Metallic Pd–Cu Alloy Phases Drive Selective Heterogeneous Electrochemical Ketonization of 1-Butene

Jiang, Chenyu; Moss, Benjamin; Lindenfelser, Alexis; Kim, Jung Tae; Li, Yuzhang; Manthiram, Karthish

doi:10.1021/acscatal.5c08675

Title: Metallic Pd–Cu Alloy Phases Drive Selective Heterogeneous Electrochemical Ketonization of 1-Butene

Journal Article · Tue Mar 31 00:00:00 UTC 2026 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.5c08675 · OSTI ID:3366386

Jiang, Chenyu ^[1]; Moss, Benjamin ^[1]; Lindenfelser, Alexis ^[1]; Kim, Jung Tae ^[1];

^[1];

^[1]

California Institute of Technology, Pasadena, CA (United States)

Electrification of 2-butanone synthesis via ketonization of 1-butene offers a viable pathway to reduce emissions associated with its production as a commodity chemical and enhance its prospects as a clean carbon-based synthetic fuel. However, the direct electrochemical ketonization of alkenes remains underexplored, with previous studies largely limited to epoxides and glycols. Herein, we report an electrochemical heterogeneous system optimized for 1-butene ketonization, converting 1-butene to 2- butanone using a bimetallic PdCu catalyst in aqueous electrolytes. The system achieves a Faradaic efficiency of 20% and a partial current density of 0.6 mA/cm² at 1.8 V_RHE. In comparison to monometallic Pd and oxidized PdCu analogs, the PdCu catalyst doubles the ketonization Faradaic efficiency and quadruples the production rate. Postelectrolysis characterization reveals that PdCu preserves the surface metallic alloy phase under anodic polarization, which likely accounts for the enhanced ketonization activity. This work demonstrates the significance of the Pd−Cu speciation dynamics and provides a framework for designing selective electrocatalysts for alkene ketonization.

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Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States); California Institute of Technology, Pasadena, CA (United States)

Sponsoring Organization:: Camille Dreyfus Teacher Scholar; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0021266; SC0022955

OSTI ID:: 3366386

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 8 Vol. 16; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
alkyls
catalyst characterization
catalysts
electrocatalysis
electrochemical 1-butene oxidation
heterogeneous catalysis
ketonization
methyl ethyl ketone
oxidation
oxides
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Title: Metallic Pd–Cu Alloy Phases Drive Selective Heterogeneous Electrochemical Ketonization of 1-Butene

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