Yang Mengya, Jiao Long, Dong Huilong, Zhou Liujiang, Teng Changqing, Yan Dongming, Ye Tian-Nan, Chen Xiaoxin, Liu Yi, Jiang Hai-Long
Institute for Composites Science Innovation (InCSI), School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China.
Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China.
Sci Bull (Beijing). 2021 Feb 15;66(3):257-264. doi: 10.1016/j.scib.2020.06.036. Epub 2020 Jun 26.
The rational design and construction of inexpensive and highly active electrocatalysts for hydrogen evolution reaction (HER) is of great importance for water splitting. Herein, we develop a facile approach for preparation of porous carbon-confined Ru-doped Cu nanoparticles (denoted as Ru-Cu@C) by direct pyrolysis of the Ru-exchanged Cu-BTC metal-organic framework. When served as the electrocatalyst for HER, strikingly, the obtained Ru-Cu@C catalyst exhibits an ultralow overpotential (only 20 mV at 10 mA cm) with a small Tafel slope of 37 mV dec in alkaline electrolyte. The excellent performance is comparable or even superior to that of commercial Pt/C catalyst. Density functional theory (DFT) calculations confirm that introducing Ru atoms into Cu nanocrystals can significantly alter the desorption of H to achieve a close-to-zero hydrogen adsorption energy and thereby boost the HER process. This strategy gives a fresh impetus to explore low-cost and high-performance catalysts for HER in alkaline media.
设计并构建用于析氢反应(HER)的廉价且高活性的电催化剂对于水分解至关重要。在此,我们开发了一种简便的方法,通过对Ru交换的Cu-BTC金属有机框架进行直接热解来制备多孔碳限制的Ru掺杂Cu纳米颗粒(表示为Ru-Cu@C)。令人惊讶的是,当用作HER的电催化剂时,所获得的Ru-Cu@C催化剂在碱性电解质中表现出超低的过电位(在10 mA cm时仅为20 mV),塔菲尔斜率小至37 mV dec。其优异的性能与商业Pt/C催化剂相当甚至更优。密度泛函理论(DFT)计算证实,将Ru原子引入Cu纳米晶体中可以显著改变H的解吸,从而实现接近零的氢吸附能,进而促进HER过程。该策略为探索碱性介质中用于HER的低成本高性能催化剂提供了新的动力。