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Triethanolamine-mediated photodeposition formation of amorphous Ni-P alloy for improved H2-evolution activity of g-C3N4

非晶镍磷合金助剂的三乙醇胺调控光沉积制备及 其增强氮化碳光催化产氢活性

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Abstract

Developing efficient, stable, and low-cost novel electron-cocatalysts is crucial for photocatalytic hydrogen evolution reaction. Herein, amorphous Ni-P alloy particles were successfully modified onto g-C3N4 to construct the Ni-P/ g-C3N4 photocatalyst through a simple and green triethanol-amine (TEOA)-mediated photodeposition method. It was found that the TEOA could serve as an excellent complexing agent to coordinate with Ni2+ to form [Ni(TEOA)]2+ complex, which can promote the rapid and effective deposition of amorphous Ni-P alloy on the g-C3N4 surface. Photocatalytic tests suggest that the hydrogen-evolution performance of g-C3N4 can be greatly promoted through integrating amorphous Ni-P alloy. Especially, the Ni-P/g-C3N4 (5 wt%) exhibits the superior H2-generation activity (118.2 μmol h-1 g-1), which is almost 35.8 times that of bare g-C3N4. Furthermore, the amorphous Ni-P alloy cocatalyst can also serve as the general hydrogen-production cocatalyst to greatly enhance the photocatalytic performance of traditional semiconductor materials such as TiO2 and CdS. Based on the present results, the mechanism of the amorphous Ni-P alloy as the high-efficiency electron transfer medium was proposed for the boosted H2-generation rate. The present facile route may broaden the horizons for the efficient development of highly active cocatalysts in photocatalytic field.

摘要

开发高效、稳定且低成本的新型助催化剂对于光催化制氢 反应至关重要. 本文通过简单、绿色的三乙醇胺(TEOA)诱导的光 沉积方法, 将非晶态Ni-P合金颗粒成功修饰到石墨相氮化碳(g- C3N4)上, 以构建Ni-P/g-C3N4光催化剂. TEOA是一种可以与Ni2+配 位形成[Ni(TEOA)]2+络合物的优良络合剂, 在光照下能够促进非晶 态Ni-P合金在g-C3N4表面快速有效沉积. 光催化产氢测试表明, 非 晶态Ni-P合金的负载可以显著提高g-C3N4的光催化产氢性能, 其中 Ni-P/g-C3N4 (5 wt%)样品具有最佳产氢性能(118.2 μmol h−1 g−1), 是纯g-C3N4的35.8倍. 此外, 非晶态Ni-P合金还可以作为具有通用 性的制氢助催化剂, 可显著提高传统半导体材料(如TiO2和CdS)的 光催化产氢性能. 基于相关表征结果, 本文提出了非晶态Ni-P合金 作为高效电子传递介质以提高产氢速率的机理. 该三乙醇胺调控 的光沉积方法为新型高效助催化剂的合成与开发提供了新的思路.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (21771142 and 51672203), and the Fundamental Research Funds for the Central Universities (WUT 2019IB002).

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Authors and Affiliations

  1. Department of Chemistry, School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan, 430070, China

    Huogen Yu  (余火根), Jiachao Xu  (许家超) & Duoduo Gao  (高朵朵)

  2. State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan, 430070, China

    Huogen Yu  (余火根)

  3. School of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450002, China

    Jiajie Fan  (范佳杰)

  4. State Key Laboratory of Advanced Technology for Material Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070, China

    Jiaguo Yu  (余家国)

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  1. Huogen Yu  (余火根)
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  2. Jiachao Xu  (许家超)
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Contributions

Yu H and Xu J designed the project; Yu H, Xu J, and Gao D performed the experiments; Fan J and Yu J performed the data analysis; Xu J, Yu H and Yu J wrote the paper. All authors contributed to the general discussion.

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Correspondence to Huogen Yu  (余火根) or Jiajie Fan  (范佳杰).

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The authors declare that they have no conflict of interest.

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Supporting data are available in the online version of the paper.

Jiajie Fan was born in 1985 and received her PhD degree in 2012 from WHUT. She currently works as an associate professor at the State Centre for International Cooperation on Designer Low-carbon and Environmental Materials (CDLCEM), and the UK-China Centre for Multifunctional Nanomaterials, School of Materials Science and Engineering, Zhengzhou University, China. Her research interests include photocatalytic hydrogen production, thin film solar cells, hydrogen sensors, dye-sensitized solar cells; nanostructure metal oxide semiconductors, TiO2, CuO/Cu4O3/ Cu2O, thin films; graphene, nano-carbons, and related process technology. Her H-index is 14.

Huogen Yu was born in 1978 and received his PhD in 2007 from Wuhan University of Technology (WHUT). He worked as a post-doctoral fellow for two years at the University of Tokyo, from 2008 to 2010. He then returned to the WHUT and was promoted to be a full professor in 2010. His research interests mainly focus on the high-performance photocatalytic materials and their photocatalytic mechanisms for water splitting and environmental purification. Prof. Yu is the author or co-author of more than 100 peer-reviewed papers with over 7000 citations and his H-index is about 50. He was selected as the Most Cited Chinese Researchers in 2014–2018, based on the Scopus database from Elsevier.

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Yu, H., Xu, J., Gao, D. et al. Triethanolamine-mediated photodeposition formation of amorphous Ni-P alloy for improved H2-evolution activity of g-C3N4. Sci. China Mater. 63, 2215–2227 (2020). https://doi.org/10.1007/s40843-020-1298-x

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