Triple-Phase Photocatalytic H2O2 Production on a Janus Fiber Membrane with Asymmetric Hydrophobicity

Yunxiang Li; Zhihao Pei; Deyan Luan; Xiong Wen David Lou

doi:10.1021/jacs.3c12465

Triple-Phase Photocatalytic H₂O₂ Production on a Janus Fiber Membrane with Asymmetric Hydrophobicity

Yunxiang Li, Zhihao Pei, Deyan Luan^*, Xiong Wen David Lou^*

^*Corresponding author for this work

Department of Chemistry

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

51 Citations (Scopus)

31 Downloads (CityUHK Scholars)

Abstract

Photocatalytic O₂ reduction is an intriguing approach to producing H₂O₂, but its efficiency is often hindered by the limited solubility and mass transfer of O₂ in the aqueous phase. Here, we design and fabricate a two-layered (2L) Janus fiber membrane photocatalyst with asymmetric hydrophobicity for efficient photocatalytic H₂O₂ production. The top layer of the membrane consists of superhydrophobic polytetrafluoroethylene (PTFE) fibers with a dispersed modified carbon nitride (mCN) photocatalyst. Amphiphilic Nafion (Naf) ionomer is sprayed onto this layer to modulate the microenvironment and achieve moderate hydrophobicity. In contrast, the bottom layer consists of bare PTFE fibers with high hydrophobicity. The elaborate structural configuration and asymmetric hydrophobicity feature of the optimized membrane photocatalyst (designated as 2L-mCN/F-Naf; F, PTFE) allow most mCN to be exposed with gas-liquid-solid triple-phase interfaces and enable rapid mass transfer of gaseous O₂ within the hierarchical membrane, thus increasing the local O₂ concentration near the mCN photocatalyst. As a result, the optimized 2L-mCN/F-Naf membrane photocatalyst shows remarkable photocatalytic H₂O₂ production activity, achieving a rate of 5.38 mmol g^-1 h^-1 under visible light irradiation. © 2024 American Chemical Society.

Original language	English
Pages (from-to)	3343-3351
Journal	Journal of the American Chemical Society
Volume	146
Issue number	5
Online published	23 Jan 2024
DOIs	https://doi.org/10.1021/jacs.3c12465
Publication status	Published - 7 Feb 2024

Funding

The authors acknowledge the funding support from the Ministry of Education of Singapore through the Academic Research Fund (AcRF) Tier-2 grant (MOE2019-T2-2-049). The authors thank Prof. Shuxin Ouyang from Central China Normal University for the help with underwater bubble contact angle and in situ ESR tests.

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COPYRIGHT TERMS OF DEPOSITED POSTPRINT FILE: This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © 2024 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/jacs.3c12465.

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title = "Triple-Phase Photocatalytic H2O2 Production on a Janus Fiber Membrane with Asymmetric Hydrophobicity",

abstract = "Photocatalytic O2 reduction is an intriguing approach to producing H2O2, but its efficiency is often hindered by the limited solubility and mass transfer of O2 in the aqueous phase. Here, we design and fabricate a two-layered (2L) Janus fiber membrane photocatalyst with asymmetric hydrophobicity for efficient photocatalytic H2O2 production. The top layer of the membrane consists of superhydrophobic polytetrafluoroethylene (PTFE) fibers with a dispersed modified carbon nitride (mCN) photocatalyst. Amphiphilic Nafion (Naf) ionomer is sprayed onto this layer to modulate the microenvironment and achieve moderate hydrophobicity. In contrast, the bottom layer consists of bare PTFE fibers with high hydrophobicity. The elaborate structural configuration and asymmetric hydrophobicity feature of the optimized membrane photocatalyst (designated as 2L-mCN/F-Naf; F, PTFE) allow most mCN to be exposed with gas-liquid-solid triple-phase interfaces and enable rapid mass transfer of gaseous O2 within the hierarchical membrane, thus increasing the local O2 concentration near the mCN photocatalyst. As a result, the optimized 2L-mCN/F-Naf membrane photocatalyst shows remarkable photocatalytic H2O2 production activity, achieving a rate of 5.38 mmol g-1 h-1 under visible light irradiation. {\textcopyright} 2024 American Chemical Society.",

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N2 - Photocatalytic O2 reduction is an intriguing approach to producing H2O2, but its efficiency is often hindered by the limited solubility and mass transfer of O2 in the aqueous phase. Here, we design and fabricate a two-layered (2L) Janus fiber membrane photocatalyst with asymmetric hydrophobicity for efficient photocatalytic H2O2 production. The top layer of the membrane consists of superhydrophobic polytetrafluoroethylene (PTFE) fibers with a dispersed modified carbon nitride (mCN) photocatalyst. Amphiphilic Nafion (Naf) ionomer is sprayed onto this layer to modulate the microenvironment and achieve moderate hydrophobicity. In contrast, the bottom layer consists of bare PTFE fibers with high hydrophobicity. The elaborate structural configuration and asymmetric hydrophobicity feature of the optimized membrane photocatalyst (designated as 2L-mCN/F-Naf; F, PTFE) allow most mCN to be exposed with gas-liquid-solid triple-phase interfaces and enable rapid mass transfer of gaseous O2 within the hierarchical membrane, thus increasing the local O2 concentration near the mCN photocatalyst. As a result, the optimized 2L-mCN/F-Naf membrane photocatalyst shows remarkable photocatalytic H2O2 production activity, achieving a rate of 5.38 mmol g-1 h-1 under visible light irradiation. © 2024 American Chemical Society.

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