Science China Chemistry最新文献_第2页

In-situ liquid-phase transmission electron microscopy for two-dimensional energy materials

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-11-11 DOI: 10.1007/s11426-024-2262-8

Junyu Zhang, Liangping Xiao, Mi Lu

{"title":"In-situ liquid-phase transmission electron microscopy for two-dimensional energy materials","authors":"Junyu Zhang, Liangping Xiao, Mi Lu","doi":"10.1007/s11426-024-2262-8","DOIUrl":"10.1007/s11426-024-2262-8","url":null,"abstract":"<div><p>Two-dimensional (2D) materials are vital for the development of advanced materials in the next-generation energy conversion and storage devices. <i>In-situ</i> liquid-phase transmission electron microscopy (LP-TEM) acts as a powerful tool for characterizing the dynamic evolution of materials under work condition in real time and <i>in operando</i>. Herein, this mini-review highlights the considerable advances in the utilization of <i>in-situ</i> LP-TEM for studying the physical and chemical process dynamics of 2D materials, such as their nucleation growth and phase transformation. The electrocatalytic water splitting reactions and CO<sub>2</sub> electroreduction of 2D energy materials are highlighted. The underlying electrochemical reaction mechanisms of the 2D electrode materials in rechargeable batteries are discussed and summarized. Finally, the current challenges and perspectives for future research are proposed. This min-review aims to inspire and stimulate further innovation and encourage the broader adoption of LP-TEM in exploring the fascinating dynamics of 2D energy materials.</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":"414 - 429"},"PeriodicalIF":10.4,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143446412","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

Unraveling the complex interactions between plasmonic Ag nanoparticles and biomolecules for enhancing molecular chirality

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-11-07 DOI: 10.1007/s11426-024-2364-3

Chen Wang, Yunlong Tao, Qingqing Cheng, Dandan Lu, Chuang Liu, Guizeng Yang, Xuehao Sun, Lichao Sun, Qingfeng Zhang

{"title":"Unraveling the complex interactions between plasmonic Ag nanoparticles and biomolecules for enhancing molecular chirality","authors":"Chen Wang, Yunlong Tao, Qingqing Cheng, Dandan Lu, Chuang Liu, Guizeng Yang, Xuehao Sun, Lichao Sun, Qingfeng Zhang","doi":"10.1007/s11426-024-2364-3","DOIUrl":"10.1007/s11426-024-2364-3","url":null,"abstract":"<div><p>Plasmonic nanostructures have been widely employed to enhance the chiral light-matter interactions for chirality sensing owing to their intriguing optical properties. However, a quantitative understanding of the correlation between enhanced molecular chirality and plasmonic properties in plasmonic nanoparticle-molecule complexes remains a challenge yet to be addressed. Here we demonstrate the complex interactions between Ag nanoparticles and biomolecules that generate distinct plasmonic circular dichroism signals ranging from UV to visible wavelengths. By deliberately changing the surface coverage of chiral molecules, the geometry of Ag nanoparticles, and the aggregation states of the complexes, three distinct underlying mechanisms were found to be intertwined and hybridized for enhancing circular dichroism signals. We further employed the chiral plasmonic nano-particle-molecule complexes to quantify the enantiomeric purity of cysteine and explore their possible applications in other chiral molecules. The insights gained from this work shed light on the underlying mechanisms dictating the enhanced circular dichroism signals of chiral plasmonic nanoparticle-molecule complexes.</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":"543 - 551"},"PeriodicalIF":10.4,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143446417","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

Dative B-N bonds weaven toward two-dimensional purely organic materials for single crystals 添加B-N键织向二维纯有机材料单晶

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-11-06 DOI: 10.1007/s11426-024-2385-1

Wei-Lei Zhou, Siwei Wang, Yong Chen

引用次数: 0

Solid-state synthesis of mesoporous metals via mechanochemical coordination self-assembly

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-11-05 DOI: 10.1007/s11426-024-2393-4

Hailong Xiong, Chunyu Qi, Lantian Xue, Ling Zhang, Hanyu Liu, Zhen-An Qiao

{"title":"Solid-state synthesis of mesoporous metals via mechanochemical coordination self-assembly","authors":"Hailong Xiong, Chunyu Qi, Lantian Xue, Ling Zhang, Hanyu Liu, Zhen-An Qiao","doi":"10.1007/s11426-024-2393-4","DOIUrl":"10.1007/s11426-024-2393-4","url":null,"abstract":"<div><p>Mesoporous metals with large surface area, high pore volume, and uniform pore structure hold excellent advantages for various applications. However, the state-of-the-art synthesis methods are still limited to wet chemistry, which requires excessive solvents and a time-consuming drying process. Here, we report a facile and general mechanochemical coordination self-assembly strategy to prepare mesoporous metals (<i>e.g.</i>, Rh, Ru, Ir, Pt, Pd, Ag, Co, and Ni) with remarkable porous properties by using metal chlorides and cationic polymer interplay. Compared with the wet chemistry process, this method proceeds without solvents and does not need complicated experimental conditions and long synthetic periods, which not only greatly reduces the consumption of cost and energy and environmental pollution, but also improves the synthesis efficiency and yield of target products. We believe the developed approach will provide a general pathway for the scalable preparation of advanced porous materials.</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":"492 - 498"},"PeriodicalIF":10.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143446415","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

Deciphering fungal metabolon coupling tandem inverse-electron-demand Diels-Alder reaction and semipinacol rearrangement for the biosynthesis of spiro polycyclic alkaloids 螺旋体多环生物碱生物合成中偶联反电按需Diels-Alder反应和半品萘酚重排的真菌代谢解译

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-31 DOI: 10.1007/s11426-024-2134-0

Shuai Liu, Wen-Qiang Xu, Ying-Tong Di, Man-Cheng Tang, Ding-Kang Chen, Ming-Ming Cao, Yao-Wen Chang, Hong-Yu Tang, Chun-Mao Yuan, Jun-Bo Yang, Zhi-Li Zuo, Han Guo, Zi-Fei Xu, Ying Zeng, Yun-Dong Wu, Xiao-Jiang Hao

{"title":"Deciphering fungal metabolon coupling tandem inverse-electron-demand Diels-Alder reaction and semipinacol rearrangement for the biosynthesis of spiro polycyclic alkaloids","authors":"Shuai Liu, Wen-Qiang Xu, Ying-Tong Di, Man-Cheng Tang, Ding-Kang Chen, Ming-Ming Cao, Yao-Wen Chang, Hong-Yu Tang, Chun-Mao Yuan, Jun-Bo Yang, Zhi-Li Zuo, Han Guo, Zi-Fei Xu, Ying Zeng, Yun-Dong Wu, Xiao-Jiang Hao","doi":"10.1007/s11426-024-2134-0","DOIUrl":"10.1007/s11426-024-2134-0","url":null,"abstract":"<div><p>In the intricate process of natural product biosynthesis, a metabolon can enhance metabolic flux by associating sequential enzymes. A fungal metabolon, comprising of flavin-dependent monooxygenase SpeF and P450 monooxygenase SpeG, is identified in the biosynthesis of spiro polycyclic alkaloids (+)-notoamide B and its diastereomer (+)-versicolamide B. Using notoamide E as a substance, SpeF/SpeG metabolon can control the stereoselectivity of its 2,3-epoxidation, followed by hydrogen atom ion at C-17 to generate reactive epoxide tau-mA with dienyl iminium unit. Subsequently, (+)-notoamide B and (+)-versicolamide B are produced <i>via</i> tandem nonenzymatic inverse-electron-demand Diels-Alder reaction and semipinacol rearrangement. This provides the first example of metabolon in the biosynthesis of spiro-prenylated indole alkaloids.\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":"288 - 296"},"PeriodicalIF":10.4,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925476","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

Phenyl-extended resorcin[4]arene opens up a new avenue for highly efficient iodine adsorption

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-30 DOI: 10.1007/s11426-024-2343-5

Jingyu Chen, Jiong Zhou

引用次数: 0

Unraveling the impacts of intermolecular interaction on morphology evolution for highly efficient organic solar cells and modules 揭示分子间相互作用对高效有机太阳能电池和组件形态进化的影响

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-28 DOI: 10.1007/s11426-024-2272-3

Xueqing Ma, Yingying Cheng, Yuqiang Liu, Xinming Zheng, Guangliu Ran, Hongxiang Li, Xinyue Cui, Andong Zhang, Wenkai Zhang, Pei Cheng, Wenchao Huang, Zhishan Bo

{"title":"Unraveling the impacts of intermolecular interaction on morphology evolution for highly efficient organic solar cells and modules","authors":"Xueqing Ma, Yingying Cheng, Yuqiang Liu, Xinming Zheng, Guangliu Ran, Hongxiang Li, Xinyue Cui, Andong Zhang, Wenkai Zhang, Pei Cheng, Wenchao Huang, Zhishan Bo","doi":"10.1007/s11426-024-2272-3","DOIUrl":"10.1007/s11426-024-2272-3","url":null,"abstract":"<div><p>Understanding the effect of intermolecular interaction on the growth dynamic of active layers is critical for advancing organic solar cells (OSCs). However, the diverse structure of donors and acceptors makes the research challenging. Additives with customizable structures and properties could simplify this complexity. Herein, we meticulously tailor two additives of 3,4-ethylenedioxythiophene (EDOT) and 2,5-dibromo-3,4-ethylenedioxythiophene (DBEDOT), possessing distinct intermolecular interaction features to elaborate the inherent relationship. It is found that varied interaction strengths can alter film formation processes. The enhanced intermolecular interaction between the DBEDOT and non-fullerene acceptor BTP-eC9-4F results in pre-aggregation and longer crystallization duration of BTP-eC9-4F, facilitating the formation of films with compact molecular packing and decent phase separation. Thus, exciton dissociation and charge transport become more efficient. Finally, devices processed with DBEDOT exhibit a remarkable power conversion efficiency of 19.35% in small-area OSCs and 14.11% in blade-coated 5 cm × 5 cm organic solar mini-modules. Especially, OSCs can maintain 80% of their initial efficiency after continuous annealing at 85 °C for over 2,100 h.</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":"264 - 272"},"PeriodicalIF":10.4,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925752","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

Controlled cationic ring-opening polymerization of L-lactide by organic ion pair: novel approach to isotactic-rich and crystalline polylactide 有机离子对控制l -丙交酯阳离子开环聚合：制备富等规结晶型聚丙交酯的新方法

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-28 DOI: 10.1007/s11426-024-2370-6

Zhiqiang Ding, Mingqian Wang, Zijing Zhou, Bin Wang, Yuesheng Li

{"title":"Controlled cationic ring-opening polymerization of L-lactide by organic ion pair: novel approach to isotactic-rich and crystalline polylactide","authors":"Zhiqiang Ding, Mingqian Wang, Zijing Zhou, Bin Wang, Yuesheng Li","doi":"10.1007/s11426-024-2370-6","DOIUrl":"10.1007/s11426-024-2370-6","url":null,"abstract":"<div><p>Living/controlled cationic ring-opening polymerization (ROP) of <i>L</i>-lactide is a promising approach to isotactic-rich and crystalline poly(<i>L</i>-lactide). In contrast with the unsubstituted lactones, <i>L</i>-LA can not be polymerized by organic Lewis acids or carbenium ions, and the state of the art in this field is the cationic ROP of <i>L</i>-LA catalyzed by Brønsted acid/alcohol system <i>via</i> activated monomer mechanism. Herein, we reported the first example of controlled cationic ROP of <i>L</i>-LA by using Meerweintype ion pair [Me<sub>3</sub>O]<sup>+</sup>[B(C<sub>6</sub>F<sub>5</sub>)<sub>4</sub>]<sup>−</sup> as the catalyst. [Me<sub>3</sub>O]<sup>+</sup>[B(C<sub>6</sub>F<sub>5</sub>)<sub>4</sub>]<sup>−</sup> promoted rapid <i>L</i>-LA cationic polymerization in the absence of alcohol, producing isotactic-rich and crystalline PLLA without transesterification and epimerization side reactions. An activated chain end mechanism, involving twice S<sub>N</sub>2 substitution and configuration-inversion (<i>S</i>→<i>R</i>→<i>S</i>) with the assistance of released Me<sub>2</sub>O, was proposed and further verified by density functional theory and control experiments. This work expands the catalytic toolbox of isotactic-rich and crystalline polylactide synthesis. It represents a unique example of cationic-controlled polymerization of <i>L</i>-LA catalyzed by an organic ion pair.</p></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"394 - 402"},"PeriodicalIF":10.4,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925780","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

Donor-acceptor modulation of coordination polymers for effective photothermal conversion 配位聚合物有效光热转换的供体-受体调制

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

Enantioselective copper-catalyzed dearomative borylative cyclization of indoles and mechanistic insights

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-23 DOI: 10.1007/s11426-024-2214-0

Yanfei Li, Xuetao Li, Zheng Zhang, Yiliang Zhang, Xiuping Yuan, Jianjun Yin, Simin Wang, Wei Guan, Qian Zhang, Tao Xiong

{"title":"Enantioselective copper-catalyzed dearomative borylative cyclization of indoles and mechanistic insights","authors":"Yanfei Li, Xuetao Li, Zheng Zhang, Yiliang Zhang, Xiuping Yuan, Jianjun Yin, Simin Wang, Wei Guan, Qian Zhang, Tao Xiong","doi":"10.1007/s11426-024-2214-0","DOIUrl":"10.1007/s11426-024-2214-0","url":null,"abstract":"<div><p>Alicyclic nitrogen heterocycles, such as enantioenriched polycyclic fused [1,2-a]indoline derivatives, are widespread in natural products, agrochemicals and pharmaceutical agents. Existing methods predominantly rely on the recent emerging Heck-type catalytic asymmetric dearomatization (CADA) protocol, wherein noble palladium catalysts commonly necessitate the form aryl-Pd species-triggered these transformations. In contrast, a more sustainable base metal catalysis paradigm through alkyl metal species disrupting the aromaticity, that is, the utilization of challenging asymmetric Csp<sup>3</sup>–Csp<sup>3</sup> bond formation entry to such important chiral densely functionalized polycyclic molecular scaffolds, remains an elusive task. Herein, we report the first copper-catalyzed dearomative borylative cyclization of indoles under mild reaction conditions, affording an array of valuable Bpin-containing pyrrolo-fused [1,2-a]indolines bearing four consecutive stereogenic centers with excellent enantio- and diastereoselectivity. The synthetic potential was documented <i>via</i> an array of useful transformations. Density functional theory (DFT) calculation studies elucidated the origin of the chemo-, regio-, enantio- and diastereoselectivities of this conversion.</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":"670 - 678"},"PeriodicalIF":10.4,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143446559","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