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Potassium‐Ion‐Assisted Regeneration of Active Cyano Groups in Carbon Nitride Nanoribbons: Visible‐Light‐Driven Photocatalytic Nitrogen Reduction
Author(s) -
Wang Weikang,
Zhang Haimin,
Zhang Shengbo,
Liu Yanyan,
Wang Guozhong,
Sun Chenghua,
Zhao Huijun
Publication year - 2019
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201908640
Subject(s) - photocatalysis , carbon nitride , visible spectrum , nitrogen , catalysis , materials science , chemistry , potassium , photochemistry , chemical engineering , organic chemistry , optoelectronics , engineering
As a metal‐free nitrogen reduction reaction (NRR) photocatalyst, g‐C 3 N 4 is available from a scalable synthesis at low cost. Importantly, it can be readily functionalized to enhance photocatalytic activities. However, the use of g‐C 3 N 4 ‐based photocatalysts for the NRR has been questioned because of the elusive mechanism and the involvement of N defects. This work reports the synthesis of a g‐C 3 N 4 photocatalyst modified with cyano groups and intercalated K + ( m CNN), possessing extended visible‐light harvesting capacity and superior photocatalytic NRR activity (NH 3 yield: 3.42 mmol g −1 h −1 ). Experimental and theoretical studies suggest that the ‐C≡N in m CNN can be regenerated through a pathway analogous to Mars van Krevelen process with the aid of the intercalated K + . The results confirm that the regeneration of the cyano group not only enhances photocatalytic activity and sustains the catalytic cycle, but also stabilizes the photocatalyst.