Jiao Jiqing, Zhang Nan-Nan, Zhang Chao, Sun Ning, Pan Yuan, Chen Chen, Li Jun, Tan Meijie, Cui Ruixue, Shi Zhaolin, Zhang Jiangwei, Xiao Hai, Lu Tongbu
MOE International Joint Laboratory of Materials Microstructure, Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, China.
Haihe Laboratory of Sustainable Chemical Transformations, Tianjin, 300192, China.
Adv Sci (Weinh). 2022 May;9(15):e2200010. doi: 10.1002/advs.202200010. Epub 2022 Mar 25.
For heterogeneous catalysts, the active sites exposed on the surface have been investigated intensively, yet the effect of the subsurface-underlying atoms is much less scrutinized. Here, a surface-engineering strategy to dope Ru into the subsurface/surface of Co matrix is reported, which alters the electronic structure and lattice strain of the catalyst surface. Using hydrogen evolution (HER) as a model reaction, it is found that the subsurface doping Ru can optimize the hydrogen adsorption energy and improve the catalytic performance, with overpotentials of 28 and 45 mV at 10 mA cm in alkaline and acidic media, respectively, and in particular, 28 mV in neutral electrolyte. The experimental results and theoretical calculations indicate that the subsurface/surface doping Ru improves the HER efficiency in terms of both thermodynamics and kinetics. The approach here stands as an effective strategy for catalyst design via subsurface engineering at the atomic level.
对于多相催化剂，人们已对其表面暴露的活性位点进行了深入研究，然而，对其表面下原子的影响却很少受到关注。在此，报道了一种将钌掺杂到钴基体表面下/表面的表面工程策略，该策略改变了催化剂表面的电子结构和晶格应变。以析氢反应（HER）作为模型反应，发现表面下掺杂钌可以优化氢吸附能并提高催化性能，在碱性和酸性介质中，在10 mA cm时的过电位分别为28和45 mV，特别是在中性电解质中为28 mV。实验结果和理论计算表明，表面下/表面掺杂钌在热力学和动力学方面均提高了析氢反应效率。本文所述方法是一种通过原子水平的表面下工程进行催化剂设计的有效策略。
