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用于光催化CO还原的介孔半金属高熵尖晶石氧化物纳米纤维的低温合成

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

作者信息

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

机构信息

College of Textiles, Donghua University, Shanghai 201620, People's Republic of China.

Innovation Center for Textile Science and Technology, Donghua University, Shanghai 200051, People's Republic of China.

出版信息

ACS Nano. 2024 Feb 9. doi: 10.1021/acsnano.3c09559.

DOI:10.1021/acsnano.3c09559
PMID:38334301
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 °C 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)O show a high specific surface area of 66.48 m/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 CO into CH and CO with high yields of 8.03 and 15.89 μmol g h, respectively, without using photosensitizers or sacrificial agents.

摘要

高熵氧化物(HEOs)因其组成多样、化学适应性强、光吸收能力可调节以及稳定性强而展现出巨大的前景。在本研究中,我们报道了一种通过溶胶 - 凝胶静电纺丝技术在400℃的低温下合成一系列多孔高熵尖晶石氧化物(HESO)纳米纤维(NFs)的策略。关键在于选择六种具有相似配位能力的乙酰丙酮盐前驱体,在从稳定溶胶转变为凝胶纳米纤维的过程中保持高熵无序状态。所合成的(NiCuMnCoZnFe)O HESO纳米纤维具有66.48 m²/g的高比表面积、多样的元素组成、双带隙、半金属特性以及丰富的缺陷。多样的元素提供了各种协同催化位点,氧空位作为电子 - 空穴分离的活性位点,而半金属性和双带隙结构提供了优异的光吸收能力,从而将其适用性扩展到广泛的光催化过程。结果,HESO纳米纤维在不使用光敏剂或牺牲剂的情况下,能够分别以8.03和15.89 μmol g⁻¹ h⁻¹的高产率将CO高效转化为CH₄和CO₂。

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