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Low-Temperature Synthesis of Mesoporous Half-Metallic High-Entropy Spinel Oxide Nanofibers for Photocatalytic CO2 Reduction

Liang Zhang, Shuhui Xia, Xiaohua Zhang, Yonggang Yao, Yuanyuan Zhang, Shuo Chen, Yuehui Chen, Jianhua Yan

ACS NANO(2024)

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Abstract
High-entropy oxides (HEOs) exhibit great prospects owing to their varied composition, chemical adaptability, adjustable light-absorption ability, and strong stability. In this study, we report a strategy to synthesize a series of porous high-entropy spinel oxide (HESO) nanofibers (NFs) at a low temperature of 400 degree celsius by a sol-gel electrospinning technique. The key lies in selecting six acetylacetonate salt precursors with similar coordination abilities, maintaining a high-entropy disordered state during the transformation from stable sols to gel NFs. The as-synthesized HESO NFs of (NiCuMnCoZnFe)(3)O-4 show a high specific surface area of 66.48 m(2)/g, a diverse elemental composition, a dual bandgap, half-metallicity property, and abundant defects. The diverse elements provide various synergistic catalytic sites, and oxygen vacancies act as active sites for electron-hole separation, while the half-metallicity and dual-bandgap structure offer excellent light absorption ability, thus expanding its applicability to a wide range of photocatalytic processes. As a result, the HESO NFs can efficiently convert CO2 into CH4 and CO with high yields of 8.03 and 15.89 mu mol g(-1) h(-1), respectively, without using photosensitizers or sacrificial agents.
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Key words
Uniform coordination strategy,Low-temperature synthesis,High-entropy oxide nanofibers,Half-metallicity,Synergistic Zn-Cu-Mn-Fe photocatalysis
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