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
Inorganic Chemistry and Catalysis Debye Institute for Nanomaterials Science Utrecht University 3584 CG Utrecht (The Netherlands.
Laboratory of Inorganic Materials and Catalysis Department of Chemical Engineering and Chemistry Eindhoven University of Technology 5600 MB Eindhoven (The Netherlands.
ChemCatChem. 2022 Sep 20;14(18):e202200754. doi: 10.1002/cctc.202200754. Epub 2022 Jul 14.
It remains a real challenge to control the selectivity of the electrocatalytic CO reduction (eCOR) 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. The metal ions were extracted from the metallurgical waste through simple chemical treatment with ammonium chloride, and CuPb electrocatalysts with tunable compositions were fabricated through electrodeposition at varying cathodic potentials. X-ray spectroscopy techniques showed that the pristine electrocatalysts consist of Cu, Cu and Pb domains, and no evidence for alloy formation was found. We found a volcano-shape relationship between eCOR 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 CuPb, which was four times higher than that of pure Cu, under the same electrocatalytic conditions. Raman spectroscopy revealed that the optimal amount of Pb effectively improved the reducibility of the pristine Cu and Pb 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 CO reduction through valorization of metallurgical waste.
控制电催化CO还原(eCOR)反应对有价值化学品和燃料的选择性仍然是一项真正的挑战。大多数电催化剂由不可再生金属资源制成,这阻碍了它们的大规模应用。在此,我们报告了从工业冶金废料制备双金属铜铅(CuPb)电催化剂的方法。通过用氯化铵进行简单化学处理从冶金废料中提取金属离子,并通过在不同阴极电位下进行电沉积制备了成分可调的CuPb电催化剂。X射线光谱技术表明,原始电催化剂由Cu、Cu和Pb域组成,未发现合金形成的证据。我们发现eCOR对双电子产物(如CO)的选择性与Cu和Pb的元素比之间存在火山形状关系。在相同电催化条件下,CuPb对CO的法拉第效率最高,比纯Cu高四倍。拉曼光谱表明,适量的Pb有效地提高了原始Cu和Pb域还原为金属Cu和Pb的能力,通过协同效应提高了对CO的选择性。这项工作为通过冶金废料的价值化设计和调节双金属电催化剂用于CO还原的选择性提供了一个思路框架。