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通过负载在硫化镍基导电纳米纤维上的低铂和无铂催化剂实现显著增强的节能析氢与尿素氧化反应耦合。

Significantly Enhanced Energy-Saving H Production Coupled with Urea Oxidation by Low- and Non-Pt Anchored on NiS-Based Conductive Nanofibers.

作者信息

Zhong Mengxiao, Yang Junyu, Xu Meijiao, Ren Siyu, Chen Xiaojie, Wang Ce, Gao Mingbin, Lu Xiaofeng

机构信息

Alan G. MacDiarmid Institute, College of Chemistry, Jilin University, 2699 Qianjin Street, Changchun, 130012, P. R. China.

Division of Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, P. R. China.

出版信息

Small. 2024 Jan;20(1):e2304782. doi: 10.1002/smll.202304782. Epub 2023 Aug 30.

Abstract

Rational designing electrocatalysts is of great significance for realizing high-efficiency H production in the water splitting process. Generally, reducing the usage of precious metals and developing low-potential nucleophiles oxidation reaction to replace anodic oxygen evolution reaction (OER) are efficient strategies to promote H generation. Here, NiS-coated nickel-carbon nanofibers (NiS@Ni-CNFs) are prepared for low-content Pt deposition (Pt-NiS@Ni-CNFs) to attain the alkaline HER catalyst. Due to the reconfiguration of NiS phase and synergistic effect between Pt and nickel sulfides, the Pt-NiS@Ni-CNFs catalyst shows a high mass activity of 2.74-fold of benchmark Pt/C sample. In addition, the NiS@Ni-CNFs catalyst performs a superior urea oxidation reaction (UOR) activity with the potential of 1.366 V versus reversible hydrogen electrode (RHE) at 10 mA cm , which demonstrates the great potential in the replacement of OER. Thus, a urea-assisted water splitting electrolyzer of Pt-NiS@Ni-CNFs (cathode)||NiS@Ni-CNFs (anode) is constructed to exhibit small voltages of 1.44 and 1.65 V to reach 10 and 100 mA cm , which is much lower than its overall water splitting process, and presents a 6.5-fold hydrogen production rate enhancement. This work offers great opportunity to design new catalysts toward urea-assisted water splitting with significantly promoted hydrogen productivity and reduced energy consumption.

摘要

合理设计电催化剂对于在水分解过程中实现高效产氢具有重要意义。一般来说,减少贵金属的使用并开发低电位亲核试剂氧化反应以替代阳极析氧反应(OER)是促进产氢的有效策略。在此,制备了硫化镍包覆的镍碳纳米纤维(NiS@Ni-CNFs)用于低含量铂沉积(Pt-NiS@Ni-CNFs)以获得碱性析氢反应催化剂。由于NiS相的重构以及铂与硫化镍之间的协同效应,Pt-NiS@Ni-CNFs催化剂表现出相对于基准Pt/C样品2.74倍的高质量活性。此外,NiS@Ni-CNFs催化剂在10 mA cm²电流密度下相对于可逆氢电极(RHE)的电位为1.366 V时表现出优异的尿素氧化反应(UOR)活性,这表明其在替代OER方面具有巨大潜力。因此,构建了Pt-NiS@Ni-CNFs(阴极)||NiS@Ni-CNFs(阳极)的尿素辅助水分解电解槽,在达到10和100 mA cm²电流密度时分别表现出1.44 V和1.65 V的低电压,这远低于其整体水分解过程,并实现了6.5倍的产氢速率提升。这项工作为设计新型催化剂用于尿素辅助水分解提供了绝佳机会,可显著提高产氢效率并降低能耗。

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