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Electron-Deficient Au Nanoparticles Confined in Organic Molecular Cages for Catalytic Reduction of 4-Nitrophenol

Liu, Y; Dong, H; Huang, H; Zong, W; Miao, Y-E; He, G; Parkin, IP; ... Liu, T; + view all (2022) Electron-Deficient Au Nanoparticles Confined in Organic Molecular Cages for Catalytic Reduction of 4-Nitrophenol. ACS Applied Nano Material , 5 (1) pp. 1276-1283. 10.1021/acsanm.1c03859. Green open access

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Abstract

Noble-metal nanoparticles are regarded as one of the most promising catalysts to reduce the organic pollutant 4-nitrophenol (4-NP). However, the inevitable agglomeration of noble-metal nanoparticles and their poor distributions in catalytic systems limit their performance. Here, we propose a strategy to encapsulate Au nanoparticles inside porous organic cages (POCs) of soluble RCC3 and stabilize the size of Au nanoparticles at ∼3.25 nm. Typically, the Au@RCC3 composite exhibits excellent 4-NP catalytic reduction performance, which is superior to the corresponding Au bulk catalyst and is also closely related to the size of Au nanoparticles. The normalized X-ray absorption near-edge structure (XANES) results indicate that the electron deficiency at the Au atoms in Au@RCC3 is due to the existence of the RCC3 cage, which is beneficial to accelerate the electron transfer from BH4– to 4-NP during the hydrogenation process. This is also shown by density functional theory (DFT), in which a low energy barrier of 1.03 eV exists for the Au12 cluster compared with 1.37 eV for the Au25 cluster. Therefore, the encapsulation of noble-metal nanoparticles with soluble POCs is an effective way to design and develop stable active catalysts rationally.

Type: Article
Title: Electron-Deficient Au Nanoparticles Confined in Organic Molecular Cages for Catalytic Reduction of 4-Nitrophenol
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/acsanm.1c03859
Publisher version: https://doi.org/10.1021/acsanm.1c03859
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: porous organic cage, metal nanoparticle, organic catalysis, 4-nitrophenol, pollutant degradation
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10142270
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