Engineering Amorphous Carbon onto Ultrathin g‐C3N4 to Suppress Intersystem Crossing for Efficient Photocatalytic H2 Evolution. Issue 19 (30th July 2018)

• Record Type: Journal Article
• Authors: Luo, Xiaoxu; Wu, Zuozuo; Liu, Ye; Ding, Shuoping; Zheng, Yang; Jiang, Qingqing; Zhou, Tengfei; Hu, Juncheng
• Is Part Of: Advanced materials interfaces. Volume 5:Issue 19(2018)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2018-07-30
• Subjects: amorphous carbon -- steric‐hindrance effect -- suppress the intersystem crossing -- ultrathin g‐C3N4; Materials science -- Periodicals; 620.11
• DOI: 10.1002/admi.201800859
• Languages: English
• ISSNs: 2196-7350

Abstract

Abstract: Tuning photochemistry conversion efficiency by atomic‐level tailoring will unlock great potential for pursuing higher photocatalytic performance for graphitic carbon nitride (g‐C3 N4 ). Here, a novel strategy to fabricate amorphous carbon–engineered ultrathin g‐C3 N4 nanocomposites, endowing the engineered g‐C3 N4 with a much higher H2 evolution rate, reaching an optimum value as high as 746.95 µmol h −1 g −1, 15.4 times higher than that of bulk g‐C3 N4, is described. Interestingly, with the formation of intimate interfaces between amorphous carbon and ultrathin g‐C3 N4, the interfacial charge transfer is boosted significantly and the recombination rate of photogenerated electrons and holes could be highly reduced, thus leading to a higher quantum yield. Moreover, the thickness of the g‐C3 N4 is significantly reduced by the steric‐hindrance effect of amorphous carbon grown in situ, and the as‐prepared ultrathin g‐C3 N4 shows a suppressed intersystem crossing rate in the photocatalytic H2 evolution process, thus leading to a lower triplet exciton concentration in the energy conversion process, and also faint triplet–triplet annihilation. It is believed that the present work identifies a new pathway to understanding the role of carbon in nanostructure construction, and will be of broad interest in research on engineering metal‐free carbon‐based catalysts and on solar conversion systems. Abstract : The thickness of the g‐C3 N4 is significantly reduced by the steric‐hindrance effect of in situ grown amorphous carbon. The ultrathin g‐C3 N4 shows suppressed intersystem crossing rate in photocatalytic H2 evolution process, thus leading to a much higher H2 evolution rate, 15.4 times higher than that of bulk g‐C3 N4 .