三维百合花状的CoNi2S4作为先进的双功能电催化剂用于氢析出和氧析出反应

doi:10.1016/S1872-2067(18)63053-0

催化学报 ›› 2018, Vol. 39 ›› Issue (8): 1403-1410.DOI: 10.1016/S1872-2067(18)63053-0

三维百合花状的CoNi₂S₄作为先进的双功能电催化剂用于氢析出和氧析出反应

黎景卫, 庄秋娜, 许培蔓, 张大维, 韦丽成, 袁定胜

暨南大学化学与材料学院, 广东广州 510632

收稿日期:2018-01-24 修回日期:2018-02-27 出版日期:2018-08-18 发布日期:2018-07-04
通讯作者: 袁定胜
基金资助:
国家自然科学基金（21376105，21576113）.

Three-dimensional lily-like CoNi₂S₄ as an advanced bifunctional electrocatalyst for hydrogen and oxygen evolution reaction

Jingwei Li, Qiuna Zhuang, Peiman Xu, Dawei Zhang, Licheng Wei, Dingsheng Yuan

School of Chemistry and Materials Science, Jinan University, Guangzhou 510632, Guangdong, China

Received:2018-01-24 Revised:2018-02-27 Online:2018-08-18 Published:2018-07-04
Contact: 10.1016/S1872-2067(18)63053-0
Supported by:
This work was supported by the National Natural Science Foundation of China (21376105, 21576113).

摘要/Abstract

摘要：

为简化电解水催化剂的合成过程和优化电解水操作系统，双功能电解水催化剂的研究，特别是在碱性条件下同时具有优异催化氢析出和氧析出反应性能的双功能电催化剂的研究尤为重要.其中，过渡金属硫化物，特别是CoNi硫化物，被报道有与氢化酶类似的催化活性中心，从而具有优异的催化氢析出和催化氧析出反应性能.虽然有关对过渡金属硫化物的研究很多，但主要集中在具有一维纳米线和二维纳米片形貌结构的过渡金属硫化物.不幸的是，这些形貌结构的过渡金属硫化物在电催化过程中容易聚集和受限于电荷传输能力.三维纳米结构的材料具有较大的比表面积以分布更多的活性位点和拥有良好的电子传输能力，所以，开发三维纳米结构的过渡金属硫化物材料可能是改进其催化电解水性能的一个好途径.本文采用简单的两步水热法，通过硫化合成的CoNi前体得到了长于泡沫镍上的三维百合花状的CoNi₂S₄（CoNi₂S₄/Ni）.它只需要54mV的过电位即可获得10mA cm^-2的催化氢析出反应电流，是最好的碱性催化氢析出反应电极材料之一.它在驱动100mA cm^-2的催化氧析出反应电流时也只需要328mV的过电位.另外，把CoNi₂S₄/Ni分别作为阴极和阳极组装成双电极碱性水电解槽时，它只需要1.56V的电压即可获取10mA cm^-2的催化全电解水电流并具有良好的催化全电解水稳定性.
扫描电子显微镜、透射电子显微镜和N₂吸脱附曲线测试结果表明，该三维百合花状的CoNi₂S₄/Ni的表面粗糙度高和拥有多孔特性.多孔结构的CoNi₂S₄/Ni可提供更多可接触的催化活性位点，也有利于催化过程中的电解质和生成的气体的扩散与传递.交流阻抗图谱测试结果表明，CoNi₂S₄/Ni具有良好的电子传输能力.另外，不同于前期对尖晶石结构的硫化物AB₂S₄的研究结果，XPS结果表明，CoNi₂S₄/Ni中含有Ni^σ⁺和S^σ-活性物种，表明CoNi₂S₄具有与活性氢化酶类似的活性中心.Ni^δ⁺和S^δ-可分别作为氢氧根和质子的接收体，协助促进吸附的水分子的分离，从而提高材料的催化性能.所以，Ni^δ⁺和S^δ-活性物种的出现，大比表面积的三维百合花状多孔结构和良好的电荷传输能力等特性集合于CoNi₂S₄/Ni上使得CoNi₂S₄/Ni具有优异的催化氢析出和催化氧析出反应性能.

关键词: 双功能电催化剂, 氢析出反应, 氧析出反应, 百合花状的CoNi₂S₄, 全电解水

Abstract:

Designing low-cost, highly efficient, and stable bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is of vital significance for water splitting. Herein, three-dimensional lily-like CoNi₂S₄ supported on nickel foam (CoNi₂S₄/Ni) has been fabricated by sulfuration of the Co-Ni precursor. As expected, CoNi₂S₄/Ni possesses such outstanding electrocatalytic properties that it requires an overpotential of only 54 mV at 10 mA cm^-2 and 328 mV at 100 mA cm^-2 for HER and OER, respectively. Furthermore, by utilizing the CoNi₂S₄/Ni electrodes as bifunctional electrocatalysts for overall water splitting, a current density of 10 mA cm^-2 can be obtained at a voltage of only 1.56 V.

Key words: Bifunctional electrocatalyst, Hydrogen evolution reaction, Oxygen evolution reaction, Lily-like CoNi₂S₄, Overall water splitting

黎景卫, 庄秋娜, 许培蔓, 张大维, 韦丽成, 袁定胜. 三维百合花状的CoNi₂S₄作为先进的双功能电催化剂用于氢析出和氧析出反应[J]. 催化学报, 2018, 39(8): 1403-1410.

Jingwei Li, Qiuna Zhuang, Peiman Xu, Dawei Zhang, Licheng Wei, Dingsheng Yuan. Three-dimensional lily-like CoNi₂S₄ as an advanced bifunctional electrocatalyst for hydrogen and oxygen evolution reaction[J]. Chinese Journal of Catalysis, 2018, 39(8): 1403-1410.

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三维百合花状的CoNi₂S₄作为先进的双功能电催化剂用于氢析出和氧析出反应

Three-dimensional lily-like CoNi₂S₄ as an advanced bifunctional electrocatalyst for hydrogen and oxygen evolution reaction

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