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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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    Supramolecular Template-Assisted Catalytic[2+2]Photocycloaddition in Homogeneous Solution

    Fang WangSha BaiQing-Wen ZhuZi-Hang Wei...
    633-640页
    查看更多>>摘要：Supramolecular interactions can help recognize and organize substrates around an enzyme's active sites and subsequently assemble a new molecule in a cer-tain way.Inspired by nature's control of reactions,in this work we designed a template catalyst equipped with ditopic Au(Ⅰ)-N-heterocyclic carbene(NHC)func-tional sites that direct olefin substrates into reactive geometries via collaboration of coordination-driven interactions.Notably,this catalyst enables the realiza-tion of catalytic[2+2]photocycloadditions with as low as 2 mol％catalyst loading in homogeneous solution and the delivery of a series of cyclobutane derivatives with excellent conversions and stereoselectivities.The success of gram-scale reactions further demonstrates the feasibility of this strategy,which lays a solid foun-dation for the large-scale preparation of cyclobutane derivatives in the future.
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    Overcharge to Remove Cathode Passivation Layer for Reviving Failed Li-O2 Batteries

    Kai ChenDong-Yue YangJin WangGang Huang...
    641-653页
    查看更多>>摘要：Prolonging the lifetime of batteries is a long-term pursuit,and it is also one of the prerequisites for the practical application of batteries.However,this endeavor is challenging for high-energy Li-O2 batteries due to their poor charge efficiency and cathode passivation-induced by-products accumula-tion.Here,we demonstrated that overcharging Li-O2 batteries could facilitate the decomposition of accu-mulated residue products and revive the cathode;thus,the battery lifespan could be significantly ex-tended.This long battery lifetime not only made full use of the Li anode but also enabled the battery to recycle in a safer way without the risk of firing and explosion.Furthermore,overcharge could be used in Li-O2 batteries with high mass loading,high rate,and large capacity.This overcharge strategy simplified the cathode regenerating procedures and realized system-level efficient use of battery components,thereby prolonging the life of Li-O2 batteries to meet the requirements of practical applications.
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    Near-Infrared All-Fused-Ring Nonfullerene Acceptors Achieving an Optimal Efficiency-Cost-Stability Balance in Organic Solar Cells

    Wenrui LiuShengjie XuHanjian LaiWuyue Liu...
    654-668页
    查看更多>>摘要：Synergistically achieving stability,cost,and efficiency is crucial for the commercialization of organic solar cells(OSCs).Despite the rapid development of 2-(3-oxo-2,3-dihydro-1H-inden-1-ylidene)malononitrile-typenonfullereneacceptors(NFAs),they are inherently unstable due to the vulnerable exocyclic double bond and possess high synthesis complexity(SC).Based on the"all-fused-ring electron acceptor(AFAR)"concept,we report two new near-infrared NFAs,F11 and F13,featuring all fused dodecacyclic rings.By developing a whole set of synthetic procedures,F11 and F13 can be conveniently prepared at a 10 g scale within a notably short period,displaying both the low SC and the lowest costs among reported NFAs,even comparable to the classical photovoltaic material,P3HT.In comparison with the one-dimensional stacking of ITYM(ITYM=2,2'-(7,7,15,15-tetrahexyl-7,15-dihydro-s-indaceno[1,2-b:5,6-b']diindeno[1,2-d]thiophene-2,10(2H)-diylidene)dimalononitrile),the first AFRA,and mixed J-and H-aggregations in Y6,F-acceptors show a compact honeycomb-type three-dimensional stacking with ex-clusive J-aggregations,favoring multichannel charge transport.By matching a medium-bandgap polymer donor,F13 delivers greater than 13％power conversion efficiencies,which is the highest performance among non-INCN acceptors,and shows device stability super-ior to the typical ITIC-and Y6-based OSCs as evidenced by the negligible burn-in losses.This work presents a first and successful example of NFAs achieving an opti-mal efficiency-cost-stability balance in OSCs.
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    Biocompatible Chemically Fueled Transient Polymer Nanoparticles for Temporally Programmable in Vivo Imaging

    Chunyu PanJiajun XuLiang WangYiyang Jia...
    669-681页
    查看更多>>摘要：Chemically fueled dissipative self-assembly paves the way for innovative materials with lifelike proper-ties and functions.Achievement of nonequilibrium systems with biocompatibility and biofunctions remains an important and challenging task.Here,we present biocompatible chemically fueled transient polymer nanoparticles and their applications in tem-porally programmable in vivo imaging.The lifetime of the transient polymer nanoparticles can be tuned by varying the concentration of polymer,adenosine triphosphate,and phosphatase.Moreover,the tran-sient assembly of polymer nanoparticles can be paused for storage and then subsequently restored.The transient polymer nanoparticles exhibit good biocompatibility.Notably,we implement in vivo im-aging in a temporally programmable fashion by using an autonomous fluorescence modulator of transient nanoparticles assembled from polymers with a fluorescence moiety.The results in this work provide a valuable way to achieve nonequilibrium self-assembly of synthetic systems with good biocompatibility and programmable biofunctions,accelerating innovative developments of nonequi-librium soft biomaterials.
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    Plasma-Assisted Dinitrogen Activation via Dual Platinum Cluster Catalysis:A Strategy for Ammonia Synthesis under Mild Conditions

    Chaonan CuiYuhan JiaHanyu ZhangLijun Geng...
    682-694页
    查看更多>>摘要：The activation and reduction of N2 to produce ammo-nia under mild conditions is of great interest,but challenges remain.Here,we report a breakthrough in efficient dinitrogen cleavage by employing small Ptn+(n=1-4)clusters and convenient plasma assistance.The reactivity of Pt3+is found to be substantially higher than that of other clusters,and the formed Pt3N7+shows prominent mass abundance among the odd-nitrogen products.We illustrate that a chain re-action path within dual cluster cooperation,especially via a"3+2"mode,is beneficial to N≡N triple bond dissociation,embodying efficient synergistic cataly-sis.A key intermediate containing a bridged N2 of binding with two Pt clusters facilitates N2 activation with significantly enhanced interactions between the d orbitals of Pt and the antibonding π*-orbitals of N2.Furthermore,by reacting the PtnNm+clusters with H2,we observed hydrogenation products of both even-and odd-hydrogen species,indicative of ammonia release.The in situ synthesized platinum nitride clus-ters,typically Pt3N7+,induce a highly active N site for hydrogen anchoring,enabling a cost-effective hydro-treating process for ammonia synthesis.
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    Topological Defects Induced High-Spin Quartet State in Truxene-Based Molecular Graphenoids

    Can LiYu LiuYufeng LiuFu-Hua Xue...
    695-703页
    查看更多>>摘要：Topological defects in graphene materials introduce exotic properties with both fundamental impor-tance and technological implications,absent in their defect-free counterparts.Although individual topo-logical defects have been widely studied,collective magnetic behaviors originating from well-organized multiple topological defects remain a great chal-lenge.Here,we examined the collective magnetic properties originating from three pentagon topo-logical defects in truxene-based molecular graphe-noids using scanning tunneling microscopy(STM)and non-contact atomic force microscopy.Unpairedπ electrons were introduced into the aromatic topol-ogy of truxene molecular graphenoids one by one by dissociating hydrogen atoms at the pentagon defects via atom manipulation.STM measurements,together with density functional theory calculations,suggested that the unpaired electrons were ferro-magnetically coupled,forming a collective high-spin quartet state of S=3/2.Our work demonstrates that collective spin ordering could be realized through engineering regular patterned topological defects in molecular graphenoids,providing a new platform for designing one-dimensional ferromagnet-ic spin chains and two-dimensional ferromagnetic networks.
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    Interfacial Reinitiation of Free Radicals Enables the Regeneration of Broken Polymeric Hydrogel Actuators

    Baoyi WuHuanhuan LuYukun JianDachuan Zhang...
    704-717页
    查看更多>>摘要：Living organisms,from plants to animals,have in-spired and guided the design and fabrication of polymeric hydrogels with biomimetic morphology,shape deformation,and actuation behavior.Howev-er,the existing polymeric hydrogels are fragile and vulnerable,which seriously hinders further applica-tion.Therefore,endowing hydrogels with a biomi-metic self-growth property and regenerating the macroscopic shape of hydrogels after they suffer significant damage are highly desirable for the next generation of adaptive biomimetic hydrogels.In-spired by the tail regeneration of geckos,we herein report an efficient and universal strategy of interfa-cial diffusion polymerization(IDP),which can regen-erate the polymeric layer at a solid-liquid interface,thereby growing new hydrogels on the existing hy-drogel layers.Through changing the solvent viscosi-ty and/or monomer type of the hydrogel precursor,diverse new hydrogels have been regenerated to endow the initial hydrogels with additional fluores-cent functions and/or actuating properties.Due to the high efficiency and universality of IDP,an injured hydrogel actuator can be repaired,regenerated,and recovered to its initial condition,even after suffering severe damage such as cutting or piercing.We be-lieve that the regeneration strategy of polymeric hydrogels will inspire the design of biomimetic mate-rials and motivate the fabrication of the next gener-ation of soft robots with adaptive and multifunctional properties.
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    Visualization of Macrophase Separation and Transformation in Immiscible Polymer Blends

    Zhiyuan WuChunyu ZhangYouliang ZhuZhongyuan Lu...
    718-728页
    查看更多>>摘要：Identification and visualization of phase structures in-side polymer blends are of critical importance in the understanding of their intrinsic structure and dynamics.However,the direct optical observation of the individ-ual component phase in a dense bulk material poses a significant challenge.Herein,three-dimensional fluorescence imaging of phase separation and real-time visualization of phase transformation in immisci-ble polymer blends of polypropylene and polystyrene is realized through multiphoton laser scanning micros-copy.Owing to the specific fluorescence behavior of the cyanostyrene derivative 2-(4-bromophenyl)-3-(4-(4-(diphenylamino)styryl)phenyl)fumaronitrile,the high-contrast imaging of the macrophase of the com-ponent polymer in two and three dimensions with a maximum depth of 140 μm and a high signal-to-noise ratio of 300 can be achieved.Detailed spectroscopic and structural studies reveal that the distinctive fluo-rescence features of each phase domain should origi-nate from the formation of a completely different aggregate between probes and component polymer.Furthermore,visualizations of the internal morphology deformation and macrophase transformation were re-alized by employing a stretched dumbbell sample un-der constant tension.
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    Dual Triplet Sensitization Strategy for Efficient and Stable Triplet-Triplet Annihilation Upconversion Perovskite Solar Cells

    Wangping ShengJia YangXiang LiJiaqi Zhang...
    729-740页
    查看更多>>摘要：The novel triplet-triplet annihilation(TTA)upcon-version(UC)field of rubrene(Rub)and dibenzote-traphenylperiflanthene(DBP)sensitized by bulk metal halide perovskite,integrated with copper-2,3,9,10,16,17,23,24-octafluorophthalocyanine(F8CuPc)as cosensitizer,have been investigated in perovskite solar cells(PVSCs)to minimize sub-bandgap pho-ton transmission loss.The firm hydrogen bonding interaction(F.H-N between F8CuPc and MA+),cat-ion-π interaction(MA+with Rub),and the hydropho-bic characteristic of additives enable F8CuPc:Rub:DBP dually-sensitized p-i-n PVSCs based on MAPbl3 and Cs0.05(FA0.83MA0.17)0.95Pb(Br0.17I0.83)3 absor-bers to attain champion efficiencies of 20.83％and 21.51％,respectively.Furthermore,due to the excel-lent photochemical and thermal stability of F8CuPc,the corresponding PVSCs can maintain nearly 80％of the original efficiencies exposed to air with 50～70％relative humidity over 1100 h and N2 at 85 ℃ for 300 h.
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    Palladium-Catalyzed One-Step Synthesis of Stereodefined Difunctionalized Glycals

    Xiao-Ping GongYuke LiHong-Chao LiuZhe Zhang...
    741-749页
    查看更多>>摘要：Efficiently modifying glycals by directly introducing functional groups into their double bonds is a long-standing challenge.Here,the strategy of introducing two different functional groups into 1-iodoglycals to obtain modified glycals in one step through palladium catalysis was reported for the first time,and the modi-fied glycals contained stereodefined tetrasubstituted olefins.Using this method,various difunctionalized glycals that were difficult to form by other routes were synthesized in moderate to good yields.Control experiments and density functional theory calcula-tions show that the palladium catalyst played dual roles in this transformation,namely,inducing nucleo-philic substitution and catalyzing Suzuki coupling.The reaction intermediate was isolated and confirmed by X-ray crystallographic analysis.Furthermore,the gram-scale synthesis and facile deprotection of the target compound enhances the practicality of this strategy.
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