In Situ Modulation of NiFeOOH Coordination Environment for Enhanced Electrocatalytic‐Conversion of Glucose and Energy‐Efficient Hydrogen Production

Abstract Glucose electrocatalytic‐conversion reaction (GCR) is a promising anode reaction to replace the slow oxygen evolution reaction (OER), thus promoting the development of hydrogen production by electrochemical water splitting. Herein, NiFe‐based metal‐organic framework (MOF) is used as a precu...

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Main Authors: Ning Wei, Sufeng Zhang, Xue Yao, Qinglu Li, Nan Li, Jinrui Li, Dingjie Pan, Qiming Liu, Shaowei Chen, Scott Renneckar
Format: Article
Language:English
Published: Wiley 2025-02-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202412872
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author Ning Wei
Sufeng Zhang
Xue Yao
Qinglu Li
Nan Li
Jinrui Li
Dingjie Pan
Qiming Liu
Shaowei Chen
Scott Renneckar
author_facet Ning Wei
Sufeng Zhang
Xue Yao
Qinglu Li
Nan Li
Jinrui Li
Dingjie Pan
Qiming Liu
Shaowei Chen
Scott Renneckar
author_sort Ning Wei
collection DOAJ
description Abstract Glucose electrocatalytic‐conversion reaction (GCR) is a promising anode reaction to replace the slow oxygen evolution reaction (OER), thus promoting the development of hydrogen production by electrochemical water splitting. Herein, NiFe‐based metal‐organic framework (MOF) is used as a precursor to prepare W‐doped nickel‐iron phosphide (W‐NiFeP) nanosheet arrays by ion exchange and phosphorylation, which exhibit a high electrocatalytic activity toward the hydrogen evolution reaction (HER), featuring an overpotential of only −179 mV to achieve the current density of 100 mA cm−2 in alkaline media. Notably, electrochemical activation of W‐NiFeP facilitates the in situ formation of phosphate groups producing W,P‐NiFeOOH, which, in conjunction with the W co‐doped amorphous layers, leads to a high electrocatalytic performance toward GCR, due to enhanced proton transfer and adsorption of reaction intermediates, as confirmed in experimental and theoretical studies. Thus, the two‐electrode electrolyzer of the W‐NiFeP/NF||W,P‐NiFeOOH/NF for HER||GCR needs only a low cell voltage of 1.56 V to deliver 100 mA cm−2 at a remarkable hydrogen production efficiency of 1.86 mmol h−1, with a high glucose conversion (98.0%) and formic acid yields (85.2%). Results from this work highlight the significance of the development of effective electrocatalysts for biomass electrocatalytic‐conversion in the construction of high‐efficiency electrolyzers for green hydrogen production.
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spelling doaj-art-186b773184b6413d919d9d5ea8426b482025-02-04T13:14:54ZengWileyAdvanced Science2198-38442025-02-01125n/an/a10.1002/advs.202412872In Situ Modulation of NiFeOOH Coordination Environment for Enhanced Electrocatalytic‐Conversion of Glucose and Energy‐Efficient Hydrogen ProductionNing Wei0Sufeng Zhang1Xue Yao2Qinglu Li3Nan Li4Jinrui Li5Dingjie Pan6Qiming Liu7Shaowei Chen8Scott Renneckar9National Demonstration Center for Experimental Light Chemistry Engineering Education Shaanxi Provincial Key Laboratory of Papermaking Technology and Specialty Paper Development College of Bioresources Chemical and Materials Engineering Shaanxi University of Science and Technology Xi'an Shaanxi 710021 ChinaNational Demonstration Center for Experimental Light Chemistry Engineering Education Shaanxi Provincial Key Laboratory of Papermaking Technology and Specialty Paper Development College of Bioresources Chemical and Materials Engineering Shaanxi University of Science and Technology Xi'an Shaanxi 710021 ChinaNational Demonstration Center for Experimental Light Chemistry Engineering Education Shaanxi Provincial Key Laboratory of Papermaking Technology and Specialty Paper Development College of Bioresources Chemical and Materials Engineering Shaanxi University of Science and Technology Xi'an Shaanxi 710021 ChinaNational Demonstration Center for Experimental Light Chemistry Engineering Education Shaanxi Provincial Key Laboratory of Papermaking Technology and Specialty Paper Development College of Bioresources Chemical and Materials Engineering Shaanxi University of Science and Technology Xi'an Shaanxi 710021 ChinaNational Demonstration Center for Experimental Light Chemistry Engineering Education Shaanxi Provincial Key Laboratory of Papermaking Technology and Specialty Paper Development College of Bioresources Chemical and Materials Engineering Shaanxi University of Science and Technology Xi'an Shaanxi 710021 ChinaNational Demonstration Center for Experimental Light Chemistry Engineering Education Shaanxi Provincial Key Laboratory of Papermaking Technology and Specialty Paper Development College of Bioresources Chemical and Materials Engineering Shaanxi University of Science and Technology Xi'an Shaanxi 710021 ChinaDepartment of Chemistry and Biochemistry University of California 1156 High Street Santa Cruz CA 96064 USADepartment of Chemistry Rice University Houston TX 77005 USADepartment of Chemistry and Biochemistry University of California 1156 High Street Santa Cruz CA 96064 USAAdvanced Renewable Materials Lab Faculty of Forestry The University of British Columbia Vancouver BC V6T 1Z4 CanadaAbstract Glucose electrocatalytic‐conversion reaction (GCR) is a promising anode reaction to replace the slow oxygen evolution reaction (OER), thus promoting the development of hydrogen production by electrochemical water splitting. Herein, NiFe‐based metal‐organic framework (MOF) is used as a precursor to prepare W‐doped nickel‐iron phosphide (W‐NiFeP) nanosheet arrays by ion exchange and phosphorylation, which exhibit a high electrocatalytic activity toward the hydrogen evolution reaction (HER), featuring an overpotential of only −179 mV to achieve the current density of 100 mA cm−2 in alkaline media. Notably, electrochemical activation of W‐NiFeP facilitates the in situ formation of phosphate groups producing W,P‐NiFeOOH, which, in conjunction with the W co‐doped amorphous layers, leads to a high electrocatalytic performance toward GCR, due to enhanced proton transfer and adsorption of reaction intermediates, as confirmed in experimental and theoretical studies. Thus, the two‐electrode electrolyzer of the W‐NiFeP/NF||W,P‐NiFeOOH/NF for HER||GCR needs only a low cell voltage of 1.56 V to deliver 100 mA cm−2 at a remarkable hydrogen production efficiency of 1.86 mmol h−1, with a high glucose conversion (98.0%) and formic acid yields (85.2%). Results from this work highlight the significance of the development of effective electrocatalysts for biomass electrocatalytic‐conversion in the construction of high‐efficiency electrolyzers for green hydrogen production.https://doi.org/10.1002/advs.202412872dopingelectrocatalytic‐conversion of glucoseelectrochemical activationelectrolyzerhydrogen evolution reactionNiFeOOH
spellingShingle Ning Wei
Sufeng Zhang
Xue Yao
Qinglu Li
Nan Li
Jinrui Li
Dingjie Pan
Qiming Liu
Shaowei Chen
Scott Renneckar
In Situ Modulation of NiFeOOH Coordination Environment for Enhanced Electrocatalytic‐Conversion of Glucose and Energy‐Efficient Hydrogen Production
Advanced Science
doping
electrocatalytic‐conversion of glucose
electrochemical activation
electrolyzer
hydrogen evolution reaction
NiFeOOH
title In Situ Modulation of NiFeOOH Coordination Environment for Enhanced Electrocatalytic‐Conversion of Glucose and Energy‐Efficient Hydrogen Production
title_full In Situ Modulation of NiFeOOH Coordination Environment for Enhanced Electrocatalytic‐Conversion of Glucose and Energy‐Efficient Hydrogen Production
title_fullStr In Situ Modulation of NiFeOOH Coordination Environment for Enhanced Electrocatalytic‐Conversion of Glucose and Energy‐Efficient Hydrogen Production
title_full_unstemmed In Situ Modulation of NiFeOOH Coordination Environment for Enhanced Electrocatalytic‐Conversion of Glucose and Energy‐Efficient Hydrogen Production
title_short In Situ Modulation of NiFeOOH Coordination Environment for Enhanced Electrocatalytic‐Conversion of Glucose and Energy‐Efficient Hydrogen Production
title_sort in situ modulation of nifeooh coordination environment for enhanced electrocatalytic conversion of glucose and energy efficient hydrogen production
topic doping
electrocatalytic‐conversion of glucose
electrochemical activation
electrolyzer
hydrogen evolution reaction
NiFeOOH
url https://doi.org/10.1002/advs.202412872
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