituted mesoporous covalent organic frame-works(COFs)have been synthesized for enhanced photocatalytic organic transformations.Photoelectro-chemical measurements indicate that the introduction of semi-metallic Se atom and the enlargement of conjugation degree can not only reduce the exciton binding energy accelerating the charge separation,but also reduce the band gap of COFs.As a result,the COF-NUST-36 with the lowest exciton binding energy(39.5 meV)shows the highest photocatalytic performance for selective oxidation of amines(up to 98％Conv.and 97.5％Sel.).This work provides a feasible method for designing COFs with high photocatalytic activity by adjusting exciton binding energy.
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    Studying the variable energy band structure for energy storage materials in charge/discharge process

    Xuancheng ChenYu HuanNingqiang SunYuanhui Su...
    584-589页
    查看更多>>摘要：So far,a clear understanding about the relationship of variable energy band structure with the corre-sponding charge-discharge process of energy storage materials is still lacking.Here,using optical spec-troscopy(red-green-blue(RGB)value,reflectivity,transmittance,UV-vis,XPS,UPS)to study α-Co(OH)2 electrode working in KOH electrolyte as the research object,we provide direct experimental evidence that:(1)The intercalation of OH-ions will reduce the valence/conduction band(VB and CB)and band gap energy(Eg)values;(2)The deintercalation of OH-ions corresponds with the reversion of VB,CB and Eg to the initial values;(3)The color of Co(OH)2 electrode also exhibit regular variations in RGB value during the charge-discharge process.
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    Self-powered stimuli responsive material for dual stimulation of heat and guest molecules

    Jintao MenKe XuTaiting ShaLei He...
    590-593页
    查看更多>>摘要：Stimuli-responsive smart materials exhibit reverse chemical/physical changes in response to external stimuli and research on stimuli-responsive smart materials with self-powered properties is still un-cultivated ground.Here,we report perovskite crystalline self-powered multiple stimuli-responsive ma-terials triggered by chemical and thermal stimuli.[HMEP]PbI3·(H2O)(1;HMEP is a hydroxytris(1-methylethyl)phosphorus cation)crystallizes in a chiral space group P21 at 293 K and has the piezoelec-tric reaction(d33=10 pC/N and output voltage=1V)of self-powered modes,this value is larger than the value of 3 pC/N for the classical piezoelectric material ZnO.Piezoelectric materials can generate en-ergy due to mechanical deformation,and using thermal heating to lose water,[HMEP]PbI3(2)can be obtained.2 crystallizes in the non-centrosymmetric space group,undergoes two reversible phase transi-tions at 243/255K and 315/348 K,and shows second harmonic generation switching.Interestingly,2 can return to the hydrated form 1 after absorbing water.This work will lay the foundation for self-powered stimuli-responsive compounds and contribute to the construction of novel organic-inorganic hybrid ma-terials with second harmonic generation switching.
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    Copper-induced formation of heterostructured Co3O4/CuO hollow nanospheres towards greatly enhanced lithium storage performance

    Junjun ZhangHuiying LuTianhao YaoXin Ji...
    594-598页
    查看更多>>摘要：We report a facile template-free fabrication of heterostructured Co3O4/CuO hollow nanospheres us-ing pre-synthesized Co/Cu-glycerate as conformal precursor.The introduction of copper nitrate in the solvothermal reaction system of glycerol/isopropanol/cobalt nitrate readily induces the conversion from solid Co-glycerate to hollow Co/Cu-glycerate nanospheres,and the effect of the Co/Cu atomic ratio on the structure evolution of the metal glycerates as well as their corresponding oxides were investigated.When examined as anode materials for lithium-ion batteries,the well-defined Co3O4/CuO hollow nanospheres with Co/Cu molar ratio of 2.0 demonstrate excellent lithium storage performance,delivering a high re-versible capacity of 930 mAh/g after 300 cycles at a current density of 0.5 A/g and a stable capacity of 650 mAh/g after 500 cycles even at a higher current density of 2.0 A/g,which are much better than their counterparts of bare CuO and Co3O4.The enhanced lithium storage performance can be attributed to the synergistic effect of the CuO and Co3O4 heterostructure with hollow spherical morphology,which greatly enhances the charge/electrolyte transfer and effectively buffers the volume changes upon lithia-tion/delithiation cycling.
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    Ultrathin ternary PtNiGa nanowires for enhanced oxygen reduction reaction

    Giday FissehaYiping HuYanan YuShaojie Lu...
    599-603页
    查看更多>>摘要：Achieving high activity and durability for the oxygen reduction reaction(ORR)with an ultra-low amount of platinum is significant to promote the widespread application of proton exchange membrane fuel cells(PEMFCs).Here we report a new ultrathin(～1 nm)ternary PtNiGa alloy nanowires(PtNiGa NWs)elec-trocatalyst,in which the presence of gallium(Ga)enhances the oxidation resistance of platinum(Pt)and nickel(Ni)and suppresses the dissolution of Ni.The mass and specific activities of PtNiGa NWs are about 11.2 and 7.6 times higher than those of commercial Pt/C catalysts for ORR.Moreover,the mass activity of PtNiGa/C NWs nanocatalyst decreased only by 12.8％and largely retained its electrochemical surface area(ECSA)after 10,000 potential cycles,compared with 38％loss of ECSA for commercial Pt/C catalyst.There-fore,this work provides a general guideline for preparing ternary alloy electrocatalysts and enhancing the activity and stability of the cathode ORR reaction of PEMFCs.
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    Synergy of phosphorus vacancies and build-in electric field into NiCo/NiCoP Mott-Schottky integrated electrode for enhanced water splitting performance

    Xiaochen ZhangHui XueJing SunNiankun Guo...
    604-610页
    查看更多>>摘要：Vacancy engineering and Mott-Schottky heterostructure can accelerate charge transfer,regulate adsorp-tion energy of reaction intermediates,and provide additional active sites,which are regarded as valid means for improving catalytic activity.However,the underlying mechanism of synergistic regulation of interfacial charge transfer and optimization of electrocatalytic activity by combining vacancy and Mott-Schottky junction remains unclear.Herein,the growth of a bifunctional NiCo/NiCoP Mott-Schottky elec-trode with abundant phosphorus vacancies on foam nickel(NF)has been synthesized through continuous phosphating and reduction processes.The obtained NiCo/NiCoP heterojunctions show remarkable OER and HER activities,and the overpotentials for OER and HER are as low as 117 and 60 mV at 10mA/cm2 in 1 mol/L KOH,respectively.Moreover,as both the cathode and anode of overall water splitting,the voltage of the bifunctional NiCo/NiCoP electrocatalyst is 1.44 V at 10mA/cm2,which are far exceeding the bench-mark commercial electrodes.DFT theoretical calculation results confirm that the phosphorus vacancies and build-in electric field can effectively accelerate ion and electron transfer between NiCo alloy and NiCoP semiconductor,tailor the electronic structure of the metal centers and lower the Gibbs free energy of the intermediates.Furthermore,the unique self-supported integrated structure is beneficial to facili-tate the exposure of the active site,avoid catalyst shedding,thus improving the activity and structural stability of NiCo/NiCoP.This study provides an avenue for the controllable synthesis and performance optimization of Mott-Schottky electrocatalysts.
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    Interfacial charge redistribution to promote the catalytic activity of Vs-CoP-CoS2/C n-n heterojunction for oxygen evolution

    Jiawen SunHui XueJing SunNiankun Guo...
    611-616页
    查看更多>>摘要：Modulating surface charge redistribution based on interface and defect engineering has been considered as a resultful means to boost electrocatalytic activity.However,the mechanism of synergistic regulation of heterojunction and vacancy defects remains unclear.Herein,a Vs-CoP-CoS2/C n-n heterojunction with sulfur vacancies is successfully constructed,which manifests superior electrocatalytic activity for oxy-gen evolution,as demonstrated by a low overpotential of 170 mV to reach 10mA/cm2.The experimental results and density functional theory calculations testify that the outstanding OER performance of Vs-CoP-CoS2/C heterojunction is owed to the synergistic effect of sulfur vacancies and built-in electric field at n-n heterogeneous interface,which accelerates the electron transfer,induces the charge redistribu-tion,and regulates the adsorption energy of active intermediates during the reaction.This study affords a promising means to regulate the electrocatalytic performance by the construction of heterogeneous inter-faces and defects,and in-depth explores the synergistic mechanisms of n-n heterojunction and vacancies.
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