Science China Chemistry最新文献_第5页

Biphenyl-dihydrothiazole-cyclized peptide libraries for peptide ligand and drug discovery 用于肽配体和药物发现的联苯-二氢噻唑环化肽文库

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2291-x

Junjie Liu, Xiangnan Sun, Jie Zhuang, Ziyan Liu, Chaoying Xu, Dalei Wu, Chuanliu Wu

{"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}

引用次数: 0

A versatile synthetic strategy towards rare earth based metal-organic frameworks 稀土基金属有机骨架的多功能合成策略

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2322-9

Quan Shi, Yun-Hao Xu, Ming-Hui Chen, Peng Zhao, Wen-Bo Deng, Ji Xiong, Kai Guo, Ya-Qing Feng, Bao Zhang

{"title":"A versatile synthetic strategy towards rare earth based metal-organic frameworks","authors":"Quan Shi, Yun-Hao Xu, Ming-Hui Chen, Peng Zhao, Wen-Bo Deng, Ji Xiong, Kai Guo, Ya-Qing Feng, Bao Zhang","doi":"10.1007/s11426-024-2322-9","DOIUrl":"10.1007/s11426-024-2322-9","url":null,"abstract":"<div><p>Rare earth metal-organic frameworks (RE-MOFs) have drawn wide attention owing to diverse network structures and various application prospects. However, due to the unpredictable formation of the nodes, it is still challenging to design novel RE-MOFs. A novel versatile strategy was developed employing a RE-acetate complex (RE<sub>2</sub>(CH<sub>3</sub>COO)<sub>6</sub>·4H<sub>2</sub>O) as a precursor to construct RE-MOFs. 2D RE-MOFs (RE-DBP) and 3D RE-MOFs (RE-TCPP) could be obtained by using dicarboxylic porphyrin ligands H<sub>2</sub>DBP and tetracarboxylic porphyrin ligands H<sub>2</sub>TCPP, respectively. Ten RE-MOFs were further synthesized to verify the universality of the methodology. Highly crystalline RE-MOFs could also be prepared at room temperature via the developed strategy, which could significantly promote large-scale preparation and practical application of RE-MOFs. As proof of the concept, the performance of porphyrin-based RE-MOFs was investigated in the photocatalytic cycloaddition of CO<sub>2</sub> with epoxides. Among the RE-DBP(Co) MOFs, Tb-DBP(Co) exhibited the best photocatalytic performance, which was also greater than that of the corresponding 3D MOF Tb-TCPP(Co) due to the optimal 2D structure and thus the accelerated photogenerated charge separation and transfer process. This work not only provides a novel versatile strategy to design and develop RE-MOFs, but also proposes a promising approach for the potential bulk production of RE-MOFs at room temperature.</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":"1362 - 1371"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716765","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}

引用次数: 0

High-selectivity electroreduction of low-concentration CO2 with large concentration fluctuation 低浓度CO2的高选择性电还原，浓度波动大

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2307-y

Mengyu Qi, Yanbin Ma, Chao Zhang, Bingwei Li, Xueqing Yang, Zhaolin Shi, Simeng Liu, Changhua An, Jiqing Jiao, Tongbu Lu

{"title":"High-selectivity electroreduction of low-concentration CO2 with large concentration fluctuation","authors":"Mengyu Qi, Yanbin Ma, Chao Zhang, Bingwei Li, Xueqing Yang, Zhaolin Shi, Simeng Liu, Changhua An, Jiqing Jiao, Tongbu Lu","doi":"10.1007/s11426-024-2307-y","DOIUrl":"10.1007/s11426-024-2307-y","url":null,"abstract":"<div><p>Electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) has been regarded as one of the most promising solutions to achieving “zero carbon emission”. In most of the CO<sub>2</sub>RR-related studies, high-purity CO<sub>2</sub> has been employed as the feed gas; however, in practice, CO<sub>2</sub> is generally emitted in low concentrations, so it is of great significance to realize high-selectivity electroreduction of low-concentration CO<sub>2</sub> with large concentration fluctuation. In this work, we constructed a dual-active-site catalyst and successfully achieved CO<sub>2</sub> local enrichment and conversion for low-concentration CO<sub>2</sub>. <i>Operando</i> experiments reveal that the catalyst has one type of site for activating CO<sub>2</sub> and one type of site for binding the reaction intermediates. The dual-active-site catalyst displays a selectivity for formic acid consistently above 97% over a broad potential window (from −0.9 to −1.6 V <i>vs.</i> RHE). Even when fed with a low-concentration CO<sub>2</sub> stream (volume ratio from 50% down to 10%), the dual-active-site catalyst could display high activity and selectivity (>91%). In particular, the selectivity is still above 85% when the CO<sub>2</sub> volume ratio is as low as 5%. This work offers a feasible route for converting low-concentration CO<sub>2</sub> via a synergistic effect for dual-active-site catalysts.</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":"1620 - 1626"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716767","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}

引用次数: 0

2D free-standing ultra-large ferromagnetic nanosheets via a topotactic transformation strategy 基于拓扑策略的二维独立超大铁磁纳米片

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2340-0

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}

引用次数: 0

Guest-induced topological transformation and near-infrared photothermal conversion featuring the Cp*Rh unit via coordination-driven self-assembly 通过协调驱动自组装的Cp*Rh单元的客源诱导拓扑变换和近红外光热转换

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2304-9

Xin-Yu Wang, Qiu-Shui Mu, Xiang Gao, Guo-Xin Jin

{"title":"Guest-induced topological transformation and near-infrared photothermal conversion featuring the Cp*Rh unit via coordination-driven self-assembly","authors":"Xin-Yu Wang, Qiu-Shui Mu, Xiang Gao, Guo-Xin Jin","doi":"10.1007/s11426-024-2304-9","DOIUrl":"10.1007/s11426-024-2304-9","url":null,"abstract":"<div><p>Herein, we perform a topological transformation by guest induction, converting [2]catenane <b>Rh-1</b> into the <b>Rh-3</b> molecular figure-of-eight. The transformation involves the interaction of longer <i>π</i>-acceptor half-sandwich Rh<sup>III</sup> bimetallic building block <b>B1</b> [(Cp*Rh)<sub>2</sub>(TPPHZ)](OTf)<sub>4</sub> and <i>π</i>-donor bipyridyl ligands 4,4′-bis((pyridin-4-ylthio)methyl)-1,1′-biphenyl with four molecules of pyrene under ambient temperature in high yields. Intriguingly, despite the involvement of a single pyrene molecule in modifying [2]catenane <b>Rh-2</b> by transitioning <b>B1</b> to <b>B2</b>, the underlying skeleton of <b>Rh-2</b> remains unaltered. Furthermore, we explored the application of these substances before and after the reaction for near-infrared (NIR) photothermal conversion. Through meticulous structural analysis, the <i>π</i>–<i>π</i> stacking interactions play a pivotal role in stabilizing the abovementioned structures, enhancing the nonradiative transitions and initiating photothermal conversion in solution. Based on the results, the introduction of pyrene significantly intensified the <i>π</i>–<i>π</i> stacking interactions but diminished the electron density between the adjacent NDI units, leading to a decrease in the NIR photothermal conversion efficiency (from 58.29% to 51.60%). In this study, an innovative approach is introduced for fabricating valuable half-sandwich-structured NIR photothermal conversion materials, and this research has promising prospects for enhancing the field of materials science with potential candidates for future development.</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":"1345 - 1354"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716752","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}

引用次数: 0

Efficient photocatalytic H2 evolution over tubular mesoporous carbon nitride with N-vacancy by microwave-assisted synthesis 微波辅助合成具有n空位的管状介孔氮化碳上的高效光催化析氢

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2237-1

Yuanlong Pan, Qiang Zhang, Guangzheng Huang, Yannan Luo, Honglin Gao

{"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}

引用次数: 0

Lung-targeted polyzwitterionic lipid nanoparticles for effective treatment of lung inflammation 肺靶向多两性离子脂质纳米颗粒有效治疗肺部炎症

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2295-8

Wen Zhang, Jiaxin Li, Nan Wang, Muzi Li, Chen Peng, Xinyue Zhang, Guanghui Ouyang, Yan Li

{"title":"Lung-targeted polyzwitterionic lipid nanoparticles for effective treatment of lung inflammation","authors":"Wen Zhang, Jiaxin Li, Nan Wang, Muzi Li, Chen Peng, Xinyue Zhang, Guanghui Ouyang, Yan Li","doi":"10.1007/s11426-024-2295-8","DOIUrl":"10.1007/s11426-024-2295-8","url":null,"abstract":"<div><p>Lipid nanoparticles (LNPs) are non-viral nucleic acid delivery systems that show great potential in vaccine development and disease treatment. Although LNPs are particularly advantageous for <i>in vivo</i> delivery, the wide application of LNPs is impeded as their systemic delivery of nucleic acid drugs to extrahepatic tissues remains highly challenging. To address this issue, we developed lung-targeted polyzwitterionic LNPs with zwitterionic polymer poly(2-methyacryloyloxyethyl phosphorylcholine) (PMPC) modified 1,2-dimyristoyl-sn-glycerol lipid for the delivery of small interfering RNA (siRNA). Three libraries with 90 PMPC-LNPs@siRNA were established. The polyzwitterionic PMPC-LNPs had high siRNA encapsulation efficiency of about 90%. The findings revealed that polyzwitterionic PMPC-LNPs@siRNA absorbed protein corona with the main component of Vitronectin, mediating lung-targeted delivery of siRNA. With good cellular uptake and endo/lysosomal escape ability, <i>in vitro</i> and <i>in vivo</i> studies demonstrated that polyzwitterionic PMPC-LNPs with siRNA against tumor necrosis factor-α (TNF-α) could significantly down-regulate the TNF-α in mRNA and protein levels, and improved the pathological features of lung inflammation. Polyzwitterionic PMPC-LNPs@siRNA achieved safe and efficient treatment of lung inflammation. Therefore, this work offered a promising siRNA therapeutic approach for lung diseases.</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":"1107 - 1116"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475117","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}

引用次数: 0

Near-infrared organic photosensitizers with aggregation-induced emission and switchable fluorescence for fungal infection therapy 具有聚集诱导发射和可切换荧光的近红外有机光敏剂用于真菌感染治疗

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2325-2

Xinzhe Yang, Zixuan Huang, Keke Ding, Huili Yang, Lirong Wang, Qing Xia, Rong Hu, Guang Shi, Bingjia Xu, Anjun Qin

{"title":"Near-infrared organic photosensitizers with aggregation-induced emission and switchable fluorescence for fungal infection therapy","authors":"Xinzhe Yang, Zixuan Huang, Keke Ding, Huili Yang, Lirong Wang, Qing Xia, Rong Hu, Guang Shi, Bingjia Xu, Anjun Qin","doi":"10.1007/s11426-024-2325-2","DOIUrl":"10.1007/s11426-024-2325-2","url":null,"abstract":"<div><p>The development of near-infrared (NIR) photosensitizers with aggregation-induced emission (AIE) properties, switchable luminescence colors, and satisfactory photodynamic therapy (PDT) effects on the treatment of fungal infection is of great importance but very challenging. Herein, two ionic organic luminogens are constructed by employing diphenylamine, diphenylacrylonitrile/1,2-diphenylethene, and methylated quinoline cation as building blocks. It is found that the resulting compounds TCQF and TQF show apparent AIE properties and produce intense fluorescence with high photoluminescence quantum yields of up to 31.2% in the solid state. In the meantime, their emission colors can be switched between red and NIR and in the NIR region by mechanical force and solvent vapor, respectively, thereby enabling remarkable and reversible mechanochromism with emission variations of up to 104 nm. More excitingly, TCQF and TQF can efficiently generate ROS under the illumination of white light and show excellent antimicrobial activities and satisfactory PDT capabilities. Inspired by the unique anti-fungus properties, TCQF is employed as a biocompatible NIR photosensitizer for treating wound infection with <i>C. albicans</i>, and apparent PDT effects are achieved. This work provides a new direction for the development of multifunctional NIR materials with AIE properties.</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":"1426 - 1433"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716760","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}

引用次数: 0

Encapsulating perovskite quantum dots into 3D COF for visible light-driven CO2 reduction 将钙钛矿量子点封装到三维碳纳米管中，用于可见光驱动的二氧化碳还原

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2300-8

Xinxin Wang, Yucheng Jin, Xiya Yang, Qingyu Luan, Tianyu Wang, Dongdong Qi, Kang Wang, Jianzhuang Jiang

{"title":"Encapsulating perovskite quantum dots into 3D COF for visible light-driven CO2 reduction","authors":"Xinxin Wang, Yucheng Jin, Xiya Yang, Qingyu Luan, Tianyu Wang, Dongdong Qi, Kang Wang, Jianzhuang Jiang","doi":"10.1007/s11426-024-2300-8","DOIUrl":"10.1007/s11426-024-2300-8","url":null,"abstract":"<div><p>Lead halide perovskite quantum dots (LHP QDs) have been revealed to possess great potential in photocatalytic applications including CO<sub>2</sub> reduction, which however suffer from poor stability. Herein, a high crystalline hydrazine-linked three-dimensional (3D) covalent organic framework, USTB-17, was fabricated from the reaction between 12-connected building block and 4-connected 3,5,7-tetrakis(4-aldophenyl)-adamantane. Post-modification with Ni<sup>2+</sup> affords the metallic framework USTB-17(Ni) followed by sequential deposition of the CH<sub>3</sub>NH<sub>2</sub>PbI<sub>3</sub> (MAPbI<sub>3</sub>) perovskite QDs into its pores, generating the USTB-17(Ni)@MAPbI<sub>3</sub> composite. Powder X-ray diffraction analysis together with theoretical simulations and transmission electron microscopy discloses the crystalline nature of USTB-17, USTB-17(Ni), and USTB-17(Ni)@MAPbI<sub>3</sub> with an unprecedented non-interpenetrated <b>hpt</b> topology. The close contact of QDs inside the COF pores with the Ni catalytic site locating at the pore surface of COF allows a rapid transfer of the photogenerated electrons in QDs to the Ni catalytic sites, enhancing the photocatalytic activity for CO<sub>2</sub> reduction. This endows USTB-17(Ni)@MAPbI<sub>3</sub> with efficient photocatalysis performance for photocatalytic CO<sub>2</sub> reduction with CO generation rate of 365 µmol g<sup>−1</sup> h<sup>−1</sup> and CO selectivity up to 96% under visible-light irradiation, 7 times higher than that of USTB-17(Ni). After four cycles of reactions, the photocatalytic CO generation rate remains almost unchanged, demonstrating its excellent cycle stability.</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":"1478 - 1485"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716762","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}

引用次数: 0

Tailor-made high elasticity and low-hysteresis hydrogels based on asymmetric H-bonding crosslinking for wearable applications 基于非对称氢键交联的高弹性低迟滞水凝胶可穿戴应用

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2297-0

Xiaofang Shi, Nan Shi, Miaomiao Dang, Chengyu Ji, Yingjie Li, Peiyi Wu, Zhiguo Hu

{"title":"Tailor-made high elasticity and low-hysteresis hydrogels based on asymmetric H-bonding crosslinking for wearable applications","authors":"Xiaofang Shi, Nan Shi, Miaomiao Dang, Chengyu Ji, Yingjie Li, Peiyi Wu, Zhiguo Hu","doi":"10.1007/s11426-024-2297-0","DOIUrl":"10.1007/s11426-024-2297-0","url":null,"abstract":"<div><p>The conventional method of fabricating hydrogels constantly confronts the conflict between elasticity and toughness, limiting their repetitive application. Achieving the desired elasticity through a simple and low-cost approach is a significant challenge for hydrogels, particularly through rational molecular design. Here, low-hysteresis and high-toughness hydrogels are developed from the design of a new feature monomer, <i>N</i>-acryloylethylsemicarbazide (NACE). Based on a concept of “asymmetric H-bonding design”, the unique double and triple H-bonding of NACE can result in a novel asymmetric crosslinking polymer with alternating strong and weak H-bonding regions. The NACE is copolymerized with acrylamide (AM) to regulate the mechanical properties of hydrogel via H-bonding density. The P(NACE-AM) ionic hydrogels are obtained simply and rapidly via one-step photopolymerization without a chemical cross-linking agent. The P(NACE-AM) hydrogels combine superb mechanical elasticity and toughness, and excellent ionic conductivity, showing great potential as durable ionic conductive devices for wearable utilization.</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":"1117 - 1125"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475121","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}

引用次数: 0