{"title":"Color-Tunable Thermally Activated Delayed Fluorescence Polymeric Materials Constructed by Host–Guest Complexation Revealing Rewritable Advanced Information Encryption","authors":"Ji-Hua Ma, Ying Han, Wei-Chen Guo, Hai-Yan Lu, Chuan-Feng Chen","doi":"10.31635/ccschem.024.202404657","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404657","url":null,"abstract":"<p>In this work, we report a facile and efficient supramolecular strategy for the construction of color-tunable thermally activated delayed fluorescence polymeric materials (TADF PMs) through host–guest complexation. Consequently, new kinds of TADF PMs exhibiting multicolor emissions were constructed conveniently by mixing a calix[3]acridan-modified polymer and various commercially available receptors. This emergent TADF property was attributed to the formation of the through-space charge transfer (TSCT) interactions between the macrocyclic donor in the polymer and the guest acceptors. Moreover, multicolor emission and high photoluminescence quantum yield (PLQY) of up to 40% were achieved readily by tailoring the guests with different electron-withdrawing abilities. Further, we found that the TADF PMs could be prepared readily on a large scale with good processability; thus, the approach could achieve potential application on rewritable advanced information encryption. Therefore, this work not only develops an efficient supramolecular strategy to design and construct color-tunable TADF PMs but also offers a new perspective for their practical applications in materials science.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142536372","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 : 2024-10-26DOI: 10.31635/ccschem.024.202404698
Hang Jiang, Lin Qi, Yunxing Li, Bingtian Zhao, Xin Guan, Panfei Ma, Wei Liu, Cheng Yang, Jianzhong Jiang, Bernard P. Binks, To Ngai
{"title":"Localizing Anaerobic Microbial Cultivation and Recovery Through Intelligent Pickering Emulsion Phase Inversion","authors":"Hang Jiang, Lin Qi, Yunxing Li, Bingtian Zhao, Xin Guan, Panfei Ma, Wei Liu, Cheng Yang, Jianzhong Jiang, Bernard P. Binks, To Ngai","doi":"10.31635/ccschem.024.202404698","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404698","url":null,"abstract":"<p>Microbial cultivation in microcompartments using water-in-oil (w/o) emulsion droplets has greatly advanced the study of strict anaerobic bacteria. However, a major challenge lies in the separation and recovery of the bacterial liquid. In this study, we address this challenge by localizing strict anaerobes within w/o Pickering emulsion droplets stabilized by modified microgel particles. This approach demonstrates remarkable efficiency in bacterial microencapsulation, growth and separation. The microgel particles are modified in-situ with hydrophobic silica allowing for stabilization of w/o emulsions at the optimum cultivation temperature of 37 °C while the continuous oil phase prevents oxygen ingress thereby maximizing anaerobic fermentation. Additionally, a temperature decrease triggers the microgel particles to swell and become hydrophilic, causing an immediate inversion of the emulsion to oil-in-water type. This facilitates complete separation and collection of the bacterial suspension without any damage or loss. The intelligent phase inversion of the emulsion presents exciting possibilities for various applications in anaerobic fermentation, synthetic biology and biomanufacturing.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142490808","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":"Potential-Driven Structural Evolution of Single-Atom Rhenium Sites Enables High-Performance Oxygen Electrode Reaction and Rechargeable Zn-Air Battery","authors":"Luoluo Qi, Xue Bai, Yin Wang, Zhiyao Duan, Lina Li, Jingqi Guan","doi":"10.31635/ccschem.024.202404810","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404810","url":null,"abstract":"<p>The availability of high-quality and durable bifunctional oxygen electrode catalysts remains a significant linchpin for rechargeable zinc-air batteries (ZABs). Modulating the d/f orbitals of isolated single-atom metal sites to enhance the reaction kinetics is an eloquent strategy. Herein, we fabricate a single-atom rhenium catalyst (Re-NG) with Re-N<sub>4</sub> sites on N-doped graphene, which renders exceptional oxygen reduction reaction (ORR) catalytic capacity, delivering a half-wave potential of 0.86 V and excellent oxygen evolution reaction (OER) activity with low overpotential (η<sub>10</sub> = 368 mV). Furthermore, the Re-NG performs satisfactorily on the cathode of a rechargeable ZAB with cell voltages as high as 1.53 V and specific capacities as high as 828.7 mA h g<sub>Zn</sub><sup>−1</sup>, which is close to theoretical value, and outstanding cycling stability. The excellent performance of the Re-NG can be attributed to the structural evolution at different reaction potentials as revealed by in situ X-ray absorption spectrum characterization and theoretical simulations, resulting in the formation of different active sites (ReN<sub>4</sub>-O/Re-N<sub>4</sub>-2O), which effectively and stably catalyze the reactions, thus accelerating the ORR/OER kinetics and enabling high activity. Our study clearly elucidates the mechanisms by which Re-NGs efficiently catalyze oxygen electrode reactions, providing a valuable reference for the as yet unknown catalytic mechanism of single-atom oxygen catalysts.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142490807","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 : 2024-10-26DOI: 10.31635/ccschem.024.202404796
Zhikai Li, Yu Yan, Zhi Chen, Runxu Tang, Ningxu Han, Runlin Han, Fang Fang, Jichun Jiang, Lei Hua, Xiujun Yu, Ming Wang, Jianfeng Cai, Haiyang Li, Heng Wang, Xiaopeng Li
{"title":"Multidimensional Decryption of Metallopolymer at Single-Chain Level","authors":"Zhikai Li, Yu Yan, Zhi Chen, Runxu Tang, Ningxu Han, Runlin Han, Fang Fang, Jichun Jiang, Lei Hua, Xiujun Yu, Ming Wang, Jianfeng Cai, Haiyang Li, Heng Wang, Xiaopeng Li","doi":"10.31635/ccschem.024.202404796","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404796","url":null,"abstract":"<p>Decrypting information from polymer chains is crucial in investigating molecular data storage media. However, decoding structural information about polymers at the single-chain level remains a significant challenge. Here, we design and construct tetraphenylethylene-based metallopolymers through covalent polymerization followed by intramolecular coordination. The tetratopic monomer as a mixture of <i>Z</i>/<i>E</i>-isomers contains two terminal alkynyl groups for polymerization and two 2,2′:6′,2′′-terpyridine moieties for coordination with Zn(II) or Fe(II) ions. Through incorporating coordination junctions into the polymer backbone, we are able to directly visualize individual metallopolymer chains using scanning tunneling microscopy and obtain multidimensional structural details of metallopolymers, including polymerization degree, <i>Z</i>/<i>E</i> configuration ratio, and the exact configuration sequence of a single polymer. Furthermore, we deduce the relationship between the conformation and corresponding persistence length of metallopolymer chains based on the distribution of bright lobes of coordination junctions in each polymer chain. As such, this study offers an alternative approach to obtaining multidimensional structural information at the single-chain level.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142490819","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 : 2024-10-25DOI: 10.31635/ccschem.024.202404983
{"title":"Radical-Mediated N–C Crosslinking in the Biosynthesis of Dynobactin A, a Ribosomally-Derived Peptide Targeting Gram-Negative Bacteria","authors":"","doi":"10.31635/ccschem.024.202404983","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404983","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142490393","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 : 2024-10-25DOI: 10.31635/ccschem.024.202404812
Yuanning Feng, Xingang Zhao, Daniel A. Appleton, Han Han, Ryan M. Young, Wenqi Liu, Christopher K. Lee, Weixingyue Li, Bai-Tong Liu, Yong Wu, Chun Tang, Aspen X.-Y. Chen, Charlotte L. Stern, Dong Jun Kim, Michael R. Wasielewski, Yunyan Qiu, J. Fraser Stoddart
{"title":"Chalcogenoviologen Enhanced Host–Guest Recognition","authors":"Yuanning Feng, Xingang Zhao, Daniel A. Appleton, Han Han, Ryan M. Young, Wenqi Liu, Christopher K. Lee, Weixingyue Li, Bai-Tong Liu, Yong Wu, Chun Tang, Aspen X.-Y. Chen, Charlotte L. Stern, Dong Jun Kim, Michael R. Wasielewski, Yunyan Qiu, J. Fraser Stoddart","doi":"10.31635/ccschem.024.202404812","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404812","url":null,"abstract":"<p>In the field of supramolecular chemistry, cyclophanes with novel properties are highly sought after since they can be tailored to fulfill specific tasks. In this article, we incorporate chalcogenoviologen-based units into tetracationic cyclophanes, resulting in enhanced host–guest recognition. The cyclophanes can be tuned through the addition of chalcogen bridging atoms—S, Se, and Te—which enhance their rigidity, regulate bond rotation and introduce additional steric bulk. Three cyclophanes containing chalcogen bridging atoms were synthesized and characterized in both the solution and solid states. The energy barriers for their interconversion between <i>syn-</i> and <i>anti-</i>conformations in solution were found to be correlated with chalcogen atom size. The photophysical properties of the cyclophanes are strongly dependent on the chalcogen atomic number, with intersystem crossing rates increasing from S to Se to Te. UV–vis-NIR spectroscopic and fluorometric titrations revealed that the chalcogenoviologen-based cyclophanes exhibit significantly stronger binding with electron-rich guests compared to the well-known, unsubstituted cyclobis(paraquat-<i>p</i>-phenylene). This enhancement in binding can be attributed to restricted rotation within the chalcogenoviologen units. This research provides insight into the rational design and tailored synthesis of cationic cyclophanes.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142490396","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 : 2024-10-25DOI: 10.31635/ccschem.024.202404866
{"title":"Introducing Polymer-to-Polymer Transformation into Multipath Closed-Loop Chemical Recycling by the Ring-Opening Polymerization of Thionolactone for Enhanced Versatility","authors":"","doi":"10.31635/ccschem.024.202404866","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404866","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142490395","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 : 2024-10-08DOI: 10.31635/ccschem.024.202404469
{"title":"Paving “Pt···Ti” Hot Electron Transportation Bridge for Outstanding Photothermal Catalytic Reduction of CO2","authors":"","doi":"10.31635/ccschem.024.202404469","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404469","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142385664","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 : 2024-10-08DOI: 10.31635/ccschem.024.202404882
{"title":"Boosting CO2 Electroreduction by Preactivation Strategy over Carbene-Based Metal–Organic Framework","authors":"","doi":"10.31635/ccschem.024.202404882","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404882","url":null,"abstract":"CCS Chemistry, Ahead of Print.<br/>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142385665","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}