铋掺杂的二氧化钌催化剂用于高效酸性水氧化

doi:10.1016/S1872-2067(23)64554-1

催化学报 ›› 2023, Vol. 55: 182-190.DOI: 10.1016/S1872-2067(23)64554-1

铋掺杂的二氧化钌催化剂用于高效酸性水氧化

吴立清^a, 梁庆^b, 赵家仪^a, 朱娟^a, 贾宏男^a, 张伟^b^,^*(), 蔡苹^a^,^*(), 罗威^a^,^*()

^a武汉大学化学与分子科学学院, 湖北武汉 430072
^b吉林大学材料科学与工程学院, 吉林省高效清洁能源材料国际合作重点实验室, 吉林省高效清洁能源材料国际科技合作重点实验室, 未来科学国际中心, 未来科学国际合作联合实验室, 吉林长春 130012

收稿日期:2023-09-27 接受日期:2023-10-25 出版日期:2023-12-18 发布日期:2023-12-07
通讯作者: *电子信箱: weizhang@jlu.edu.cn (张伟), applecaiping@163.com (蔡苹), wluo@whu.edu.cn (罗威).
基金资助:
国家自然科学基金(22272121);国家自然科学基金(21972107);国家自然科学基金(51872115)

A Bi-doped RuO₂ catalyst for efficient and durable acidic water oxidation

Liqing Wu^a, Qing Liang^b, Jiayi Zhao^a, Juan Zhu^a, Hongnan Jia^a, Wei Zhang^b^,^*(), Ping Cai^a^,^*(), Wei Luo^a^,^*()

^aCollege of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, Hubei, China
^bKey Laboratory of Automobile Materials MOE, and School of Materials Science & Engineering, and Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials, and Electron Microscopy Center, and International Center of Future Science, Jilin University, Changchun 130012, Jilin, China

Received:2023-09-27 Accepted:2023-10-25 Online:2023-12-18 Published:2023-12-07
Contact: *E-mail: weizhang@jlu.edu.cn (W. Zhang), applecaiping@163.com (P. Cai), wluo@whu.edu.cn (W. Luo).
Supported by:
National Natural Science Foundation of China(22272121);National Natural Science Foundation of China(21972107);National Natural Science Foundation of China(51872115)

摘要/Abstract

摘要：

目前, 电解水是一种很有前景的制氢方式, 它能够将可持续能源产生的电能转化为储存在氢键中的化学能, 实现高效的能源转换. 与传统碱性电解槽相比, 质子交换膜水电解槽(PEMWE)由于工作温度低、电压效率高、电流密度高和兼容性好, 是一种很有发展潜力的绿色制氢技术. 然而, PEMWE阳极析氧反应(OER)缓慢的反应动力学通常需要消耗更多能量, 极大降低工作效率并限制了其发展. 目前氧化铱(IrO₂)仍然是唯一能商业应用的PEMFC阳极催化剂. 但铱储量少且成本高严重阻碍了PEMFC大规模应用. 近年来, 氧化钌(RuO₂)因其高固有活性且价格相对低廉被认为是IrO₂在酸性OER中潜在的替代品. 然而, RuO₂在酸性OER中稳定性较差, 长时间会发生晶体结构崩塌和溶解. 因此, 开发出一种有效的策略来平衡RuO₂基催化剂的稳定性和活性之间的关系对PEMWE的实际应用至关重要.

本文采用铋(Bi)掺杂来调控RuO₂的酸性OER电催化剂(Bi_0.15Ru_0.85O₂), 同时提高了其酸性OER的活性和稳定性. 在0.5 mol L^-1 H₂SO₄溶液中, Bi_0.15Ru_0.85O₂在10 mA cm^-2下酸性OER的过电位为200.0 mV, 远低于RuO₂和商业RuO₂, 且具有长达100 h的稳定性. X射线光电子能谱(XPS)和Ru L_2,3边X射线吸收近边结构(XANES)结果表明, 引入Bi元素后, Bi_0.15Ru_0.85O₂中Ru的初始氧化态升高, 有利于OER过程中Ru活性中心的氧化, 激活活性位点, 从而提高催化活性. 电化学实验、紫外光发射光谱和紫外可见光谱等结果表明, Bi_0.15Ru_0.85O₂比RuO₂具有更快的电子转移能力和更好的导电性, 从而提升了催化过程的反应动力学. Bi和Ru之间的强电子相互作用也有利于提高催化剂结构的稳定性以及在OER过程中的稳定性. 此外, 本文还通过原位拉曼光谱研究了Bi_0.15Ru_0.85O₂和RuO₂的催化机理, 更加深入地了解其构效关系. 表观活化能测试和密度泛函理论结果表明, Bi的引入可以有效降低速率决定步骤的表观活化能和能垒, 从而大大提升催化性能.

综上所述, 本文成功制备了高性能的RuO₂基电催化剂, 并将其应用于酸性OER中. Bi_0.15Ru_0.85O₂中Ru活性位点的激活以及强电子相互作用有利于平衡活性和稳定性之间的关系, 实现同时提高催化活性和稳定性, 对酸性OER催化剂的设计提供了新思路.

关键词: 析氧反应, 二氧化钌基催化剂, Bi掺杂, 活性, 稳定性

Abstract:

Ruthenium oxide-based electrocatalysts have been regarded as promising alternatives to the state-of-the-art Iridium oxide (IrO₂) towards acidic oxygen evolution reaction (OER). However, their practical applications of proton exchange membrane water electrolyzer (PEMWE) are severely limited by the lack of efficient strategy to balance the seesaw relation between stability and activity of ruthenium oxide (RuO₂)-based catalysts. Herein, we report that both the activity and stability of RuO₂ can be significantly boosted though bismuth (Bi) doping. We find that the introduction of Bi can increase the initial valance state of Ru in Bi_0.15Ru_0.85O₂, which can promote the activation of Ru active sites, and facilitate the reaction kinetics of acidic OER. Besides, the presence of Bi can strengthen the electron interaction to maintain the structure stability and improve the electrocatalytic performance by reducing the energy barriers and avoiding the overoxidation of active species. The obtained Bi_0.15Ru_0.85O₂ catalyst shows a low overpotential of 200.0 mV to reach a current density of 10 mA cm^-2 under acidic media, and a long-term stability for over 100 hours. Our work provides an important inspiration to rational design RuO₂-based electrocatalysts with high activity and durability toward acidic OER.

Key words: Oxygen evolution reaction, RuO₂-based catalyst, Bismuth doping, Activity, Stability

吴立清, 梁庆, 赵家仪, 朱娟, 贾宏男, 张伟, 蔡苹, 罗威. 铋掺杂的二氧化钌催化剂用于高效酸性水氧化[J]. 催化学报, 2023, 55: 182-190.

Liqing Wu, Qing Liang, Jiayi Zhao, Juan Zhu, Hongnan Jia, Wei Zhang, Ping Cai, Wei Luo. A Bi-doped RuO₂ catalyst for efficient and durable acidic water oxidation[J]. Chinese Journal of Catalysis, 2023, 55: 182-190.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(23)64554-1

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图/表 4

Fig. 1. Morphology and structure analysis. (a) XRD patterns of Bi0.15Ru0.85O2 and RuO2. (b) and (c) HAADF-STEM image of Bi0.15Ru0.85O2. (d) HAADF-STEM image and corresponding EDS elemental mapping of Bi0.15Ru0.85O2. (e) The high-resolution XPS spectrum of Ru 3p in Bi0.15Ru0.85O2 and RuO2. (f) Experimental Ru L2,3-edges XANES spectra of Bi0.15Ru0.85O2 and RuO2.

Fig. 2. Electrochemical performance of Bi0.15Ru0.85O2 in acidic medium. (a) LSV curves of Bi0.15Ru0.85O2, RuO2, and C-RuO2, recorded with a scan rate of 5 mV s?1. (b) Tafel plots of Bi0.15Ru0.85O2, RuO2, and C-RuO2, derived from the LSV curves. The operando Bode phase plots of (c) Bi0.15Ru0.85O2 and (d) RuO2. (e) Phase peak angles varies with the changes of potentials for Bi0.15Ru0.85O2 and RuO2. (f) Chronopotentiometric stability test of Bi0.15Ru0.85O2.

Fig. 3. Kinetic analysis. (a) LSV curves of Bi0.15Ru0.85O2 and RuO2 recorded at 25 and 65 °C, respectively. (b) The corresponding Eapp data at different potentials of Bi0.15Ru0.85O2, derived from the LSV curves at different temperatures. (c) The corresponding Eapp data at different potentials of RuO2, derived from the LSV curves at different temperatures. (d) UPS spectra of Bi0.15Ru0.85O2 and RuO2. (e) UV spectra of Bi0.15Ru0.85O2 and RuO2. (f) Summary of some major OER performance metrics of Bi0.15Ru0.85O2 and RuO2. The Eapp was calculated at 1.45 V vs. RHE.

Fig. 4. Theoretical analysis. In situ Raman spectra of Bi0.15Ru0.85O2 (a) and RuO2 (b), in which the red square indicating the formation of the OOH*. (c) Charge density distribution image for Bi0.15Ru0.85O2 based on DFT analysis. (d) Reaction pathways of Bi0.15Ru0.85O2 and RuO2 for OER.

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铋掺杂的二氧化钌催化剂用于高效酸性水氧化

A Bi-doped RuO₂ catalyst for efficient and durable acidic water oxidation

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铋掺杂的二氧化钌催化剂用于高效酸性水氧化

A Bi-doped RuO2 catalyst for efficient and durable acidic water oxidation

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A Bi-doped RuO₂ catalyst for efficient and durable acidic water oxidation