Two-Step Carbothermal Welding To Access Atomically Dispersed Pd1 on Three-Dimensional Zirconia Nanonet for Direct Indole Synthesis
journal contributionposted on 2019-06-12, 00:00 authored by Yafei Zhao, Huang Zhou, Wenxing Chen, Yujing Tong, Chao Zhao, Yue Lin, Zheng Jiang, Qingwei Zhang, Zhenggang Xue, Weng-Chon Cheong, Benjin Jin, Fangyao Zhou, Wenyu Wang, Min Chen, Xun Hong, Juncai Dong, Shiqiang Wei, Yadong Li, Yuen Wu
Herein, we report a novel carbothermal welding strategy to prepare atomically dispersed Pd sites anchored on a three-dimensional (3D) ZrO2 nanonet (Pd1@ZrO2) via two-step pyrolysis, which were evolved from isolated Pd sites anchored on linker-derived nitrogen-doped carbon (Pd1@NC/ZrO2). First, the NH2–H2BDC linkers and Zr6-based [Zr6(μ3-O)4(μ3-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 Pd1–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 Pd1 species, leaving a sintering-resistant Pd1@ZrO2 catalyst via atom trapping. This Pd1@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.
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Two-Step Carbothermal Weldingnovel carbothermal welding strategyUiO -66-NH 2OHThree-Dimensional Zirconia NanonetZrO 2 nanoclustersBDCPd 1intramolecular condensation processesN-doped carbon skeletonsNCAccess Atomically Dispersed Pd 1ZrO 2 nanonetlinker-derived nitrogen-doped carbonZrO 2 catalystDirect Indole Synthesis Hereinsintering-resistant Pd 1Pd sitesPd 1 species