CCS ChemistryPub Date : 2026-08-31DOI: 10.31635/ccschem.026.202608010
Zhongqiang Wu, Minghao Wei, Bin Zhu & Yan Qiao1Beijing National Laboratory for Molecular Sciences (BNLMS), Laboratory of Polymer Physics and Chemistry, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 1001902University of Chinese Academy of Sciences, Beijing 1000493Department of Orthopaedics, Beijing Friendship Hospital, Capital Medical University, Beijing 100050
{"title":"Engineering Synthetic Membraneless Organelles Towards Efficient Hydrogen Production in Escherichia coli","authors":"Zhongqiang Wu, Minghao Wei, Bin Zhu & Yan Qiao1Beijing National Laboratory for Molecular Sciences (BNLMS), Laboratory of Polymer Physics and Chemistry, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 1001902University of Chinese Academy of Sciences, Beijing 1000493Department of Orthopaedics, Beijing Friendship Hospital, Capital Medical University, Beijing 100050","doi":"10.31635/ccschem.026.202608010","DOIUrl":"https://doi.org/10.31635/ccschem.026.202608010","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>The construction of compartmentalized synthetic organelles offers a compelling strategy to optimize metabolic pathways and enhance the efficiency of microbial cell factories. Conventional biohydrogen production relies on microalgae, photosynthetic bacteria, or fermentative bacteria, which often face limitations in genetic manipulation, suboptimal growth kinetics, or by-product accumulation. Although engineered Escherichia coli provides a versatile and genetically tractable chassis, its endogenous hydrogenase activity is low, and heterologously expressed hydrogenases suffer from inefficient spatial organization. To address this, we engineer hydrogen-producing membraneless organelles in E. coli through liquid–liquid phase separation of the intrinsically disordered protein I16, enabling selective sequestration of the hydrogenase system. I16 condensate formation reduced cell size while increasing intracellular structural complexity. Both in vitro reconstitution and intracellular experiments confirmed that dynamic, liquid-like SZ1-I16-RFP condensates recruit SZ2-tagged proteins via coiled-coil interactions of specific zipper peptides, and concentrate relevant substrates for hydrogen production. By promoting colocalization and finely modulating the condensate volume fraction via T7 promoter engineering, hydrogen production reached 152,375 ± 9354 nmol·L−1 within 36 h and was further elevated to 175,789 ± 5823 nmol·L−1, surpassing previously reported benchmarks. This work demonstrates a modular and programmable strategy for spatial organization of enzymatic pathways, providing a scalable framework for efficient microbial energy conversion and biosynthesis of high-value chemicals in engineered cell factories.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"185 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148870221","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}
CCS ChemistryPub Date : 2026-08-27DOI: 10.31635/ccschem.026.202608002
Lingyi Meng, Hui-Ying Sun, Meiyuan Liu, Zhen Shao, Yi-Fei Deng, Yin-Shan Meng & Yuan-Zhu Zhang1Department of Chemistry, Southern University of Science and Technology, Shenzhen 5180552School of Chemistry and Chemical Engineering, Xi’an University of Architecture and Technology, Xi’an 7100553State Key Laboratory of Fine Chemicals, Frontier Science Center for Smart Materials, Dalian University of Technology, Dalian 1160244Core Facility, Wuhan University, Wuhan 430072
{"title":"Lattice-Solvent Gating of Spin-Transition Pathways in {FeCo} Cyanometallates","authors":"Lingyi Meng, Hui-Ying Sun, Meiyuan Liu, Zhen Shao, Yi-Fei Deng, Yin-Shan Meng & Yuan-Zhu Zhang1Department of Chemistry, Southern University of Science and Technology, Shenzhen 5180552School of Chemistry and Chemical Engineering, Xi’an University of Architecture and Technology, Xi’an 7100553State Key Laboratory of Fine Chemicals, Frontier Science Center for Smart Materials, Dalian University of Technology, Dalian 1160244Core Facility, Wuhan University, Wuhan 430072","doi":"10.31635/ccschem.026.202608002","DOIUrl":"https://doi.org/10.31635/ccschem.026.202608002","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>Mastering the intermediate dynamics of electron-transfer-coupled spin transition (ETCST) in switchable Fe/Co cyanometallates requires decoupling and independently controlling their constituent steps: Co(II) spin crossover (SCO) and Fe-to-Co electron transfer (ET). Such precise control is essential for directing spin-state switching in advanced molecular devices. We report here a series of isostructural {FeCo} dinuclear cyanometallates with the general formula, [(Tp*)Fe(CN)3Co(LN3py2)][ClO4]·sol (1·sol = 1·2MeCN, 1·DMF·2H2O, 1·3MeOH·H2O, 1·MeCN·5H2O, and 1·8H2O). In all compounds, identical {FeCo}+ cations assemble into a three-dimensional supramolecular framework with solvent-accessible channels, enabling ready solvent exchange, via single-crystal-to-single-crystal transformation or through recrystallization. Structural, spectroscopic, and magnetic analyses reveal two distinct switching behaviors: Co(II)-based SCO dominates in 1·2MeCN and 1·DMF·2H2O, whereas full ETCST occurs in the other three. This mechanistic divergence is traced to solvent-induced modulations of the cobalt coordination sphere and intermolecular cyanide contacts, which collectively fine-tune the ligand-field strengths and redox balance of the Fe/Co pair. Consequently, an SCO-derived intermediate state can be selectively stabilized or suppressed, thus gating the ET pathway within an otherwise identical molecular framework. These findings establish a solvent-directed strategy for controlling the SCO-ET interface and provide a new paradigm for steering spin-transition pathways in switchable magnetic materials through deliberate lattice-solvent engineering.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"49 1","pages":"1-11"},"PeriodicalIF":11.2,"publicationDate":"2026-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148870218","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":"Supramolecular Nanoarchitectonics of Manganese-Biliverdin for Orally Delivered Transabdominal Photothermal Therapy","authors":"Luyang Zhao, Kaiwei Chen, Mengqian Shi, Yazhou Liu, Huadan Xue, Xuehai Yan, Ruirui Xing","doi":"10.31635/ccschem.026.202608171","DOIUrl":"https://doi.org/10.31635/ccschem.026.202608171","url":null,"abstract":"Photothermal therapy (PTT) offers a non-invasive approach to tumor ablation, yet current agents suffer from limited deep-tissue penetration and lack integrated mechanisms to address the interconnected pathologies of gastrointestinal malignancies. Herein, we introduce a supramolecular nanoarchitectonics strategy that leverages manganese-biliverdin (Mn-BV) coordination chemistry to overcome these limitations. Coordination of Mn (III) with the endogenous pigment BV induces a ligand-to-metal charge transfer (LMCT), shifting absorption from 680 nm to 880 nm—a 200 nm red-shift that enables deep-tissue penetration for transabdominal PTT. Supramolecular assembly with a hyaluronic acid-lipid conjugate (DPHA) imparts gastrointestinal stability, CD44-targeted delivery, and a photothermal conversion efficiency of 58.1 %. In orthotopic colorectal cancer (CRC) models, oral administration of MnBV@DPHA nanoparticles followed by transabdominal NIR irradiation achieves complete tumor ablation, resulting in >80 % survival at 120 days. Beyond local tumor eradication, this nanoarchitectonic platform reprograms the gut microbiota by suppressing pathogenic taxa and enriching probiotic commensals, while concurrently reversing immunosuppression within the tumor microenvironment-evidenced by increased CD8+ T-cell infiltration and depletion of regulatory T cells. Germ-free animal studies confirm that this antitumor immunity is strictly dependent on the gut microbiota, establishing a causal link between supramolecular design and host immune modulation. By unifying metal-coordination-driven photothermal function, supramolecular stabilization, and bidirectional regulation of the microbiota-immune axis into a single oral platform. This work establishes a conceptual paradigm for CRC intervention rooted in supramolecular nanoarchitectonics.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"64 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148682304","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":"Subtle Structural Tailoring Enables Improved Crystallinity and Miscibility for High-Efficiency, Stable Organic Photovoltaics","authors":"Mingpeng Li, Waqar Ali Memon, Xue Lai, Yongmin Luo, Yufei Wang, Zhiqiang Wang, Zijian Xiao, Guangye Zhang, Jiaying Wu, Feng He","doi":"10.31635/ccschem.026.202608095","DOIUrl":"https://doi.org/10.31635/ccschem.026.202608095","url":null,"abstract":"Organic photovoltaics (OPVs) offer a promising renewable energy route, yet balancing high power conversion efficiency (PCE) with long-term stability remains challenging. This study presents a precise molecular engineering strategy to design non-fullerene acceptors (NFAs) addressing this trade-off. Starting from the 1,4-diazepine-core 7C-2F, three NFAs, were synthesized through strategic modifications of side-chain length and terminal group π-conjugation. Characterization revealed that shortening the side chains (7C-BO-2F and 7C-eC9-2F) or extending the terminal π-conjugation (7C-N2F) enhances molecular crystallinity, reduces π-π stacking distance, and suppresses non-radiative energy loss. In bulk heterojunction devices, the PM6:7C-eC9-2F system achieved a champion PCE of 19.67%, with an energy loss of only 0.539 eV. Notably, devices based on 7C-eC9-2F exhibited exceptional photostability and thermal stability (retaining 80% of their initial PCE for 2728 h under continuous illumination and 1242 h after thermal annealing at 65 °C), greatly exceeding other controls. When incorporated into quasi-planar heterojunction architectures, these NFAs likewise exhibited superior performance, highlighting their processing versatility. In short, precise molecular engineering offers a robust route to high-efficiency, low-loss, and intrinsically stable OPVs, paving the way for their practical deployment in next-generation photovoltaics.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"9 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148682303","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}
CCS ChemistryPub Date : 2026-08-05DOI: 10.31635/ccschem.026.202608070
Zihao Yu, Lin Sun, Xincan Hu, Yubin He, Tongwen Xu
{"title":"Recent advances in ion exchange membranes for water electrolysis","authors":"Zihao Yu, Lin Sun, Xincan Hu, Yubin He, Tongwen Xu","doi":"10.31635/ccschem.026.202608070","DOIUrl":"https://doi.org/10.31635/ccschem.026.202608070","url":null,"abstract":"As the key component of water electrolysis (WE), ion exchange membranes (IEMs) determine the energy efficiency, gas purity, and device durability. A typical IEM provides conductivity through its hydrated ion transport channels. However, the same channel is also responsible for water absorption, membrane swelling, and gas crossover. Therefore, recent membrane research has moved from maximizing conductivity toward controlling the chemical and structural environment in which ions, water, and gases move. This review covers this shift across proton exchange, anion exchange, ion-solvating, and bipolar membranes. The influence of polymer backbones, ionic or solvating groups, confined channels, and reinforced architectures on membrane conductivity, dimensional stability, gas separation, and chemical durability are discussed. We further provide perspectives on why device-level durability cannot be inferred from ex situ membrane stability, since water distribution, gas evolution, electrode contact, and heat accumulation in operating cells can introduce additional failure modes.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"17 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148682302","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}
CCS ChemistryPub Date : 2026-07-31DOI: 10.31635/ccschem.026.202607930
Neng Gong, Guodong Xie, Yanhang Ma, Quanzheng Deng, Wanning Zhang, Yongping Cui, Hao Chen, Wendi Zhang, Lu Han, Yingying Duan, Shunai Che, Yuxi Fang
{"title":"Chiral Nanostructured Ultrasmall Co Nanoparticles Confined in MFI Zeolite for Syngas Conversion to Gasoline","authors":"Neng Gong, Guodong Xie, Yanhang Ma, Quanzheng Deng, Wanning Zhang, Yongping Cui, Hao Chen, Wendi Zhang, Lu Han, Yingying Duan, Shunai Che, Yuxi Fang","doi":"10.31635/ccschem.026.202607930","DOIUrl":"https://doi.org/10.31635/ccschem.026.202607930","url":null,"abstract":"Syngas conversion may enable the conversion of non-petroleum carbon sources into chemical products sustainably. Co-loaded zeolite is a promising catalyst in syngas conversion for gasoline production. However, achieving high utilization efficiency of Co remains challenging, as high Co loadings are currently necessary in selective syngas conversion to long-chain hydrocarbons. Herein, we propose that the chiral nanostructured ultrasmall Co nanoparticles (CNUCN) can significantly enhance the Co utilization efficiency. CNUCNs with an average Co particle size of ∼2.8 nm were confined in H-type mesoporous <b xmlns:bkstg=\"http://www.atypon.com/backstage-ns\" xmlns:fn=\"http://www.w3.org/2005/xpath-functions\" xmlns:pxje=\"java:com.atypon.frontend.services.impl.PassportXslJavaExtentions\" xmlns:urlutil=\"java:com.atypon.literatum.customization.UrlUtil\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"><b>MFI</b></b> zeolite (HMMZ) by impregnation method using chiral molecules as symmetry breaking agents. Chirality-induced spin polarization promotes the formation of triplet OCCO by aligning parallel electron spin, while helical lattice dis-tortion reduces its adsorption energy, subsequently promoting C<sub>2+</sub> alcohols and gasoline and minimizing CH<sub>4</sub> byproduct. The CNUCN-confined HMMZ achieves Co metal time yield of 867 mol<sub>CO</sub> kg<sub>Co</sub><sup>−1</sup> h<sup>−1</sup> and 653 mol<sub>gasoline</sub> kg<sub>Co</sub><sup>−1</sup> h<sup>−1</sup>, using ∼1/3 of the Co loading required for previous comparable Co-based catalysts with nearly the highest gasoline selectivity of ∼75% currently available.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"152 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148682305","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":"Zwitterionic Polymer Electrolytes with Enhanced Ion Transport Efficiency and Interfacial Stability for All-Solid-State Lithium Batteries","authors":"Jie Zhang, Yujie Ning, Jinyu Zhang, Ruohao Tang, Zhenyu Fan, Yawen Li, Huaqing Yu, Xiaotian Wang, Shuangxin Ren, Jichi Yang, Lanqing Wu, Lianqiang Peng, Weiwei Xie, Qing Zhao","doi":"10.31635/ccschem.026.202608062","DOIUrl":"https://doi.org/10.31635/ccschem.026.202608062","url":null,"abstract":"All-solid-state batteries based on polymer electrolytes are promising due to their high energy density, enhanced safety, and facile processability. However, their development is still hindered by low lithium-ion transport efficiency in the bulk phase and high instability towards the electrode-electrolyte interphase. In this work, we resolve the above issues by designing zwitterionic solid polymer electrolytes incorporating with lithium-salt optimization. The zwitterionic polymer matrix synthesized via reversible addition-fragmentation chain transfer copolymerization is endowed with a narrow distribution of molecular weight (M<sub>w</sub>), enabling the high mechanical strength and mitigating the decomposition of low-M<sub>w</sub> polymers. The intrinsically high dielectric environment of zwitterionic polymers not only facilitates Li<sup>+</sup> transport with a high Li<sup>+</sup> transference number (<i>t</i><sub>Li</sub><sup>+</sup>) of 0.66, but enables the dissociation of interphase-preferable lithium salts such as LiNO<sub>3</sub>, thus inducing the formation of stable and inorganic-rich interphases towards the lithium metal anode and highvoltage cathodes. As results, lithium metal batteries (LMBs) using a 50 μm lithium anode coupled with LiFePO<sub>4</sub> and LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> cathodes achieve capacity retentions of 96.85% after 400 cycles and 92.17% after 150 cycles, respectively. Finally, the zwitterionic polymer electrolytes also enable operation of LMBs under ultrathin condition (> 10 μm), thus presenting an effective strategy for building energy-dense batteries.","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":"294 1","pages":""},"PeriodicalIF":11.2,"publicationDate":"2026-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148624132","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}