Formate is identified as economically viable chemical fuel from electrochemical carbon dioxide reduction. However, the selectivity of current catalysts toward formate is limited by the competitive reaction such as HER. Herein, we propose a CeO modification strategy to improve the selectivity of catalysts for formate through tuning of the *OCHO intermediate, which is important for formate production.
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http://dx.doi.org/10.1021/acs.inorgchem.2c03844 | DOI Listing |
Angew Chem Int Ed Engl
January 2025
University of Electronic Science and Technology of China, State Key Laboratory of Electronic Thin Films and Integrated Devices, No. 2006, Xiyuan Avenue, High-tech Zone (West Area), 610054, Chengdu, CHINA.
Bismuth oxide (Bi2O3) emerges as a potent catalyst for converting CO2 to formic acid (HCOOH), leveraging its abundant lattice oxygen and the high activity of its Bi-O bonds. Yet, its durability is usually impeded by the loss of lattice oxygen causing structure alteration and destabilized active bonds. Herein, we report an innovative approach via the interstitial incorporation of indium (In) into the Bi2O3, significantly enhancing bond stability and preserving lattice oxygen.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies, College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing, 210016, P. R. China.
Halide anion adsorption on transition metals can improve the performance of electrochemical CO reduction reaction (CORR), while the specific reaction mechanisms governing selective CORR pathways remain unclear. In this study, we reveal for the first time the distinct pathway switching between gaseous (CO) and liquid products (formate and ethanol) on the well-defined Ag-Cu nanostructures with controlled chlorination. We show that CO conversion to CO on Ag/AgCl can be tuned by adjusting the thickness of AgCl layer, achieving a high selectivity over a broad potential range in a 0.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
November 2024
Department of Chemical and Biomolecular Engineering, National, University of Singapore, Singapore, 117585, Republic of Singapore.
The electrochemical conversion of low-concentration CO feedstock to value-added chemicals and fuels is a promising pathway for achieving direct valorization of waste gas streams. However, this is challenging due to significant competition from the hydrogen evolution reaction (HER) and lowered CO reduction (COR) kinetics as compared to systems that employ pure CO. Here we show that terephthalic acid (TPA) functionalization can boost selectivity towards COR and suppress HER over a range of catalysts including Bi, Cu and Zn.
View Article and Find Full Text PDFJ Colloid Interface Sci
January 2025
Guizhou Provincial Key Laboratory of Green Chemical and Clean Energy Technology, School of Chemistry and Chemical Engineering, Guizhou University, Guiyang 550025, China; School of Civil Engineering, Guizhou Institute of Technology, Guiyang 550003, China. Electronic address:
Electrochemical CO reduction reaction (CORR) is one of the most attractive measures to achieve the carbon neutral goal by converting CO into high-value chemicals such as formate. Si in Bi silicates is promising to enhance CO adsorption and activation due to its strong oxygenophilicity. Whereas, its role in boosting CORR via the cheap Bi-based catalysts is still not clear.
View Article and Find Full Text PDFNanoscale
August 2024
School of Energy and Chemical Engineering, Xiamen University Malaysia, Sepang, Selangor Darul Ehsan, 43900, Malaysia.
In the context of catalytic CO reduction (CORR), the interference of the inherent hydrogen evolution reaction (HER) and the possible selectivity towards CO have posed a significant challenge to the generation of formic acid. To address this hurdle, in this work, we have investigated the impact of different single-atom metal catalysts on tuning selectivity by employing density functional theory (DFT) calculations to scrutinize the reaction pathways. Single-atom catalysts supported on carbon-based systems have proven to be pivotal in altering both the activity and selectivity of the CORR.
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