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Engineering Amorphous Carbon onto Ultrathin g-C3N4 to Suppress Intersystem Crossing for Efficient Photocatalytic H2 Evolution

Journal Article


Abstract


  • Tuning photochemistry conversion efficiency by atomic-level tailoring will unlock great potential for pursuing higher photocatalytic performance for graphitic carbon nitride (g-C3N4). Here, a novel strategy to fabricate amorphous carbon���engineered ultrathin g-C3N4 nanocomposites, endowing the engineered g-C3N4 with a much higher H2 evolution rate, reaching an optimum value as high as 746.95 ��mol h���1 g���1, 15.4 times higher than that of bulk g-C3N4, is described. Interestingly, with the formation of intimate interfaces between amorphous carbon and ultrathin g-C3N4, 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-C3N4 is significantly reduced by the steric-hindrance effect of amorphous carbon grown in situ, and the as-prepared ultrathin g-C3N4 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.

UOW Authors


  •   Zhou, Tengfei (external author)

Publication Date


  • 2018

Citation


  • Luo, X., Wu, Z., Liu, Y., Ding, S., Zheng, Y., Jiang, Q., . . . Hu, J. (2018). Engineering Amorphous Carbon onto Ultrathin g-C3N4 to Suppress Intersystem Crossing for Efficient Photocatalytic H2 Evolution. Advanced Materials Interfaces, 5(19). doi:10.1002/admi.201800859

Scopus Eid


  • 2-s2.0-85051072683

Volume


  • 5

Issue


  • 19

Place Of Publication


Abstract


  • Tuning photochemistry conversion efficiency by atomic-level tailoring will unlock great potential for pursuing higher photocatalytic performance for graphitic carbon nitride (g-C3N4). Here, a novel strategy to fabricate amorphous carbon���engineered ultrathin g-C3N4 nanocomposites, endowing the engineered g-C3N4 with a much higher H2 evolution rate, reaching an optimum value as high as 746.95 ��mol h���1 g���1, 15.4 times higher than that of bulk g-C3N4, is described. Interestingly, with the formation of intimate interfaces between amorphous carbon and ultrathin g-C3N4, 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-C3N4 is significantly reduced by the steric-hindrance effect of amorphous carbon grown in situ, and the as-prepared ultrathin g-C3N4 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.

UOW Authors


  •   Zhou, Tengfei (external author)

Publication Date


  • 2018

Citation


  • Luo, X., Wu, Z., Liu, Y., Ding, S., Zheng, Y., Jiang, Q., . . . Hu, J. (2018). Engineering Amorphous Carbon onto Ultrathin g-C3N4 to Suppress Intersystem Crossing for Efficient Photocatalytic H2 Evolution. Advanced Materials Interfaces, 5(19). doi:10.1002/admi.201800859

Scopus Eid


  • 2-s2.0-85051072683

Volume


  • 5

Issue


  • 19

Place Of Publication