摘要
相工程被认为是调节催化剂电子结构和催化活性的有效方法。非晶材料的无序构型允许表面电子结构的灵活重整,显示出其作为析氢反应(HER)催化剂的吸引力。在此,我们设计并开发了一种具有无序Ru-O构型的非晶催化剂(a-RuO_(2))。结合先进的电镜技术和详细的电化学测试,建立了Ru-O有序性与HER性能的构效关系。具体来说,无序的Ru-O配位显著增强了酸性和碱性HER中的催化活性,最终使经济性更高的a-RuO_(2)催化性能接近商业Pt/C。此外,在10 mA·cm^(-2)下进行10 h电流-时间(i-t)测试后,a-RuO_(2)表现出极好的稳定性。进一步的理论模拟显示a-RuO_(2)较低的d带中心和优化的电子输运调制了活性位点对中间反应物的吸附强度,促进了HER动力学。这项工作为通过相工程探索高活性HER催化剂提供了新的观点。
Phase engineering is considered as an effective method for modulating the electronic structure and catalytic activity of catalysts. The disordered conformation of amorphous materials allows flexible reforming of the surface electronic structure,showing their attractiveness as catalysts for hydrogen evolution reaction(HER). Herein, we designed and developed an amorphous ruthenium dioxide(a-RuO_(2)) catalyst with a disordered Ru-O configuration. The conformational relationship between Ru-O ordering and HER performance is established by combining advanced electron microscopic techniques with detailed electrochemical tests.Specifically, the disordered Ru-O coordination significantly enhanced the HER catalytic activity in both acidic and alkaline media,ultimately leading to HER performance of a-RuO_(2)approaching that of commercial Pt/C with higher economics. In addition, a-RuO_(2)exhibited excellent stability after 10 h current-time(i-t) testing at 10 mA·cm^(-2). Further theoretical simulations showed that the lowered d-band center and optimized electron transport of a-RuO_(2)modulated the adsorption strength of the active site to the intermediate reactants, promoting HER kinetics. This work provides a new perspective for exploring highly active HER catalysts through phase engineering.
作者
孙雪
宋亚杰
李仁龙
王家钧
Xue Sun;Ya-Jie Song;Ren-Long Li;Jia-Jun Wang(MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage,Harbin Institute of Technology,Harbin,150001,China;Chongqing Research Institute of HIT,Chongqing 401135,P.R.China.)
出处
《电化学》
CAS
CSCD
北大核心
2022年第10期79-89,共11页
Journal of Electrochemistry
基金
supported by National Natural Science Foundation of China (No. 22075063, No. U1932205, No. 22102041)
Fundamental Research Funds for the Central Universities (FRFCU5710092520)
Chinesisch-Deutschen Zentrum für Wissenschaftsf?rderung (M0281)
Natural Science Funds of Heilongjiang Province (No. ZD2019B001)
Heilongjiang Touyan Team (HITTY-20190033)
the Natural Science Fund for Distinguished Young Scholars of Chongqing ( cstc2021jcyj-jqX0003)
“Young Scientist Studio” and Chongqing Research Institute of HIT。
关键词
相工程
电化学析氢
非晶催化剂
电子结构
phase engineering
hydrogen evolution reaction
amorphous catalyst
electronic structure
