Size-Selective Photoelectrochemical Reactions in Microporous Environments: Clark Probe Investigation of Pt@g-C3N4 Embedded into Intrinsically Microporous Polymer (PIM-1)

Yuanzhu Zhao; Richard Malpass-Evans; Mariolino Carta; Neil B. McKeown; Philip J. Fletcher; Gabriele Kociok-Köhn; Diana Lednitzky; Frank Marken

doi:10.1002/celc.202100732

Size-Selective Photoelectrochemical Reactions in Microporous Environments: Clark Probe Investigation of Pt@g-C₃N₄ Embedded into Intrinsically Microporous Polymer (PIM-1)

Yuanzhu Zhao, Richard Malpass-Evans, Mariolino Carta, Neil B. McKeown, Philip J. Fletcher, Gabriele Kociok-Köhn, Diana Lednitzky, Frank Marken^*

^*Corresponding author for this work

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

Abstract / Description of output

Graphitic carbon nitride (g-C₃N₄) with photo-attached platinum (Pt@g-C₃N₄) is known to generate hydrogen under illumination in aqueous environments in the presence of carbohydrate hole quenchers. Here, Pt@g-C₃N₄ is embedded into a polymer of intrinsic microporosity (PIM-1) host material with a molecularly rigid structure to maintain active unblocked catalyst surfaces and to control transport to/from the photocatalyst. A Clark-type oxygen/hydrogen sensor is employed with Pt@g-C₃N₄ embedded into PIM-1 applied as a film to be the gas-permeable sensor membrane. Oxygen reduction and hydrogen production are observed in situ as a function of light exposure and quencher concentration. Significant size-selectivity favouring smaller more flexible saccharides or carbohydrate/ hydrocarbon quenchers is observed and attributed to rate limiting PIM-1 micropore transport. Effective hydrogen production through a Teflon membrane is demonstrated. The underlying hydrogen production/ photocurrent enhancing effects of the microporous PIM-1 film on the photochemical process are revealed.

Original language	English
Pages (from-to)	3499-3505
Number of pages	7
Journal	ChemElectroChem
Volume	8
Issue number	18
Early online date	14 Jun 2021
DOIs	https://doi.org/10.1002/celc.202100732
Publication status	E-pub ahead of print - 14 Jun 2021

Keywords / Materials (for Non-textual outputs)

biomass
hydrogen
microporous host-guest interactions
photocatalysis
reaction monitoring

Access to Document

10.1002/celc.202100732

20211223_McKeown_Zhao-VoRFinal published version, 1.41 MBLicence: Creative Commons: Attribution (CC-BY)

https://chemistry-europe.onlinelibrary.wiley.com/doi/full/10.1002/celc.202100732

Cite this

Zhao, Y., Malpass-Evans, R., Carta, M., McKeown, N. B., Fletcher, P. J., Kociok-Köhn, G., Lednitzky, D., & Marken, F. (2021). Size-Selective Photoelectrochemical Reactions in Microporous Environments: Clark Probe Investigation of Pt@g-C₃N₄ Embedded into Intrinsically Microporous Polymer (PIM-1). ChemElectroChem, 8(18), 3499-3505. Advance online publication. https://doi.org/10.1002/celc.202100732

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title = "Size-Selective Photoelectrochemical Reactions in Microporous Environments: Clark Probe Investigation of Pt@g-C3N4 Embedded into Intrinsically Microporous Polymer (PIM-1)",

abstract = "Graphitic carbon nitride (g-C3N4) with photo-attached platinum (Pt@g-C3N4) is known to generate hydrogen under illumination in aqueous environments in the presence of carbohydrate hole quenchers. Here, Pt@g-C3N4 is embedded into a polymer of intrinsic microporosity (PIM-1) host material with a molecularly rigid structure to maintain active unblocked catalyst surfaces and to control transport to/from the photocatalyst. A Clark-type oxygen/hydrogen sensor is employed with Pt@g-C3N4 embedded into PIM-1 applied as a film to be the gas-permeable sensor membrane. Oxygen reduction and hydrogen production are observed in situ as a function of light exposure and quencher concentration. Significant size-selectivity favouring smaller more flexible saccharides or carbohydrate/ hydrocarbon quenchers is observed and attributed to rate limiting PIM-1 micropore transport. Effective hydrogen production through a Teflon membrane is demonstrated. The underlying hydrogen production/ photocurrent enhancing effects of the microporous PIM-1 film on the photochemical process are revealed.",

keywords = "biomass, hydrogen, microporous host-guest interactions, photocatalysis, reaction monitoring",

author = "Yuanzhu Zhao and Richard Malpass-Evans and Mariolino Carta and McKeown, {Neil B.} and Fletcher, {Philip J.} and Gabriele Kociok-K{\"o}hn and Diana Lednitzky and Frank Marken",

note = "Funding Information: Y.Z. thanks the China Scholarship Council (CSC scholarship No 20180935006) for a PhD scholarship. F.M. thanks the EPSRC (EP/N013778/1) for support. Publisher Copyright: {\textcopyright} 2021 The Authors. ChemElectroChem published by Wiley-VCH GmbH",

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Zhao, Y, Malpass-Evans, R, Carta, M, McKeown, NB, Fletcher, PJ, Kociok-Köhn, G, Lednitzky, D & Marken, F 2021, 'Size-Selective Photoelectrochemical Reactions in Microporous Environments: Clark Probe Investigation of Pt@g-C₃N₄ Embedded into Intrinsically Microporous Polymer (PIM-1)', ChemElectroChem, vol. 8, no. 18, pp. 3499-3505. https://doi.org/10.1002/celc.202100732

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T2 - Clark Probe Investigation of Pt@g-C3N4 Embedded into Intrinsically Microporous Polymer (PIM-1)

AU - Zhao, Yuanzhu

AU - Malpass-Evans, Richard

AU - Carta, Mariolino

AU - McKeown, Neil B.

AU - Fletcher, Philip J.

AU - Kociok-Köhn, Gabriele

AU - Lednitzky, Diana

AU - Marken, Frank

N1 - Funding Information: Y.Z. thanks the China Scholarship Council (CSC scholarship No 20180935006) for a PhD scholarship. F.M. thanks the EPSRC (EP/N013778/1) for support. Publisher Copyright: © 2021 The Authors. ChemElectroChem published by Wiley-VCH GmbH

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N2 - Graphitic carbon nitride (g-C3N4) with photo-attached platinum (Pt@g-C3N4) is known to generate hydrogen under illumination in aqueous environments in the presence of carbohydrate hole quenchers. Here, Pt@g-C3N4 is embedded into a polymer of intrinsic microporosity (PIM-1) host material with a molecularly rigid structure to maintain active unblocked catalyst surfaces and to control transport to/from the photocatalyst. A Clark-type oxygen/hydrogen sensor is employed with Pt@g-C3N4 embedded into PIM-1 applied as a film to be the gas-permeable sensor membrane. Oxygen reduction and hydrogen production are observed in situ as a function of light exposure and quencher concentration. Significant size-selectivity favouring smaller more flexible saccharides or carbohydrate/ hydrocarbon quenchers is observed and attributed to rate limiting PIM-1 micropore transport. Effective hydrogen production through a Teflon membrane is demonstrated. The underlying hydrogen production/ photocurrent enhancing effects of the microporous PIM-1 film on the photochemical process are revealed.

AB - Graphitic carbon nitride (g-C3N4) with photo-attached platinum (Pt@g-C3N4) is known to generate hydrogen under illumination in aqueous environments in the presence of carbohydrate hole quenchers. Here, Pt@g-C3N4 is embedded into a polymer of intrinsic microporosity (PIM-1) host material with a molecularly rigid structure to maintain active unblocked catalyst surfaces and to control transport to/from the photocatalyst. A Clark-type oxygen/hydrogen sensor is employed with Pt@g-C3N4 embedded into PIM-1 applied as a film to be the gas-permeable sensor membrane. Oxygen reduction and hydrogen production are observed in situ as a function of light exposure and quencher concentration. Significant size-selectivity favouring smaller more flexible saccharides or carbohydrate/ hydrocarbon quenchers is observed and attributed to rate limiting PIM-1 micropore transport. Effective hydrogen production through a Teflon membrane is demonstrated. The underlying hydrogen production/ photocurrent enhancing effects of the microporous PIM-1 film on the photochemical process are revealed.

KW - biomass

KW - hydrogen

KW - microporous host-guest interactions

KW - photocatalysis

KW - reaction monitoring

U2 - 10.1002/celc.202100732

DO - 10.1002/celc.202100732

M3 - Article

AN - SCOPUS:85108998052

SN - 2196-0216

VL - 8

SP - 3499

EP - 3505

JO - ChemElectroChem

JF - ChemElectroChem

IS - 18

ER -