Two-Step Carbothermal Welding To Access Atomically Dispersed Pd-1 on Three-Dimensional Zirconia Nanonet for Direct Indole Synthesis
文献类型:期刊论文
作者 | Zhao, YF; Zhou, H; Chen, WX; Tong, YJ; Zhao, C; Lin, Y; Jiang, Z; Zhang, QW; Xue, ZG; Cheong, WC |
刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY |
出版日期 | 2019 |
卷号 | 141期号:27页码:10590-10594 |
ISSN号 | 0002-7863 |
关键词 | SINGLE-ATOM CATALYST WATER TEMPERATURE PLATINUM OXYGEN COORDINATION HYDROGEN |
DOI | 10.1021/jacs.9b03182 |
文献子类 | 期刊论文 |
英文摘要 | Herein, we report a novel carbothermal welding strategy to prepare atomically dispersed Pd sites anchored on a three-dimensional (3D) ZrO2 nanonet (Pd-1@ZrO2) via two-step pyrolysis, which were evolved from isolated Pd sites anchored on linker-derived nitrogen-doped carbon (Pd-1@NC/ZrO2). First, the NH2-H2BDC linkers and Zr-6-based [Zr-6(mu(3)-O)(4)(mu(3)-OH)(4)](12+) nodes of UiO-66-NH2 were transformed into amorphous N-doped carbon skeletons (NC) and ZrO2 nanoclusters under an argon atmosphere, respectively. The NC supports can simultaneously reduce and anchor the Pd sites, forming isolated Pd-1-N/C sites. Then, switching the argon to air, the carbonaceous skeletons are gasified and the ZrO2 nanoclusters are welded into a rigid and porous nanonet. Moreover, the reductive carbon will result in abundant oxygen (O*) defects, which could help to capture the migratory Pd-1 species, leaving a sintering-resistant Pd-1@ZrO2 catalyst via atom trapping. This Pd-1@ZrO2 nanonet can act as a semi-homogeneous catalyst to boost the direct synthesis of indole through hydrogenation and intramolecular condensation processes, with an excellent turnover frequency (1109.2 h(-1)) and 94% selectivity. |
语种 | 英语 |
源URL | [http://ir.sinap.ac.cn/handle/331007/32267] |
专题 | 上海应用物理研究所_中科院上海应用物理研究所2011-2017年 |
作者单位 | 1.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China; 2.Univ Sci & Technol China, IChEM Collaborat Innovat Ctr Chem Energy Mat, Hefei Natl Lab Phys Sci Microscale, Dept Chem, Hefei 230026, Anhui, Peoples R China; 3.Shanghai Inst Appl Phys, Natl Synchrotron Radiat Lab, Shanghai 201800, Peoples R China; 4.Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230026, Anhui, Peoples R China 5.Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China; 6.Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Construct Tailorable Adv Funct Ma, Beijing 100081, Peoples R China; |
推荐引用方式 GB/T 7714 | Zhao, YF,Zhou, H,Chen, WX,et al. Two-Step Carbothermal Welding To Access Atomically Dispersed Pd-1 on Three-Dimensional Zirconia Nanonet for Direct Indole Synthesis[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2019,141(27):10590-10594. |
APA | Zhao, YF.,Zhou, H.,Chen, WX.,Tong, YJ.,Zhao, C.,...&Wu, Y.(2019).Two-Step Carbothermal Welding To Access Atomically Dispersed Pd-1 on Three-Dimensional Zirconia Nanonet for Direct Indole Synthesis.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,141(27),10590-10594. |
MLA | Zhao, YF,et al."Two-Step Carbothermal Welding To Access Atomically Dispersed Pd-1 on Three-Dimensional Zirconia Nanonet for Direct Indole Synthesis".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 141.27(2019):10590-10594. |
入库方式: OAI收割
来源:上海应用物理研究所
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