Single atom accelerates ammonia photosynthesis

• 来源期刊: 中国科学:化学（英文版）
• 年，卷（期）: 2018,（9）
• 页码范围: 1187-1196
• 页数: 10页
• 语种: 英文

摘要

Atomically dispersed metal has gained much attention because of the new opportunities they offer in catalysis.However,it is still crucial to understand the mechanism of single-atom catalysis at molecular level for expanding them to other more difficult catalytic reactions,such as ammonia synthesis from nitrogen.In fact,developing ammonia synthesis under ambient conditions to overcome the high energy consumption in well-established Haber-Bosch process has fascinated scientists for many years.Herein,we demonstrate that single Cu atom yields facile valence-electron isolation from the conjugated π electron cloud of p-CN.Electron spin resonance measurements reveal that these isolated valence electrons can be easily excited to generate free electrons under photo-illumination,thus inducing high efficient photo-induced ammonia synthesis under ambient conditions.The NH3 producing rate of copper modified carbon nitride (Cu-CN) reached 186 μmol g-1 h-1 under visible light irradiation with the quantum efficiency achieved 1.01％ at 420 nm monochromatic light.This finding surely offers a model to open up a new vista for the ammonia synthesis at gentle conditions.The introduction of single atom to isolate the valence electron also represents a new paradigm for many other photocatalytic reactions,since the most photoinduced processes have been successfully exploited sharing the same origin.