Science China Chemistry最新文献_第2页

Donor-acceptor modulation of coordination polymers for effective photothermal conversion

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-25 DOI: 10.1007/s11426-024-2253-y

Bo Zhang, Xing-Wang Li, Han Fang, Chang-Tai Li, Si-Jia Yu, Mei-Hui Yu, Ze Chang, Xian-He Bu

{"title":"Donor-acceptor modulation of coordination polymers for effective photothermal conversion","authors":"Bo Zhang, Xing-Wang Li, Han Fang, Chang-Tai Li, Si-Jia Yu, Mei-Hui Yu, Ze Chang, Xian-He Bu","doi":"10.1007/s11426-024-2253-y","DOIUrl":"10.1007/s11426-024-2253-y","url":null,"abstract":"<div><p>The targeted construction of donor-acceptor (D-A) materials featuring efficient photothermal (PT) conversion properties has been an attractive but challenging goal. Herein, a new series of coordination polymers (CPs) featuring different PT performances were constructed with flexible linker 1,1′-Ferrocenedicarboxylic acid (FCA) and 2,4,6-tri(pyridin-4-yl)-1,3,5-triazine (TPT) as acceptor and donor molecules including coronene and tetrathiafulvalene (TTF). Based on the flexible configurations of FCA ligand and the directing of donor dependent D-A interactions, the structures of <b>TF-1</b> to <b>TF-3</b> featuring distinctive dimension were obtained based on Cd(II) ions for investigating the PT property in configurational perspectives. A systematic investigation of the PT properties of the CPs was performed. Notably, <b>TF-3</b> exhibits the finest PT conversion effect under the irradiation of 560 nm laser, while <b>TF-2</b> shows optimal PT conversion under 808 nm laser irradiation required for biological PT therapy, illustrating the correlation between the structural and component features of the CPs and their PT performances. Furthermore, Zn(II) as bio-friendly ion was utilized to construct hypotoxic <b>TF-4</b> that reveals similar structure to that of <b>TF-2</b> for potential application. Polydimethylsiloxane (PDMS) patches doped with <b>TF-4</b> exhibits considerable NIR PT conversion effect under 808 nm, represented by the nearly 80 °C temperature increased in 120 s for <b>TF-4</b>@PDMS patch (1.2 wt%) under 0.9 W cm<sup>−2</sup> irradiation, the results of which herein indicate the potential of D-A CPs as versatile platform for the modulation of PT materials.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 12","pages":"4175 - 4183"},"PeriodicalIF":10.4,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142757993","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

Visualization of the protective role of estrogen against female liver fibrosis via an ER viscosity NIR fluorescent probe

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-23 DOI: 10.1007/s11426-024-2061-7

Zheng Liu, Changyu Zhang, Zipeng Li, Wanying Ma, Jia Liu, Xiang Xia, Ning Xu, Wen Sun, Jianjun Du, Jiangli Fan, Xiaojun Peng

{"title":"Visualization of the protective role of estrogen against female liver fibrosis via an ER viscosity NIR fluorescent probe","authors":"Zheng Liu, Changyu Zhang, Zipeng Li, Wanying Ma, Jia Liu, Xiang Xia, Ning Xu, Wen Sun, Jianjun Du, Jiangli Fan, Xiaojun Peng","doi":"10.1007/s11426-024-2061-7","DOIUrl":"10.1007/s11426-024-2061-7","url":null,"abstract":"<div><p>Endoplasmic reticulum (ER) viscosity has emerged as a new potential biomarker for hepatic fibrosis (HF). Herein, we report the first ER-targeting viscosity-responsive near-infrared (NIR) fluorescent probe HBT-PP for investigations of HF pathogenesis. The twisted intramolecular charge transfer (TICT) and the excited state intramolecular proton transfer (ESIPT) are combined to endow HBT-PP with the selective response towards viscosity (∼62-fold) and a super large stokes shift (∼320 nm). HBT-PP mainly targets organelle ER and is able to image the drug- or alcohol-induced viscosity elevation in living cells. Significantly, HBT-PP was successfully applied to visualize the gender difference in HF and the protective role of estrogen in restraining HF progression. Of note, after 10 min of stain with HBT-PP, HF lesions showed a stage-based response, indicating the potential of this probe in fast and early diagnosis of HF. These results clearly demonstrated the promising application of HBT-PP as a new tool for exploring ER viscosity-involved physiological and pathological processes.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"360 - 368"},"PeriodicalIF":10.4,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925605","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

Potassium ions and cyano group modified g-C3N4 for effective generation of H2O2 through two-electron oxygen reduction

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-22 DOI: 10.1007/s11426-024-2200-1

Dongying Wang, Shulan Pu, Yongmin Chen, Ke Lei, Yujie Duan, Linjiao Mao, Xuhui Zeng, Xi Luo, Yuntao Zhang, Yuqin Dong, Jin Zhong Zhang, Yan Sun

{"title":"Potassium ions and cyano group modified g-C3N4 for effective generation of H2O2 through two-electron oxygen reduction","authors":"Dongying Wang, Shulan Pu, Yongmin Chen, Ke Lei, Yujie Duan, Linjiao Mao, Xuhui Zeng, Xi Luo, Yuntao Zhang, Yuqin Dong, Jin Zhong Zhang, Yan Sun","doi":"10.1007/s11426-024-2200-1","DOIUrl":"10.1007/s11426-024-2200-1","url":null,"abstract":"<div><p>Potassium ions (K<sup>+</sup>) doped graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) was prepared by a thermal etching method using potassium hydroxide (KOH) as an ion source. Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) results showed that the generation of the cyano group was detected while introducing K<sup>+</sup>. Under simulated sunlight irradiation, the sample with a K<sup>+</sup> doping amount of 10% showed the highest hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) generation rate of 2,140.2 µmol h<sup>−1</sup> g<sup>−1</sup>. The apparent quantum yield (AQY) at 400 nm and the solar-to-chemical conversion (SCC) are 4.35% and 1.23%, respectively. K<sup>+</sup> acted as a bridge between g-C<sub>3</sub>N<sub>4</sub> layers, which enhanced charge transfer efficiency. Meanwhile, the cyano group enhanced the adsorption capacity of protons (H<sup>+</sup>) and promoted the yield of H<sub>2</sub>O<sub>2</sub>. The catalyst exhibited excellent photocatalytic stability based on four-cycle experiments. In addition, a mechanism study showed that superoxide radicals (·O<sub>2</sub><sup>−</sup>) were the most important active species in the reaction system. Photocatalytic production of H<sub>2</sub>O<sub>2</sub> was achieved through consecutive single-electron steps. This study deepens the understanding of the oxygen reduction reaction process and opens up a new venue for improving H<sub>2</sub>O<sub>2</sub> generation.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"192 - 200"},"PeriodicalIF":10.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925575","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

Mechanically robust and dynamic supramolecular polymer networks enabled by [an]daisy chain backbones

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-21 DOI: 10.1007/s11426-024-2329-7

Yongming Wang, Yi Ding, Yuhang Liu, Shaolei Qu, Wenbin Wang, Wei Yu, Zhaoming Zhang, Feng Liu, Xuzhou Yan

{"title":"Mechanically robust and dynamic supramolecular polymer networks enabled by [an]daisy chain backbones","authors":"Yongming Wang, Yi Ding, Yuhang Liu, Shaolei Qu, Wenbin Wang, Wei Yu, Zhaoming Zhang, Feng Liu, Xuzhou Yan","doi":"10.1007/s11426-024-2329-7","DOIUrl":"10.1007/s11426-024-2329-7","url":null,"abstract":"<div><p>Supramolecular polymer networks (SPNs) have garnered significant research interest due to their dynamic properties. However, while current developments primarily focus on managing supramolecular crosslinks, the role of polymer backbones—equally crucial to SPN properties—has not yet been sufficiently explored. Herein, we utilize mechanically interlocked [<i>a</i>n]daisy chain as backbone to prepare a class of SPNs, where the force-induced motion of successive mechanical bonds toughens and reinforces the networks. In specific, the [<i>a</i>n]daisy chain backbones connect with polynorbornene chains through quadruple H-bonding in the SPN networks. Compared to the control with non-slidable backbone, The representative SPN-<b>2</b> exhibits a robust feature in tensile tests with high maximum stress (14.7 vs. 7.89 MPa) and toughness (83.8 vs. 48.6 MJ/m<sup>3</sup>). Moreover, it also has superior performance in energy dissipation benefitting from the [<i>a</i>n]daisy chain backbones as well as supramolecular crosslinks. Additionally, the SPN-<b>2</b> displayed exceptional self-healing and reprocessing capabilities due to their dynamic quadrable H-bonding crosslinkers. These findings demonstrate the untapped potential of [<i>a</i>n]daisy chain as a polymer skeleton to develop SPNs and open the door to design mechanically robust supramolecular materials with diverse smart functions.</p></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 12","pages":"4234 - 4241"},"PeriodicalIF":10.4,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142757929","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

Emerging trends in the selective production of value-added aromatics

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-17 DOI: 10.1007/s11426-024-2354-3

Yuchao Wu, Houliang Dai, Weisheng Yang, Yaxing Li, Lichen Liu

引用次数: 0

Bifunctional bridging capping layer enables 24.5% efficiency of perovskite solar cells with polymer-based hole transport materials

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-15 DOI: 10.1007/s11426-024-2142-4

Can Zhu, Yiyang Wang, Lei Meng, Beibei Qiu, Jing Li, Shucheng Qin, Ke Hu, Xin Jiang, Wenbin Lai, Minchao Liu, Zhe Liu, Chenxing Lu, Jinyuan Zhang, Yongfang Li

{"title":"Bifunctional bridging capping layer enables 24.5% efficiency of perovskite solar cells with polymer-based hole transport materials","authors":"Can Zhu, Yiyang Wang, Lei Meng, Beibei Qiu, Jing Li, Shucheng Qin, Ke Hu, Xin Jiang, Wenbin Lai, Minchao Liu, Zhe Liu, Chenxing Lu, Jinyuan Zhang, Yongfang Li","doi":"10.1007/s11426-024-2142-4","DOIUrl":"10.1007/s11426-024-2142-4","url":null,"abstract":"<div><p>Developing a bridge capping layer between perovskite and hole transport layer materials (HTMs) in the <i>n-i-p</i> perovskite solar cells (pero-SCs) is an effective approach to modify the morphology of HTMs and passivate the perovskite simultaneously. Herein, we select the quinoxaline-based bifunctional passivation agent, quinoxalin-6-yl-methylamine hydrochloride (QxMACl), as the bridging layer, and a D-A copolymer PBQ12 containing the same quinoxaline unit as an HTM for the <i>n-i-p</i> pero-SCs. Due to the <i>π-π</i> stacking among the common quinoxaline units in the bridge layer and HTM, QxMACl induces the <i>π</i>-<i>π</i> stacking of the PBQ12 film and improves the film morphology of HTMs with better conductivity. Additionally, QxMACl can effectively passivate the perovskite surface, and PBQ12 possesses appropriate energy levels and high hole mobility. The pero-SCs based on FAPbI<sub>3</sub> with PBQ12/QxMACl treatment showed a higher power conversion efficiency (PCE) of 24.05% and outstanding stability, maintaining 95.4% and 92.1% of its initial PCE after 750 h of storage and after over 800 h of thermal annealing at 85 °C, respectively. To further enhance the PCE of the PBQ12/QxMACl-based devices, we developed a non-metal ion dopant for the PBQ12 HTM. Through trace doping of PBQ12 HTM by the non-metal ion dopant, the PCE of the PBQ12/QxMACl-based devices reached 25.24% (the calibrated PCE of 24.55% by the National Institute of Metrology, China).\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"350 - 359"},"PeriodicalIF":10.4,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925746","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

Small modifications of endo-functionalized cavities lead to large changes in molecular interaction in water

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-14 DOI: 10.1007/s11426-024-2120-0

Song-Meng Wang, Hao Nian, Yan-Fang Wang, Li-Shuo Zheng, Yu-Tao Zheng, Yi-Wei Dong, Liping Huang, Xiaoping Wang, Wei Jiang, Liu-Pan Yang

引用次数: 0

Trinuclear gold-catalyzed site-selective alkylation of peptides

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-14 DOI: 10.1007/s11426-024-2169-4

Qing-Yun Fang, Chengyihan Gu, Yinghan Chen, Wencheng Yan, Yong Liang, Weipeng Li, Chengjian Zhu, Jie Han, Jin Xie

{"title":"Trinuclear gold-catalyzed site-selective alkylation of peptides","authors":"Qing-Yun Fang, Chengyihan Gu, Yinghan Chen, Wencheng Yan, Yong Liang, Weipeng Li, Chengjian Zhu, Jie Han, Jin Xie","doi":"10.1007/s11426-024-2169-4","DOIUrl":"10.1007/s11426-024-2169-4","url":null,"abstract":"<div><p>Selective modification of peptides has always been a challenging issue. The selective alkylation of peptides can alter the biological activity and physical properties of molecules, and it has gained significant research interest. We herein disclose an intriguing gold-catalyzed alkylation of peptides using bench-stable unactivated alkyl bromides under photoredox catalysis. A wide range of structurally diverse primary, secondary and tertiary alkyl bromides serve as effective coupling partners to precisely connect with the α-C(sp<sup>3</sup>)–H in glycine residue of peptides. This protocol demonstrates an exceptionally broad scope for alkyl halides and excellent tolerance for a wide range of useful functional groups. A series of relay transformations to construct cyclic peptides, to proceed click reaction and to realize peptide fluorescence labeling further enhance its synthetic practicality. In addition, mechanistic studies and density functional theory (DFT) calculations reveal an inner-sphere and subsequent outer-sphere single electron transfer (SET) mechanism.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"249 - 256"},"PeriodicalIF":10.4,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925695","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

Cobalamin-dependent radical S-adenosyl-L-methionine protein functions with a partner to successively methylate tricyclic indole alkaloid for chuangxinmycin maturation and derivatization

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-14 DOI: 10.1007/s11426-024-2188-x

Sili Wang, Jiancheng Huang, Yanan Du, Wei Huang, Yufeng Xue, Xiaokun Xu, Guannan Zhong, Yuanyuan Shi, Bin Hong, Xiaoying Bian, Wen Liu

{"title":"Cobalamin-dependent radical S-adenosyl-L-methionine protein functions with a partner to successively methylate tricyclic indole alkaloid for chuangxinmycin maturation and derivatization","authors":"Sili Wang, Jiancheng Huang, Yanan Du, Wei Huang, Yufeng Xue, Xiaokun Xu, Guannan Zhong, Yuanyuan Shi, Bin Hong, Xiaoying Bian, Wen Liu","doi":"10.1007/s11426-024-2188-x","DOIUrl":"10.1007/s11426-024-2188-x","url":null,"abstract":"<div><p>Cobalamin (Cbl)-dependent radical <i>S</i>-adenosyl-L-methionine (SAM) proteins constitute the largest collection of the radical SAM superfamily that has hundreds of thousands of individual members. Many of these proteins are involved in the biosynthesis of pharmaceutically important natural products to catalyze chemically demanding reactions. In the biosynthetic pathway of chuangxinmycin (CXM), a unique indole alkaloid antibiotic with potent anti-infective activity, functionalization of the characteristic thiopyrano[4,3,2-<i>cd</i>]indole scaffold by regio- and stereoselective C3-methylation is believed to rely on a Cbl-dependent radical process, which, however, remained to be reconstituted biochemically. We here report the dissection of this enzymatic process, which requires the incorporation of Cxm8, a Cbl-dependent radical SAM protein, with Cxm9, a DUF5825 family protein that shares no homology to any proteins of known functions. Cxm8 and Cxm9 function together by forming an unexpected heterodimeric complex that selectively catalyzes C3-methylation of the tricyclic indole<i>-S</i>-hetero ring system in a successive manner, achieving CXM and a recently identified, C3-dimethylated congener. Detailed biochemical characterization, isotope labeling, structural simulation and bioinformatics analysis rationalized the catalysis of the Cxm8/Cxm9 complex and particularly the necessity of the DUF5825 protein for C3-methylase activity. This is the first example that a Cbl-dependent protein acts with a partner to exhibit radical SAM activity.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"308 - 316"},"PeriodicalIF":10.4,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925694","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

Molecular catalysts for electrocatalytic ammonia oxidation

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-14 DOI: 10.1007/s11426-024-2137-5

Jun Li, Feiyang Zhang, Huatian Xiong, Yuanyuan Cai, Biaobiao Zhang

引用次数: 0