CCS Chemistry最新文献

{"title":"Ambient Ammonia Production from Nitrogen and Hydrogen Gases Enabled by Dissociative High-Energy Electron Impact Interactions","authors":"Zijian Lin, Zhaoqing Chu, Sinan Chen,Yifan Li, Zhiwen Jiang, Changjiang Hu, Xun Chen, Degao Wang & Jun Ma1School of Nuclear Science and Technology, University of Science and Technology of China, Hefei, Anhui 2300262Engineering Laboratory of Advanced Energy Materials, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, Zhejiang 3152013Advanced Interdisciplinary Sciences Research (AiR) Center, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, Zhejiang 3152014University of Chinese Academy of Sciences, Shijingshan District, Beijing 100049","doi":"10.31635/ccschem.026.202607688","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607688","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>Primary ammonia synthesis via the Haber–Bosch process operates under harsh conditions (15–25 MPa, 400–500 °C), largely constrained by the high dissociation energy of the N≡N triple bond and the scaling relations between adsorption and transition-state energies. Here, we present ambient-condition NH3 synthesis driven by MeV-level electron beam irradiation. Optimizing the beam parameters in a catalyst-free system alone achieves an industrially relevant yield of 0.14 μmol·L−1·s−1, a two-order-of-magnitude enhancement compared to conventional electrocatalytic/photocatalytic methods. Macroscopic-microscopic Monte Carlo simulations identify that the reaction initiation is primarily driven by a cascade of low-energy secondary electrons (150–250 eV). Upon further introduction of Ru nanoclusters, irradiation enables the catalytic system to achieve a peak yield 2.8-fold higher than the maximum yield of the noncatalytic baseline. Density functional theory calculations reveal that the Ru catalyst acts as an energy ladder, lowering the N2 dissociation barrier by ∼32.7 kcal·mol−1 compared to the gas phase and stabilizing intermediates via a radical-mediated surface pathway (N· + H·). This combined physical-chemical insight informed an electron-beam scale-up strategy, showing promising energy-performance potential under mild conditions. As the system can be directly powered by renewable electricity, our work presents a simple, decentralized, and high-efficiency alternative for sustainable ammonia production.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"33 1","pages":"1-14"},"PeriodicalIF":11.2,"publicationDate":"2026-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148394038","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enantioselective Construction of 1,3-Nonadjacent Stereocenters via 1,2-Difunctionalization of Alkenes Under Visible Light","authors":"Xue-Song Zhou, Wen-Yuan Qu, Wen-Jing Xiao, Ying Cheng & Jia-Rong Chen1Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, College of Chemistry, Central China Normal University, Wuhan, Hubei 4300792Wuhan Institute of Photochemistry and Technology, Wuhan, Hubei 430083","doi":"10.31635/ccschem.026.202607790","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607790","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>Achieving simultaneous chemo-, regio-, and stereocontrol in the 1,2-difunctionalization of alkenes represents a formidable challenge in organic synthesis. While significant advances have enabled access to products bearing a single stereocenter, catalytic enantioselective methods that forge nonadjacent stereocenters through this transformation remain largely unexplored. Here, we report a synergistic photoredox-nickel-copper triple catalytic platform that enabled the enantioselective 1,2-difunctionalization of alkenes to construct 1,3-nonadjacent stereocenters. This protocol operated through a sequential radical process: photoredox-generated β-ketocarbonyl radicals add to alkenes to generate a benzylic radical and establish the first quaternary stereocenter, which subsequently underwent copper-catalyzed enantioselective cyanation to install the second stereocenter with high fidelity. This modular approach provided direct access to valuable chiral architectures featuring 1,3-nonadjacent stereocenters from readily available starting materials. Mechanistic investigations revealed that the differential oxidation potentials of nickel- and copper-enolate complexes played a decisive role in orchestrating this triple catalytic cascade.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"9 1","pages":"1-11"},"PeriodicalIF":11.2,"publicationDate":"2026-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148394097","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"One Methyl Distance from Stoichiometric Glycosylation to Catalytic Glycosylation","authors":"Zhiwen Liao, Lingkui Meng, Yue Li, Shuaiqing Li, Sicheng Zhou, Zhihua Liang, Ruohan Zhang, Jing Zeng & Qian WanHubei Key Laboratory of Natural Medicinal Chemistry and Resource Evaluation, School of Pharmacy, Huazhong University of Science and Technology, Wuhan, 430030 Hubei","doi":"10.31635/ccschem.026.202607701","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607701","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>We report the development of glycosyl 4-methylpent-4-enoate (MPE), containing an unactivated alkene moiety, as a class of glycosyl donors characterized by structural simplicity, facile accessibility, and suitability for catalytic activation. These C6-donors were efficiently activated through a proton-catalyzed hydrolactonization mechanism, proceeding under mild reaction conditions and exhibiting exceptional tolerance toward diverse functional groups. The utility of this approach is exemplified by the large-scale, chromatography-free synthesis of C6-NHS esters and the successful employment of these C6 MPE donors in the assembly of various oligosaccharides and complex natural products. This study demonstrates that deliberate molecular simplification can yield highly effective and broadly applicable glycosylation methodologies.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"26 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148394037","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synthesis of Glycans: State of the Art and Future Perspectives","authors":"Jiahao Fan, Shengzhou Ma, Weizhun Yang, Liuqing Wen, You Yang, Dapeng Zhu & Biao Yu1State Key Laboratory of Bioreactor Engineering, Shanghai Frontiers Science Center of Optogenetic Techniques for Cell Metabolism, Shanghai Key Laboratory of New Drug Design, School of Pharmacy, East China University of Science and Technology, Shanghai 2002372State Key Laboratory of Chemical Biology, Shanghai Institute of Materia Medica, Chinese Academy of Sciences, Shanghai 2012033Key Laboratory of Glyco-drug Research of Zhejiang Province, School of Chemistry and Materials Science, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou 3100244Center for Chemical Glycobiology, Zhangjiang Institute for Advanced Study, Institute of Translational Medicine, National Center for Translational Medicine (Shanghai), Shanghai Jiao Tong University, Shanghai 2002405State Key Laboratory of Chemical Biology, Shanghai Institute of Organic Chemistry, Chinese Academy of Scienc..","doi":"10.31635/ccschem.026.202607552","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607552","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>Structure-defined glycans are essential research tools in the field of glycoscience. However, natural glycans occur to be micro-heterogeneous, rendering homogeneous glycans difficult to obtain and thus posing a major obstacle to deciphering life’s glyco-code. Therefore, precision synthesis of glycans constitutes a fundamental topic at the chemistry-biology interface. In this review, we reflect current developments for the chemical and enzymatic synthesis of glycans, with emphasis being placed on the methodologies for glycosidic bond formation and the strategies for streamlined glycan assembly. Representative synthesis of complex glycans such as those with ultralong chain and novel arrangement patterns, bacterial surface glycans bearing rare sugar residues, as well as human N-glycans, O-glycans, and glycosaminoglycans, are highlighted. Moreover, the remaining challenges, including the lack of universal glycosylation methods, insufficient control over stereo- and regioselectivity, limited availability and uncontrollable catalytic efficiency of enzymes are discussed.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"366 1","pages":"1-25"},"PeriodicalIF":11.2,"publicationDate":"2026-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148394022","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Chiral Surfactants Reveal Supramolecular Asymmetry and Enable Its Amplification by Biocatalysis","authors":"Freek V. de Graaf, Puck Springintveld, Christian Zoister, Riccardo Bellan, Ghislaine Vantomme, Rainer Haag, Ivo A. W. Filot & E. W. Meijer1Institute for Complex Molecular Systems, Laboratory of Macromolecular and Organic Chemistry, Eindhoven University of Technology, 5600 MB, Eindhoven2Institute of Chemistry and Biochemistry, Freie Universität Berlin, 14195 Berlin3School of Chemistry and RNA Institute, University of New South Wales, NSW 2052 Sydney4Max Planck Institute for Polymer Research, 55128 Mainz","doi":"10.31635/ccschem.026.202607686","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607686","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>Noncovalent synthesis is an essential strategy in the development of complex molecular systems that show resemblance to biological systems. One such characteristic is homochirality, though its establishment remains elusive. Recently, it was reported that chiral surfactants can effectively induce and amplify the asymmetry of synthetic helical supramolecular polymers in water. In this study, we explored the broader applicability of this process by a first demonstration using a relatively new class of water-compatible supramolecular polymers assembled from achiral monomers. Using quantum chemical calculations on the electronic structure, we reconstructed the supramolecular organization and explained the new chiroptical properties observed. Furthermore, by applying in situ biocatalysis, we exploited the initial weak induction of asymmetry by a saccharide-based surfactant and achieved an amplification that exceeded expectations. Kinetic experiments revealed that the rate of amplification was limited by the rearrangement of supramolecular polymers in response to the changes in the surfactant composition. Therefore, our study highlights the nonequilibrium chiral rearrangement of water-compatible supramolecular polymers undergoing a nonreversible reaction, and demonstrates the effective role played by enzymes via a noncovalent synthetic approach to enhance the amplification of asymmetry.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"21 1","pages":"1-11"},"PeriodicalIF":11.2,"publicationDate":"2026-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148394041","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Infrared Spectroscopy of Neutral Distrontium Hydroxides Unravels Configuration Transformation in Growing Water Clusters","authors":"Shuai Jiang, Shangdong Li, Wenhui Yan, Jianxing Zhuang, Ailin Wang, Shiying Jiang, Yue Zhu, Hongwei Li, Hua Xie, Chuanfan Ding, Gang Li, Yinghua Yan, Ling Jiang & Xueming Yang1State Key Laboratory of Chemical Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 1160232University of Chinese Academy of Sciences, Beijing 1000493School of Materials Science and Chemical Engineering, Ningbo University, Ningbo 3152114Hefei National Laboratory, Hefei 2300885Department of Chemistry and Guangdong Provincial Key Laboratory of Catalytic Chemistry, Southern University of Science and Technology, Shenzhen 518055","doi":"10.31635/ccschem.026.202608054","DOIUrl":"https://doi.org/10.31635/ccschem.026.202608054","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>Elucidating the hydration dynamics of polynuclear metals is vital for understanding the fundamental physicochemical properties of various interfacial processes. Nevertheless, the structural characterization of these neutral complexes is hindered by the inherent difficulties associated with experimental size selection. Here, the microhydration pathways and structural transformations of neutral Sr2(OH)3(H2O)n (n = 1–5) clusters were unveiled through size-selected infrared-vacuum ultraviolet spectroscopy, coupled with quantum chemical calculations as well as ab initio molecular dynamics simulations. The results reveal that three water molecules are sufficient to trigger the configuration transformation from Sr2(μ2-OH)2(η1-OH) to Sr2(μ2-OH)3. This intriguing transition is found to be driven by hydration-induced structural deformation, achieving thermodynamic stability through the rearrangement of the hydrogen-bonding network. The current system affords a model for clarifying the metal-oxygen skeleton and hydration dynamics in the microenvironment of perovskite catalysts and opens new avenues for systematic understanding of hydration-driven lattice rearrangements, active site modulation, and catalyst activation.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"65 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148394107","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Anatase Clusters Embedded in Zeolite Enabling Ethane Photo-Dehydrogenation","authors":"Dapeng Hao, Zhendong Feng, Yida Zhou, Yi-Chi Wang, Tianjun Zhang, Guangyuan He, Zhaochi Feng, Donghai Mei, Shutao Xu, Xiao Chen, Can Li & Jihong Yu1State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 1300122International Center of Future Science, Jilin University, Changchun 1300123State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 1160234National Engineering Research Center of Lower-Carbon Catalysis Technology, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 1160235Beijing National Center for Electron Microscopy and Key Laboratory of Advanced Materials (MOE), School of Materials Science and Engineering, Tsinghua University, Beijing 1000846State Key Laboratory of New Pharmaceutical Preparations and Excipients, Key Laboratory of Medicinal Chemistry and Molecular Diagnosis of the Ministry of Education, College of Chemistry and M..","doi":"10.31635/ccschem.026.202607982","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607982","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>Ethylene is a key platform chemical extensively utilized in the modern petrochemical and fine chemical industries. The dehydrogenation of ethane to produce ethylene is currently a focal point of research, but the existing catalytic process predominantly occurs at elevated temperatures. In this study, we develop the anatase clusters confined in TS-1 zeolite (TiO2@TS-1) as efficient photocatalysts to successfully achieve photocatalytic dehydrogenation of ethane to ethylene at room temperature. The photocatalytic active center, made up of anatase clusters with a size comparable to a single unit cell of anatase, was confined within the channels of the TS-1 zeolite. The semiconductor quantum size effect endowed these ultrasmall anatase species with enhanced redox capabilities, enabling the ethane photodehydrogenation to form ethylene. In contrast, P25 (TiO2 nanoparticles) with a particle size of 21 nm exclusively catalyzed the photochemical cleavage of ethane C–C bonds, leading to methane formation. The incorporation of 0.43 wt % Pd onto TiO2@TS-1 facilitated the effective separation of photogenerated electrons and holes, thereby further enhancing their photocatalytic efficiency (6.25 mmol g(TiO2)−1 h−1 C2H4 generation rate and 100% C2H4 selectivity). This work provides a pathway to the design of zeolite-based photocatalysts and opens new prospects for their photocatalytic applications.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"5 1","pages":"1-11"},"PeriodicalIF":11.2,"publicationDate":"2026-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148394039","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Hydrogen Bond-Induced Resonant Charge Transport at the Single-Molecule Scale","authors":"Jieyao Lv, Qingqing Wu, Nan Guo, Chaochao Pan, Shiqi Sheng, Songjun Hou, Ruiqin Sun, Jun Chen, Shiyong Yu, Colin J. Lambert, Wenjing Hong & Zhibing Tan1College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 0100212State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 3610053Department of Physics, Lancaster University, Lancaster LA1 4YB","doi":"10.31635/ccschem.026.202607679","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607679","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>Hydrogen bonds are essential for life science and play a vital role in charge transport in supramolecular and biological systems. Here, we investigate the role of hydrogen bonds in charge transport through a series of hydrogen-bonded supramolecular junctions using the scanning tunneling microscopy break junction technique. We found that the insertion of a single pair of hydrogen bonds leads to the decrease of the decay constant β from 3.42 to 1.01 nm−1, which significantly enhances charge transport through the hydrogen-bonded supramolecular junctions with a distance of more than one nanometer. Density functional theory calculations show that hydrogen bonds introduce new resonances within the hydrogen-bonded molecular junctions, which change the charge transport from off-resonance transport to resonant transport. This work provides a new fundamental understanding of the role of hydrogen bonds in enhancing charge transport in natural and artificial supramolecular systems.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"41 1","pages":"1-10"},"PeriodicalIF":11.2,"publicationDate":"2026-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148394040","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Quantify Electrode Polarization for Designing High-Rate Li-Ion Batteries","authors":"Zhe Pu, Yuansheng Lin, Bowen Nan, Jingjing Xiong, Ziyan Wu, Pufan Han, Wenguang Zhao, Hai Lin, Zhongxin Chen, Mingjian Zhang","doi":"10.31635/ccschem.026.202607901","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607901","url":null,"abstract":"Electrode polarization represents a primary obstacle to achieving high-rate lithium-ion batteries by impeding electron and Li⁺ transport. While the intrinsic correlation between electrode polarization and electrode architecture has been widely recognized, a quantitative physical model that precisely describes the relationship between key structural parameters — including electrochemical active surface area, porosity, and internal resistance — with polarization magnitude is lacking. Here, we systematically deconvolute the unique contribution of each structural parameter to electronic conductivity and Li⁺ diffusivity through a series of rationally designed LiCoO₂ electrodes with gradient mass loadings. Based on comprehensive experimental analysis, we establish a novel and generalized equation that enables accurate quantification and prediction of electrode polarization for the first time. The validity of our model is demonstrated in LiNi_0.8Co_0.1Mn_0.1O₂ and LiFePO₄ electrodes that achieve both high mass loading and superior rate capability. This work not only deepens the fundamental understanding of the structure-performance correlation of battery electrodes but also provides a robust quantitative tool for the rational design and optimization of high-performance electrodes for advanced Li-ion batteries.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"30 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148348833","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"On/Off Spin Crossover Switching of an Iron(II) Metal-Organic Framework via Orthogonal Redox-Modulations","authors":"Lu Yu, Guang Yang, Si-Guo Wu, Ming-Liang Tong","doi":"10.31635/ccschem.026.202607877","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607877","url":null,"abstract":"Integrating multiple stimulus-responsive modules into spin crossover (SCO) materials enables programmable functions, yet orthogonal control over distinct switching units remains challenging. Herein, we report an iron(II) SCO metal-organic framework that incorporates both a redox-active tetra(4-pyridyl)tetrathiafuvalene (TTF(py)₄) spacer and dicyanoaurate(I) pillar, unlocking two mechanistically independent, sequentially addressable post-synthetic modification (PSM) pathways. Site-specific one-electron oxidation of the TTF moiety, triggered by tetrachloroethane, induces a conformational change from a boat-like to a nearly planar geometry and produces a radical species with enlarged thermal hysteresis. Site-selective oxidative addition of iodine to the linear dicyanoaurate(I) pillar generates square planar <i>trans</i>-[Auᴵᴵᴵ(CN)₂I₂]⁻, which strengthens the ligand field and suppresses the SCO behavior. These two PSM events operate orthogonally: TTF oxidation leaves the Au center untouched, while Au oxidation preserves the neutral TTF state. Sequential application of both modifications yields a fully oxidated low-spin product, and the entire process is reversed by mild chemical reduction with L-ascorbic acid and/or sodium thiosulfate. As a proof of concept, this study establishes a tandem redox-modification strategy for achieving structural transformability and on/off SCO switching within a unified platform.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"31 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148348836","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}