Science China Chemistry最新文献_第7页

Surface ligand-promoted heterogeneous CO2 catalysis 表面配体促进异相二氧化碳催化

IF 9.445 1区化学

Science China Chemistry Pub Date : 2024-09-13 DOI: 10.1007/s11426-024-2205-y

Zhe Lu, Lu Wang

引用次数: 0

Light-activated tautomeric transition enhanced buried heterointerface for highly efficient and ultraviolet robust perovskite solar cells 光激活同分异构转换增强型埋藏异质界面，用于高效和紫外线稳健型过氧化物太阳能电池

IF 9.445 1区化学

Science China Chemistry Pub Date : 2024-09-13 DOI: 10.1007/s11426-024-2194-0

Sheng Jiang, Shaobing Xiong, Shuaifei Mao, Yefan Zhang, Dongyang Zhao, Xiaomeng You, Vladimir Gaishun, Dmitry Kovalenk, Qinye Bao

{"title":"Light-activated tautomeric transition enhanced buried heterointerface for highly efficient and ultraviolet robust perovskite solar cells","authors":"Sheng Jiang, Shaobing Xiong, Shuaifei Mao, Yefan Zhang, Dongyang Zhao, Xiaomeng You, Vladimir Gaishun, Dmitry Kovalenk, Qinye Bao","doi":"10.1007/s11426-024-2194-0","DOIUrl":"https://doi.org/10.1007/s11426-024-2194-0","url":null,"abstract":"The buried heterointerface of perovskite solar cells (PSCs) suffers from serious nonradiative recombination and ultraviolet (UV) light stress, relentlessly limiting further increase in their power conversion efficiency and operational stability. Herein, we develop an emerging strategy of incorporating a thin UV-activated tautomeric transition layer onto underlying charge transport layer and then depositing perovskite layer to construct an efficient hole-selective buried heterojunction. It is revealed that the UV-activated tautomeric transition interlayer not only improves upper perovskite crystallinity, diminishes thermionic loss for collecting hole and passivates defect site at such buried contact that significantly promote charge transport and suppress nonradiative recombination, but also effectively protects adjacent perovskite from UV degradation through “UV sunscreen” effect. As a result, we report a remarkably enhanced efficiency of 24.76% compared to 22.02% of the control device. More importantly, the achieved high-efficiency PSC features excellent resistance against UV radiation at 365 nm of 100 and 850 mW cm−2, which are approximately 21 and 184 times of UV flux (4.6 mW cm−2) under AM 1.5G solar illumination. This work provides a promising approach of strengthening buried heterointerface for simultaneous realization of highly efficient and UV robust PSCs.","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"3 1","pages":""},"PeriodicalIF":9.445,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249232","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

Tandem asymmetric dearomatized functionalization reaction of phenols with Evans-ynamides enabled by divergent electrophiles 利用发散亲电体实现苯酚与伊文炔酰胺的串联不对称脱芳烃官能化反应

IF 9.445 1区化学

Science China Chemistry Pub Date : 2024-09-13 DOI: 10.1007/s11426-024-2211-y

Ying-Qi Zhang, Gan-Lu Qian, Yun Liu, Jia-Hui Li, Xin Hong, Zhou Xu, Bo Zhou, Long-Wu Ye

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Combating periodontitis with an ATP-responsive metal-organic framework through synergistic ion-interference-induced pyroptosis 通过协同离子干扰诱导的热渗透作用，利用 ATP 响应型金属有机框架防治牙周炎

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-12 DOI: 10.1007/s11426-024-2192-9

Yuling Xu, Mengrong He, Xuechuan Hong

引用次数: 0

Metal-organic frameworks with dinuclear metal centers for synergistically boosting CO2 photoreduction 具有双核金属中心的金属有机框架可协同促进二氧化碳光还原

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-10 DOI: 10.1007/s11426-024-2108-2

Hui-Feng Wang, Wen-Jie Shi, Yu-Xin Yang, Bao-Xia Dong, Tong-Bu Lu, Di-Chang Zhong

{"title":"Metal-organic frameworks with dinuclear metal centers for synergistically boosting CO2 photoreduction","authors":"Hui-Feng Wang, Wen-Jie Shi, Yu-Xin Yang, Bao-Xia Dong, Tong-Bu Lu, Di-Chang Zhong","doi":"10.1007/s11426-024-2108-2","DOIUrl":"10.1007/s11426-024-2108-2","url":null,"abstract":"<div>Dinuclear metal synergistic catalysis (DMSC) has been proved powerful in boosting CO2 reduction, while this has not been achieved in heterogeneous catalysts with long-range order structures. In this study, we, by introduction of metal catalytic centers into an indium-based metal-organic framework (MOF), obtained a series of isostructural In-MOFs, including three MOFs with mononuclear metal catalytic center (M-In), three MOFs with dinuclear homometallic catalytic centers (MM-In), and three MOFs with dinuclear heterometallic catalytic centers (MM′-In, M/M′ = Co(II), Ni(II), Zn(II)). It was found that all these MOFs can serve as catalysts for photochemical CO2 reduction to CO. Compared with M-In, the catalytic activities of MM-In were obviously enhanced, and that of MM′-In was further significantly enhanced. For example, the CO yield of CoZn-In reaches a record value of 12,700 µmol g−1 h−1, which is 4.0, 8.1, 9.4, and 18.6-fold higher than that of CoCo-In, ZnZn-In, Co-In, andZn-In, respectively. Similarly, the catalytic activities of CoNi-In and NiZn-In also show different fold increase than those of corresponding dinuclear homometallic and mononuclear metallic MOFs. The results of control experiments and theoretical calculation reveal that the higher catalytic activities of MM-In over M-In can be ascribed to the DMSC effect, and the higher catalytic activity of MM′-In over MM-In can be ascribed to the strengthened DMSC effect. The work reveals the relationship between DMSC effect and bimetal centers in CO2 reduction, which provides new insights into the DMSC and paves a new way to design highly active catalysts for photochemical CO2 reduction.\u0000<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":"201 - 208"},"PeriodicalIF":10.4,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142225137","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

Integration of metal-organic layers with quantum dots for artificial photosynthesis 将金属有机层与量子点集成用于人工光合作用

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-10 DOI: 10.1007/s11426-024-2025-2

Hong Yuan, Min Zhang, Ji-Hua Deng, Tong-Bu Lu, Di-Chang Zhong

{"title":"Integration of metal-organic layers with quantum dots for artificial photosynthesis","authors":"Hong Yuan, Min Zhang, Ji-Hua Deng, Tong-Bu Lu, Di-Chang Zhong","doi":"10.1007/s11426-024-2025-2","DOIUrl":"10.1007/s11426-024-2025-2","url":null,"abstract":"<div>Metal-organic layers (MOLs), a type of new-emerging two-dimensional ultrathin metal-organic framework materials with large surface areas and highly exposed active sites, have shown promising applications in photocatalytic CO2 reduction. However, due to a lack of photosensitivity and photooxidation capability, photosensitizers and sacrificial reductants are usually necessary for MOLs-based photocatalytic CO2 reduction systems. In this article, by integration of MOLs and quantum dots (QDs), we constructed MOLs-based catalysts with multi-functions of photosensitivity, photoreduction and photooxidation, which thus can serve as photocatalysts for CO2 reduction with H2O as an electron donor. Specifically, by an electrostatic self-assembly approach, nickel(II)-based MOLs (Ni-MOLs) and CsPbBr3 QDs have been assembled, constructing valid II-Scheme Ni-MOLs/CsPbBr3 heterojunctions with close Ni-MOLs/CsPbBr3 heterointerface. Such a close heterointerface shortens the charge transfer distance, thus effectively boosting the charge separation and transfer. As a result, upon illumination by visible light (λ ⩾ 400 nm, 100 mW cm−2), the optimized photocatalyst shows high efficiency and stability in photochemical CO2 reduction in the absence of any photosensitizers and sacrificial reductants. The CO yield reaches as high as 124 µmol g−1 in 4 h, over 6 times higher than that achieved by CsPbBr3. Additionally, the selectivity reaches 100%. This work provides a new way to construct MOL-based catalysts for artificial photosynthesis.\u0000<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":"3712 - 3718"},"PeriodicalIF":10.4,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142225135","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

Engineering Ru(N^N)3-modified covalent organic framework for photocatalytic olefin epoxidation 用于光催化烯烃环氧化的 Ru(N^N)3 改性共价有机框架工程设计

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-10 DOI: 10.1007/s11426-024-2043-2

Yan-Lin Li, Sheng-Li Huang, Guo-Yu Yang

{"title":"Engineering Ru(N^N)3-modified covalent organic framework for photocatalytic olefin epoxidation","authors":"Yan-Lin Li, Sheng-Li Huang, Guo-Yu Yang","doi":"10.1007/s11426-024-2043-2","DOIUrl":"10.1007/s11426-024-2043-2","url":null,"abstract":"<div>Photocatalytic olefin oxidation using air as an oxidant is an environmentally friendly method for producing epoxides. Covalent organic frameworks (COFs) have emerged as promising photocatalysts in various organic synthesis reactions. The combination of tri-(2-pyridinal aldehyde)-containing precursor with 4,4′,4″-(1,3,5-triazine-2,4,6-triyl)trianiline generated (N^N)-I-COF. Via imine-to-quinoline transformation and coordination anchorage of Ru(N^N)3 unit, Ru(N^N)3@Q-COF was obtained with improved chemical stability, skeleton conjugation, and novel photochemical characteristics, and demonstrated excellent photocatalytic activity in olefin epoxidation with a wide range of substrates. The presence of H2O played a crucial role in the formation of reactive oxygen species (ROSs), which in turn influenced the olefin oxidation process. The hydrophilicity of Ru(N^N)3 facilitated the approach of H2O and O2 to the photogenerated charges, thereby promoting ROSs generation. The lipophilicity of Q-COF allowed for the absorption of olefin substrates, and its nano-channels increased encountering possibility between olefins and ROSs. Consequently, Ru(N^N)3@Q-COF provided an intriguing platform for olefin photooxidation and could be recycled multiple times without any degradation in performance. This report revealed that the conversion of classical ROSs into less potent oxidants with rapid kinetic rates played a crucial role in achieving highly efficient and selective epoxidation of terminal olefins.\u0000<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":"3719 - 3728"},"PeriodicalIF":10.4,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197150","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 Z/E isomeric cation designed organic-inorganic cadmium chloride ferroelectric with broadband white-light emission 具有宽带白光发射功能的 Z/E 异构阳离子设计有机无机氯化镉铁电体

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-10 DOI: 10.1007/s11426-024-2175-2

Jun-Chao Qi, Yan Qin, Hang Peng, Hui-Peng Lv, Yong-Ju Bai, Xin Shen, Zhang-Tian Xia, Wei-Qiang Liao

{"title":"A Z/E isomeric cation designed organic-inorganic cadmium chloride ferroelectric with broadband white-light emission","authors":"Jun-Chao Qi, Yan Qin, Hang Peng, Hui-Peng Lv, Yong-Ju Bai, Xin Shen, Zhang-Tian Xia, Wei-Qiang Liao","doi":"10.1007/s11426-024-2175-2","DOIUrl":"10.1007/s11426-024-2175-2","url":null,"abstract":"<div>Hybrid organic-inorganic metal halides (HOMHs) have attracted tremendous interest in the past decades due to their diverse functional properties, such as ferroelectricity and luminescence. However, although a large number of ferroelectric HOMHs and luminescent HOMHs have been reported, the HOMH ferroelectrics with white-light emission remain very sparse. Here, for the first time, by using the Z/E isomeric organic cation, we designed a cadmium-based HOMH ferroelectric [EE-PMU]CdCl4 (EE-PMU = pyridin-2-ylmethanamide muconate) with broadband white-light emission. In contrast to the [ZZ-PMU]CdCl4 with centrosymmetric crystal structure at room temperature, [EE-PMU]CdCl4 adopts the polar crystal symmetry, which shows piezoelectricity with a piezoelectric coefficient of d33 up to 19 pC/N and ferroelectricity with the saturated polarization of 1.52 µC/cm2. Moreover, [EE-PMU]CdCl4 exhibits a broadband white-light emission with an ultra-high color rendering index of 91 under UV excitation, which is related to the severely distorted [CdCl4]2− tetrahedron in the structure. To our knowledge, [EE-PMU]CdCl4 is the first example of Z/E isomeric cation-designed HOMH ferroelectric and the first cadmium halide white-light emissive ferroelectric. This finding paves a new way for the design of organic-inorganic molecular ferroelectrics with white-light emission.</div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 12","pages":"4167 - 4174"},"PeriodicalIF":10.4,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197149","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

De novo synthesis of atropisomeric benzofurans via Cu/SPDO complex catalyzed asymmetric formal [3 + 2] annulation 通过 Cu/SPDO 复合物催化的不对称形式 [3 + 2] 环化从头合成异构苯并呋喃

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-09 DOI: 10.1007/s11426-024-2174-x

Fan-Xiao Meng, Xing-Yu Wang, Ka Lu, Ju-Song Yang, Fu-Min Zhang, Ai-Jun Ma, Bao Du, Yong-Qiang Tu

引用次数: 0

Zeolite-based materials for greenhouse gas capture and conversion 用于温室气体捕获和转化的沸石基材料

IF 9.445 1区化学

Science China Chemistry Pub Date : 2024-09-09 DOI: 10.1007/s11426-024-2287-6

Qiang Zhang, Jialiang Li, Li Li, Jihong Yu

{"title":"Zeolite-based materials for greenhouse gas capture and conversion","authors":"Qiang Zhang, Jialiang Li, Li Li, Jihong Yu","doi":"10.1007/s11426-024-2287-6","DOIUrl":"https://doi.org/10.1007/s11426-024-2287-6","url":null,"abstract":"The global warming caused by greenhouse gas emissions, principally carbon dioxide (CO2) and methane (CH4), has become a great threat to human survival. The capture and conversion of CO2 and CH4 not only provide an effective method to reduce the greenhouse gas emissions towards achieving carbon neutrality but also produce sustainable chemicals and fuels to meet the increasing demand for chemicals and energy. Zeolite-based materials are excellent adsorbents and catalysts for CO2 and CH4 capture and conversion. In this mini-review, we present the recent progress in zeolite-based materials for CO2 and CH4 capture and conversion. We first discuss the key factors of zeolites on the CO2 and CH4 adsorption performance. Then, we demonstrate the catalytic conversion of CO2 and CH4 into value-added chemicals, including hydrocarbons, oxygenates, and syngas. Finally, we provide an outlook regarding the opportunities and challenges for the capture and conversion of CO2 and CH4 towards achieving carbon neutrality and sustainable development.","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"27 1","pages":""},"PeriodicalIF":9.445,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197148","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