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磷改性非晶态高熵CoFeNiCrMn化合物作为肼辅助水电解的高性能电催化剂

Phosphorus-Modified Amorphous High-Entropy CoFeNiCrMn Compound as High-Performance Electrocatalyst for Hydrazine-Assisted Water Electrolysis.

作者信息

Li Kaixun, He JinFeng, Guan Xuze, Tong Yun, Ye Yutong, Chen Lu, Chen Pengzuo

机构信息

School of Chemistry and Chemical Engineering, Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Zhejiang Sci-Tech University, Hangzhou, Zhejiang, 310018, China.

Department of Chemical Engineering, University College London, Roberts Building, Torrington Place, London, WC1E 7JE, UK.

出版信息

Small. 2023 Oct;19(42):e2302130. doi: 10.1002/smll.202302130. Epub 2023 Jun 22.

Abstract

Exploiting highly active and bifunctional catalysts for both hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR) is a prerequisite for the hydrogen acquisition. High-entropy materials have received widespread attention in catalysis, but the high-performance bifunctional electrodes are still lacking. Herein, a novel P-modified amorphous high-entropy CoFeNiCrMn compound is developed on nickel foam (NF) by one-step electrodeposition strategy. The achieved CoFeNiCrMnP/NF delivers remarkable HER and HzOR performance, where the overpotentials as low as 51 and 268 mV are realized at 100 mA cm . The improved cell voltage of 91 mV is further demonstrated at 100 mA cm by assessing CoFeNiCrMnP/NF in the constructed hydrazine-assisted water electrolyser, which is almost 1.54 V lower than the HER||OER system. Experimental results confirm the important role of each element in regulating the bifuncational performance of high-entropy catalysts. The main influencing elements seem to be Fe and Ni for HER, while the P-modification and Cr metal may contribute a lot for HzOR. These synergistic advantages help to lower the energy barriers and improve the reaction kinetics, resulting in the excellent bifunctional activity of the CoFeNiCrMnP/NF. The work offers a feasible strategy to develop self-supporting electrode with high-entropy materials for overall water splitting.

摘要

开发用于析氢反应(HER)和肼氧化反应(HzOR)的高活性双功能催化剂是获取氢气的前提条件。高熵材料在催化领域受到了广泛关注,但高性能双功能电极仍然匮乏。在此,通过一步电沉积策略在泡沫镍(NF)上制备了一种新型的P修饰非晶态高熵CoFeNiCrMn化合物。所制备的CoFeNiCrMnP/NF展现出卓越的HER和HzOR性能,在100 mA cm 时实现了低至51和268 mV的过电位。通过在构建的肼辅助水电解槽中评估CoFeNiCrMnP/NF,在100 mA cm 时进一步证明了91 mV的电池电压改善,这比HER||OER系统低近1.54 V。实验结果证实了各元素在调节高熵催化剂双功能性能中的重要作用。对于HER,主要影响元素似乎是Fe和Ni,而P修饰和Cr金属可能对HzOR有很大贡献。这些协同优势有助于降低能垒并改善反应动力学,从而使CoFeNiCrMnP/NF具有优异的双功能活性。这项工作为开发用于全水分解的高熵材料自支撑电极提供了一种可行的策略。

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