College of Chemistry and Environmental Engineering, Institute of Low-dimensional Materials Genome Initiative, Shenzhen University, Shenzhen, 518071, China.
School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China.
Angew Chem Int Ed Engl. 2023 Mar 13;62(12):e202300879. doi: 10.1002/anie.202300879. Epub 2023 Feb 14.
Charge redistribution on surface of Ru nanoparticle can significantly affect electrocatalytic HER activity. Herein, a double atomic-tuned RuBi SAA/Bi@OG nanostructure that features RuBi single-atom alloy nanoparticle supported by Bi-O single-site-doped graphene was successfully developed by one-step pyrolysis method. The alloyed Bi single atom and adjacent Bi-O single site in RuBi SAA/Bi@OG can synergistically manipulate electron transfer on Ru surface leading to optimum charge redistribution. Thus, the resulting RuBi SAA/Bi@OG exhibits superior alkaline HER activity. Its mass activity is up to 65000 mA mg at an overpotential of 150 mV, which is 72.2 times as much as that of commercial Pt/C. DFT calculations reveal that the RuBi SAA/Bi@OG possesses the optimum charge redistribution, which is most beneficial to strengthen adsorption of water and weaken hydrogen-adsorption free energy in HER process. This double atomic-tuned strategy on surface charge redistribution of Ru nanoparticle opens a new way to develop highly efficient electrocatalysts.
表面的 Ru 纳米颗粒上的电荷再分配可以显著影响电催化 HER 活性。在此，通过一步热解法成功地开发了一种具有 RuBi 单原子合金纳米颗粒负载于 Bi-O 单原子掺杂石墨烯的双原子调谐 RuBi SAA/Bi@OG 纳米结构。RuBi SAA/Bi@OG 中的合金化 Bi 单原子和相邻的 Bi-O 单原子位点可以协同地操纵 Ru 表面的电子转移，从而实现最佳的电荷再分配。因此，所得到的 RuBi SAA/Bi@OG 表现出优异的碱性 HER 活性。其在 150 mV 过电势下的质量活性高达 65000 mA·mg，是商业 Pt/C 的 72.2 倍。DFT 计算表明，RuBi SAA/Bi@OG 具有最佳的电荷再分配，这最有利于加强对水的吸附并减弱 HER 过程中氢吸附自由能。这种对 Ru 纳米颗粒表面电荷再分配的双原子调谐策略为开发高效电催化剂开辟了新途径。
