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Concurrent Oxidation-Reduction Reactions in a Single System Using a Low-Plasma Phenomenon: Excellent Catalytic Performance and Stability in the Hydrogenation Reaction.

Authors:
Wail Al Zoubi Abdul Wahab Allaf Bassem Assfour Young Gun Ko

ACS Appl Mater Interfaces 2022 Feb 26;14(5):6740-6753. Epub 2022 Jan 26.

Materials Electrochemistry Laboratory, School of Materials Science and Engineering, Yeungnam University, Gyeongsan 38541, Republic of Korea.

The catalytic activity and stability of metal nanocatalysts toward agglomeration and detachment during their preparation on a support surface are major challenges in practical applications. Herein, we report a novel, one-step, synchronized electro-oxidation-reduction "bottom-up" approach for the preparation of small and highly stable Cu nanoparticles (NPs) supported on a porous inorganic ([email protected]) coating with significant catalytic activity and stability. This unique embedded structure restrains the sintering of CuNPs on a porous [email protected] surface at a high temperature and exhibits a high reduction ratio (100% in 60 s) and no decay in activity even after 30 cycles (>98% conversion in 3 min). This occurs in a model reaction of 4-nitrophenol (4-NP) hydrogenation, far exceeding the performance of most common catalysts observed to date. More importantly, nitroarene, ketone/aldehydes, and organic dyes were reduced to the corresponding compounds with 100% conversion. Density functional theory (DFT) calculations of experimental model systems with six Cu, two Fe, and four Ag clusters anchored on the TiO surface were conducted to verify the experimental observations. The experimental results and DFT calculations revealed that CuNPs not only favor the adsorption on the TiO surface over those of Fe and AgNPs but also boost the adsorption energy and activity of 4-NP. This strategy has also been extended to the preparation of other single-atom catalysts (e.g., [email protected] and [email protected]), which exhibit excellent catalytic performance.

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http://dx.doi.org/10.1021/acsami.1c22192DOI Listing
February 2022

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