Amorphization activated FeB2 porous nanosheets enable efficient electrocatalytic N2 fixation

• 作者: Ke Chu Weicong Gu Qingqing Li Yaping Liu Ye Tian Wuming Liu
• 来源期刊: 能源化学
• 年，卷（期）: 2021,（2）
• 页码范围: 82-89
• 页数: 8页
• 语种: 英文

摘要

Designing active,robust and cost-effective catalysts for the nitrogen reduction reaction (NRR) is of paramount significance for sustainable electrochemical NH3 synthesis.Transition-metal diborides (TMB2) have been recently theoretically predicted to be a new class of potential NRR catalysts,but direct experimental evidence is still lacking.Herein,we present the first experimental demonstration that amorphous FeB2 porous nanosheets (a-FeB2 PNSs) could be a highly efficient NRR catalyst,which exhibited an NH3 yield of 39.8 μg h-1 mg-1 (-0.3 V) and a Faradaic efficiency of 16.7％ (-0.2 V),significantly outperforming their crystalline counterpart and most of existing NRR catalysts.First-principle calculations unveiled that the amorphization could induce the upraised d-band center of a-FeB2 to boost d-2π* coupling between the active Fe site and *N2H intermediate,resulting in enhanced *N2H stabilization and reduced reaction barrier.Out study may facilitate the development and understanding of earth-abundant TMB2-based catalysts for electrocatalytic N2 fixation.