Plasmon-Enhanced Electrochemical CO 2 Reduction on Dendritic Gold Nanostructures with High Selectivity and Turnover Frequency

作者：Yubin Huang, Yen-Ken Li, Shivaraj B. Patil, Di‐Yan Wang, U‐Ser Jeng, Ying‐Huang Lai · 发表于：ACS Applied Energy Materials · 年份：2025 · DOI：10.1021/acsaem.5c01299 · 被引用次数：4 · 研究领域：CO2 Reduction Techniques and Catalysts、Electrocatalysts for Energy Conversion、Advanced Thermoelectric Materials and Devices

High Resolution Image Download MS PowerPoint Slide The electrochemical reduction of carbon dioxide (CO 2 RR) to carbon monoxide (CO) presents a promising pathway for sustainable fuel production and greenhouse gas mitigation. Herein, we report the fabrication of three-dimensional dendritic gold (Au-D) nanostructures via pulsed electrodeposition for efficient and selective CO 2 RR under both electrochemical and photoelectrochemical conditions. The dendritic morphology features high-curvature tips and abundant high-index facets, resulting in a large electrochemically active surface area and strong localized surface plasmon resonance (LSPR) effect. Under AM1.5G illumination, the LSPR-induced hot carriers and local heating synergistically enhance the CO 2 reduction activity while suppressing the competing hydrogen evolution reaction (HER). The Au-D electrode achieves a maximum CO Faradaic efficiency of 88.8% and a turnover frequency (TOF) of 14.8 s –1 at −0.525 V vs RHE under illumination, representing one of the highest reported performances for Au-based CO 2 RR catalysts. In situ surface-enhanced Raman spectroscopy (SERS) reveals the formation of *CO 2 – and *COOH intermediates, indicating that the formation of *CO 2 – is the rate-determining step. Temperature-dependent and light modulation experiments confirm that LSPR activation enhances both the electronic and thermal catalytic pathways, enabling low-overpotential CO 2 -to-CO conversion with high stability. These findings pro...