Hydrogen-Mediated Photoelectrocatalysis with Nickel-Modified Poly(Heptazine Imides)

Sirlon Blaskievicz; Ivo F.  Teixeira; Lucia Helena Mascaro; Mariolino Carta; Neil B. Mckeown; Yuanzhu Zhao; Frank Marken

doi:10.1007/s12678-023-00852-9

Hydrogen-Mediated Photoelectrocatalysis with Nickel-Modified Poly(Heptazine Imides)

Sirlon Blaskievicz
, Ivo F. Teixeira
, Lucia Helena Mascaro
, Mariolino Carta
, Neil B. Mckeown
, Yuanzhu Zhao
, Frank Marken

University of Edinburgh
Edinburgh Napier University
Swansea University
Universidade Federal de São Carlos

Research output: Contribution to journal › Article › peer-review

6 Citations (SciVal)

Abstract

Polymeric carbon nitrides (C ₃N ₄) are photochemically active organic semiconductors that can be produced in a wide range of structural types. Here, a poly-(heptazine imide) containing nickel single atoms (Ni-PHI) is employed for photochemical hydrogen production and is compared to the non-nickel-doped semiconductor. Film deposits are formed on a platinum disk electrode (to detect hydrogen) and a coating of the molecularly rigid polymer of intrinsic microporosity PIM-1 is applied to (i) mechanically stabilize the photo-catalyst film without impeding photocatalysis and (ii) assist in the interfacial hydrogen capture/oxygen suppression process. In the presence of hole quenchers such as methanol or ethanol, anodic photocurrents linked to hydrogen production/oxidation are observed. A comparison with an experiment on glassy carbon confirms the formation of interfacial hydrogen as a mediator. The effects of hole quencher concentration are evaluated. The system Pt/Ni-PHI/PIM-1 is employed in a single-compartment photo-fuel cell. Graphical Abstract: [Figure not available: see fulltext.]

Original language	English
Pages (from-to)	42-51
Number of pages	10
Journal	Electrocatalysis
Volume	15
Issue number	1
Early online date	11 Nov 2023
DOIs	https://doi.org/10.1007/s12678-023-00852-9
Publication status	Published - 31 Jan 2024

Data Availability Statement

Data and materials are available from the authors.

Funding

S.F.B. thanks to the financial support of the CAPES Foundation for a sandwich doctorate scholarship (CAPES-PRINT Process 88887.465542/2019-00). L.H.M. thanks to FAPESP (2017/11986-5, 2020/14741-6, 2014/50249-8). Y.Z. (201809350006) is grateful to the China Scholarship Council for a PhD scholarship.

Funders	Funder number
Fundação de Amparo à Pesquisa do Estado de São Paulo
Coordenacao de Aperfeicoamento de Pessoal de Nivel Superior	88887.465542/2019-00
China Scholarship Council	201809350006
Centros de Pesquisa, Inovação e Difusão, Fundação Amazônia Paraense de Amparo à Pesquisa	2020/14741-6, 2014/50249-8, 2017/11986-5

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Keywords

Biomass
Hydrogen
Intrinsic Microporosity
Photocatalysis
Photofuel cell

ASJC Scopus subject areas

Electrochemistry

Access to Document

10.1007/s12678-023-00852-9Licence: CC BY

Cite this

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title = "Hydrogen-Mediated Photoelectrocatalysis with Nickel-Modified Poly(Heptazine Imides)",

abstract = "Polymeric carbon nitrides (C 3N 4) are photochemically active organic semiconductors that can be produced in a wide range of structural types. Here, a poly-(heptazine imide) containing nickel single atoms (Ni-PHI) is employed for photochemical hydrogen production and is compared to the non-nickel-doped semiconductor. Film deposits are formed on a platinum disk electrode (to detect hydrogen) and a coating of the molecularly rigid polymer of intrinsic microporosity PIM-1 is applied to (i) mechanically stabilize the photo-catalyst film without impeding photocatalysis and (ii) assist in the interfacial hydrogen capture/oxygen suppression process. In the presence of hole quenchers such as methanol or ethanol, anodic photocurrents linked to hydrogen production/oxidation are observed. A comparison with an experiment on glassy carbon confirms the formation of interfacial hydrogen as a mediator. The effects of hole quencher concentration are evaluated. The system Pt/Ni-PHI/PIM-1 is employed in a single-compartment photo-fuel cell. Graphical Abstract: [Figure not available: see fulltext.]",

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author = "Sirlon Blaskievicz and Teixeira, \{Ivo F.\} and Mascaro, \{Lucia Helena\} and Mariolino Carta and Mckeown, \{Neil B.\} and Yuanzhu Zhao and Frank Marken",

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T1 - Hydrogen-Mediated Photoelectrocatalysis with Nickel-Modified Poly(Heptazine Imides)

AU - Blaskievicz, Sirlon

AU - Teixeira, Ivo F.

AU - Mascaro, Lucia Helena

AU - Carta, Mariolino

AU - Mckeown, Neil B.

AU - Zhao, Yuanzhu

AU - Marken, Frank

PY - 2024/1/31

Y1 - 2024/1/31

N2 - Polymeric carbon nitrides (C 3N 4) are photochemically active organic semiconductors that can be produced in a wide range of structural types. Here, a poly-(heptazine imide) containing nickel single atoms (Ni-PHI) is employed for photochemical hydrogen production and is compared to the non-nickel-doped semiconductor. Film deposits are formed on a platinum disk electrode (to detect hydrogen) and a coating of the molecularly rigid polymer of intrinsic microporosity PIM-1 is applied to (i) mechanically stabilize the photo-catalyst film without impeding photocatalysis and (ii) assist in the interfacial hydrogen capture/oxygen suppression process. In the presence of hole quenchers such as methanol or ethanol, anodic photocurrents linked to hydrogen production/oxidation are observed. A comparison with an experiment on glassy carbon confirms the formation of interfacial hydrogen as a mediator. The effects of hole quencher concentration are evaluated. The system Pt/Ni-PHI/PIM-1 is employed in a single-compartment photo-fuel cell. Graphical Abstract: [Figure not available: see fulltext.]

AB - Polymeric carbon nitrides (C 3N 4) are photochemically active organic semiconductors that can be produced in a wide range of structural types. Here, a poly-(heptazine imide) containing nickel single atoms (Ni-PHI) is employed for photochemical hydrogen production and is compared to the non-nickel-doped semiconductor. Film deposits are formed on a platinum disk electrode (to detect hydrogen) and a coating of the molecularly rigid polymer of intrinsic microporosity PIM-1 is applied to (i) mechanically stabilize the photo-catalyst film without impeding photocatalysis and (ii) assist in the interfacial hydrogen capture/oxygen suppression process. In the presence of hole quenchers such as methanol or ethanol, anodic photocurrents linked to hydrogen production/oxidation are observed. A comparison with an experiment on glassy carbon confirms the formation of interfacial hydrogen as a mediator. The effects of hole quencher concentration are evaluated. The system Pt/Ni-PHI/PIM-1 is employed in a single-compartment photo-fuel cell. Graphical Abstract: [Figure not available: see fulltext.]

KW - Biomass

KW - Hydrogen

KW - Intrinsic Microporosity

KW - Photocatalysis

KW - Photofuel cell

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DO - 10.1007/s12678-023-00852-9

M3 - Article

SN - 1868-2529

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EP - 51

JO - Electrocatalysis

JF - Electrocatalysis

IS - 1

ER -

Hydrogen-Mediated Photoelectrocatalysis with Nickel-Modified Poly(Heptazine Imides)

Abstract

Data Availability Statement

Funding

UN SDGs

Keywords

ASJC Scopus subject areas

Access to Document

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