Abstract
We report the development of the C3N4 structure by integrating two different structures: (i) two identical layers as AA-stacked C3N4 and (ii) intercalating one different layer between two identical layers as ABA-stacked C3N4. This in turn endows C3N4 with significantly promoted charge migration, up-shifted conduction-band (CB) level, enhanced CB potential from -0.89 eV (AA-stacked C3N4) to -1.03 eV (ABA-stacked C3N4), broadened band gap as well as enhanced surface area, all of which favor the enhancement of the photocatalytic performance. The optical absorption level exhibited significant enhancement in the visible light region when shifting from AA-stacked C3N4 to ABA-stacked C3N4, where the absorption edge moves from λ = 508.1 → λ = 454.1 nm. This corresponds to the direct optical band gap of 2.44 eV → 2.73 eV, which is well matched with the solar spectrum and the sufficient negative CB potential for H+/H2 reduction. Based on these results, we can conclude that AA-stacked and ABA-stacked C3N4 satisfies all the requirements to be efficient photocatalysts. This study will significantly improve the search efficiency and considerably aid the experimentalists in the exploration of novel photocatalysts.
References
May 15, 1990·Physical Review. B, Condensed Matter·A Y Liu, M L Cohen
Oct 28, 1996·Physical Review Letters·J P PerdewM Ernzerhof
Aug 9, 2003·Physical Review Letters·Faming GaoYongjun Tian
Apr 29, 2004·Journal of the American Chemical Society·Dale R MillerEdward G Gillan
Oct 21, 2004·Angewandte Chemie·My Hang V HuynhRichard Gilardi
Aug 25, 1989·Science·A Y Liu, M L Cohen
Nov 11, 2008·Nature Materials·Xinchen WangMarkus Antonietti
Aug 8, 2009·Physical Review Letters·Fabien Tran, Peter Blaha
Feb 24, 2010·Langmuir : the ACS Journal of Surfaces and Colloids·S C YanZ G Zou
Apr 20, 2010·Journal of the American Chemical Society·Yuanjian ZhangMarkus Antonietti
Aug 5, 2010·Journal of the American Chemical Society·Gang LiuHui-Ming Cheng
May 17, 2012·Chemical Communications : Chem Comm·Guohui DongLizhi Zhang
Nov 8, 2012·Chemical Communications : Chem Comm·Jianghua LiYilin Chen
Feb 22, 2013·Langmuir : the ACS Journal of Surfaces and Colloids·Qiao Liu, Junyan Zhang
May 18, 2013·Scientific Reports·Xingxing LiJinlong Yang
Sep 21, 2013·The Analyst·Li XuHuaming Li
Sep 21, 2013·Journal of Molecular Modeling·Sigismund T A G MelissenLaurent Joubert
Jun 4, 2014·Advanced Materials·Peng ZhouMietek Jaroniec
Sep 16, 2014·Angewandte Chemie·Yun ZhengXinchen Wang
Dec 20, 2014·ACS Applied Materials & Interfaces·Hongwei HuangYihe Zhang
Nov 6, 2015·Chemical Communications : Chem Comm·Shunji XieYe Wang
Aug 27, 2016·ChemSusChem·Zhiming PanXinchen Wang
Jul 22, 2017·Angewandte Chemie·Hongwei HuangYihe Zhang
Sep 2, 2017·Chemistry : a European Journal·Na SunFeng Chen
Sep 6, 2017·Physical Chemistry Chemical Physics : PCCP·A H Reshak