Ni3N/MoO2平面异质结构实现增强的碱性氢氧化

doi:10.1016/S1872-2067(22)64126-3

催化学报 ›› 2022, Vol. 43 ›› Issue (12): 3154-3160.DOI: 10.1016/S1872-2067(22)64126-3

Ni₃N/MoO₂平面异质结构实现增强的碱性氢氧化

安露露^a^,^†, 邓邵峰^a^,^†, 郭煦昀^b, 刘旭坡^a, 赵桐辉^a, 陈科^a, 朱叶^b, 付玉喜^a, 赵旭^a^,^#(), 王得丽^a^,^*()

^a华中科技大学化学化工学院, 能源转换与存储材料化学教育部重点实验室, 材料化学与服役失效湖北省重点实验室, 湖北武汉430074
^b香港理工大学智能能源研究所应用物理系, 香港

收稿日期:2022-03-30 接受日期:2022-05-09 出版日期:2022-12-18 发布日期:2022-10-18
通讯作者: 赵旭,王得丽
作者简介:第一联系人：
^†共同第一作者.
基金资助:
国家自然科学基金(22002046);国家自然科学基金(91963109);国家重点研发计划项目(2018YFB0905600);能源转化与储存材料化学教育部重点实验室开放课题基金(华中科技大学)(2021JYBKF01)

Enhancing hydrogen electrocatalytic oxidation on Ni₃N/MoO₂ in-plane heterostructures in alkaline solution

Lulu An^a^,^†, Shaofeng Deng^a^,^†, Xuyun Guo^b, Xupo Liu^a, Tonghui Zhao^a, Ke Chen^a, Ye Zhu^b, Yuxi Fu^a, Xu Zhao^a^,^#(), Deli Wang^a^,^*()

^aKey laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China
^bDepartment of Applied Physics, Research Institute for Smart Energy, The Hong Kong Polytechnic University, Hong Kong, China

Received:2022-03-30 Accepted:2022-05-09 Online:2022-12-18 Published:2022-10-18
Contact: Xu Zhao, Deli Wang
About author:First author contact:^†Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(22002046);National Natural Science Foundation of China(91963109);National Key R&D Program of China(2018YFB0905600);Open Research Fund of Key Laboratory of Material Chemistry for Energy Conversion and Storage (HUST), Ministry of Education(2021JYBKF01)

摘要/Abstract

摘要：

氢氧燃料电池技术的发展有利于缓解化石燃料短缺和环境污染等问题. 近年来, 碱性阴离子交换膜燃料电池因可以使用非贵金属催化剂而得到广泛关注, 但其阳极氢氧化反应(HOR)的动力学相对于酸性条件下有2‒3个数量级的降低. 因此, 亟需开发低成本高活性的碱性氢氧化电催化剂.

镍(Ni)基材料是非常具有应用前景的非贵金属碱性氢氧化反应催化剂. 然而, 纯金属Ni对氢物种的吸附过强, 导致其对氢氧化反应的催化活性不高. 因此, 研究学者们采取了多种改性策略以提高Ni基催化剂的催化活性. 目前报道的比较有效的策略是构造Ni基氮化物, 调节Ni的电子结构, 减弱Ni位点对H物种的吸附, 进一步增强其对碱性HOR的催化性能. 另一种行之有效的策略是构筑Ni基异质结构, 通过组成异质结构的两相之间的电子转移优化催化剂对反应中间体氢和氢氧物种的吸附, 从而提升对碱性HOR的催化性能. 综上所述, 通过催化剂结构设计提升其催化活性是一个值得研究的课题.

本文通过构建氮化物结构和异质结构以调节催化位点对碱性氢氧化反应中间体H和OH物种的吸附能力, 从而增强Ni基催化剂的活性. 采用多步溶剂热和氨气退火方法合成了Ni₃N/MoO₂平面异质结, 电化学测试结果表明, Ni₃N/MoO₂平面异质结表现出了较高的催化活性, 其质量活性达到了16.4 mA mg^‒1, 分别是纯氮化镍的4.4倍和纯镍的8.6倍; 同时, Ni₃N/MoO₂平面异质结还表现出了较好的循环稳定性, 在2000次CV循环后, 性能基本无变化; 另外, Ni₃N/MoO₂平面异质结还具有较好的CO耐受性, 即使在1000 ppm的CO存在时, 其活性衰减也较小. 进一步通过CO剥离和氢气氮气条件下的循环伏安法研究其对OH和H物种的吸附能力, 分析了Ni₃N/MoO₂平面异质结对碱性HOR性能的增强机制. CO剥离实验结果显示, Ni₃N/MoO₂平面异质结表现出较Ni₃N低的CO剥离峰, 表明由于MoO₂的引入, Ni₃N/平面异质结对OH物种的吸附能力增强. 循环伏安结果显示, 相比于N₂饱和的0.1 mol L^‒1 KOH电解液中催化材料的氧化峰位置, Ni₃N/MoO₂平面异质结在H₂饱和的0.1 mol L^‒1 KOH电解液中的氧化峰较Ni₃N正移更明显, 表明Ni₃N/MoO₂平面异质结对H物种的吸附减弱, 这归因于MoO₂与Ni₃N之间的电子转移对Ni电子结构的优化. 因此, 由于Ni₃N/MoO₂平面异质结构对H物种的吸附减弱和OH物种的吸附增强, 从而加速了碱性氢氧化反应进程. 综上, 本文为设计高性能碱性氢氧化电催化剂提供了一种简便的方法.

关键词: 氮化镍, 平面异质结构, 吸附, 氢氧化反应, 碱性溶液

Abstract:

Nickel (Ni)-based materials act as one of the most promising candidates as platinum-group-metal-free (PGM-free) electrocatalysts for hydrogen oxidation reaction (HOR) in alkaline solution. Nevertheless, the electrocatalytic activity of pure Ni is significantly limited due to the sluggish kinetics under alkaline condition. To accelerate the kinetics, constructing heterostructures and nitride structures have been developed as two representative strategies. Here, we combined the two methods and presented a facile synthesis of the sheet-like Ni₃N/MoO₂ in-plane heterostructures for enhanced HOR in alkaline electrolytes. Relative to Ni or Ni₃N, the Ni₃N/MoO₂ in-plane heterostructures exhibited a significantly increased mass activity by 8.6-fold or 4.4-fold, respectively. Mechanistic studies revealed that the enhanced activity of Ni₃N/MoO₂ could be attributed to the weakened hydrogen adsorption and strengthened hydroxyl adsorption. This work provides a facile approach to design high-efficiency catalysts for hydrogen-oxidation catalysis and beyond.

Key words: Nickel nitride, In-plane heterostructures, Adsorption, Hydrogen oxidation reaction, Alkaline solution

安露露, 邓邵峰, 郭煦昀, 刘旭坡, 赵桐辉, 陈科, 朱叶, 付玉喜, 赵旭, 王得丽. Ni₃N/MoO₂平面异质结构实现增强的碱性氢氧化[J]. 催化学报, 2022, 43(12): 3154-3160.

Lulu An, Shaofeng Deng, Xuyun Guo, Xupo Liu, Tonghui Zhao, Ke Chen, Ye Zhu, Yuxi Fu, Xu Zhao, Deli Wang. Enhancing hydrogen electrocatalytic oxidation on Ni₃N/MoO₂ in-plane heterostructures in alkaline solution[J]. Chinese Journal of Catalysis, 2022, 43(12): 3154-3160.

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https://www.cjcatal.com/CN/Y2022/V43/I12/3154

图/表 5

Fig. 1. (a) Schematic illustration of the preparation of Ni3N/MoO2 in-plane heterostructures. SEM (b), TEM (c), HRTEM (d) images, and element mapping (e?i) of Ni3N/MoO2 in-plane heterostructures.

Fig. 2. (a) XRD patterns of Ni3N and Ni3N/MoO2 in-plane heterostructures; Ni 2p (b), N 1s (c) and Mo 3d (d) XPS spectra of Ni3N/MoO2 in-plane heterostructures.

Fig. 3. (a) HOR polarization curves of Ni3N/MoO2, Ni3N, MoO2, Ni and commercial Pt/C with a sweep rate of 2 mV s-1 in H2-saturated KOH solution of 0.1 mol L?1. (b) Polarization curves of Ni3N/MoO2 at varied rotation rate. The inset showed the Koutecky-Levich plot. (c) Polarization curves of Ni3N/MoO2 before and after CV. (d) HOR polarization curves of Ni3N/MoO2 and Pt/C with and without CO.

Fig. 4. (a) Micro-polarization regions of Ni, Ni3N, and Ni3N/MoO2 in-plane heterostructures. (b) Exchange current density and mass activity of Ni, Ni3N, and Ni3N/MoO2 in-plane heterostructures. (c) Tafel plots of the kinetic current densities on Ni3N/MoO2, Ni3N, and Ni in-plane heterostructures. (d) Comparison of the mass activity of various studied HOR catalysts.

Fig. 5. (a) CO stripping curves of Ni3N and Ni3N/MoO2 in KOH solution of 0.1 mol L?1 with a sweep rate of 20 mV s-1. (b) CV curves of Ni3N and Ni3N/MoO2 in H2 or N2-saturated 0.1 mol L?1 KOH, respectively. (c) Schematic illustration of the mechanism for enhanced HOR catalyzed by Ni3N/MoO2 in-plane heterostructures.

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Ni₃N/MoO₂平面异质结构实现增强的碱性氢氧化

Enhancing hydrogen electrocatalytic oxidation on Ni₃N/MoO₂ in-plane heterostructures in alkaline solution

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