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Incorporating p ‐Phenylene as an Electron‐Donating Group into Graphitic Carbon Nitride for Efficient Charge Separation
Author(s) -
Gao Honglin,
Guo Yong,
Yu Zhiwu,
Zhao Meiming,
Hou Yang,
Zhu Zhongqi,
Yan Shicheng,
Liu Qingju,
Zou Zhigang
Publication year - 2019
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.201901239
Subject(s) - graphitic carbon nitride , photocurrent , carbon nitride , phenylene , materials science , nitride , poly(p phenylene) , photocatalysis , condensation polymer , photochemistry , carbon fibers , chemistry , chemical engineering , nanotechnology , catalysis , organic chemistry , composite number , polymer , optoelectronics , composite material , layer (electronics) , engineering
Low charge‐separation transport efficiency resulting from structural defects largely limits photocatalytic hydrogen production over polymeric graphitic carbon nitride (PCN) photocatalyst. Herein, an electron‐donating group, namely p ‐phenylene, is incorporated into PCN by a polycondensation reaction between carbon nitride and p ‐phenylenediamine (or p ‐benzoquinone) to repair the structural defects. The p ‐phenylene‐modified PCN exhibits an almost fivefold increase in H 2 evolution, a threefold increase in photocurrent density, and higher nonradiative rate (0.285 ns −1 ). Spectroscopic studies confirm that p ‐phenylene tends to bridge the heptazine‐based oligomers through a polycondensation reaction. Theoretical calculations reveal that anchoring of the heptazine units by p ‐phenylene induces localization of h + and e − on the phenylene and melem moieties, respectively, which effectively separates the charge carriers. This strategy provides an opportunity to overcome structural defects in carbon nitride for efficient photocatalytic solar energy conversion.