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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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    Enhancing stability of diradical polycyclic hydrocarbons via P=O-attaching

    Jingyuan YangXinyu TianLiuzhong YuanYu Liu...
    309-313页
    查看更多>>摘要：Diradical polycyclic hydrocarbons(PHs)have unique open-shell structures and interesting physical prop-erties.However,owing to high reactivity of unpaired electrons,such open-shell organic diradicaloids are usually less stable than closed-shell systems,limiting their practical applications.In this study,we report P=O-attaching of diradical PHs as a new strategy to enhance their stability while maintaining diradi-cal properties.Three P=O-attached PHs containing the indeno[1,2-b]fluorene,fluoreno[3,2-b]fluorene and indeno[2,1-b]fluorene π-skeletons,respectively,were designed and synthesized.As theoretically and ex-perimentally proved,two of them have the relatively large diradical characters and open-shell singlet diradical nature.In comparison to their all-carbon analogues,the attached electron-withdrawing P=O groups endow them with much lower LUMO/HOMO energy levels but preserved magnetic activities and physical properties,such as thermally accessible triplet species and multi-redox ability.Moreover,the P=O groups effectively decrease their oxidation activities and thereby lead to their remarkably excellent ambient stabilities.Thus,this P=O-attaching strategy will be applicable to other diradical PH systems and may promote the generation of stable organic diradicaloids for radical chemistry and materials.
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    Surface reconstruction enabled o-PdTe@Pd core-shell electrocatalyst for efficient oxygen reduction reaction

    Min SongQian ZhangTao ShenGuanyu Luo...
    314-318页
    查看更多>>摘要：Palladium-based alloy catalysts have been employed as one of the potential candidates for oxygen reduc-tion reaction(ORR),but the dissolution of transition metal hinders their application.Herein,structure or-dered PdTe intermetallic with Pd shell(o-PdTe@Pd)are synthesized via an electrochemical etching driven surface reconstruction strategy.The surface reconstruction could tune the electronic structure,weaken the adsorption energy of reaction intermediates on o-PdTe@Pd,resulting in enhanced electrocatalytic ac-tivity for ORR.The mass activity of o-PdTe@Pd is about 3.3 and 2.7 times higher than that of Pd/C in acid and alkaline,respectively.Besides,the half-potentials for ORR decay only about 44 mV and 12 mV after 30 k cycles accelerated durability test in acid and alkaline media,respectively.The enhanced dura-bility originates from the resistance of Te atoms dissolve in the ordered PdTe intermetallic core and the core-shell structure.When assembled in a Zn-air battery,o-PdTe@Pd electrode delivers a higher specific capacity(794 mAh/g)and better cycling stability than Pt/C.
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    Ambient electrosynthesis of urea from carbon dioxide and nitrate over Mo2C nanosheet

    Yue ZhangXiaoya FanXun HeTingyu Yan...
    319-323页
    查看更多>>摘要：Electrocatalytic synthesis of urea through C-N bond formation,converting carbon dioxide(CO2)and ni-trate(NO3-),presents a promising,less energy-intensive alternative to industrial urea production process.In this communication,we report the application of Mo2C nanosheets-decorated carbon sheets(Mo2C/C)as a highly efficient electrocatalyst for facilitating C-N coupling in ambient urea electrosynthesis.In CO2-saturated 0.2mol/L Na2SO4 solution containing 0.05mol/L NO3-,the Mo2C/C catalyst achieves an impres-sive urea yield of 579.13 μg h-1 mg-1 with high Faradaic efficiency of 44.80％at-0.5 V versus the reversible hydrogen electrode.Further theoretical calculations reveal that the multiple Mo active sites enhance the formation of*CO and*NH2 intermediates and facilitate their C-N coupling.This research propels the use of Mo2C-based electrodes in electrocatalysis and accentuates the capabilities of binary metal-based catalysts in C-N coupling reactions.
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    Synergy of sodium doping and nitrogen defects in carbon nitride for promoted photocatalytic synthesis of hydrogen peroxide

    Fabrice Nelly HabarugiraDucheng YaoWei MiaoChengcheng Chu...
    324-329页
    查看更多>>摘要：Photocatalytic synthesis of hydrogen peroxide has gradually become a promising method for in-situ pro-duction of hydrogen peroxide,which relies on sustainable solar energy.However,the commonly used photocatalyst,i.e.,carbon nitride(CN),still suffers from the drawbacks of narrow light absorption range and fast charge recombination.Here,we report a facile method to introduce nitrogen defects into carbon nitride together with sodium ion.By adjusting the ratio of sodium dicyandiamide,the band gap of carbon nitride can be controlled,while the carrier separation and transfer ability of carbon nitride is improved.The modified CN with sodium doping and nitrogen defect(SD-CN)demonstrates outstanding H2O2 pro-duction performance(H2O2 yield rate of 297.2 μmol L-1 h-1)under visible light irradiation,which is approximately 9.8 times higher than that of pristine CN.This work deepens the understanding of the coordinated effect of structural defect and element doping of carbon nitride on the photocatalytic H2O2 production performance,and provides new insight into the design of photocatalytic system for efficient production of H2O2.
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    POV-based molecular catalysts for highly efficient esterification of alcohols with aldehydes as acylating agents

    Zhikang WuGuoyong DaiQi LiZheyu Wei...
    330-334页
    查看更多>>摘要：The selective oxidative esterification of aldehydes with alcohols to the corresponding esters has been one of the hot spots in scientific research and industrial synthesis.However,the application of precious metal catalytic systems is limited by their complicated synthetic steps and high cost.Thus a highly efficient,green,recyclable selective synthesis method of esters catalyzed by polyoxovanadate(POV)-based molecu-lar catalysts has been developed in this paper.The results show that supramolecular interaction between POV and 1,3-dibenzylimidazolium bromide(Act2lm)can efficiently convert alcohols and aldehydes to the corresponding esters in high yield under much milder conditions.Mechanistic insight is also provided based on the control experiments,single crystal X-ray diffraction and cyclic voltammetry studies.
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    A new Keggin-type polyoxometallate-based bifunctional catalyst for trace detection and pH-universal photodegradation of phenol

    Shuang LiJiayu SunGuocheng LiuShuo Zhang...
    335-340页
    查看更多>>摘要：The widespread application of phenolic substances in the field of food,medicine and industry,is harmful to the environment and human health.Therefore,it is very important to develop a con-venient and effective method to detect and degrade phenolic compounds.Herein,we report a new keggin-type polyoxometallate-based metal-organic complex self-assembled under solvothermal condition,{[Cu(dap)(3-PA)]4(SiW12O40)(H2O)2}·2H2O(1,dap=1,2-diaminopropane,3-HPA=3-pyridineacrylic acid).1 shows an interesting 1D ladder-like structure.As a bifunctional catalyst,1 can be employed as a colori-metric sensor toward phenol with the relatively low detection limit(LOD)of 0.36 μmol/L(S/N=3)in the wide range(0.001-0.1 mmol/L).The title colorimetric sensor is applied to determine phenol in various water environment with good recoveries ranging from 95％-105％.In addition,1 also exhibits excellent photocatalytic degradation toward phenol under visible light with the highest removal efficiency at 96％for 100 min and wide pH universality.The selectivity,stability and reliability of the detection of 1 towards phenol,as well as the detection for 4-chlorophenol,o-cresol,4-nitrophenol and phloroglucinol were stud-ied.Furthermore,the photocatalytic reaction kinetics and the mechanisms of photodegradation of phenol were also investigated in detail.
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    Revealing the intrinsic mechanisms for accelerating nitrogen removal efficiency in the Anammox reactor by adding Fe(Ⅱ)at low temperature

    Linjing LiWenlai XuJianyong NingYaping Zhong...
    341-348页
    查看更多>>摘要：Fe(Ⅱ)is an essential trace element for anaerobic ammonium oxidation bacteria(AAOB)metabolism,and can improve the nitrogen removal efficiency of anaerobic ammonia oxidation(Anammox).Here we oper-ated two identical expanded granular sludge bed(EGSB)reactors at low temperature(15±3 ℃)for 154 days.Reactor 1(R1)received additional Fe(Ⅱ)(0.12mmol/L)during the late startup phase,while reactor 0(R0)served as the control and did not receive extra Fe(Il).Nitrogen removal in R1 became stable at 55 d of operation,ten days earlier than R0.The nitrogen removal rate(NRR)of R1 was 1.64kg N m-3 d-1 and its TN removal rate was as high as 89％,while R0 only reached 75％.The addition of Fe(Ⅱ)was fur-ther beneficial to aggregation and stability of the granular sludge,and the used sludge of both reactors showed enrichment for AAOB populations compared to the inoculum,for instance,increased abundance of Candidatus-Kuenenia and in particular of Candidatus-Brocadia(from 0.17％to 10.10％in R0 and 7.79％in R1).Diverse microbial species and complex microbial network structure in R1 compared to R0 promoted the coupled denitrogenation by Anammox,dissimilatory nitrate reduction to ammonium(DNRA),nitrate-dependent Fe oxidation(NDFO),and ferric ammonium oxidation(Feammox).In addition,the microbial community in R1 was more resistant to short-term low temperature(2-7 ℃)starvation,illustrating a further positive effect of adding Fe(Ⅱ)during the startup phase of an Anammox reactor.
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    Insights into the electron transfer mechanisms of peroxydisulfate activation by modified metal-free acetylene black for degradation of sulfisoxazole

    Chunxiu YuZelin WuHongle ShiLingyun Gu...
    349-356页
    查看更多>>摘要：Herein,a modified metal-free acetylene black(MMF-AB)catalyst was synthesized by a simple solvothermal-calcination method and designed successfully to activate peroxodisulfate(PDS)for the degradation of sulfisoxazole(SIZ).Due to the doping of N,S and O metal-free elements,the modified catalyst showed excellent catalytic performance with 100％SIZ removal within 30 min.Pseudo first-order reaction rate constants(evaluating catalytic efficiencies and activity)of MMF-AB(kobs=0.105 min-1)was 3 times higher than pure-AB(kobs=0.029 min-1).Interestingly,it was demonstrated that the reaction sys-tem is based on the transfer of electrons from SIZ to PDS to realize an electron-transfer-based mechanism by the evidence of premixing,electron paramagnetic resonance(EPR)spectroscopy,salt-bridge experi-ments and electrochemical analyses.The introduction of recyclable filtration device solved the secondary pollution caused by the dispersion of the powdered catalyst in the treated water,which further proved the practicality and superiority of the MMF-AB catalyst.
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    Insights on selective Pb adsorption via O 2p orbit in UiO-66 containing rich-zirconium vacancies

    Yu-Hang LiShuai GaoLu ZhangHanchun Chen...
    357-361页
    查看更多>>摘要：Herein,we constructed defective UiO-66 with rich Zr vacancy structure model,in which the defective structure was verified by various characterizations.Also,the Pb adsorption experiments affirmed that defective UiO-66 could display better adsorption and selective adsorption ability than that of perfect UiO-66.The results of partial density of states(PDOS)and Mulliken charge population indicated that the blue shift of O 2p and Zr 4d orbit induced the electron rearrangement of atoms closed to the bonding sites,while the positive charge number of Zr atoms decreased than before.Combining with the expansion of pore size,Pb atom was more inclined to transfer and bond with unsaturated coordination oxygens.More significantly,quantitative structure-activity relationships(QSARs)demonstrated that selective capture of Pb instead of Zn,Cu,Cd and Hg displayed by defective UiO-66 was determined jointly by bond strength,adsorption energy and electron transfer.This work provided some theoretical direction for the purpose of the fabrication of adsorbent and the investigation of mechanism.
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    Fe nanoclusters anchored in biomass waste-derived porous carbon nanosheets for high-performance supercapacitor

    Yuchen WangYaoyu LiuXiongfei HuangGuanjie He...
    362-366页
    查看更多>>摘要：Metal-nanocluster materials have gradually become a promising electrode candidate for supercapaci-tor application.The high-efficient and rational architecture of these metal-nanocluster electrode mate-rials with satisfied supercapacitive performance are full of challenges.Herein,Fe-nanocluster anchored porous carbon(FAPC)nanosheets were constructed through a facile and low-cost impregnation-activation strategy.Various characterization methods documented that FAPC nanosheets possessed a mesopore-dominated structure with large surface area and abundant Fe-N4 active sites,which are crucial for su-percapacitive energy storage.The optimal FAPC electrode exhibited a high specific capacitance of 378 F/g at a specific current of 1 A/g and an excellent rate capability(271 F/g at 10 A/g),which are comparable or even superior to that of most reported carbon candidates.Furthermore,the FAPC-based device achieved a desired specific energy of 14.8Wh/kg at a specific power of 700W/kg.This work opens a new avenue to design metal-nanocluster materials for high-performance biomass waste-based supercapacitors.
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