Single-Atom Pd–N3 Sites on Carbon-Deficient g-C3N4 for Photocatalytic H2 Evolution

Guimei Liu; Haiqin Lv; Yubin Zeng; Mingzhe Yuan; Qingguo Meng; Yuanhao Wang; Chuanyi Wang

doi:10.1007/s12209-020-00279-z

Transactions of Tianjin University ›› 2021, Vol. 27 ›› Issue (2) : 139 -146. DOI: 10.1007/s12209-020-00279-z

Research Article

Single-Atom Pd–N₃ Sites on Carbon-Deficient g-C₃N₄ for Photocatalytic H₂ Evolution

Guimei Liu ¹^,²
, Haiqin Lv ¹^,³
, Yubin Zeng ²^,^c
, Mingzhe Yuan ¹^,³^,^d
, Qingguo Meng ¹^,³
, Yuanhao Wang ⁴
, Chuanyi Wang ¹^,²^,³^,^g

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¹ Shenyang Institute of Automation, Guangzhou, Chinese Academy of Science, 511400, Guangzhou, China

² Hubei Key Laboratory of Accoutrement Technique in Fluid Machinery and Power Engineering, 430072, Hubei, China

³ Guangdong Engineering Technology Research Center for Environmental Purification and Functional Materials, 511400, Guangzhou, China

⁴ SUSTech Engineering Innovation Center, School of Environmental Science and Engineering, Southern University of Science and Technology, 518000, Shenzhen, China

^c zengyubin@whu.edu.c

^d mzyuan@sia.cn

^g wangchuanyi@sust.edu.cn

Yubin Zeng obtained her PhD degree from Department of Environmental Science and Engineering, Huazhong University of Science and Technology, China, in 2007. She worked in Korea (Department of Civil and Environmental Engineering, Seoul National University) as a postdoctor fellowship with Prof. Junboum Park from 2008 to 2009. Currently, she is an associate professor at Wuhan University, China. Her research interest mainly focuses on environmental photocatalysis.

Mingzhe Yuan is a researcher of Shenyang Institute of Automation, Guangzhou, Chinese Academy of Science (CAS). He obtained his PhD degree from Shenyang Institute of Automation of CAS in 2006. Currently, his research interest covers functional materials and environmental photocatalysis. By far, he has published over 100 papers in peer-reviewed journals.

Chuanyi Wang Fellow of Royal Society of Chemistry, is a distinguished professor of Chinese Academy of Sciences (CAS) and an adjunct professor at Wuhan University. He obtained his PhD degree from Institute of Photographic Chemistry of CAS in 1998, worked in Germany (Institute for Solar Energy Research in Hannover and Free University Berlin) as an Alexander von Humboldt research fellow with Prof. Detlef Bahnemann from 1999 to 2000, and then worked in USA (Tufts University and Missouri University-Kansas City) as a research faculty from 2000 to 2010. Currently, Dr. Wang also serves as an associate editor of Environmental Chemistry Letters and an editorial board member for number of international journals. His research interest covers eco-materials and environmental photocatalysis. By far, he has published over 200 papers in peer-reviewed journals.

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Abstract

Photocatalytic hydrogen evolution is an attractive field for future environment-friendly energy. However, fast recombination of photogenerated charges severely inhibits hydrogen efficiency. Single-atom cocatalysts such as Pt have emerged as an effective method to enhance the photocatalytic activity by introduction of active sites and boosting charge separation with low-coordination environment. Herein, we demonstrated a new strategy to develop a highly active Pd single atom in carbon-deficient g-C₃N₄ with a unique coordination. The single-atom Pd–N₃ sites constructed by oil bath heating and photoreduction process were confirmed by HADDF-STEM and XPS measurements. Introduction of single-atom Pd greatly improved the separation and transportation of charge carriers, leading to a longer lifespan for consequent reactions. The obtained single-atom Pd loaded on the carbon-deficient g–C₃N₄ showed excellent photocatalytic activity in hydrogen production with about 24 and 4 times higher activity than that of g–C₃N₄ and nano-sized Pd on the same support, respectively. This work provides a new insight on the design of single-atom catalyst.

Keywords

Single-atom / Pd / g-C₃N₄ / Active sites / Hydrogen / Photocatalytic

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Guimei Liu, Haiqin Lv, Yubin Zeng, Mingzhe Yuan, Qingguo Meng, Yuanhao Wang, Chuanyi Wang. Single-Atom Pd–N₃ Sites on Carbon-Deficient g-C₃N₄ for Photocatalytic H₂ Evolution. Transactions of Tianjin University, 2021, 27(2): 139-146 DOI:10.1007/s12209-020-00279-z

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