Simultaneous Photocatalytic Production of H 2 and Acetal from Ethanol with Quantum Efficiency over 73% by Protonated Poly(heptazine imide) under Visible Light.

Autor:	Shvalagin V; Max Planck Institute of Colloids and Interfaces, Am Mühlenberg 1, Potsdam 14476, Germany., Tarakina N; Max Planck Institute of Colloids and Interfaces, Am Mühlenberg 1, Potsdam 14476, Germany., Badamdorj B; Max Planck Institute of Colloids and Interfaces, Am Mühlenberg 1, Potsdam 14476, Germany., Lahrsen IM; Energy & Process Systems Engineering, Department of Mechanical and Process Engineering, ETH Zurich, Tannenstrasse 3, Zurich 8092, Switzerland., Bargiacchi E; Energy & Process Systems Engineering, Department of Mechanical and Process Engineering, ETH Zurich, Tannenstrasse 3, Zurich 8092, Switzerland., Bardow A; Energy & Process Systems Engineering, Department of Mechanical and Process Engineering, ETH Zurich, Tannenstrasse 3, Zurich 8092, Switzerland., Deng Z; Department of Chemistry, The University of Hong Kong, Kowloon, Hong Kong SAR 999077, China., Wang W; Department of Chemistry, The University of Hong Kong, Kowloon, Hong Kong SAR 999077, China., Phillips DL; Department of Chemistry, The University of Hong Kong, Kowloon, Hong Kong SAR 999077, China., Guo Z; Department of Chemistry, The University of Hong Kong, Kowloon, Hong Kong SAR 999077, China., Zhang G; State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fujian 350116, China., Tang J; Industrial Catalysis Center, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China., Savateev O; Department of Chemistry, The Chinese University of Hong Kong, Shatin, New Territories, Kowloon 999077, Hong Kong.
Jazyk:	angličtina
Zdroj:	ACS catalysis [ACS Catal] 2024 Sep 23; Vol. 14 (19), pp. 14836-14854. Date of Electronic Publication: 2024 Sep 23 (Print Publication: 2024).
DOI:	10.1021/acscatal.4c04180
Abstrakt:	In this work, protonated poly(heptazine imide) (H-PHI) was obtained by adding acid to the suspension of potassium PHI (K-PHI) in ethanol. It was established that the obtained H-PHI demonstrates very high photocatalytic activity in the reaction of hydrogen formation from ethanol in the presence of Pt nanoparticles under visible light irradiation in comparison with K-PHI. This enhancement can be attributed to improved efficiency of photogenerated charge transfer to the photocatalyst's surface, where redox processes occur. Various factors influencing the system's activity were evaluated. Notably, it was discovered that the conditions of acid introduction into the system can significantly affect the size of Pt (cocatalyst metal) deposition on the H-PHI surface, thereby enhancing the photocatalytic system's stability in producing molecular hydrogen. It was established that the system can operate efficiently in the presence of air without additional components on the photocatalyst surface to block air access. Under optimal conditions, the apparent quantum yield of molecular hydrogen production at 410 nm is around 73%, the highest reported value for carbon nitride materials to date. The addition of acid not only increases the activity of the reduction part of the system but also leads to the formation of a value-added product from ethanol-1,1-diethoxyethane (acetal) with high selectivity. Competing Interests: The authors declare the following competing financial interest(s): The patents EP 3 700 910 B1 and US 11,813,596 B2 have been issued, in which OS is listed as the inventor. (© 2024 The Authors. Published by American Chemical Society.)
Databáze:	MEDLINE
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