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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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    Alcohothermal synthesis of sulfidated zero-valent iron for enhanced Cr(Ⅵ)removal

    Zhongsen WangLijun QiuYunhua HuangMeng Zhang...
    192-195页
    查看更多>>摘要：Sulfidation of zero-valent iron(ZⅥ)has attracted broad attention in recent years for improving the se-questration of contaminants from water.However,sulfidated ZⅥ(S-ZⅥ)is mostly synthesized in the aqueous phase,which usually causes the formation of a thick iron oxide layer on the ZⅥ surface and hinders the efficient electron transfer to the contaminants.In this study,an alcohothermal strategy was employed for S-ZⅥ synthesis by the one-step reaction of iron powder with elemental sulfur.It is found that ferrous sulfide(FeS)with high purity and fine crystallization was formed on the ZⅥ surface,which is extremely favorable for electron transfer.Cr(Ⅵ)removal experiments confirm that the rate constant of S-ZⅥ synthesized by the alcohothermal method was 267.1-and 5.4-fold higher than those of un-sulfidated ZVI and aqueous-phase synthesized S-ZⅥ,respectively.Systematic characterizations proved that Cr(Ⅵ)was reduced and co-precipitated on S-ZⅥ in the form of a Fe(Ⅲ)/Cr(Ⅲ)/Cr(Ⅵ)composite,suggesting its environmental benignancy.
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    Can perfluorooctanoic acid be effectively degraded using β-PbO2 reactive electrochemical membrane?

    Xubin QianLei XuXu GeZhun Liu...
    196-199页
    查看更多>>摘要：Aqueous perfluorooctanoic acid(PFOA)elimination has raised significant concerns due to its persistence and bioaccumulation.Although β-PbO2 plate anodes have shown efficient mineralization of PFOA,it re-mains unclear whether PFOA can be effectively degraded using β-PbO2 reactive electrochemical mem-brane(REM).Herein,we assessed the performance of Ti/SnO2-Sb/La-PbO2 REM for PFOA removal and proposed a possible degradation mechanism.At a current density of 10mA/cm2 and a membrane flux of 8500(liters per square meter per hour,LMH),the degradation efficiency of 10mg/L PFOA was merely 8.8%,whereas the degradation efficiency of 0.1mg/L PFOA increased to 96.6% .Although the porous struc-ture of the β-PbO2 REM provided numerous electroactive sites for PFOA,the generated oxygen bubbles in the pores could block the pore channels and adsorb PFOA molecules.These hindered the protonation process and significantly impeded the degradation of high-concentration PFOA.Quenching experiments indicated that·OH played dominant role in PFOA degradation.The electrical energy per order to re-move 0.1mg/L PFOA was merely 0.74 Wh/L,which was almost an order of magnitude lower than that of other anode materials.This study presents fresh opportunities for the electrochemical degradation of low-concentration PFOA using β-PbO2 REM.
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    Regulating the electronic structure of Ir single atoms by ZrO2 nanoparticles for enhanced catalytic oxidation of formaldehyde at room temperature

    Shiqi PengYongfang RaoTan LiYufei Zhang...
    200-205页
    查看更多>>摘要：Developing low-loading single-atom catalysts with superior catalytic activity and selectivity in formalde-hyde(HCHO)oxidation at room temperature remains challenging.Herein,ZrO2 nanoparticles cou-pled low-loading Ir single atoms in N-doped carbon(Ir1-N-C/ZrO2)was prepared.The optimal Ir1-N-C/ZrO2 with 0.25 wt％ Ir loading delivers the high HCHO removal and conversion efficiency(>95％ )at 20℃,which is higher than that over Ir1-N-C with the same Ir loading.The specific rate can reach 1285.6 mmol gIr-1 h-1,surpassing the Ir based catalysts reported to date.Density functional theory cal-culation results and electron spin resonance spectra indicate that the introduction of ZrO2 nanoparticles modulate the electronic structure of the Ir single atoms,promoting O2 activation to·O2-.Moreover,the Ir-C-Zr channel is favorable for the dissociation of·O2-to active oxygen atom(O),and further acceler-ates the transformation of HCHO and intermediates(dioxymethylene and formates)to CO2 and H2O.This work provides a facile strategy to design low-loading single-atom catalysts with high catalytic activity toward HCHO oxidation.
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    Double active sites promoting hydrogen evolution activity and stability of CoRuOH/Co2P by rapid hydrolysis

    Bin DongNing YuQiu-Yue WangJing-Ke Ren...
    206-211页
    查看更多>>摘要：Cobalt-based phosphides show excellent hydrogen evolution reaction(HER)performance,however,im-proving the intrinsic activity and stability of it in alkaline electrolyte still remains a challenge.Herein,CoRuOH/Co2P/CF with heterojunction structure was developed by means of molten salt and rapid hydrol-ysis(30 s).The OH- from rapid surface hydrolysis of Co2P as a hydrogen adsorption site can facilitate the formation of thin CoRuOH layer as a water dissociation site,which may bring out better synergistic ef-fect for alkaline HER.Moreover,the covering of CoRuOH can improve the stability of Co2P for HER.When drives at 100 mA/cm2,it only requires overpotential of 81 mV in 1.0 mol/L KOH(25 ℃).Even at higher current density(1000 mA/cm2),CoRuOH/Co2P/CF can also operate stability for at least 100 h.When cou-pling with NiFe-LDH/IF in a two-electrode system,the voltage of NiFe-LDH/IF(+)||CoRuOH/Co2P/CF(-)at 1000 mA/cm2 is merely 1.77 V with 100 h,demonstrating great potential for water splitting.The imple-mentation of this work provides a new strategy and reference for the further improvement of transition metal phosphides as HER electrocatalysts.
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    Yolk shell-structured pyrite-type cobalt sulfide grafted by nitrogen-doped carbon-needles with enhanced electrical conductivity for oxygen electrocatalysis

    Jiahao XieJin LiuBin LiuXin Meng...
    212-217页
    查看更多>>摘要：Pyrite-type sulfides(PTS)exhibit promising intrinsic activities for oxygen reduction and evolution re-actions(ORR/OER).However,their poor electrical conductivities may limit the charge transfer rate to inevitably lower activity.Here,yolk-shell structured cobalt-pyrite nanospheres(CoS2 YSS)are prepared and modified with amino groups as nucleation sites for coupling highly-conductive needle-like nitrogen-doped carbon via a facile solvothermal method(CoS2 YSS@NC).The as-marked CoS2 YSS@NC-0.5 shows a gap between yolk and shell,and an obvious exterior layer of grafted NC,which can provide an inte-grated structure,an interior place,and three exposed surfaces on CoS2.CoS2 YSS@NC-0.5 reveals higher ORR activity(half-wave potential of 0.88 V)and methanol resistance than commercial Pt/C.Due to in-situ formation of highly-active CoOOH,CoS2 YSS@NC-0.5 shows a better overpotential(244mV at 10mA/cm2)and Tafel slope(135mV/dec)than RuO2.Zinc-air battery with CoS2 YSS@NC-0.5 air-cathode exhibits good open circuit potential(1.44 V),specific capacity(772.5 mAh/g)and cycling stability.Needle-like NC layer coated on the yolk-shell structure of CoS2 effectively lowers the charge transfer resistance to obtain ex-traordinary ORR/OER activities.It indicates that the integration of highly-conductive carbon onto pyrite-type sulfides is an effective strategy to acquire durable bifunctional ORR/OER catalysts.
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    Enhanced degradation of florfenicol by microscale SiC/Fe:Dechlorination via hydrogenolysis

    Yun-Fei ZhangChun-Hui ZhangJian-Hui XuLei Li...
    218-221页
    查看更多>>摘要：Herein,the degradation of florfenicol(FLO)over zero-valent iron(ZⅥ)enhanced by SiC was sys-tematically investigated.It was found that 5 g/L of ZVI/SiC(1:3)at pH 3.0 could completely degrade 20 mg/L of FLO within 1 h,with a Kobs value of 0.0873 min-1,12.5 times greater than that of pure ZⅥ(0.0069 min-1).Vibrating sample magnetometer(VSM)characterizations revealed that the use of SiC supporter reduces the magnetic intensity of ZⅥ,which mitigates iron particle agglomeration,in-creases Brunauer-Emmett-Teller(BET)surface area,and enhances FLO degradation efficiency.Further-more,ZⅥ/SiC exhibits a much lower hydrogen evolution potential(HEP)and significantly higher corrosion currents compared to pure ZⅥ.FLO was proposed to undergo degradation via reductive dechlorination,involving a hydrogenolysis mechanism that entails the cleavage of the σ bond.This study provides new insights into the reduction hydrogenation mechanism of ZⅥ.
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    Light/pH dual-responsive magnetic metal-organic frameworks composites for phosphorylated peptide enrichment

    Rui WangHe QiHaijiao ZhengQiong Jia...
    222-226页
    查看更多>>摘要：Metal-organic frameworks(MOFs)combined with specific ligands are highly adaptable smart materials that can respond to external and physiological stimuli.In this study,we introduced a pyridinyl zwitteri-onic ligand with light/pH dual response into magnetic MOF composite(Fe3O4@ZW-MOF)for enrichment of phosphorylated peptides for the first time.The introduction of the developed ligand gives MOF ma-terial dual response properties.Light stimulation affects the generation/disappearance of free radicals of the pyridine derivative,resulting in a change in the charge gradient of the zwitterion,and zwitterion can also regulate the pH of the solution by adding acid or base.Therefore,the reversible capture and release of phosphorylated peptides can be easily achieved by adjusting light and pH.The established phospho-rylated peptide enrichment platform exhibits high sensitivity(detection limit of 1 fmol),high selectivity(β-casein:BSA,1:1000),and good reusability(7 cycles).In addition,the method was applied to the en-richment of phosphorylated peptides in complex systems(non-fat milk and human serum),demonstrat-ing the feasibility of this method for phosphoproteom analysis.In conclusion,the synthesized Fe3O4@ZW-MOF is a promising MOF material,which provides the possibility to advance the application of responsive MOFs materials in proteomics.
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    Intelligent laser-induced graphene sensor for multiplex probing catechol isomers

    Tian CaoXuyin DingQiwen PengMin Zhang...
    227-234页
    查看更多>>摘要：Herein,we unveil the intelligent detection of multiple catechol isomers in complex environments utilizing both laser-induced graphene(LIG)and artificial neural network(ANN).The large scale-up manufacturing of LIG-based sensors(LIGS)with three-electrode configuration on polyimide(PI)is achieved by direct laser-writing and screen-printing technologies.Our LIGS shows excellent electrochemical performance toward catechol isomers,i.e.,hydroquinone(1,4-dihydroxybenzene,HQ),catechol(1,2-dihydroxybenzene,CT),and resorcinol(1,3-dihydroxybenzene,RC),with a low limit of detection(LOD)(CC,0.079 μmol/L;HQ,0.093 μmol/L;RC,1.18 μmol/L).Moreover,the ANN model is developed for machine-intelligent to predict concentrations of catechol isomers under an interfering environment via a single LIGS.Using six unique parameters extracted from the differential pulse voltammetry(DPV)response,the machine learning-based regression provides a coefficient of correlation with 0.998 and is able to correctly predict the total and individual concentrations in complex river samples.Hence,this work provides a guide for the preparation and application of LIGS via facile and cost-efficient mass production and the development of an intelligent sensing platform based on the ANN model.
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    Allosteric DNAzyme-based encoder for molecular information transfer

    Minghao HuTianci XieYuqiang HuLongjie Li...
    235-241页
    查看更多>>摘要：Dynamic DNA nanotechnology plays a significant role in nanomedicine and information science due to its high programmability based on Watson-Crick base pairing and nanoscale dimensions.Intelligent DNA machines and networks have been widely used in various fields,including molecular imaging,biosen-sors,drug delivery,information processing,and logic operations.Encoders serve as crucial components for information compilation and transfer,allowing the conversion of information from diverse application scenarios into a format recognized and applied by DNA circuits.However,there are only a few encoder designs with DNA outputs.Moreover,the molecular priority encoder is hardly designed.In this study,we introduce allosteric DNAzyme-based encoders for information transfer.The design of the allosteric do-main and the recognition arm allows the input and output to be independent of each other and freely programmable.The pre-packaged mode design achieves uniformity of baseline dynamics and dynamics controllability.We also integrated non-nucleic acid molecules into the encoder through the aptamer de-sign of the allosteric domain.Furthermore,we developed the 2n-n encoder and the Endo Ⅳ-assisted pri-ority encoder inspired by immunoglobulin's molecular structure and effector patterns.To our knowledge,the proposed encoder is the first enzyme-free DNA encoder with DNA output,and the priority encoder is the first molecular priority encoder in the DNA reaction network.Our encoders avoid complex operations on a single molecule,and their simple structure facilitates their application in complex DNA circuits and biological scenarios.
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    Bioinspired synthesis of cochlearol B and ganocin A

    Zhenhao WangYuliang TangRuyu LiShuai Tian...
    242-246页
    查看更多>>摘要：Described here is a divergent,biosynthetically inspired synthesis of cochlearol B and ganocin A.Key steps of the synthesis include the chromene unit construction through a biomimetic acid-catalyzed[4+2]ring cyclization.A photochemical[2+2]cycloaddition was featured to construct the cyclobutane core of cochlearol B.Different skeletal rearrangements of cochlearol B afforded ganocin A,that one of them was Lewis acid mediated epoxide rearrangement and another was DDQ induced cyclobutane formed tetrahy-drofuran ring.The described syntheses not only achieved these natural products in an efficient manner,but also provided insight into the biosynthetic relationship between the two different skeletons.
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