The development of low-cost, efficient, and high atomic economy electrocatalysts for hydrogen evolution reaction(HER) in the entire p H range for sustainable hydrogen production is of great importance but still challe...The development of low-cost, efficient, and high atomic economy electrocatalysts for hydrogen evolution reaction(HER) in the entire p H range for sustainable hydrogen production is of great importance but still challenging. Herein, we synthesize a highly dispersed N-doped carbon frames(NCFs) anchored with Co single atoms(SAs) and Co nanoparticles(NPs) catalyst by a doping-adsorption-pyrolysis strategy for electrocatalytic hydrogen evolution. The Co SAs-Co NPs/NCFs catalyst exhibits an excellent HER activity with small overpotential, low Tafel slope, high turnover frequency as well as remarkable stability. It also exhibits a superior HER performance in the entire p H range. Combining with experimental and theoretical calculation, we find that Co SAs with Co-N_(3) coordination structure and Co NPs have a strong interaction for promoting synergistic HER electrocatalytic process. The H_(2)O molecule is easily activated and dissociated on Co NPs, while the generated H^(*) is easily adsorbed on Co SAs for HER, which makes the Co SAs-Co NPs/NCFs catalyst exhibit more suitable H adsorption strength and more conducive to the activation and dissociation of H_(2)O molecules. This work not only proposes a novel idea for constructing coupling catalyst with atomic-level precision, but also provides strong reference for the development of high-efficiency HER electrocatalysts for practical application.展开更多
基金supported by the Taishan Scholars Program of Shandong Province(tsqn201909065)the Shandong Provincial Natural Science Foundation(ZR2020QB174)+3 种基金the Petro China Innovation Foundation(2019D-5007-0401)the National Natural Science Foundation of China(21776315,22108306)the Fundamental Research Funds for the Central Universities(19CX02008A,19CX05001A)the Postgraduate Innovation Fund of China University of Petroleum(East China)(YCX2020037)。
文摘The development of low-cost, efficient, and high atomic economy electrocatalysts for hydrogen evolution reaction(HER) in the entire p H range for sustainable hydrogen production is of great importance but still challenging. Herein, we synthesize a highly dispersed N-doped carbon frames(NCFs) anchored with Co single atoms(SAs) and Co nanoparticles(NPs) catalyst by a doping-adsorption-pyrolysis strategy for electrocatalytic hydrogen evolution. The Co SAs-Co NPs/NCFs catalyst exhibits an excellent HER activity with small overpotential, low Tafel slope, high turnover frequency as well as remarkable stability. It also exhibits a superior HER performance in the entire p H range. Combining with experimental and theoretical calculation, we find that Co SAs with Co-N_(3) coordination structure and Co NPs have a strong interaction for promoting synergistic HER electrocatalytic process. The H_(2)O molecule is easily activated and dissociated on Co NPs, while the generated H^(*) is easily adsorbed on Co SAs for HER, which makes the Co SAs-Co NPs/NCFs catalyst exhibit more suitable H adsorption strength and more conducive to the activation and dissociation of H_(2)O molecules. This work not only proposes a novel idea for constructing coupling catalyst with atomic-level precision, but also provides strong reference for the development of high-efficiency HER electrocatalysts for practical application.
