Atomic nickel on graphitic carbon nitride as a visible light-driven hydrogen production photocatalyst studied by x-ray spectromicroscopy
學年 111
學期 2
出版（發表）日期 2023-03-29
作品名稱 Atomic nickel on graphitic carbon nitride as a visible light-driven hydrogen production photocatalyst studied by x-ray spectromicroscopy
作品名稱（其他語言）
著者 Yu Cheng Huang, Yanrui Li, K. Thanigai Arul, Takuji Ohigashi, Ta Thi Thuy Nga, Ying Rui Lu, Chi Liang Chen, Jeng Lung Chen, Shaohua Shen, Way Faung Pong, Chung Li Dong, Wu Ching Chou
單位
出版者
著錄名稱、卷期、頁數 ACS Sustainable Chemistry & Engineering 11(14), 5390-5399
摘要 The photocatalytic production of solar hydrogen through water splitting by graphitic carbon nitride (g-C3N4) has gained substantial interest due to its advantageous characteristics, such as eco-friendliness, wealth on the earth, favorable bandgap, and easy preparation. Nevertheless, the performance for photocatalytic overall water splitting has been significantly restricted owing to the rapid recombination of charge carriers and slow catalytic kinetics. This investigation demonstrates the utilization of a single-atom Ni-terminating agent to coordinate with the heptazine moieties of g-C3N4, resulting in the formation of a new electronic orbital. g-C3N4 with single-atom Ni-termination can achieve highly efficient photocatalytic overall water splitting into H2 and H2O2 upon visible light irradiation, without requiring the use of any additional cocatalysts. The underlying cause of the enhanced photocatalytic performance of single-atom Ni-incorporated g-C3N4 in hydrogen evolution reaction is identified using synchrotron X-ray spectroscopy and microscopy. The X-ray spectro-microscopic results discover that the new hybrid orbital that is critical for optimizing photocatalysis is associated with carbon defects. The atomic and electronic structures and the band gap of g-C3N4 are adjusted by the new hybrid orbital. Moreover, it synergistically enhances visible light absorption, thereby promoting the separation and transfer of photogenerated charge carriers. The single-atom Ni and the adjacent C atom are recognized as the active sites for water oxidation and reduction, respectively, supporting the efficient photocatalytic splitting of water via a two-electron transfer pathway. This study demonstrated a promising material design for promoting photocatalytic activity in solar energy conversion applications.
關鍵字 Single-Atom Catalysts; X-Ray Absorption Spectroscopy (XAS); Scanning Transmission X-Ray Microscopy (STXM); Defect; Local Atomic Structure
語言 en_US
ISSN 2168-0485
期刊性質 國外
收錄於 SCI
產學合作
通訊作者
審稿制度 否
國別 USA
公開徵稿
出版型式 ,電子版
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機構典藏連結 ( http://tkuir.lib.tku.edu.tw:8080/dspace/handle/987654321/125724 )