High-entropy-perovskite subnanowires for photoelectrocatalytic coupling of methane to acetic acid

Siyang Nie, Liang Wu, Qinghua Zhang, Yunwei Huang, Qingda Liu () and Xun Wang ()
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Siyang Nie: Tsinghua University
Liang Wu: Shanghai Jiao Tong University
Qinghua Zhang: Chinese Academy of Sciences
Yunwei Huang: Tsinghua University
Qingda Liu: Tsinghua University
Xun Wang: Tsinghua University

Nature Communications, 2024, vol. 15, issue 1, 1-15

Abstract: Abstract The incorporation of multiple immiscible metals in high-entropy oxides can create the unconventional coordination environment of catalytic active sites, while the high formation temperature of high-entropy oxides results in bulk materials with low specific surface areas. Here we develop the high-entropy LaMnO3-type perovskite-polyoxometalate subnanowire heterostructures with periodically aligned high-entropy LaMnO3 oxides and polyoxometalate under a significantly reduced temperature of 100 oC, which is much lower than the temperature required by state-of-the-art calcination methods for synthesizing high-entropy oxides. The high-entropy LaMnO3-polyoxometalate subnanowires exhibit excellent catalytic activity for the photoelectrochemical coupling of methane into acetic acid under mild conditions (1 bar, 25 oC), with a high productivity (up to 4.45 mmol g‒1cat h‒1) and selectivity ( > 99%). Due to the electron delocalization at the subnanometer scale, the contiguous active sites of high-entropy LaMnO3 and polyoxometalate in the heterostructure can efficiently activate C − H bonds and stabilize the resulted *COOH intermediates, which benefits the in situ coupling of *CH3 and *COOH into acetic acid.

Date: 2024
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DOI: 10.1038/s41467-024-50977-8

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