Corrosion-Induced Cl-Doped Ultrathin Graphdiyne toward Electrocatalytic Nitrogen Reduction at Ambient Conditions

作者：Haiyuan Zou, Weifeng Rong, Baihua Long, Yongfei Ji, Lele Duan · 发表于：ACS Catalysis · 年份：2019 · DOI：10.1021/acscatal.9b02794 · 被引用次数：128 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Advanced Photocatalysis Techniques、Caching and Content Delivery

Electrochemical nitrogen fixation under ambient conditions is an attractive prospect to produce ammonia, yet the process still suffers from the sluggish kinetics and is extremely sensitive to the structures of catalysts. Metal-free materials with tunable structures and electronic properties represent as alternative catalysts for electroreduction of N 2 . Here, we develop a corrosion engineering strategy that enables the heteroatom doping and etching of host graphdiyne (GDY) simultaneously, leading to the consequent Cl-doped ultrathin GDY (Cl-GDY) catalyst to realize effective N 2 electroreduction. The as-synthesized Cl-GDY can afford a relatively high NH 3 yield rate of 10.7 μg h –1 cm –2 associated with a Faradaic efficiency of 8.7% at −0.45 and −0.4 V versus the reversible hydrogen electrode, respectively. This has been the first report so far that the halogen-doped nonmetallic GDY efficiently drives the N 2 reduction reaction, and it dramatically broadens the scope of metal-free catalysts for artificial nitrogen fixation.