Rh/Al Nanoantenna Photothermal Catalyst for Wide-Spectrum Solar-Driven CO<sub>2</sub> Methanation with Nearly 100% Selectivity.

Fu, Gao; Jiang, Minghang; Liu, Jie; Zhang, Kaiqiang; Hu, Yi; Xiong, Yan; Tao, Anyang; Tie, Zuoxiu et al. · Nano Lett · 2021

basic_science · Level V

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Abstract

Solar-powered CO<sub>2</sub> 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 CO<sub>2</sub> 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 CO<sub>2</sub> methanation, achieving a high CH<sub>4</sub> selectivity of nearly 100% and an unprecedented CH<sub>4</sub> productivity of 550 mmol·g<sup>-1</sup>·h<sup>-1</sup> under concentrated simulated solar irradiation (11.3 W·cm<sup>-2</sup>). Detailed control experiment results verified that the CO<sub>2</sub> 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 CO<sub>2</sub> 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 CO<sub>2</sub>-to-fuel conversion.