Hu Chun, Yue Kaihang, Han Jiajia, Liu Xiaozhi, Liu Lijia, Liu Qiunan, Kong Qingyu, Pao Chih-Wen, Hu Zhiwei, Suenaga Kazu, Su Dong, Zhang Qiaobao, Wang Xianying, Tan Yuanzhi, Huang Xiaoqing
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
CAS Key Laboratory of Materials for Energy Conversion, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China.
Sci Adv. 2023 Sep 15;9(37):eadf9144. doi: 10.1126/sciadv.adf9144.
Designing an efficient catalyst for acidic oxygen evolution reaction (OER) is of critical importance in manipulating proton exchange membrane water electrolyzer (PEMWE) for hydrogen production. Here, we report a fast, nonequilibrium strategy to synthesize quinary high-entropy ruthenium iridium-based oxide (M-RuIrFeCoNiO) with abundant grain boundaries (GB), which exhibits a low overpotential of 189 millivolts at 10 milliamperes per square centimeter for OER in 0.5 M HSO. Microstructural analyses, density functional calculations, and isotope-labeled differential electrochemical mass spectroscopy measurements collectively reveal that the integration of foreign metal elements and GB is responsible for the enhancement of activity and stability of RuO toward OER. A PEMWE using M-RuIrFeCoNiO catalyst can steadily operate at a large current density of 1 ampere per square centimeter for over 500 hours. This work demonstrates a pathway to design high-performance OER electrocatalysts by integrating the advantages of various components and GB, which breaks the limits of thermodynamic solubility for different metal elements.
设计一种用于酸性析氧反应(OER)的高效催化剂对于操控质子交换膜水电解槽(PEMWE)制氢至关重要。在此,我们报道了一种快速、非平衡策略来合成具有大量晶界(GB)的五元高熵钌铱基氧化物(M-RuIrFeCoNiO),其在0.5 M HSO中对于OER在10毫安每平方厘米时表现出189毫伏的低过电位。微观结构分析、密度泛函计算以及同位素标记的差分电化学质谱测量共同表明,外来金属元素与晶界的整合是RuO对OER活性和稳定性增强的原因。使用M-RuIrFeCoNiO催化剂的PEMWE能够在1安培每平方厘米的大电流密度下稳定运行超过500小时。这项工作展示了一条通过整合各种组分和晶界的优势来设计高性能OER电催化剂的途径,这打破了不同金属元素的热力学溶解度限制。