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

CHEMELECTROCHEM(2021)

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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 mu mol(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.
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Key words
electrochemical hydrogenation, tensile strain, icosahedra, anisaldehyde, alloy
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