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  Overcoming electron transfer efficiency bottlenecks for hydrogen production in highly crystalline carbon nitride-based materials

Teixeira, I., Tarakina, N. V., Silva, I. F., Lopez Salas, N., Savateev, A., & Antonietti, M. (2022). Overcoming electron transfer efficiency bottlenecks for hydrogen production in highly crystalline carbon nitride-based materials. Advanced Sustainable Systems, 6(3): 2100429. doi:10.1002/adsu.202100429.

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 Creators:
Teixeira, Ivo1, Author              
Tarakina, Nadezda V.2, Author              
Silva, Ingrid F.1, Author              
Lopez Salas, Nieves3, Author              
Savateev, Aleksandr4, Author              
Antonietti, Markus1, Author              
Affiliations:
1Markus Antonietti, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863321              
2Nadezda V. Tarakina, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2522693              
3Nieves Lopez Salas, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_3029702              
4Aleksandr Savateev, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2421702              

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Free keywords: carbon nitrides; HER; hydrogen; Na-PHI, photocatalysis; poly(heptazine imide)
 Abstract: The hydrogen evolution reaction (HER) is a complex reaction involving many interdependent physicochemical steps. Highly ordered carbon nitride-based materials, such as Na-PHI and K-PHI, display some of the highest activities for H2 evolution among the carbon nitride-based materials, due to their electronic properties, but also the presence of cyanimide terminations, which favors the charge transfer for the Pt cocatalyst nanoparticles (NPs). For such highly optimized semiconductor structures, the necessity to control and improve other steps of the photocatalytic process becomes essential, in particular the poor electron transfer from the Pt NPs to the protons in solution over the Helmholtz or Stern layer. Taking highly ordered Na-PHI as a test material, the influence of water-dissolved alkali cations on the HER is systematically studied and it is experimentally verified that the electron transfer from the Pt NPs to the protons in solution limits the efficiency of heterogeneous carbon nitride-based catalysts. This paper explains how hydrated alkali cations influence electron transfer and are able to boost the H2 evolution rate of the same Na-PHI from 2401 up to 5330 µmol h-1 g-1 with an apparent quantum yield of 13% at 420 nm.

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Language(s): eng - English
 Dates: 2022-01-132022
 Publication Status: Published in print
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 Identifiers: DOI: 10.1002/adsu.202100429
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Title: Advanced Sustainable Systems
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: - Volume / Issue: 6 (3) Sequence Number: 2100429 Start / End Page: - Identifier: ISSN: 2366-7486