Waste-Derived Copper-Lead Electrocatalysts for CO2 Reduction
Yang, Shuang; An, Hongyu; Anastasiadou, Dimitra; Xu, Wenjie; Wu, Longfei; Wang, Hui; de Ruiter, Jim; Arnouts, Sven; Figueiredo, Marta C.; Bals, Sara; Altantzis, Thomas; van der Stam, Ward; Weckhuysen, Bert M.
(2022) ChemCatChem, volume 14, issue 18, pp. 1 - 10
(Article)
Abstract
It remains a real challenge to control the selectivity of the electrocatalytic CO2 reduction (eCO2R) reaction to valuable chemicals and fuels. Most of the electrocatalysts are made of non-renewable metal resources, which hampers their large-scale implementation. Here, we report the preparation of bimetallic copper-lead (CuPb) electrocatalysts from industrial metallurgical waste.
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The metal ions were extracted from the metallurgical waste through simple chemical treatment with ammonium chloride, and CuxPby electrocatalysts with tunable compositions were fabricated through electrodeposition at varying cathodic potentials. X-ray spectroscopy techniques showed that the pristine electrocatalysts consist of Cu0, Cu1+ and Pb2+ domains, and no evidence for alloy formation was found. We found a volcano-shape relationship between eCO2R selectivity toward two electron products, such as CO, and the elemental ratio of Cu and Pb. A maximum Faradaic efficiency towards CO was found for Cu9.00Pb1.00, which was four times higher than that of pure Cu, under the same electrocatalytic conditions. In situ Raman spectroscopy revealed that the optimal amount of Pb effectively improved the reducibility of the pristine Cu1+ and Pb2+ domains to metallic Cu and Pb, which boosted the selectivity towards CO by synergistic effects. This work provides a framework of thinking to design and tune the selectivity of bimetallic electrocatalysts for CO2 reduction through valorization of metallurgical waste.
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Keywords: Catalysis, Physical and Theoretical Chemistry, Organic Chemistry, Inorganic Chemistry
ISSN: 1867-3880
Publisher: Wiley - VCH Verlag GmbH & CO. KGaA
Note: Funding Information: S.Y and B.M.W. acknowledge support from the EU Framework Programme for Research and Innovation Horizon 2020 (SOCRATES-721385; project website: http://etn-socrates.eu/). W.v.d.S., M.C.F. and B.M.W. acknowledge support from the Strategic UU-TU/e Alliance project ‘Joint Centre for Chemergy Research’. S.B. acknowledges support from the European Research Council (ERC Consolidator Grant #815128 REALNANO). S.A. and T.A. acknowledge funding from the University of Antwerp Research fund (BOF). The Beijing Synchrotron Radiation Facility (1W1B, BSRF) is acknowledged for the beamtime. We are grateful to Annelies van der Bok and Bas Salzmann (Condensed Matter and Interfaces, Utrecht University, UU) for the support with the ICP-OES measurements. The authors thank dr. Robin Geitenbeek, Nikos Nikolopoulos, Ioannis Nikolopoulos, Jochem Wijten and Joris Janssens (Inorganic Chemistry and Catalysis, UU) for helpful discussions and technical support. The authors also thank Yuang Piao (Materials Chemistry and Catalysis, UU) for the help in the preparation of the figures of the article. Funding Information: S.Y and B.M.W. acknowledge support from the EU Framework Programme for Research and Innovation Horizon 2020 (SOCRATES‐721385; project website: http://etn‐socrates.eu/ ). W.v.d.S., M.C.F. and B.M.W. acknowledge support from the Strategic UU‐TU/e Alliance project ‘Joint Centre for Chemergy Research’. S.B. acknowledges support from the European Research Council (ERC Consolidator Grant #815128 REALNANO). S.A. and T.A. acknowledge funding from the University of Antwerp Research fund (BOF). The Beijing Synchrotron Radiation Facility (1W1B, BSRF) is acknowledged for the beamtime. We are grateful to Annelies van der Bok and Bas Salzmann (Condensed Matter and Interfaces, Utrecht University, UU) for the support with the ICP‐OES measurements. The authors thank dr. Robin Geitenbeek, Nikos Nikolopoulos, Ioannis Nikolopoulos, Jochem Wijten and Joris Janssens (Inorganic Chemistry and Catalysis, UU) for helpful discussions and technical support. The authors also thank Yuang Piao (Materials Chemistry and Catalysis, UU) for the help in the preparation of the figures of the article. Publisher Copyright: © 2022 The Authors. ChemCatChem published by Wiley-VCH GmbH.
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