Fangren Qian, Dengfeng Cao, Shuangming Chen, Yalong Yuan, Kai Chen, Peter Joseph Chimtali, Hengjie Liu, Wei Jiang, Beibei Sheng, Luocai Yi, Jiabao Huang, Chengsi Hu, Huxu Lei, Xiaojun Wu, Zhenhai Wen, Qingjun Chen, Li Song
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引用次数: 0
摘要
研制耐用的酸性析氧反应催化剂是工业质子交换膜水电解槽的关键。我们通过退火将高熵原子（Co, Ni, Cu, Mn, Sm）加入到RuO2 （RuO2- heae）中，获得了非常高的稳定性（在100 mA cm−2下1500小时）。原位差分电化学质谱分析和operando衰减全反射表面增强红外吸收光谱分析表明，RuO2-HEAE遵循双点氧化路径机制，而不是传统的吸附质演化机制。定量傅里叶变换扩展x射线吸收精细结构拟合和密度泛函理论计算表明，这种机制转变源于RuO2-HEAE的第二配位层中Ru-M距离的延长，从而实现了直接的O-O耦合。这种opm型催化剂在1 A cm−2和50°C下可稳定运行约1500小时，与大多数报道的基于ruo2的催化剂相比，具有优越的耐久性。这项工作为设计高稳定的质子交换膜水电解提供了基础见解。
High-entropy RuO2 catalyst with dual-site oxide path for durable acidic oxygen evolution reaction
Developing durable acidic oxygen evolution reaction catalysts is critical for industrial proton exchange membrane water electrolyzers. We incorporate high-entropy atoms (Co, Ni, Cu, Mn, Sm) into RuO2 (RuO2-HEAE) via annealing, achieving remarkably high stability (>1500 h at 100 mA cm−2). In situ differential electrochemical mass spectrometry and operando Attenuated Total Reflection Surface-Enhanced Infrared Absorption Spectroscopy reveal RuO2-HEAE follows a dual-site oxide path mechanism instead of the conventional adsorbate evolution mechanism. Quantitative Fourier-transformed extended X-ray absorption fine structure fitting and density functional theory calculations show this mechanistic shift stems from an elongated Ru-M distance in second coordination shell of RuO2-HEAE, enabling direct O-O coupling. This OPM-type catalyst delivers ~1500 h of stable operation at 1 A cm−2 and 50 °C, demonstrating superior durability versus most reported RuO2-based catalysts. This work provides fundamental insights for designing highly stable proton exchange membrane water electrolysis.
期刊介绍：
Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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