Boosting Oxygen Reduction through Microenvironment Modulation to Enhance Mass Transportation

Electroreduction of oxygen driven by renewable electricity holds significant promise for the sustainable production of value‐added hydrogen peroxide (H2O2). While water is a desirable source of protons and electrons for this reaction, its low gas solubility often limits the transportation of gas mol...

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Main Authors: Bihao Hu, Miao Wang, Danning Li, Jingyi Chen, Chunfeng Li, Lei Wang
Format: Article
Language:English
Published: Wiley-VCH 2023-12-01
Series:Advanced Energy & Sustainability Research
Subjects:
Online Access:https://doi.org/10.1002/aesr.202300143
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author Bihao Hu
Miao Wang
Danning Li
Jingyi Chen
Chunfeng Li
Lei Wang
author_facet Bihao Hu
Miao Wang
Danning Li
Jingyi Chen
Chunfeng Li
Lei Wang
author_sort Bihao Hu
collection DOAJ
description Electroreduction of oxygen driven by renewable electricity holds significant promise for the sustainable production of value‐added hydrogen peroxide (H2O2). While water is a desirable source of protons and electrons for this reaction, its low gas solubility often limits the transportation of gas molecules and consequently leads to large concentration overpotential, resulting in unsatisfactory energy efficiencies. Herein, a facile and effective strategy to promote the 2e− oxygen reduction reaction (ORR) through microenvironment modulation is presented. In this work, it is specifically aimed to facilitate oxygen transportation at the reaction interface, particularly at high rates. To achieve this, hydrophobic polytetrafluoroethylene (PTFE) particles are introduced into a catalyst layer containing amino‐group‐functionalized carbon nanotube (CNT‐NH2) as the ORR catalyst for H2O2 production. As a result, the PTFE‐modified CNT‐NH2‐based gas‐diffusion electrode (GDE) substantially improves ORR activity. At 100 mA cm−2, the PTFE‐modified CNT‐NH2 achieves a high cathodic energy efficiency of 92%, 1.5 times higher than the pristine CNT‐NH2‐based GDE (63%). Detailed kinetic analysis reveals that this enhanced ORR performance is indeed due to the enhanced oxygen transportation induced by the persistent hydrophobic microenvironment created by the PTFE‐modified catalyst layer, reducing the concentration overpotential during ORR.
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spelling doaj.art-d0bb454fa8cc4ccd9fcc0e1096aadddf2023-12-08T03:59:29ZengWiley-VCHAdvanced Energy & Sustainability Research2699-94122023-12-01412n/an/a10.1002/aesr.202300143Boosting Oxygen Reduction through Microenvironment Modulation to Enhance Mass TransportationBihao Hu0Miao Wang1Danning Li2Jingyi Chen3Chunfeng Li4Lei Wang5Department of Chemical and Biomolecular Engineering College of Design and Engineering National University of Singapore 4 Engineering Drive 4 E5 #03-12 Singapore 117585 SingaporeDepartment of Chemical and Biomolecular Engineering College of Design and Engineering National University of Singapore 4 Engineering Drive 4 E5 #03-12 Singapore 117585 SingaporeDepartment of Chemical and Biomolecular Engineering College of Design and Engineering National University of Singapore 4 Engineering Drive 4 E5 #03-12 Singapore 117585 SingaporeDepartment of Chemical and Biomolecular Engineering College of Design and Engineering National University of Singapore 4 Engineering Drive 4 E5 #03-12 Singapore 117585 SingaporeDepartment of Chemical and Biomolecular Engineering College of Design and Engineering National University of Singapore 4 Engineering Drive 4 E5 #03-12 Singapore 117585 SingaporeDepartment of Chemical and Biomolecular Engineering College of Design and Engineering National University of Singapore 4 Engineering Drive 4 E5 #03-12 Singapore 117585 SingaporeElectroreduction of oxygen driven by renewable electricity holds significant promise for the sustainable production of value‐added hydrogen peroxide (H2O2). While water is a desirable source of protons and electrons for this reaction, its low gas solubility often limits the transportation of gas molecules and consequently leads to large concentration overpotential, resulting in unsatisfactory energy efficiencies. Herein, a facile and effective strategy to promote the 2e− oxygen reduction reaction (ORR) through microenvironment modulation is presented. In this work, it is specifically aimed to facilitate oxygen transportation at the reaction interface, particularly at high rates. To achieve this, hydrophobic polytetrafluoroethylene (PTFE) particles are introduced into a catalyst layer containing amino‐group‐functionalized carbon nanotube (CNT‐NH2) as the ORR catalyst for H2O2 production. As a result, the PTFE‐modified CNT‐NH2‐based gas‐diffusion electrode (GDE) substantially improves ORR activity. At 100 mA cm−2, the PTFE‐modified CNT‐NH2 achieves a high cathodic energy efficiency of 92%, 1.5 times higher than the pristine CNT‐NH2‐based GDE (63%). Detailed kinetic analysis reveals that this enhanced ORR performance is indeed due to the enhanced oxygen transportation induced by the persistent hydrophobic microenvironment created by the PTFE‐modified catalyst layer, reducing the concentration overpotential during ORR.https://doi.org/10.1002/aesr.202300143concentration overpotentialhydrogen peroxidemicroenvironmentoxygen reduction reactionPTFE
spellingShingle Bihao Hu
Miao Wang
Danning Li
Jingyi Chen
Chunfeng Li
Lei Wang
Boosting Oxygen Reduction through Microenvironment Modulation to Enhance Mass Transportation
Advanced Energy & Sustainability Research
concentration overpotential
hydrogen peroxide
microenvironment
oxygen reduction reaction
PTFE
title Boosting Oxygen Reduction through Microenvironment Modulation to Enhance Mass Transportation
title_full Boosting Oxygen Reduction through Microenvironment Modulation to Enhance Mass Transportation
title_fullStr Boosting Oxygen Reduction through Microenvironment Modulation to Enhance Mass Transportation
title_full_unstemmed Boosting Oxygen Reduction through Microenvironment Modulation to Enhance Mass Transportation
title_short Boosting Oxygen Reduction through Microenvironment Modulation to Enhance Mass Transportation
title_sort boosting oxygen reduction through microenvironment modulation to enhance mass transportation
topic concentration overpotential
hydrogen peroxide
microenvironment
oxygen reduction reaction
PTFE
url https://doi.org/10.1002/aesr.202300143
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AT jingyichen boostingoxygenreductionthroughmicroenvironmentmodulationtoenhancemasstransportation
AT chunfengli boostingoxygenreductionthroughmicroenvironmentmodulationtoenhancemasstransportation
AT leiwang boostingoxygenreductionthroughmicroenvironmentmodulationtoenhancemasstransportation