Wang Maoyu, Muhich Brian A, He Zizhou, Yang Zhenzhen, Yang Dongqi, Lucero Marcos, Nguyen Hoan Kim Khai, Sterbinsky George E, Árnadóttir Líney, Zhou Hua, Fei Ling, Feng Zhenxing
School of Chemical, Biological and Environmental Engineering, Oregon State University, Corvallis, OR 97331, United States.
X-ray Science Division, Argonne National Laboratory, Lemont, IL, 60439, United States.
ChemSusChem. 2024 Sep 23;17(18):e202400332. doi: 10.1002/cssc.202400332. Epub 2024 Jun 7.
High-efficiency and low-cost catalysts for oxygen evolution reaction (OER) are critical for electrochemical water splitting to generate hydrogen, which is a clean fuel for sustainable energy conversion and storage. Among the emerging OER catalysts, transition metal dichalcogenides have exhibited superior activity compared to commercial standards such as RuO, but inferior stability due to uncontrolled restructuring with OER. In this study, we create bimetallic sulfide catalysts by adapting the atomic ratio of Ni and Co in CoNiS electrocatalysts to investigate the intricate restructuring processes. Surface-sensitive X-ray photoelectron spectroscopy and bulk-sensitive X-ray absorption spectroscopy confirmed the favorable restructuring of transition metal sulfide material following OER processes. Our results indicate that a small amount of Ni substitution can reshape the Co local electronic structure, which regulates the restructuring process to optimize the balance between OER activity and stability. This work represents a significant advancement in the development of efficient and noble metal-free OER electrocatalysts through a doping-regulated restructuring approach.
用于析氧反应（OER）的高效低成本催化剂对于电化学水分解制氢至关重要，氢是可持续能源转换和存储的清洁燃料。在新兴的OER催化剂中，过渡金属二硫属化物与RuO等商业标准相比表现出优异的活性，但由于在OER过程中不受控制的结构重组，其稳定性较差。在本研究中，我们通过调整CoNiS电催化剂中Ni和Co的原子比来制备双金属硫化物催化剂，以研究复杂的结构重组过程。表面敏感的X射线光电子能谱和体敏感的X射线吸收光谱证实了过渡金属硫化物材料在OER过程后有利的结构重组。我们的结果表明，少量的Ni取代可以重塑Co的局部电子结构，从而调节结构重组过程，以优化OER活性和稳定性之间的平衡。这项工作通过掺杂调节的结构重组方法，在高效无贵金属OER电催化剂的开发方面取得了重大进展。
