Bi2O3 Nanosheets Grown on Carbon Nanofiber with Inherent Hydrophobicity for High-Performance CO2 Electroreduction in a Wide Potential Window
- 21 October 2021
- journal article
- research article
- Published by American Chemical Society (ACS) in ACS Nano
- Vol. 15 (11), 17757-17768
- https://doi.org/10.1021/acsnano.1c05737
Abstract
The ever-increasing concern for adverse climate changes has propelled worldwide research on the reduction of CO2 emission. In this regard, CO2 electroreduction (CER) to formate is one of the promising approaches to converting CO2 to a useful product. However, to achieve a high production rate of formate, the existing catalysts for CER fall short of expectation in maintaining the high formate selectivity and activity over a wide potential window. Through this study, we report that Bi2O3 nanosheets (NSs) grown on carbon nanofiber (CNF) with inherent hydrophobicity achieve a peak formate current density of 102.1 mA cm–2 and high formate Faradaic efficiency of >93% over a very wide potential window of 1000 mV. To the best of our knowledge, this outperforms all the relevant achievements reported so far. In addition, the Bi2O3 NSs on CNF demonstrate a good antiflooding capability when operating in a flow cell system and can deliver a current density of 300 mA cm–2. Molecular dynamics simulations indicate that the hydrophobic carbon surface can repel water molecules to form a robust solid–liquid–gas triple-phase boundary and a concentrated CO2 layer; both can boost CER activity with the local high concentration of CO2 and through inhibiting the hydrogen evolution reaction (HER) by reducing proton contacts. This water-repelling effect also increases the local pH at the catalyst surface, thus inhibiting HER further. More significantly, the concept and methodology of this hydrophobic engineering could be broadly applicable to other formate-producing materials from CER.Keywords
Funding Information
- Natural Sciences and Engineering Research Council of Canada
- Discovery Grant (GRPIN-2016-05494)
This publication has 62 references indexed in Scilit:
- In Situ Surface-Enhanced Raman Spectroscopy of the Electrochemical Reduction of Carbon Dioxide on Silver with 3,5-Diamino-1,2,4-TriazoleThe Journal of Physical Chemistry C, 2014
- Formic acid as a hydrogen source – recent developments and future trendsEnergy & Environmental Science, 2012
- Systematic studies of covalent functionalization of carbon nanotubes via argon plasma-assisted UV graftingNanotechnology, 2007
- A general purpose model for the condensed phases of water: TIP4P/2005The Journal of Chemical Physics, 2005
- Calculation for the cathode surface concentrations in the electrochemical reduction of CO2 in KHCO3 solutionsJournal of Applied Electrochemistry, 2005
- GROMACS: Fast, flexible, and freeJournal of Computational Chemistry, 2005
- Potential energy functions for atomic-level simulations of water and organic and biomolecular systemsProceedings of the National Academy of Sciences of the United States of America, 2005
- History of the Chlor-Alkali IndustryPublished by Springer Science and Business Media LLC ,2005
- The Brønsted–Evans–Polanyi relation and the volcano curve in heterogeneous catalysisJournal of Catalysis, 2004
- Evaluation and Reparametrization of the OPLS-AA Force Field for Proteins via Comparison with Accurate Quantum Chemical Calculations on PeptidesThe Journal of Physical Chemistry B, 2001