TY - JOUR
T1 - Carbon vacancies and hydroxyls in graphitic carbon nitride
T2 - Promoted photocatalytic NO removal activity and mechanism
AU - Gu, Zhanyong
AU - Cui, Zhitao
AU - Wang, Zijing
AU - Qin, Ken Sinkou
AU - Asakura, Yusuke
AU - Hasegawa, Takuya
AU - Tsukuda, Satoshi
AU - Hongo, Kenta
AU - Maezono, Ryo
AU - Yin, Shu
N1 - Funding Information:
This work was partly supported by the JSPS Grant-in-Aid for Scientific Research on Innovative Areas “Mixed anion” (No. 16H06439,19H04692), JSPS Grant-in-Aid for Scientific Research (No. 20H00297 ), the Dynamic Alliance for Open Innovations Bridging Human, Environment and Materials, the Cooperative Research Program of “Network Joint Research Center for Materials and Devices” . The computations in this work have been performed using the facilities of Research Center for Advanced Computing Infrastructure at JAIST. R.M. is grateful for financial supports from FLAGSHIP2020 (project nos. hp190169 and hp190167 at K-computer), from Toyota Motor Corporation, from the Air Force Office of Scientific Research (AFOSR-AOARD/FA2386-17-1-4049; FA2386-19-1-4015). K.H. is grateful for financial supports from FLAGSHIP2020 (project nos. hp180206 and hp180175 at K-computer), KAKENHI grant ( 19K05029 ) and a Grant-in-Aid for Scientific Research on Innovative Areas ( 19H05169 ). We acknowledge Mr. Jiawei Xue from the Osaka University for his helpful discussion Z.G. thanks the China Scholarship Council for providing the scholarship.
Publisher Copyright:
© 2020 Elsevier B.V.
PY - 2020/12/15
Y1 - 2020/12/15
N2 - The carbon vacancies and hydroxyls co-modified CN (CH[sbnd]CN) was successfully prepared using a green hydrothermal method. During the hydrothermal process, the water played an important role in etching the unstable partial of bulk CN to introduce carbon vacancies and hydroxyls into the CH[sbnd]CN nanosheets. The carbon vacancies and hydroxyls co-modified CH[sbnd]CN displayed 2.2 times higher photocatalytic NO removal performance than that of pristine CN. Detailed experimental characterizations and density functional theory calculations revealed that the enhanced photocatalytic NO removal performance of CH[sbnd]CN nanosheet was largely ascribed to synergistic effects of carbon vacancies and hydroxyls. The carbon vacancies could narrow the bandgap of modified CH[sbnd]CN nanosheet to improve the light-absorbing capability; the hydroxyls enabled to form stable covalent bonds acted as electron transport channels to facilitate the charge carrier separation. This study may provide new insights into vacancies engineering for enhancing the photocatalytic activity of CN-based photocatalysts.
AB - The carbon vacancies and hydroxyls co-modified CN (CH[sbnd]CN) was successfully prepared using a green hydrothermal method. During the hydrothermal process, the water played an important role in etching the unstable partial of bulk CN to introduce carbon vacancies and hydroxyls into the CH[sbnd]CN nanosheets. The carbon vacancies and hydroxyls co-modified CH[sbnd]CN displayed 2.2 times higher photocatalytic NO removal performance than that of pristine CN. Detailed experimental characterizations and density functional theory calculations revealed that the enhanced photocatalytic NO removal performance of CH[sbnd]CN nanosheet was largely ascribed to synergistic effects of carbon vacancies and hydroxyls. The carbon vacancies could narrow the bandgap of modified CH[sbnd]CN nanosheet to improve the light-absorbing capability; the hydroxyls enabled to form stable covalent bonds acted as electron transport channels to facilitate the charge carrier separation. This study may provide new insights into vacancies engineering for enhancing the photocatalytic activity of CN-based photocatalysts.
KW - Carbon vacancies
KW - Graphitic carbon nitride
KW - Hydroxyls
KW - Mechanism
KW - Photocatalytic NO removal
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U2 - 10.1016/j.apcatb.2020.119376
DO - 10.1016/j.apcatb.2020.119376
M3 - Article
AN - SCOPUS:85089198890
SN - 0926-3373
VL - 279
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
M1 - 119376
ER -