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Defect Engineering Metal‐Free Polymeric Carbon Nitride Electrocatalyst for Effective Nitrogen Fixation under Ambient Conditions
Author(s) -
Lv Chade,
Qian Yumin,
Yan Chunshuang,
Ding Yu,
Liu Yuanyue,
Chen Gang,
Yu Guihua
Publication year - 2018
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201806386
Subject(s) - electrocatalyst , catalysis , faraday efficiency , nitride , carbon nitride , electron transfer , nitrogen , adsorption , chemistry , graphitic carbon nitride , redox , metal , carbon fibers , nitrogen fixation , electrochemistry , inorganic chemistry , materials science , chemical engineering , nanotechnology , photochemistry , electrode , organic chemistry , photocatalysis , composite number , layer (electronics) , composite material , engineering
Electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions provides an intriguing picture for the conversion of N 2 into NH 3 . However, electrocatalytic NRR mainly relies on metal‐based catalysts, and it remains a grand challenge in enabling effective N 2 activation on metal‐free catalysts. Here we report a defect engineering strategy to realize effective NRR performance (NH 3 yield: 8.09 μg h −1 mg −1 cat. , Faradaic efficiency: 11.59 %) on metal‐free polymeric carbon nitride (PCN) catalyst. Illustrated by density functional theory calculations, dinitrogen molecule can be chemisorbed on as‐engineered nitrogen vacancies of PCN through constructing a dinuclear end‐on bound structure for spatial electron transfer. Furthermore, the N−N bond length of adsorbed N 2 increases dramatically, which corresponds to “strong activation” system to reduce N 2 into NH 3 . This work also highlights the significance of defect engineering for improving electrocatalysts with weak N 2 adsorption and activation ability.