Shape-Controlled Metal-Free Catalysts: Facet-Sensitive Catalytic Activity Induced by the Arrangement Pattern of Noncovalent Supramolecular Chains | |
Geng, Guangwei1,2; Chen, Penglei1,2,3,4,5; Guan, Bo1; Jiang, Lang1; Xu, Zhongfei6,7; Di, Dawei8; Tu, Zeyi1; Hao, Weichang6,7; Yi, Yuanping1; Chen, Chuncheng1 | |
刊名 | ACS NANO |
2017-05-01 | |
卷号 | 11期号:5页码:4866-4876 |
关键词 | Metal-free Catalysts Organic Crystals Facet-sensitive Catalytic Activity 2d Charge Transport Network Noncovalent Supramolecular Chains |
英文摘要 | Metal-free catalytic materials have recently received broad attention as promising alternatives to metal-involved catalysts. This is owing to their inherent capability to overcome the inevitable limitations of metal-involved catalysts, such as high sensitivity to poisoning, the limited reserves, high cost and scarcity of metals (especially noble metals), etc. However, the lack of shape controlled metal-free catalysts with well-defined facets is a formidable bottleneck limiting our understandings on the underlying structure activity relationship at atomic/molecular level, which thereby restrains their rational design. Here, we report that catalytically active crystals of a porphyrin, 5,10,15,20-tetrakis-(pentafluorophenyl)porphyrin, could be shaped into well-defined cubes and sheet like tetradecahedrons (TDHD), which are exclusively and predominantly enclosed by {101} and {001} facets, respectively. Fascinatingly, compared to the cubes, the TDHDs display substantially enhanced catalytic activity toward water decontamination under visible-light irradiation, although both the architectures have identical crystalline structure. We disclose that such interesting shape-sensitive catalytic activity is ascribed to the distinct spatial separation efficiency of photogenerated electrons and holes induced by single-channel and multichannel charge transport pathways along noncovalent supramolecular chains, which are arranged as parallel-aligned and 2D network patterns, respectively. Our findings provide an ideal scientific platform to guide the rational design of next generation metal-free catalysts of desired catalytic performances. |
语种 | 英语 |
内容类型 | 期刊论文 |
源URL | [http://ir.iccas.ac.cn/handle/121111/38519] |
专题 | 化学研究所_有机固体实验室 |
作者单位 | 1.Chinese Acad Sci, Inst Chem, CAS Res Educ Ctr Excellence Mol Sci, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R China 2.Zhengzhou Univ, Coll Chem & Mol Engn, Zhengzhou 450001, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 4.Tianjin Univ, Sch Sci, Dept Chem, Tianjin 300072, Peoples R China 5.Tianjin Univ, Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China 6.Beihang Univ, Dept Phys, Beijing 100191, Peoples R China 7.Beihang Univ, Minist Educ, Key Lab Micro Nano Measurement Manipulat & Phys, Beijing 100191, Peoples R China 8.Univ Cambridge, Cavendish Lab, JJ Thomson Ave, Cambridge CB3 OHE, England |
推荐引用方式 GB/T 7714 | Geng, Guangwei,Chen, Penglei,Guan, Bo,et al. Shape-Controlled Metal-Free Catalysts: Facet-Sensitive Catalytic Activity Induced by the Arrangement Pattern of Noncovalent Supramolecular Chains[J]. ACS NANO,2017,11(5):4866-4876. |
APA | Geng, Guangwei.,Chen, Penglei.,Guan, Bo.,Jiang, Lang.,Xu, Zhongfei.,...&Hu, Wenping.(2017).Shape-Controlled Metal-Free Catalysts: Facet-Sensitive Catalytic Activity Induced by the Arrangement Pattern of Noncovalent Supramolecular Chains.ACS NANO,11(5),4866-4876. |
MLA | Geng, Guangwei,et al."Shape-Controlled Metal-Free Catalysts: Facet-Sensitive Catalytic Activity Induced by the Arrangement Pattern of Noncovalent Supramolecular Chains".ACS NANO 11.5(2017):4866-4876. |
个性服务 |
查看访问统计 |
相关权益政策 |
暂无数据 |
收藏/分享 |
除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。
修改评论