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Title: Continuous production of pure liquid fuel solutions via electrocatalytic CO 2 reduction using solid-electrolyte devices

Abstract

Electrocatalytic CO 2 reduction is often carried out in a solution electrolyte such as KHCO 3(aq), which allows for ion conduction between electrodes. Thus, liquid products that form are in a mixture with the dissolved salts, requiring energy-intensive downstream separation. In this work, we report continuous electrocatalytic conversion of CO 2 to pure liquid fuel solutions in cells that utilize solid electrolytes, where electrochemically generated cations (such as H+) and anions (such as HCOO–) are combined to form pure product solutions without mixing with other ions. Using a HCOOH-selective (Faradaic efficiencies>90%) and easily scaled Bi catalyst at the cathode, we demonstrate production of pure HCOOH solutions with concentrations up to 12M. We also show 100h continuous and stable generation of 0.1 M HCOOH with negligible degradation in selectivity and activity. Production of other electrolyte-free C 2+ liquid oxygenate solutions, including acetic acid, ethanol and n-propanol, are also demonstrated using a Cu catalyst. Lastly, we show that our CO 2 reduction cell with solid electrolytes can be modified to suit other, more complex practical applications.

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [4];  [5];  [6]; ORCiD logo [3]; ORCiD logo [2]
  1. Rice Univ., Houston, TX (United States); Harvard Univ., Cambridge, MA (United States)
  2. Rice Univ., Houston, TX (United States)
  3. King Abdullah Univ. of Science and Technology (KAUST), Thuwal (Saudi Arabia)
  4. Harvard Univ., Cambridge, MA (United States)
  5. Northeastern Univ., Burlington, MA (United States)
  6. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1571402
Report Number(s):
BNL-212214-2019-JAAM
Journal ID: ISSN 2058-7546
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Energy
Additional Journal Information:
Journal Volume: 4; Journal Issue: 9; Journal ID: ISSN 2058-7546
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Xia, Chuan, Zhu, Peng, Jiang, Qiu, Pan, Ying, Liang, Wentao, Stavitsk, Eli, Alshareef, Husam N., and Wang, Haotian. Continuous production of pure liquid fuel solutions via electrocatalytic CO2 reduction using solid-electrolyte devices. United States: N. p., 2019. Web. doi:10.1038/s41560-019-0451-x.
Xia, Chuan, Zhu, Peng, Jiang, Qiu, Pan, Ying, Liang, Wentao, Stavitsk, Eli, Alshareef, Husam N., & Wang, Haotian. Continuous production of pure liquid fuel solutions via electrocatalytic CO2 reduction using solid-electrolyte devices. United States. doi:10.1038/s41560-019-0451-x.
Xia, Chuan, Zhu, Peng, Jiang, Qiu, Pan, Ying, Liang, Wentao, Stavitsk, Eli, Alshareef, Husam N., and Wang, Haotian. Mon . "Continuous production of pure liquid fuel solutions via electrocatalytic CO2 reduction using solid-electrolyte devices". United States. doi:10.1038/s41560-019-0451-x.
@article{osti_1571402,
title = {Continuous production of pure liquid fuel solutions via electrocatalytic CO2 reduction using solid-electrolyte devices},
author = {Xia, Chuan and Zhu, Peng and Jiang, Qiu and Pan, Ying and Liang, Wentao and Stavitsk, Eli and Alshareef, Husam N. and Wang, Haotian},
abstractNote = {Electrocatalytic CO2 reduction is often carried out in a solution electrolyte such as KHCO3(aq), which allows for ion conduction between electrodes. Thus, liquid products that form are in a mixture with the dissolved salts, requiring energy-intensive downstream separation. In this work, we report continuous electrocatalytic conversion of CO2 to pure liquid fuel solutions in cells that utilize solid electrolytes, where electrochemically generated cations (such as H+) and anions (such as HCOO–) are combined to form pure product solutions without mixing with other ions. Using a HCOOH-selective (Faradaic efficiencies>90%) and easily scaled Bi catalyst at the cathode, we demonstrate production of pure HCOOH solutions with concentrations up to 12M. We also show 100h continuous and stable generation of 0.1 M HCOOH with negligible degradation in selectivity and activity. Production of other electrolyte-free C2+ liquid oxygenate solutions, including acetic acid, ethanol and n-propanol, are also demonstrated using a Cu catalyst. Lastly, we show that our CO2 reduction cell with solid electrolytes can be modified to suit other, more complex practical applications.},
doi = {10.1038/s41560-019-0451-x},
journal = {Nature Energy},
number = 9,
volume = 4,
place = {United States},
year = {2019},
month = {9}
}

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Works referenced in this record:

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