Science China Chemistry最新文献_第8页

Auxiliary ligand-induced assembly of atomically precise silver clusters

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-27 DOI: 10.1007/s11426-024-2220-4

Yeqin Feng, Xuemeng Jing, Fangyu Fu, Mengyun Zhao, Manzhou Chi, Hongjin Lv, Guo-Yu Yang

{"title":"Auxiliary ligand-induced assembly of atomically precise silver clusters","authors":"Yeqin Feng, Xuemeng Jing, Fangyu Fu, Mengyun Zhao, Manzhou Chi, Hongjin Lv, Guo-Yu Yang","doi":"10.1007/s11426-024-2220-4","DOIUrl":"10.1007/s11426-024-2220-4","url":null,"abstract":"<div><p>Establishing the correlation between inter-cluster assembly and auxiliary ligands at the atomic level is crucial for the development of metal cluster science. In this work, we report the successful preparation and characterization of three Ag clusters, discrete 0-D Ag<sub>51</sub>S<sub>6</sub>Cl<sub>3</sub>(<sup><i>i</i></sup>PrS)<sub>21</sub>(TsO)<sub>15</sub>CH<sub>3</sub>CN (<b>0-D Ag</b><sub><b>51</b></sub>, <sup><i>i</i></sup>PrS<sup>−</sup> = isopropanethiolate, TsO<sup>−</sup> = toluenesulfonate), 1-D {Ag<sub>38</sub>S<sub>4</sub> (<sup><i>i</i></sup>PrS)<sub>18</sub>(PhCOO)<sub>12</sub>}<sub>n</sub> (<b>1-D Ag</b><sub><b>38</b></sub>, PHCOO<sup>−</sup> = benzoate), and 2-D {Ag<sub>20</sub>(SO<sub>4</sub>)Cl<sub>2</sub>(<sup><i>i</i></sup>PrS)<sub>10</sub>(NO<sub>3</sub>)<sub>6</sub>}<sub>n</sub> (<b>2-D Ag</b><sub><b>20</b></sub>), using a delicate auxiliary-ligand-induced strategy. Structural analyses reveal that the types of auxiliary ligands can readily affect the structure and dimensionality of resulting Ag clusters. The addition of different surface auxiliary ligands from TsO<sup>−</sup> to PhCOO<sup>−</sup> and then to NO<sub>3</sub><sup>−</sup> leads to the formation of <b>0-D Ag</b><sub><b>51</b></sub> to <b>1-D Ag</b><sub><b>38</b></sub> and then to <b>2-D Ag</b><sub><b>20</b></sub> clusters under otherwise identical reaction conditions, respectively. The resulting Ag clusters exhibited structure-related optical/luminescence properties and distinct bathochromic shifts as revealed by the temperature-dependent luminescence and single-crystal X-ray diffraction studies.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 2","pages":"580 - 589"},"PeriodicalIF":10.4,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143446580","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

Organo-electroreduction enables arylcarboxylation of styrenes 有机电还原实现苯乙烯的芳基羧化

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-27 DOI: 10.1007/s11426-024-2154-8

Yanwei Wang, Qian Wang, Zile Zhu, Weikang Qi, Youai Qiu

{"title":"Organo-electroreduction enables arylcarboxylation of styrenes","authors":"Yanwei Wang, Qian Wang, Zile Zhu, Weikang Qi, Youai Qiu","doi":"10.1007/s11426-024-2154-8","DOIUrl":"10.1007/s11426-024-2154-8","url":null,"abstract":"<div><p>Electroreduction offers an alternative to generate high active intermediates from electrophiles (halides, alkenes, etc.) in organic synthesis. However, it still remains challenge to enable the transformations in controlled fashion for substrates with similar reduction potentials. Herein, an electroreductive arylcarboxylation of styrenes with aryl halides and CO<sub>2</sub> promoted by an organo-mediator has been developed. The reaction exhibits the remarkable reactivity control between styrenes and aryl halides bearing very similar reduction potentials, which is enabled by the addition of a simple organic mediator. The mediated process for different kinds of aryl halides (iodides and bromides) could be achieved by simply tuning the electronic effect of the skeleton of naphthalene. This protocol displays a broad substrate scope and the extension to late-stage modification of biorelevant molecules and their derivatives showed a bright prospect. Moreover, density functional theory (DFT) calculations and mechanistic studies have been conducted and provide solid support to rationalize the selectivity and reactivity control observed.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3825 - 3832"},"PeriodicalIF":10.4,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142518973","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

Copper-catalyzed C-H bond functionalization enabled by programmed alternating current 程控交流电实现铜催化的C-H键功能化

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-26 DOI: 10.1007/s11426-024-2273-y

Zhoumei Tan, Kun Xu, Chengchu Zeng

引用次数: 0

Photoinduced radical sulfur dioxide insertion with asymmetric cyclization of alkenes: accessing β-chiral sulfones bearing S-stereocentric cyclic sulfinamides 烯不对称环化的光诱导自由基二氧化硫插入：获得含s -立体中心环亚胺的β-手性砜

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-26 DOI: 10.1007/s11426-024-2151-x

Jiapian Huang, Chenxin Wang, Xu Wang, Xiaoyu Zhou, Wei Xiao, Jie Wu

引用次数: 0

Recent progress of radionuclides separation by porous materials 利用多孔材料分离放射性核素的最新进展

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-26 DOI: 10.1007/s11426-024-2218-8

Yinghui Xie, Long Yu, Long Chen, Cheng Chen, Li Wang, Fenglei Liu, Yun Liao, Peng Zhang, Tao Chen, Yihui Yuan, Yuexiang Lu, Boyang Huang, Hui Yang, Suhua Wang, Shuao Wang, Lijian Ma, Feng Luo, Yunhai Liu, Baowei Hu, Hongqing Wang, Duoqiang Pan, Wenkun Zhu, Ning Wang, Zhe Wang, Liang Mao, Shengqian Ma, Xiangke Wang

{"title":"Recent progress of radionuclides separation by porous materials","authors":"Yinghui Xie, Long Yu, Long Chen, Cheng Chen, Li Wang, Fenglei Liu, Yun Liao, Peng Zhang, Tao Chen, Yihui Yuan, Yuexiang Lu, Boyang Huang, Hui Yang, Suhua Wang, Shuao Wang, Lijian Ma, Feng Luo, Yunhai Liu, Baowei Hu, Hongqing Wang, Duoqiang Pan, Wenkun Zhu, Ning Wang, Zhe Wang, Liang Mao, Shengqian Ma, Xiangke Wang","doi":"10.1007/s11426-024-2218-8","DOIUrl":"10.1007/s11426-024-2218-8","url":null,"abstract":"<div><p>The separation of radionuclides is critical for the sustainable development of nuclear energy. It is urgent to design and prepare functionalized materials for efficient radionuclides separation. Porous materials are considered excellent candidates for the separation of radionuclides under complex conditions due to their high specific surface areas, tunable pore structures and controllable functionalities. In this review, we summarized the design, preparation and functionalization of porous materials and their application for separation of radionuclides in the past five years, discussed the separation performance and analyzed the structure-activity relationship between various radionuclides and porous materials, and systematically clarified their characterization and mechanism of different type porous materials. We also introduced the detection, irradiation and chemical toxicity of different reflective radionuclides.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3515 - 3577"},"PeriodicalIF":10.4,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142518628","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

Functionalization of covalent organic frameworks via multicomponent reactions 通过多组分反应的共价有机框架的功能化

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-25 DOI: 10.1007/s11426-024-2213-2

Xue-Hui Liu, Peng-Lai Wang, Wei Wang, San-Yuan Ding

引用次数: 0

Bisulfite-mediated base-free decarboxylative carbonylsulfination of alkenes: access to β-keto sultines

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-24 DOI: 10.1007/s11426-024-2210-2

Yongxin Zhang, Pan Zhou, Xinyue Ma, Xiaoxiao Yang, Xing Fang, Yuxi Wang, Chao Shu

引用次数: 0

Sequence-controlled dynamic covalent units enable decoupling of mechanical and self-healing performance of polymers

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-24 DOI: 10.1007/s11426-024-2209-8

Luzhi Zhang, Hongfei Huang, Lijie Sun, Xiaopeng Ma, Hui Tan, Zhengwei You

{"title":"Sequence-controlled dynamic covalent units enable decoupling of mechanical and self-healing performance of polymers","authors":"Luzhi Zhang, Hongfei Huang, Lijie Sun, Xiaopeng Ma, Hui Tan, Zhengwei You","doi":"10.1007/s11426-024-2209-8","DOIUrl":"10.1007/s11426-024-2209-8","url":null,"abstract":"<div><p>Sequence regulation provides an effective approach to controlling the properties of polymer materials. However, this approach remains an open question in the field of dynamic polymers, which emerge as more and more important new generation materials. Herein, we systematically investigate the effect of sequence control of dynamic covalent units in tuning the properties of materials. Different sequence-controlled poly(oxime-urethanes) are designed. The dynamic oxime-urethane groups are relatively dispersed (SCP-1) or concentrated (SCP-2) distributed in their molecular chains. The sequence control strategy provides an efficient way to decouple the mechanical and self-healing performance of polymers, which is one of the most pressing challenges in the field. The relatively dispersed oxime-urethane groups in SCP-1 not only facilitate the reorganization of the dynamic covalent bonds but also increase the probability of the reformation of hydrogen bonds. The reversible dissociation/reassociation of dynamic bonds is conducive to dissipating energy to enhance mechanical performance and promote self-healing properties. As a result, SCP-1 exhibits much faster self-healing than SCP-2, and its tensile strength is nearly twice that of SCP-2. In addition, energy dissipation capacity and degradation behavior also show significant sequence dependence. Overall, this work reveals a new molecular structure-property relationship and provides a powerful strategy to construct high-performance polymers.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 2","pages":"745 - 753"},"PeriodicalIF":10.4,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11426-024-2209-8.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143446538","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Hydrogen self-supplying initiators excited by visible light for the fabrication of transparent films 利用可见光激发氢气自给引发剂以制造透明薄膜

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-23 DOI: 10.1007/s11426-024-2118-0

Qingze Pan, Chiheng Liu, Wenzhe Qiao, Jianwei Li, Saihe Yang, Yangyang Xin, Pengzhong Chen, Jiangli Fan, Xiaojun Peng

{"title":"Hydrogen self-supplying initiators excited by visible light for the fabrication of transparent films","authors":"Qingze Pan, Chiheng Liu, Wenzhe Qiao, Jianwei Li, Saihe Yang, Yangyang Xin, Pengzhong Chen, Jiangli Fan, Xiaojun Peng","doi":"10.1007/s11426-024-2118-0","DOIUrl":"10.1007/s11426-024-2118-0","url":null,"abstract":"<div><p>Unimolecular Type II radical photoinitiators (PIs) have received significant attention in photocuring owing to the fact that they improve the sustainability of the overall process compared with traditional Type II radical photoinitiators. However, the photopolymerization efficiency of unimolecular Type II radical photoinitiators is hindered by their short excitation wavelengths, poor photon capture abilities, and inefficient photobleaching performance. Herein, we report a coumarin-based self-sufficient initiator (<b>C-NA</b>), which is designed by integrating “hydrogen donor” and “hydrogen acceptor” into the coumarin framework and used for single-component visible light curing. <b>C-NA</b> exhibits a visible light absorbance and high molar extinction coefficient and is completely photobleached under the irradiation of 405 nm light-emitting diodes (LEDs). The formation of free radicals arises from the transfer of hydrogen from the diethylamino group to the coumarin framework, together with a highly efficient photodegradation process of <b>C-NA</b>. Finally, <b>C-NA</b> was successfully applied to prepare a transparent film material. Therefore, <b>C-NA</b> offers new insights into the design of promising unimolecular Type II radical photoinitiators for photocuring.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3868 - 3874"},"PeriodicalIF":10.4,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142518881","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

Enantio-divergent C–H borylation with two different ligands from a single chiral source 来自单一手性源的两种不同配体的对映异构C-H硼化反应

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-23 DOI: 10.1007/s11426-024-2106-3

Rongrong Du, Senmiao Xu

引用次数: 0