{"title":"Multiple dynamic bonds enable high mechanical strength and efficient room-temperature self-healable polyurethane for triboelectric nanogenerators","authors":"Wenwen Zhang, Huixia Xuan, Xiaofei Xu, Jiaming Lou, Qingbao Guan, Zhengwei You","doi":"10.1007/s11426-024-2298-y","DOIUrl":"10.1007/s11426-024-2298-y","url":null,"abstract":"<div><p>For room temperature self-healing triboelectric nanogenerators (TENGs), the inherent contradiction between mechanical strength and self-healing properties was an urgent problem to be solved. Based on the phenol-carbamate bond, this paper proposed a strategy to design a new molecular structure and coordinate the triple dynamic bonds, which provided a feasible strategy to solve this contradiction. With polytetramethylene ether glycol (<i>M</i><sub>n</sub> = 1,000) as the soft segment in the main chain of polyurethane (PU), meanwhile methylene diphenyl diisocyanate and 4,4′-dihydroxybiphenyl (BP) as the hard segment and chain extension agent, respectively, the combination of tetrad benzene ring endowed the resultant 4BP-PU with π-π interaction. The effective reversible dissociation and association with hydrogen bond not only bestowed 4BP-PU with high mechanical strength (16.14 MPa), but also promoted high self-healing efficiency (94.8%) at room temperature. 4BP-PU was selected as the elastic substrate between polydimethylsiloxane and copper sheet to prepare a self-healing TENG to collect energy from natural motion. Consequently, the rational molecular structure design provided new ideas for developing self-healing materials and fabricating energy harvest electronics.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1468 - 1477"},"PeriodicalIF":10.4,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716838","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":"Adding new dimension to non-directed C(sp3)–H functionalizations","authors":"Konstantin P. Bryliakov","doi":"10.1007/s11426-024-2431-3","DOIUrl":"10.1007/s11426-024-2431-3","url":null,"abstract":"","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1215 - 1217"},"PeriodicalIF":10.4,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716830","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}
Shuai Huang, Shuaige Bai, Ting Luo, Bin Feng, Min Liu, Fan Zheng, Shuang Huang, Yanpeng Fang, Dan Ding, Wenbin Zeng
{"title":"Engineering high-performance chemiluminescent probes via enzymatic pocket targeting: high-throughput screening for ultralong afterglow imaging of orthotopic hepatocellular carcinoma","authors":"Shuai Huang, Shuaige Bai, Ting Luo, Bin Feng, Min Liu, Fan Zheng, Shuang Huang, Yanpeng Fang, Dan Ding, Wenbin Zeng","doi":"10.1007/s11426-024-2296-6","DOIUrl":"10.1007/s11426-024-2296-6","url":null,"abstract":"<div><p>Hepatocellular carcinoma (HCC) is a highly aggressive liver malignancy and the main form of liver cancer. Early diagnosis and treatment of HCC can effectively reduce mortality. Carboxylesterase (CE)-specific detection and imaging can be used for early diagnosis and image-guided surgical of HCC. However, traditional optical probes suffer from poor selectivity and low imaging signal-to-noise ratio. Here, we have constructed a series of chemiluminescent probes for carboxylesterase detection based on the strategy of enzymatic pocket-oriented steric tailoring techniques. The probes with different unique and excellent properties have been obtained through the structure-based steric hindrance adjustment on the recognition site. Here, <b>CE-2</b> has been successfully used for high-throughput screening of rapid carboxylesterase inhibitors due to its extremely low detection limit (2.5 × 10<sup>−4</sup> U mL<sup>−1</sup>) and fast recognition ability. <b>CE-3</b> has been successfully used for image-guided surgery of orthotopic hepatocellular carcinoma due to its ultra-long chemiluminescence imaging (over 12 h) of hepatocellular carcinoma. This study may promote advances in the rapid detection and screening of inhibitory drugs for CE and the field of surgical navigation in HCC.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 3","pages":"1175 - 1184"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475104","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}
Xueting Lu, Lei Wang, Liangxuan Ren, Wen Li, Afang Zhang
{"title":"Thermoresponsive helical dendronized poly(arylacetylene)s: modulating the dynamic chirality","authors":"Xueting Lu, Lei Wang, Liangxuan Ren, Wen Li, Afang Zhang","doi":"10.1007/s11426-024-2302-8","DOIUrl":"10.1007/s11426-024-2302-8","url":null,"abstract":"<div><p>Helical poly(arylacetylene)s have formed an intriguing class of polymers, whose chiralities are dynamic and liable to external stimuli. By combining dendronized polymer topology with dendritic oligoethylene glycols (OEGs), we here report on synthesis of a homologous series of thermoresponsive dendronized poly(arylacetylene)s with either poly(phenyl acetylene) or poly (naphthalene acetylene) as the backbones, and investigate tunability of their helical conformations. These polymers carry dendritic OEG pendants with either methoxyl- or ethoxyl-terminals to tune their unprecedent thermoresponsive behaviors, and at the same time, dendritic shielding plays an important role in mediating their thermal phase transition temperatures. Helicity of these polymers is originated from the chiral alanine or phenylalanine moieties within the dendritic pendants, which can be tailored through manipulating solvation in different organic solvents or via thermal dehydration and collapse in water. Furthermore, achiral additives such as linear or dendritic OEGs and benzene derivatives can act similarly as thermal dehydration to induce chirality transitions of these polymers in aqueous phase through interplay competitions between the additives and the polymers against their hydration.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1486 - 1496"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716761","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":"Efficient photocatalytic H2 evolution over tubular mesoporous carbon nitride with N-vacancy by microwave-assisted synthesis","authors":"Yuanlong Pan, Qiang Zhang, Guangzheng Huang, Yannan Luo, Honglin Gao","doi":"10.1007/s11426-024-2237-1","DOIUrl":"10.1007/s11426-024-2237-1","url":null,"abstract":"<div><p>Modifying the microstructure of photocatalysts while simultaneously introducing vacancies has shown significant potential in enhancing their performance for hydrogen production. Herein, a novel tubular mesoporous carbon nitride (TMCN) with nitrogen vacancies was fabricated using a microwave-assisted synthesis strategy, employing melamine-cyanuric acid supramolecular (MC-S) as the precursor. The optimized TMCN exhibited an outstanding H<sub>2</sub> production rate, approximately 29 times higher than that of pristine g-C<sub>3</sub>N<sub>4</sub>. The N-vacancies serve as sites for reactant adsorption and activation, leading to enhanced delocalization of HOMO-LUMO. Furthermore, the porous structures of TMCN facilitate the reactant diffusion, while its tubular architectures promote the oriented transfer of charge carriers. Crucially, the markedly improved photocatalytic performance of TMCN can be predominantly attributed to the synergistic effects arising from its superior structure and N-vacancy defects. This work opens new possibilities for the simultaneous formation of surface defect states as photocatalytic reaction sites and distinctive structures conducive to charge carrier transport.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 3","pages":"866 - 873"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475120","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":"Biphenyl-dihydrothiazole-cyclized peptide libraries for peptide ligand and drug discovery","authors":"Junjie Liu, Xiangnan Sun, Jie Zhuang, Ziyan Liu, Chaoying Xu, Dalei Wu, Chuanliu Wu","doi":"10.1007/s11426-024-2291-x","DOIUrl":"10.1007/s11426-024-2291-x","url":null,"abstract":"<div><p>Utilizing diverse organic crosslinkers for cyclization has proven to be an effective approach to creating peptide libraries, enabling the rapid discovery of functional peptides. Existing crosslinkers usually provide a tiny and flexible molecular scaffold to constrain peptide conformations, leading to larger cyclic peptides retaining a high degree of flexibility. Moreover, the limited structural impact of the crosslinkers undermines the feasibility of diversifying cyclic peptide structures by varying the types of crosslinker scaffolds. These limitations hamper the robustness of various cyclic peptide libraries for ligands and drug discovery and development. Herein, we present a unique crosslinker featuring a bulky and rigid biphenyl-dihydrothiazole (BDT) scaffold for the rapid and biocompatible cyclization of linear peptides. This scaffold was used to construct phage display BDT-cyclic peptide libraries, enabling the effective identification of cyclic peptide binders with low-nanomolar binding affinity toward BCL-X<sub>L</sub>, a protein target with potential for cancer therapy. Thus, this study introduces a novel method for constructing cyclic peptide libraries with rigidly constrained and diverse structures, offering a promising avenue for the <i>de novo</i> discovery of cyclic peptide ligands and drugs.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1434 - 1444"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716682","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}
Haofeng Sun, Minghao Wang, Wenjie Li, Yang Liu, Xinyu Sun, Wenjie Wang, Yuqiao Guo, Yi Xie, Changzheng Wu
{"title":"2D free-standing ultra-large ferromagnetic nanosheets via a topotactic transformation strategy","authors":"Haofeng Sun, Minghao Wang, Wenjie Li, Yang Liu, Xinyu Sun, Wenjie Wang, Yuqiao Guo, Yi Xie, Changzheng Wu","doi":"10.1007/s11426-024-2340-0","DOIUrl":"10.1007/s11426-024-2340-0","url":null,"abstract":"<div><p>Considerable progress has been made in synthesizing two-dimensional (2D) materials by exfoliating layered solids. However, for tremendous non-layered inorganic materials, especially magnet solids, usually with closely packed bulk phases by strong chemical bonds, it is challenging to obtain their high-quality 2D sheets. Herein, we highlighted a new structure of free-standing ferromagnetic nanosheets featuring (111) facets. For magnet, Fe<sub>3</sub>O<sub>4</sub>, its inversed spinel crystalline has limited abilities to exfoliate into 2D forms and rarely exists as free-standing nanosheets owing to aggregation induced by magnetic force. We realized a breakthrough in achieving free-standing ferromagnetic nanosheets with dramatically surpassing size limitations via topotactic conversion from layered counterparts. Our Fe<sub>3</sub>O<sub>4</sub> nanosheets exhibited a maximum width of 60 µm while only ∼4 nm thick, prominently exposing (111) facets. 2D Fe<sub>3</sub>O<sub>4</sub> behaved anisotropic magnetism, which displayed a 4.6 emu g<sup>−1</sup> moment (<i>H</i>=500 Oe) in the (111) plane but 2.1 emu g<sup>−1</sup> out of the (111) plane, indicating a (111) in-plane easy axis. We anticipated our topotactic conversion strategy would inspire the creation of 2D non-layered materials and enrich the 2D materials family.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1337 - 1344"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716750","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}