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Two-Step Carbothermal Welding To Access Atomically Dispersed Pd-1 on Three-Dimensional Zirconia Nanonet for Direct Indole Synthesis
Zhao, YF; Zhou, H; Chen, WX; Tong, YJ; Zhao, C; Lin, Y; Jiang, Z; Zhang, QW; Xue, ZG; Cheong, WC; Jin, BJ; Zhou, FY; Wang, WY; Chen, M; Hong, X; Dong, JC; Wei, SQ; Li, YD; Wu, Y
2019
Source PublicationJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN0002-7863
Volume141Issue:27Pages:10590-10594
Subtype期刊论文
AbstractHerein, 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.
KeywordSINGLE-ATOM CATALYST WATER TEMPERATURE PLATINUM OXYGEN COORDINATION HYDROGEN
DOI10.1021/jacs.9b03182
Indexed BySCI
Language英语
Citation statistics
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/32267
Collection中科院上海应用物理研究所2011-2020年
Affiliation1.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;
2.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China;
3.Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Construct Tailorable Adv Funct Ma, Beijing 100081, Peoples R China;
4.Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China;
5.Shanghai Inst Appl Phys, Natl Synchrotron Radiat Lab, Shanghai 201800, Peoples R China;
6.Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230026, Anhui, Peoples R China
Recommended Citation
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.
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