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Solar-Driven Reduction of 1 atm of CO_2 to Formate at 10% Energy-Conversion Efficiency by Use of a TiO_2-Protected III–V Tandem Photoanode in Conjunction with a Bipolar Membrane and a Pd/C Cathode

Zhou, Xinghao and Liu, Rui and Sun, Ke and Chen, Yikai and Verlage, Erik and Francis, Sonja A. and Lewis, Nathan S. and Xiang, Chengxiang (2016) Solar-Driven Reduction of 1 atm of CO_2 to Formate at 10% Energy-Conversion Efficiency by Use of a TiO_2-Protected III–V Tandem Photoanode in Conjunction with a Bipolar Membrane and a Pd/C Cathode. ACS Energy Letters, 1 (4). pp. 764-770. ISSN 2380-8195. http://resolver.caltech.edu/CaltechAUTHORS:20161003-141800305

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Abstract

A solar-driven CO_2 reduction (CO_2R) cell was constructed, consisting of a tandem GaAs/InGaP/TiO_2/Ni photoanode in 1.0 M KOH(aq) (pH = 13.7) to facilitate the oxygen-evolution reaction (OER), a Pd/C nanoparticle-coated Ti mesh cathode in 2.8 M KHCO_3(aq) (pH = 8.0) to perform the CO_2R reaction, and a bipolar membrane to allow for steady-state operation of the catholyte and anolyte at different bulk pH values. At the operational current density of 8.5 mA cm^(–2), in 2.8 M KHCO_3(aq), the cathode exhibited <100 mV overpotential and >94% Faradaic efficiency for the reduction of 1 atm of CO_2(g) to formate. The anode exhibited a 320 ± 7 mV overpotential for the OER in 1.0 M KOH(aq), and the bipolar membrane exhibited ∼480 mV voltage loss with minimal product crossovers and >90 and >95% selectivity for protons and hydroxide ions, respectively. The bipolar membrane facilitated coupling between two electrodes and electrolytes, one for the CO_2R reaction and one for the OER, that typically operate at mutually different pH values and produced a lower total cell overvoltage than known single-electrolyte CO_2R systems while exhibiting ∼10% solar-to-fuels energy-conversion efficiency.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/acsenergylett.6b00317DOIArticle
http://pubs.acs.org/doi/abs/10.1021/acsenergylett.6b00317PublisherArticle
http://pubs.acs.org/doi/suppl/10.1021/acsenergylett.6b00317PublisherSupporting Information
ORCID:
AuthorORCID
Zhou, Xinghao0000-0001-9229-7670
Sun, Ke0000-0001-8209-364X
Lewis, Nathan S.0000-0001-5245-0538
Additional Information:© 2016 American Chemical Society. Received: August 2, 2016; Accepted: September 9, 2016; Publication Date (Web): September 9, 2016. This material is based on work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. S.A.F. acknowledges the Resnick Sustainability Institute at Caltech for a Postdoctoral Fellowship. The authors also thank N. Dalleska (Caltech) for his assistance with measurements and analysis of the ICPMS and TIC data. The authors declare no competing financial interest.
Group:Resnick Sustainability Institute, JCAP
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Resnick Sustainability InstituteUNSPECIFIED
Record Number:CaltechAUTHORS:20161003-141800305
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20161003-141800305
Official Citation:Solar-Driven Reduction of 1 atm of CO2 to Formate at 10% Energy-Conversion Efficiency by Use of a TiO2-Protected III–V Tandem Photoanode in Conjunction with a Bipolar Membrane and a Pd/C Cathode Xinghao Zhou, Rui Liu, Ke Sun, Yikai Chen, Erik Verlage, Sonja A. Francis, Nathan S. Lewis, and Chengxiang Xiang ACS Energy Letters 2016 1 (4), 764-770 DOI: 10.1021/acsenergylett.6b00317
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:70765
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:03 Oct 2016 21:39
Last Modified:31 Mar 2017 18:32

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