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中国化学会会刊（英文）
中国化学会会刊（英文）
中国化学会会刊（英文）/Journal CCS Chemistry
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    Editorial

    Xi ZhangDonna J.Minton
    772-775页
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    Author Spotlight

    李永舫李艳梅陈于蓝陈义旺...
    776-780页
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    Selection of Functional Spacer Cations for Efficient 2D/3D Perovskite Solar Cells

    Dengxue LiZhi XingXiangchuan MengXiaotian Hu...
    781-801页
    查看更多>>摘要：In recent years,perovskite solar cells(PSCs)have gone through unparalleled rapid expansion and be-come a candidate for solar cells.Among various PSCs,though typical three-dimensional(3D)halide perovskite-based PSCs deliver the highest efficiency,they are subjected to severe instability,which con-strains their commercializability.In comparison,two-dimensional(2D)PSCs have aroused wide-spread concern due to their superior stability.After that,2D/3D perovskite materials combining high ef-ficiency and good stability have emerged as the times require,which are expected to bring about stable and efficient PSCs.Here,this review focuses on selection of functional spacer cations for efficient and stable 2D/3D PSCs.First,the unique function of different spacer groups and the selection of appro-priate spacer cations in 2D perovskites is summa-rized and proposed.Then,by selecting appropriate cations,the role of 2D perovskites is elaborated,including energy level regulation,ion migration sup-pression,defect passivation,residual stress release and improved stability.In addition,the preparation methods of 2D/3D perovskites are comprehensively summarized.Finally,current challenges and future opportunities for the further development of 2D/3D perovskites for solar cells are discussed and pros-pected.
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    Proximity Chemistry in Living Systems

    Yanjun LiuYun GeRuxin ZengWilliam Shu Ching Ngai...
    802-813页
    查看更多>>摘要：Enzyme-and catalyst-generated reactive species have been leveraged in the past decade to covalently label biomolecules within a short range of a defined site or space inside cells or at the cell-cell interface.Due to their high spatial resolution,such proximity labeling strategies have been coupled with various bioanalytical techniques for dissecting dynamic and complex biological processes.Here,we review the development of enzyme-and catalyst-triggered proximity chemistry and their applications to identi-fying protein interaction networks as well as cell-cell communications in living systems.
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    Diastereoselective and Enantioselective Nickel-Catalyzed Reductive Coupling of Imines and Unactivated Alkenes

    Biao WangXian-Ming LiuKai-Xiang ZhangWei-Min Feng...
    814-822页
    查看更多>>摘要：Herein we report a method for highly diastereoselec-tive and enantioselective nickel-catalyzed reductive coupling of imines and unactivated alkenes.A mono-dentate chiral spiro phosphoramidite ligand is the key to controlling the enantioselectivity.This efficient,straightforward method allows for the construction of chiral benzocyclic and indole-fused cyclic amines with two contiguous stereogenic centers in good yields from readily accessible starting materials.
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    A Cleavable Self-Inclusion Conjugate with Enhanced Biocompatibility and Antitumor Bioactivity

    Han WuTian XiaFeilong QiShan Mei...
    823-829页
    查看更多>>摘要：The effective encapsulation of antitumor drugs by dynamic host-guest interactions at the submicromo-lar level remains a challenge.Herein,we report a cleavable self-inclusion camptothecin-cucurbit[7]uril(CPT-CB[7])conjugate.The binding affinity of CB[7]to CPT is greatly enhanced owing to the intramolecu-lar self-inclusion,demonstrating a concentration-independent encapsulation efficiency of nearly 100％.The disulfide linker of CPT-CB[7]conjugate can be cleaved in the reductive tumor microenviron-ment,transforming the self-inclusion into a binary host-guest complexation pattern,thus releasing the CPT thoroughly.The enhanced biocompatibility and antitumor bioactivity of the cleavable self-inclusion conjugate have been confirmed by in vitro and in vivo experiments.This line of research will open new hor-izons for supramolecular drug delivery systems oper-ating in diluted and competitive conditions.
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    Optical Trapping of a Single Molecule of Length Sub-1 nm in Solution

    Biao-Feng ZengRan DengYu-Ling ZouChun-An Huo...
    830-840页
    查看更多>>摘要：Plasmonic optical manipulation has emerged as an affordable alternative to manipulate single chemical and biological molecules in nanoscience.Although the theoretical models of sub-5 nm single-molecule trapping have been considered promising,the exper-imental strategies remain a challenge due to the Brownian motions and weak optical gradient forces with significantly reduced molecular polarizability.Herein,we address direct trapping and in situ sensing of single molecules with unprecedented size,down to～5 Å in solution,by employing an adjustable plasmonic optical nanogap and single-molecule con-ductance measurement.The theoretical simulations demonstrate that local fields with a high enhance-ment factor,over 103,were generated at such small nanogaps,resulting in optical forces as large as sev-eral piconewtons to suppress the Brownian motion and trap a molecule of length sub-1 nm.This work demonstrates a strategy for directly manipulating the small molecule units,promising a vast multitude of applications in chemical,biological,and materials sciences at the single-molecule level.
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    18.55％Efficiency Polymer Solar Cells Based on a Small Molecule Acceptor with Alkylthienyl Outer Side Chains and a Low-Cost Polymer Donor PTQ10

    Xiaolei KongJinyuan ZhangLei MengChenkai Sun...
    841-850页
    查看更多>>摘要：The development of A-DA'D-A type small molecule accep-tors(SMAs)has promoted the rapid progress of polymer solar cells(PSCs)in recent years.The outer side chains on the terminal thiophene ring and inner side chains on nitrogen atoms of the pyrrole ring of the DA'D fused ring play impor-tant roles in the photovoltaic performance of the SMAs.Here,we synthesized two new SMAs,2,2'-((2Z,2'Z)-((12,13-bis(2-ethylhexyl)-3,9-bis(4-(2-ethylhexyl)thiophen-2-yl)-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2",3":4',5']thieno[2',3':4,5]pyrrolo[3,2-g]thieno[2',3':4,5]thieno[3,2-b]indole-2,10-diyl)bis(methaneylylidene))bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile(T2EH)and 2,2'-((2Z,2'Z)-((12,13-bis(2-ethylhexyl)-3,9-bis(3-(2-ethylhexyl)phenyl)-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2",3":4',5']thieno[2',3':4,5]pyrrolo[3,2-g]thieno[2',3':4,5]thieno[3,2-b]indole-2,10-diyl)bis(methaneylylidene))bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene)(P2EH),with 2-ethylhexylβ-substituted thienyl or phenyl as the outer side chains,respectively,to improve the photovoltaic properties of the SMAs.Compared with P2EH,T2EH exhibits closer π-π stack-ing,slightly red-shifted absorption,and higher electron mo-bility.Moreover,the active layer of T2EH blended with the low-cost polymer donor poly[(thiophene)-alt-(6,7-difluoro-2-(2-hexyldecyloxy)quinoxaline)](PTQ10)possesses higher mobilities,a longer lifetime,and less recombination of the charge carriers in comparison with that of the PTQ10∶P2EH active layer.Eventually,the PTQ10∶T2EH-based PSCs showed an outstanding power conversion efficiency(PCE)of 18.55％,while the PSC based on PTQ10∶P2EH displayed a PCE of 17.50％.Importantly,18.55％is the highest PCE in the PTQ10-based binary PSCs so far.The results indicate that T2EH is one of the best SMAs for the PTQ10-based PSCs and is a promising SMA for the application of PSCs.
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    Construction of Synergistic Co and Cu Diatomic Sites for Enhanced Higher Alcohol Synthesis

    Gaofeng ChenOlga A.SyzgantsevaMaria A.SyzgantsevaShuliang Yang...
    851-864页
    查看更多>>摘要：Higher alcohol synthesis(HAS)from syngas could efficiently alleviate the dependence on the traditional fossil resources.However,it is still challenging to con-struct high-performance HAS catalysts with satisfying selectivity,space-time yield(STY),and stability.Here-in,we designed a diatomic catalyst by anchoring Co and Cu sites onto a hierarchical porous N-doped car-bon matrix(Co/Cu-N-C).The Co/Cu-N-C is efficient for HAS and is among the best catalysts reported.With a CO conversion of 81.7％,C2+OH selectivity could reach 58.5％with an outstanding C2+OH STY of 851.8 mg/g.h.We found that the N4-Co1 and Cu1-N4 showed an excellent synergistic effect.The adsorption of CO occurred on the Co site,and the surrounding nitrogen sites served as a hydrogen reservoir for the CO reduction reactions to form CHxCo.Meanwhile,the Cu sites stabilized a CHOCu species to interact with CHxCo,facilitating a barrier-free formation of C2 spe-cies,which is responsible for the high selectivity of higher alcohols.
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    Ligand Modified and Light Switched On/Off Single-Chain Magnets of{Fe2Co} Coordination Polymers via Metal-to-Metal Charge Transfer

    Ji-Xiang HuHai-Lang ZhuYin-Shan MengJiandong Pang...
    865-875页
    查看更多>>摘要：It is still a formidable challenge to simultaneously switch single-chain magnet(SCM)behavior via li-gand modification and light irradiation in the field of molecular spintronics.Herein,we present a ligand-bridged layer {[pzTpFe(CN)3]4Co2(Bib)4}·3H2O(1;pzTp,tetra-kis(1-pyrazolyl)borate;Bib,1,4-bis-(1H-imidazol-1-yl)benzene)and a well-isolated double chain {[pzTpFe(CN)3]2Co(Bpi)2}·CH3CN·4H20(2;Bpi,1-Biphenyl-4-yl-1H-imidazole)that display re-versible metal-to-metal charge transfer(MMCT)be-tween FeⅢLS(μ-CN)CoⅡHS(μ-NC)FeⅢLS(LS,low spin;HS,high spin)and FeⅢLS(μ-CN)CoⅢLS(μ-NC)FeⅡLs lin-kages under alternating irradiation with 808 and 532 nm lasers.The bidirectional light irradiations induces significant changes in anisotropy and intra-chain magnetic interactions,resulting in the on/off switching of SCM behavior with observable hystere-sis loops by 808 and 532 nm light irradiations for both compounds.Because of the ligand modifica-tion,the SCM property of 2 with the monodentate ligand is greatly improved with a correlation length increased to 83,which is the largest correlation length among all reported light actuated SCMs.Furthermore,the influence of ligand modification on their thermally induced MMCT is also discussed.This study provides a rational approach for the swift and reversible control of SCM behavior via ligand modi-fied and light induced MMCT,which is crucial to the future technological demand for high-density data storage and processing.
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