Carbonized wood membrane decorated with AuPd alloy nanoparticles as an efficient self-supported electrode for electrocatalytic CO2 reduction

摘要

Efficient electrocatalytic reduction of CO2 to value-added chemicals and fuels is a promising technology for mitigating energy shortage and pollution issues yet highly relay on the development of high-performance electrocatalysts. Herein, we develop an effective strategy to fabricate carbonized wood membrane (CW) decorated with AuPd alloy nanoparticles with tunable composition (termed as AuPd@CW) as self-supported electrodes for efficient electrocatalytic CO2 reduction. The uniformly distributed AuPd nanoparticles on wood matrix are first achieved through the in-situ reduction of metal cations by the lignin content in wood. Subsequently, two-step carbonization was employed to promote the alloying of AuPd nanoparticles and the formation of CW. The AuPd@CW membrane electrode features an integrated macroscopic structure with numerous open and aligned channels for rapid electron transfer and mass diffusion and well-dispersed AuPd alloy nanoparticles as active sites for the CO2 reduction. The optimal Au95Pd5@CW electrode affords a high selectivity for CO2 electroreduction with a maximum CO faradaic efficiency (FECO) of 82 at an overpotential of 0.49 V, much higher than those obtained on Au@CW and Pd@CW electrodes. The CO current density and FECO remain relatively stable during a 12 h electrolysis reaction. In addition, density functional theory (DFT) calculations reveal that alloying Au with Pd enables a balance between the formation of intermediate COOH* and the desorption of CO on the surface of AuPd nanoparticles, thus enhancing the selectivity of CO production. This work offers an effective strategy for the fabrication of bimetallic alloys supported on wood-based carbon membrane as a practical electrode for electrochemical energy conversion. (C) 2021 Elsevier Inc. All rights reserved.