TY - JOUR
T1 - Efficient visible light photocatalysis enabled by the interaction between dual cooperative defect sites
AU - Qi, Rongjie
AU - Yu, Pengfei
AU - Zhang, Jiachen
AU - Guo, Weiqi
AU - He, Yaoyu
AU - Hojo, Hajime
AU - Einaga, Hisahiro
AU - Zhang, Qun
AU - Liu, Xiaosong
AU - Jiang, Zhi
AU - Shangguan, Wenfeng
N1 - Funding Information:
This work was supported by the funding from the National Natural Science Foundation of China ( 21872093 , 21573211 , 21633007 ), the National Key Research and Development Program of China ( 2018YFB1502001 , 2016YFA0200602 , 2018YFA0208702 ), the Shanghai Committee of Science and Technology ( 19ZR1467000 ), Center of Hydrogen Science, Shanghai Jiao Tong University , China, and the Anhui Initiative in Quantum Information Technologies ( AHY090200 ). The authors thank the staffs at BL20A1 of TLS, BL02B of SSRF and BL12B-α of NSRL for sXAS measurements and discussion, and staffs at BL14W of SSRF for hXAS measurements.
Funding Information:
This work was supported by the funding from the National Natural Science Foundation of China (21872093, 21573211, 21633007), the National Key Research and Development Program of China (2018YFB1502001, 2016YFA0200602, 2018YFA0208702), the Shanghai Committee of Science and Technology (19ZR1467000), Center of Hydrogen Science, Shanghai Jiao Tong University, China, and the Anhui Initiative in Quantum Information Technologies (AHY090200). The authors thank the staffs at BL20A1 of TLS, BL02B of SSRF and BL12B-α of NSRL for sXAS measurements and discussion, and staffs at BL14W of SSRF for hXAS measurements.
Publisher Copyright:
© 2020 Elsevier B.V.
PY - 2020/1/1
Y1 - 2020/1/1
N2 - Modifying photocatalyst with defects offers effective pathway to tailor light absorption properties, but may result in more sluggish kinetics. Therefore, enhanced light absorption often could not guarantee increased activity. Here, we report a dual defect strategy to extend light absorption with minimal loss in charge dynamics. Fine-tuned amount of dual defect, i.e., nitrogen defects and single-site copper, is simultaneously generated in polymer carbon nitride(PCN) through in-situ vapor diffusion method. Surface nitrogen defect extends the light absorption to long-wavelength via sub-band absorption. The interaction between nitrogen and single-site copper at certain concentration retains the charge dynamics by making the photogenerated electrons more delocalized through the newly-formed copper-nitrogen bonds. As a result, champion modified PCN exhibits robust hydrogen production activity, roughly 4.5-fold greater than the pristine counterpart in both visible and full light ranges. More intriguingly, this synergism provides PCN with efficient visible light activity even in faint tailing optical absorption region(>450 nm).
AB - Modifying photocatalyst with defects offers effective pathway to tailor light absorption properties, but may result in more sluggish kinetics. Therefore, enhanced light absorption often could not guarantee increased activity. Here, we report a dual defect strategy to extend light absorption with minimal loss in charge dynamics. Fine-tuned amount of dual defect, i.e., nitrogen defects and single-site copper, is simultaneously generated in polymer carbon nitride(PCN) through in-situ vapor diffusion method. Surface nitrogen defect extends the light absorption to long-wavelength via sub-band absorption. The interaction between nitrogen and single-site copper at certain concentration retains the charge dynamics by making the photogenerated electrons more delocalized through the newly-formed copper-nitrogen bonds. As a result, champion modified PCN exhibits robust hydrogen production activity, roughly 4.5-fold greater than the pristine counterpart in both visible and full light ranges. More intriguingly, this synergism provides PCN with efficient visible light activity even in faint tailing optical absorption region(>450 nm).
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U2 - 10.1016/j.apcatb.2020.119099
DO - 10.1016/j.apcatb.2020.119099
M3 - Article
AN - SCOPUS:85084445130
VL - 274
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
SN - 0926-3373
M1 - 119099
ER -