Suppressing product crossover and C-C bond cleavage in a glycerol membrane electrode assembly reformer

Generating hydrogen through water electrolysis is impeded by high costs and substantial energy consumption mainly due to high equilibrium potential and sluggish kinetics of the oxygen evolution reaction (OER). Glycerol oxidation reaction (GOR) is proposed as an alternative due to its low thermodynam...

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Main Authors: Dai, Chencheng, Wu, Qian, Wu, Tianze, Zhang, Yuwei, Sun, Libo, Wang, Xin, Fisher, Adrian C., Xu, Jason Zhichuan
Other Authors: School of Materials Science and Engineering
Format: Article
Language:English
Published: 2024
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Online Access:https://hdl.handle.net/10356/180921
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Institution: Nanyang Technological University
Language: English
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spelling sg-ntu-dr.10356-1809212024-11-05T01:34:27Z Suppressing product crossover and C-C bond cleavage in a glycerol membrane electrode assembly reformer Dai, Chencheng Wu, Qian Wu, Tianze Zhang, Yuwei Sun, Libo Wang, Xin Fisher, Adrian C. Xu, Jason Zhichuan School of Materials Science and Engineering The Cambridge Centre for Advanced Research and Education in Singapore Energy Research Institute @ NTU (ERI@N) Center for Advanced Catalysis Science and Technology Engineering Anion exchange Bond cleavages Generating hydrogen through water electrolysis is impeded by high costs and substantial energy consumption mainly due to high equilibrium potential and sluggish kinetics of the oxygen evolution reaction (OER). Glycerol oxidation reaction (GOR) is proposed as an alternative due to its low thermodynamic limit and value-added oxidation products. However, GOR in membrane electrolyzers faces challenges in achieving industrial-scale current densities as well as in addressing crossover issues. Here, we investigated five different membrane electrode assembly (MEA) configurations to perform GOR with various ion exchange membranes and catholyte. After systematic study, we present an innovative acid-alkali asymmetric cell design which operates with alkaline anolyte and acidic catholyte for electrochemical neutralization energy (ENE) harvesting to improve energy efficiency. The product anions crossover via anion exchange membrane (AEM) is also impeded since that the increasing concentration gradient-driven hydroxide ion crossover occupying the anion exchange channels in AEM and thus limits the product crossover of AEM. Such device also demonstrates the capability of impeding C-C bond cleavage to promote high-value C3 products generation and reduce carbon emission due to the lower degree of cell polarization and limited hydroxide ion supply at anode. Eventually, a whole-cell potential can be significantly reduced to 0.377 V while achieving a current density of 200 mA cm−2. Moreover, total faradaic efficiencies (FEs) of 55% and 84% for all C3 products and all liquid products can be achieved at a current density up to 1000 mA cm−2 Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) National Research Foundation (NRF) 2024-11-05T01:34:27Z 2024-11-05T01:34:27Z 2024 Journal Article Dai, C., Wu, Q., Wu, T., Zhang, Y., Sun, L., Wang, X., Fisher, A. C. & Xu, J. Z. (2024). Suppressing product crossover and C-C bond cleavage in a glycerol membrane electrode assembly reformer. Energy and Environmental Science, 17(17), 6350-6359. https://dx.doi.org/10.1039/d4ee01824a 1754-5692 https://hdl.handle.net/10356/180921 10.1039/d4ee01824a 2-s2.0-85200895824 17 17 6350 6359 en M22K2c0078 RG78/22 CREATE Energy and Environmental Science © 2024 The Authors. All rights reserved.
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering
Anion exchange
Bond cleavages
spellingShingle Engineering
Anion exchange
Bond cleavages
Dai, Chencheng
Wu, Qian
Wu, Tianze
Zhang, Yuwei
Sun, Libo
Wang, Xin
Fisher, Adrian C.
Xu, Jason Zhichuan
Suppressing product crossover and C-C bond cleavage in a glycerol membrane electrode assembly reformer
description Generating hydrogen through water electrolysis is impeded by high costs and substantial energy consumption mainly due to high equilibrium potential and sluggish kinetics of the oxygen evolution reaction (OER). Glycerol oxidation reaction (GOR) is proposed as an alternative due to its low thermodynamic limit and value-added oxidation products. However, GOR in membrane electrolyzers faces challenges in achieving industrial-scale current densities as well as in addressing crossover issues. Here, we investigated five different membrane electrode assembly (MEA) configurations to perform GOR with various ion exchange membranes and catholyte. After systematic study, we present an innovative acid-alkali asymmetric cell design which operates with alkaline anolyte and acidic catholyte for electrochemical neutralization energy (ENE) harvesting to improve energy efficiency. The product anions crossover via anion exchange membrane (AEM) is also impeded since that the increasing concentration gradient-driven hydroxide ion crossover occupying the anion exchange channels in AEM and thus limits the product crossover of AEM. Such device also demonstrates the capability of impeding C-C bond cleavage to promote high-value C3 products generation and reduce carbon emission due to the lower degree of cell polarization and limited hydroxide ion supply at anode. Eventually, a whole-cell potential can be significantly reduced to 0.377 V while achieving a current density of 200 mA cm−2. Moreover, total faradaic efficiencies (FEs) of 55% and 84% for all C3 products and all liquid products can be achieved at a current density up to 1000 mA cm−2
author2 School of Materials Science and Engineering
author_facet School of Materials Science and Engineering
Dai, Chencheng
Wu, Qian
Wu, Tianze
Zhang, Yuwei
Sun, Libo
Wang, Xin
Fisher, Adrian C.
Xu, Jason Zhichuan
format Article
author Dai, Chencheng
Wu, Qian
Wu, Tianze
Zhang, Yuwei
Sun, Libo
Wang, Xin
Fisher, Adrian C.
Xu, Jason Zhichuan
author_sort Dai, Chencheng
title Suppressing product crossover and C-C bond cleavage in a glycerol membrane electrode assembly reformer
title_short Suppressing product crossover and C-C bond cleavage in a glycerol membrane electrode assembly reformer
title_full Suppressing product crossover and C-C bond cleavage in a glycerol membrane electrode assembly reformer
title_fullStr Suppressing product crossover and C-C bond cleavage in a glycerol membrane electrode assembly reformer
title_full_unstemmed Suppressing product crossover and C-C bond cleavage in a glycerol membrane electrode assembly reformer
title_sort suppressing product crossover and c-c bond cleavage in a glycerol membrane electrode assembly reformer
publishDate 2024
url https://hdl.handle.net/10356/180921
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