Rh/Al Nanoantenna Photothermal Catalyst for Wide-Spectrum Solar-Driven CO<sub>2</sub> Methanation with Nearly 100% Selectivity
Gao Fu, Minghang Jiang, Jie Liu, Kaiqiang Zhang, Yi Hu, Yan Xiong, Anyang Tao, Zuoxiu Tie, Zhong Jin
Abstract
Solar-powered CO2 conversion represents a promising green and sustainable approach for achieving a carbon-neutral economy. However, the rational design of a wide-spectrum sunlight-driven catalysis system for effective CO2 reduction is an ongoing challenge. Herein, we report the preparation of a rhodium/aluminum (Rh/Al) nanoantenna photothermal catalyst that can utilize a broad range of sunlight (from ultraviolet to the near-infrared region) for highly efficient CO2 methanation, achieving a high CH4 selectivity of nearly 100% and an unprecedented CH4 productivity of 550 mmol·g–1·h–1 under concentrated simulated solar irradiation (11.3 W·cm–2). Detailed control experiment results verified that the CO2 methanation process was facilitated by the localized surface plasmonic resonance and nanoantenna effects of the Rh/Al nanostructure under light irradiation. In operando temperature-programmed Fourier transform infrared spectroscopy confirmed that CO2 methanation on the Rh/Al nanoantenna catalyst was a multistep reaction with CO as a key intermediate. The design of a wide-spectrum solar-driven photothermal catalyst provides a feasible strategy for boosting CO2-to-fuel conversion.