One‐Pot Synthesis of Tensile‐Strained PdRuCu Icosahedra toward Electrochemical Hydrogenation of Alkene

Abstract Electrochemical hydrogenation (ECH) uses electricity to drive proton (H + ) reduction for hydrogenation, which can greatly reduce energy supply and environmental pollution, representing an ideal alternative to traditional thermal hydrogenation. In this work, we put forward tensile‐strained PdRuCu alloy to promote ECH. Tensile strain promotes the adsorption of C=C by changing the d ‐band center. Meanwhile, alloying Ru and Cu into Pd lattice facilitates hydrogenation by weakening Pd−H bonding. Therefore, PdRuCu icosahedra display excellent ECH performance of 2‐methyl‐3‐buten‐2‐ol (MBE) with specific activity of 227.4 μmol MBE nm −2 min −1 at −0.3 V versus reversible hydrogen electrode (RHE), about 16.1 and 10.5 times higher than that of commercial Pd/C and Ru/C, respectively. In addition, PdRuCu icosahedra was excellent in the scaling up of substrate concentration combined with anisyl alcohol oxidation to produce high‐value added anisaldehyde at anode. This work provides a guideline for the rational design of highly active and durable metallic catalyst in ECH.