期刊
NANO ENERGY
卷 86, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.nanoen.2021.106099
关键词
Pd cluster catalyst; Adsorption and desorption abilities; Hydrogen substituted graphdiyne; Electrochemical nitrogen reduction
类别
资金
- GRF Scheme [CityU 11305218]
- City University of Hong Kong [9667165]
The high electron density of acetylene linkages in hydrogen substituted graphdiyne (HsGDY) can regulate nitrogen adsorption and NH3 desorption on active Pd sites, leading to impressive electrocatalytic NRR performance. The optimized Pd/HsGDY shows ultrahigh Faraday efficiency and NH3 yield, favoring a selectively facilitated electrosynthesis of NH3.
Precious metal Pd has the intrinsic superiority in adsorbing N2 molecule and wrecking the high cleavage barrier of the N equivalent to N bond, however, its over-strong adsorption ability is unfavorable to the desorption of the produced NH3 during the electrochemical N2 reduction (NRR), which weighs heavily against the NH3 productivity. Here we demonstrate that the high electron-density of acetylene linkages of hydrogen substituted graphdiyne can regulate the nitrogen adsorption and NH3 desorption on the active Pd sites (Pd/HsGDY), resulting in impressive electrocatalytic NRR performance. The optimized Pd/HsGDY features an ultrahigh Faraday efficiency of 44.45% and an NH3 yield of 115.93 mg g-1 h-1 (or 11.59 mu g cm-2 h-1). Density functional theory calculations reveal that the acetylene linkages in HsGDY can tune the d band center of active Pd atoms by downward shifting it from the Fermi level. This favors the hydrogenation of nitrogen on HsGDY-tuned Pd sites and benefits the desorption of produced NH3 from the catalyst surface to recover active sites induced by heat dissipation during the exothermic hydrogenation processes, resulting in a selectively facilitated electrosynthesis of NH3.
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