Science China Chemistry最新文献_第8页

Two-coordinate copper(I) complexes enable efficient X-ray scintillation and imaging 双坐标铜(I)配合物实现了高效的x射线闪烁和成像

IF 9.7 1区化学

Science China Chemistry Pub Date : 2025-03-20 DOI: 10.1007/s11426-024-2589-9

He Zhang, Bin Yu, Yao Tan, Ao Ying, Weihang He, Zhenglin Jia, Qianqian Lin, Shaolong Gong

{"title":"Two-coordinate copper(I) complexes enable efficient X-ray scintillation and imaging","authors":"He Zhang, Bin Yu, Yao Tan, Ao Ying, Weihang He, Zhenglin Jia, Qianqian Lin, Shaolong Gong","doi":"10.1007/s11426-024-2589-9","DOIUrl":"10.1007/s11426-024-2589-9","url":null,"abstract":"<div><p>Organic scintillators hold great promise for applications in high-energy radiation detection and medical diagnostics. However, their practical application is hindered by limited X-ray attenuation capacity and low exciton utilization efficiency. Here, we present a series of two-coordinate Cu(I)-based carbene-metal-amide (CMA) complexes featuring cyclic(amino)(barrelene) carbene ligands. These complexes exhibit pronounced thermally activated delayed fluorescence (TADF) from a metal-perturbed interligand charge transfer (ICT) excited state, together with high photoluminescence quantum yields of up to 0.86 and short decay lifetimes as low as 1.54 µs in thin films. Moreover, the Cu metal center significantly enhances the X-ray absorption cross-sections of these complexes. Under X-ray irradiation, these complexes display intense radioluminescence with high light yields of up to 30522 photons MeV<sup>−1</sup>. The optimized scintillator screens enable high-quality X-ray imaging with a spatial resolution exceeding 16.0 line pairs mm<sup>−1</sup>. This work represents the first demonstration of CMA complexes as scintillators for X-ray detection and provides a guideline for developing efficient organic X-ray scintillators.\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 9","pages":"4245 - 4254"},"PeriodicalIF":9.7,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145011455","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

Designing metal-organic frameworks for the selective removal of 99TcO4− from nuclear wastewater 设计金属有机框架选择性去除核废水中的99TcO4−

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-03-20 DOI: 10.1007/s11426-025-2556-y

Ming Lei, Mengjie Hao, Zhongshan Chen, Hui Yang, Geoffrey I. N. Waterhouse, Shengqian Ma, Xiangke Wang

引用次数: 0

Upgrading polyolefin plastics: experiences from petroleum refining and distinct characteristics 聚烯烃塑料的升级换代：石油炼制的经验和独特的特性

IF 9.7 1区化学

Science China Chemistry Pub Date : 2025-03-19 DOI: 10.1007/s11426-024-2522-x

Rongxin Zhang, Guangchao Deng, Zhuoyang Jiang, Yiyi Fan, Yanqi Guo, Zhongwen Dong, Wenjun Chen, Bo Peng, Fan Zhang

{"title":"Upgrading polyolefin plastics: experiences from petroleum refining and distinct characteristics","authors":"Rongxin Zhang, Guangchao Deng, Zhuoyang Jiang, Yiyi Fan, Yanqi Guo, Zhongwen Dong, Wenjun Chen, Bo Peng, Fan Zhang","doi":"10.1007/s11426-024-2522-x","DOIUrl":"10.1007/s11426-024-2522-x","url":null,"abstract":"<div><p>The upgrading of polyolefins poses a significant challenge in polymer recycling due to their abundance and chemical inertness. While petroleum refining technologies could be transformed into polyolefins’ upgrading due to their similarities in atomic composition, there are essential differences. Current research aims to develop a better understanding of polyolefins’ “refinery”, but there is a lack of systematic comparison with traditional refinery methods. This review provides a comprehensive overview of the most recent reactions employed in polyolefin upgrading, establishing parallels with recognized petroleum refining technologies. It starts with a comparison of physicochemical properties between feedstocks from plastics and from petroleum-based origin. Below major classes of reactions are then discussed, i.e., (1) C–C bond cleavage over solid acid catalysts and/or metallic catalysts, with their conventional refining analogues of fluidized catalytic cracking, hydrocracking and hydrogenolysis; (2) C–C bond rearrangement, mainly aromatization, with petroleum analogue of catalytic reforming; (3) heteroatom removal from impurities, with petroleum analogue of hydrotreating. The review emphasizes the scenario-dependent challenges and corresponding advancements associated with these reactions. Furthermore, we draw a conclusion by identifying key areas that are inadequately addressed in existing literature, highlighting the technological requirements necessary to progress from laboratory-scale chemistry to pilot demonstrations, and providing insight into future directions and opportunities for advancing polyolefin upgrading technologies.\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 7","pages":"2927 - 2947"},"PeriodicalIF":9.7,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145144500","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

Flexible supramolecular polymer proton conductors with high mechanical-conductive decoupling ability 具有高机械导电解耦能力的柔性超分子聚合物质子导体

IF 9.7 1区化学

Science China Chemistry Pub Date : 2025-03-19 DOI: 10.1007/s11426-024-2549-6

Haikun Guo, Xiang Li, Shengchao Chai, Haibin Li, Tingting Li, Shihao Song, Peng Zuo, Haolong Li

{"title":"Flexible supramolecular polymer proton conductors with high mechanical-conductive decoupling ability","authors":"Haikun Guo, Xiang Li, Shengchao Chai, Haibin Li, Tingting Li, Shihao Song, Peng Zuo, Haolong Li","doi":"10.1007/s11426-024-2549-6","DOIUrl":"10.1007/s11426-024-2549-6","url":null,"abstract":"<div><p>Achieving the decoupling of ion transport and mechanical relaxation, also known as superionic conduction, is a crucial goal for electrolyte materials in energy and electronics technologies. However, constructing highly efficient ionic conductive pathways to overcome the trade-off that restrained segments reduce ionic conduction in polymer electrolytes still remains challenging. Given the non-covalent binding nature of supramolecular polymers, which offers advantages such as dynamic segments and easy integration of ionophilic units, here we present the creation of supramolecular polymer proton conductors (SPPCs) based on deep eutectic solvents (DESs) and polyoxometalate (POM) nanoclusters as hybrid monomers. By innovatively incorporating glycosyl and zwitterionic groups into DES precursor, the resulting glycosyl zwitterionic DESs can be non-covalently crosslinked by POM nanoclusters through synergistic hydrogen bonding and electrostatic interactions, leading to the solidification of DESs. The dense supramolecular networks formed within SPPCs serve as mechanical support and proton-conducting pathways. This gives SPPCs significant adhesive strength, high viscosity, excellent proton conductivity, and high mechanical-conductive decoupling ability. Furthermore, vanadium-substituted POM nanoclusters in SPPCs exhibit an additional pseudocapacitance for flexible supercapacitors, achieving an impressive increase in specific capacitance compared to tungsten-containing POM nanoclusters. This work highlights the immense potential of using functional supramolecular polymers to boost the development of innovative electrolyte materials.\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 9","pages":"4338 - 4347"},"PeriodicalIF":9.7,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145011926","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

Structural regulation of imine-linked benzothiadiazole-based covalent organic frameworks for efficient photocatalysis 用于高效光催化的亚胺连接苯并噻唑基共价有机框架的结构调控

IF 9.7 1区化学

Science China Chemistry Pub Date : 2025-03-19 DOI: 10.1007/s11426-024-2507-5

Xin Zhao, Yuancheng Wang, Guangchao Han, Guoye Yu, Guanshi Ren, Xiang Li, Tongyang Zhang, Lishui Sun, Yingjie Zhao

{"title":"Structural regulation of imine-linked benzothiadiazole-based covalent organic frameworks for efficient photocatalysis","authors":"Xin Zhao, Yuancheng Wang, Guangchao Han, Guoye Yu, Guanshi Ren, Xiang Li, Tongyang Zhang, Lishui Sun, Yingjie Zhao","doi":"10.1007/s11426-024-2507-5","DOIUrl":"10.1007/s11426-024-2507-5","url":null,"abstract":"<div><p>Slightly structural variation often leads to huge changes in the properties of the covalent organic frameworks (COFs). The atom-level precisely arranged structures of COFs make it possible to understand the structure-performance relationship. Here, four highly crystalline imine-linked benzothiadiazole-based COFs were constructed from precisely designed monomers. The effects of imine linkage orientation, the π bridge between the benzothiadiazole unit and imine linkage on the photocatalysis performance were systematically studied. It is noted that photocatalytic performance can be dramatically improved when the imine carbon atoms are attached to the pyrene-based unit. In addition, the extension of the π bridge in the benzothiadiazole units could obviously enhance the photocatalytic hydrogen evolution and weaken the hydrogen peroxide generation. The PC-NPB containing the diphenylbenzothiadiazole building block exhibited the highest hydrogen evolution rate of 15.7 mmol h<sup>−1</sup> g<sup>−1</sup>, 4.4 times higher than that of non-phenyl-substituted benzothiadiazole-containing PC-NB. Interestingly, PC-NB displayed the highest hydrogen peroxide generation rate of 1376 µmol h<sup>−1</sup> g<sup>−1</sup>, 2.8 times higher than that of PC-NPB.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 8","pages":"3707 - 3713"},"PeriodicalIF":9.7,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145166535","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

Stereospecific assembly of enantiopure Archimedean polyhedra 对映纯阿基米德多面体的立体定向组装

IF 9.7 1区化学

Science China Chemistry Pub Date : 2025-03-19 DOI: 10.1007/s11426-025-2599-y

He Tian

引用次数: 0

Surface lattice carbon cycles the reverse water–gas shift reaction 表面晶格碳循环逆水气移位反应

IF 9.7 1区化学

Science China Chemistry Pub Date : 2025-03-19 DOI: 10.1007/s11426-025-2616-0

Jun Wang, Jianyong Feng, Zhaosheng Li

引用次数: 0

Gas-phase synthesis and soft-landing deposition of imidazole clusters with narrowband emission 窄带发射咪唑簇的气相合成及软着陆沉积

IF 9.7 1区化学

Science China Chemistry Pub Date : 2025-03-19 DOI: 10.1007/s11426-024-2544-y

Qiuhao Yi, Siyang Ye, Haiming Wu, Yuxi Tian, Zhixun Luo

{"title":"Gas-phase synthesis and soft-landing deposition of imidazole clusters with narrowband emission","authors":"Qiuhao Yi, Siyang Ye, Haiming Wu, Yuxi Tian, Zhixun Luo","doi":"10.1007/s11426-024-2544-y","DOIUrl":"10.1007/s11426-024-2544-y","url":null,"abstract":"<div><p>Imidazole and its derivatives are common in bioactive molecules and function as pharmacophores in diverse medications. This study examines the gas-phase reactions of imidazole and benzylimidazole using a self-developed reflectron time-of-flight mass spectrometer equipped with dual sources and a downstream tube reactor. It was found that the Cu<sup>+</sup>/Ag<sup>+</sup> ions readily coordinate with these organic molecules to create metal complexes; furthermore, the plasma-assisted Cu<sup>+</sup>/Ag<sup>+</sup> ions enable C–N coupling reactions to generate a C<sub>17</sub>H<sub>17</sub>N<sub>2</sub><sup>+·</sup> radical assigned to 1,3-dibenzylimidazole, along with hydropolymerization to form molecular clusters through hydrogen bond linkers. With Im<sub>3</sub>H<sup>+</sup> as a representative, we attained soft-landing deposition and measured its fluorescence. Interestingly, the deposited quantum dots of Im<sub>3</sub>H<sup>+</sup> clusters exhibit narrow-width emission at 516 nm, which fits well with the time-dependent density functional theory (TD-DFT) calculation results. Through DFT calculations, we also elucidated the chemical interactions in these cluster systems. This study advances the basic understanding of heteroaromatic compounds and their weakly bound clusters, and provides a solvent-free synthesis technique for organic molecular clusters and metal-organic complexes.\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 9","pages":"4459 - 4467"},"PeriodicalIF":9.7,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145011940","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

Improved photoelectric performance of perovskite solar cells with interfacial dipole molecules 界面偶极子分子改善钙钛矿太阳能电池光电性能

IF 9.7 1区化学

Science China Chemistry Pub Date : 2025-03-19 DOI: 10.1007/s11426-024-2567-7

Wenjing Li, Yongchun Li, Deng Wang, Weichun Pan, Lin Gao, Jihuai Wu, Xugang Guo, Zhang Lan

引用次数: 0

High-fidelity spatio-temporal recognition of mitochondrial esterase with an on-demand photoactivation strategy 高保真时空识别线粒体酯酶与按需光激活策略

IF 9.7 1区化学

Science China Chemistry Pub Date : 2025-03-17 DOI: 10.1007/s11426-024-2548-1

Lixin Sun, Huili Liu, Zehua Qian, Ziwen Zhang, Hongyu Wu, Kehuan Wu, Nan Guo, Da-Hui Qu, Xianfeng Gu, Chunchang Zhao

{"title":"High-fidelity spatio-temporal recognition of mitochondrial esterase with an on-demand photoactivation strategy","authors":"Lixin Sun, Huili Liu, Zehua Qian, Ziwen Zhang, Hongyu Wu, Kehuan Wu, Nan Guo, Da-Hui Qu, Xianfeng Gu, Chunchang Zhao","doi":"10.1007/s11426-024-2548-1","DOIUrl":"10.1007/s11426-024-2548-1","url":null,"abstract":"<div><p>Multiple signaling molecules work together in mitochondria to mediate complex physiological processes. However, most current fluorescent probes lack of ability to clarify the function of these actives in mitochondria due to their non-specific binding with analytes outside mitochondria. In this study, we designed an on-demand light-activated mitochondria-targeted fluorescent probe to observe <i>in situ</i> fluctuations in mitochondrial esterase. The designed probe has a natural yellow fluorescence that monitors entry into the mitochondria and maintains nonfluorescent responsiveness to esterase during cellular delivery. Following the enrichment of the probe in mitochondria, on-demand photoactivation only at the required mitochondrial location resulted in a remarkable emission response to the esterase with red fluorescence at 700 nm. Precise spatiotemporal recognition of esterase in mitochondria is successfully achieved by activating the <i>in situ</i> fluorescence response of esterase by light irradiation. This work provides a new strategy for the study of esterase-related 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 8","pages":"3699 - 3706"},"PeriodicalIF":9.7,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145166100","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