Affiliation:
1. Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University Shanghai 200438 China
2. State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering Donghua University Shanghai 201620 China
Abstract
AbstractThe electrochemical reduction of CO or CO2 into C2+ products has mostly been focused on Cu‐based catalysts. Although Ag has also been predicted as a possible catalyst for the CO‐to‐C2+ conversion from the thermodynamic point of view, however, due to its weak CO binding strength, CO rapidly desorbs from the Ag surface rather than participates in deep reduction. In this work, we demonstrate that single‐atomic Pd sites doped in Ag lattice can tune the CO adsorption behavior and promote the deep reduction of CO toward C2 products. The monodispersed Pd−Agn sites enable the CO adsorption with both Pd‐atop (PdL) and Pd−Ag bridge (PdAgB) configurations, which can increase the CO coverage and reduce the C−C coupling energy barrier. Under room temperature and ambient pressure, the Pd1Ag10 alloy catalyst exhibited a total CO‐to‐C2 Faradaic efficiency of ~37 % at −0.83 V, with appreciable current densities and electrochemical stability, thus featuring unconventional non‐Cu electrocatalytic CO‐to‐C2 conversion capability.