Gas-phase electrochemical CO2 reduction on silver-copper BTC MOF in a zero-gap membrane electrode assembly.

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Title: Gas-phase electrochemical CO2 reduction on silver-copper BTC MOF in a zero-gap membrane electrode assembly.
Authors: Nambi, Ashwin1 (AUTHOR), Chatzitakis, Athanasios2 (AUTHOR), Olsbye, Unni2 (AUTHOR), Hjelm, Johan1 (AUTHOR), Zhao, Yujie1 (AUTHOR), Kaiser, Andreas1 (AUTHOR) akai@dtu.dk
Source: Electrochimica Acta. Dec2024, Vol. 506, pN.PAG-N.PAG. 1p.
Subjects: Hydrogen evolution reactions, Carbon dioxide, Ionic structure, Water supply, Ligands (Chemistry), Electrolytic reduction
Abstract: • A fast co-precipitation method using a deprotonated BTC ligand was developed to be able to incorporate Ag ions into the structure of bimetallic AgCu-BTC MOFs. • For the first time, the electrocatalytic reduction of CO 2 was investigated in the gas phase and as a function of different humidity levels on AgCu-BTC MOF. • The presence of Ag in the Cu-BTC based framework improves the gas phase CO 2 reduction reaction towards CO and suppresses the competing H 2 evolution. • Lowering the humidity levels in the CO 2 gas stream enhances CO production due to the reduced availability of water. Bimetallic AgCu-BTC MOFs, derived from Cu-BTC (HKUST-1), have been synthesized by fast co-precipitation method and evaluated for CO 2 reduction reaction (CO 2 RR) using humidified CO 2 gas in a zero-gap configuration. Three compositions with varying Ag content – AgCu-1 (9.4 at.%), AgCu-2 (12.5 at.%), and AgCu-3 (16.5 at.%) – were characterized by SEM-EDS, PXRD, FTIR, and XPS. These structural analyzes confirmed the formation of a low-crystalline AgCu-BTC MOF with Ag+1 ions coordinated to the BTC framework. Electrochemical tests (CV and LSV) revealed that AgCu-3 MOF, with the highest Ag content (16.5 at.%), exhibited a more positive onset potential at -0.65 V vs Ag/AgCl compared to HKUST-1 MOF, indicating enhanced CO 2 RR activity, owing to Ag incorporation. Constant potential (CP) experiments showed that AgCu-3 MOF predominantly produced CO and H 2 , achieving faradaic efficiency of approximately 65 % for CO production and 5 % for H 2 production. Moreover, lowering the relative humidity (RH%) in the inlet CO 2 gas stream from 80% to 20% increased CO production by 2-fold from 6.2 µmol s-1 cm-2 to 13 µmol s-1 cm-2, simultaneously suppressing the hydrogen evolution reaction (HER). This reduction in humidity resulted in an increased local concentration of CO 2 at the catalyst site, leading to an enhanced CO 2 RR rate. However, substantial morphological changes have been observed in the AgCu-3 MOF after the CP experiment under humid CO 2 reduction conditions. [ABSTRACT FROM AUTHOR]
Copyright of Electrochimica Acta is the property of Pergamon Press - An Imprint of Elsevier Science and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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  Label: Title
  Group: Ti
  Data: Gas-phase electrochemical CO2 reduction on silver-copper BTC MOF in a zero-gap membrane electrode assembly.
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  Data: <searchLink fieldCode="AR" term="%22Nambi%2C+Ashwin%22">Nambi, Ashwin</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Chatzitakis%2C+Athanasios%22">Chatzitakis, Athanasios</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Olsbye%2C+Unni%22">Olsbye, Unni</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Hjelm%2C+Johan%22">Hjelm, Johan</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Zhao%2C+Yujie%22">Zhao, Yujie</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Kaiser%2C+Andreas%22">Kaiser, Andreas</searchLink><relatesTo>1</relatesTo> (AUTHOR)<i> akai@dtu.dk</i>
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  Data: <searchLink fieldCode="JN" term="%22Electrochimica+Acta%22">Electrochimica Acta</searchLink>. Dec2024, Vol. 506, pN.PAG-N.PAG. 1p.
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  Data: <searchLink fieldCode="DE" term="%22Hydrogen+evolution+reactions%22">Hydrogen evolution reactions</searchLink><br /><searchLink fieldCode="DE" term="%22Carbon+dioxide%22">Carbon dioxide</searchLink><br /><searchLink fieldCode="DE" term="%22Ionic+structure%22">Ionic structure</searchLink><br /><searchLink fieldCode="DE" term="%22Water+supply%22">Water supply</searchLink><br /><searchLink fieldCode="DE" term="%22Ligands+%28Chemistry%29%22">Ligands (Chemistry)</searchLink><br /><searchLink fieldCode="DE" term="%22Electrolytic+reduction%22">Electrolytic reduction</searchLink>
– Name: Abstract
  Label: Abstract
  Group: Ab
  Data: • A fast co-precipitation method using a deprotonated BTC ligand was developed to be able to incorporate Ag ions into the structure of bimetallic AgCu-BTC MOFs. • For the first time, the electrocatalytic reduction of CO 2 was investigated in the gas phase and as a function of different humidity levels on AgCu-BTC MOF. • The presence of Ag in the Cu-BTC based framework improves the gas phase CO 2 reduction reaction towards CO and suppresses the competing H 2 evolution. • Lowering the humidity levels in the CO 2 gas stream enhances CO production due to the reduced availability of water. Bimetallic AgCu-BTC MOFs, derived from Cu-BTC (HKUST-1), have been synthesized by fast co-precipitation method and evaluated for CO 2 reduction reaction (CO 2 RR) using humidified CO 2 gas in a zero-gap configuration. Three compositions with varying Ag content – AgCu-1 (9.4 at.%), AgCu-2 (12.5 at.%), and AgCu-3 (16.5 at.%) – were characterized by SEM-EDS, PXRD, FTIR, and XPS. These structural analyzes confirmed the formation of a low-crystalline AgCu-BTC MOF with Ag+1 ions coordinated to the BTC framework. Electrochemical tests (CV and LSV) revealed that AgCu-3 MOF, with the highest Ag content (16.5 at.%), exhibited a more positive onset potential at -0.65 V vs Ag/AgCl compared to HKUST-1 MOF, indicating enhanced CO 2 RR activity, owing to Ag incorporation. Constant potential (CP) experiments showed that AgCu-3 MOF predominantly produced CO and H 2 , achieving faradaic efficiency of approximately 65 % for CO production and 5 % for H 2 production. Moreover, lowering the relative humidity (RH%) in the inlet CO 2 gas stream from 80% to 20% increased CO production by 2-fold from 6.2 µmol s-1 cm-2 to 13 µmol s-1 cm-2, simultaneously suppressing the hydrogen evolution reaction (HER). This reduction in humidity resulted in an increased local concentration of CO 2 at the catalyst site, leading to an enhanced CO 2 RR rate. However, substantial morphological changes have been observed in the AgCu-3 MOF after the CP experiment under humid CO 2 reduction conditions. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
  Group: Ab
  Data: <i>Copyright of Electrochimica Acta is the property of Pergamon Press - An Imprint of Elsevier Science and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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RecordInfo BibRecord:
  BibEntity:
    Identifiers:
      – Type: doi
        Value: 10.1016/j.electacta.2024.144763
    Languages:
      – Code: eng
        Text: English
    PhysicalDescription:
      Pagination:
        PageCount: 1
        StartPage: N.PAG
    Subjects:
      – SubjectFull: Hydrogen evolution reactions
        Type: general
      – SubjectFull: Carbon dioxide
        Type: general
      – SubjectFull: Ionic structure
        Type: general
      – SubjectFull: Water supply
        Type: general
      – SubjectFull: Ligands (Chemistry)
        Type: general
      – SubjectFull: Electrolytic reduction
        Type: general
    Titles:
      – TitleFull: Gas-phase electrochemical CO2 reduction on silver-copper BTC MOF in a zero-gap membrane electrode assembly.
        Type: main
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            NameFull: Nambi, Ashwin
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            NameFull: Chatzitakis, Athanasios
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            NameFull: Olsbye, Unni
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            NameFull: Hjelm, Johan
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            NameFull: Zhao, Yujie
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            NameFull: Kaiser, Andreas
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          Dates:
            – D: 01
              M: 12
              Text: Dec2024
              Type: published
              Y: 2024
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              Value: 00134686
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              Value: 506
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            – TitleFull: Electrochimica Acta
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