Acetic Acid Production from CH<sub>4</sub> and CO<sub>2</sub> via Synergistic Catalysis between Pd Particles and Oxygen Vacancies Generated in ZrO<sub>2</sub>
Yufeng Li, Ke Zheng, Yu Shen, Mengyuan Huang, Bing Liu, Yuebing Xu, Xiaohao Liu
Abstract
Co-conversion of CO 2 and CH 4 into acetic acid is of great significance to the environment but is challenged by their chemical stability. Herein, Pd–ZrO 2 catalysts exhibit excellent performance for acetic acid production, which is about 5 times higher than that for pure ZrO 2 . Combined catalytic tests, characterization, and density functional theory (DFT) calculations have revealed a synergistic catalysis mechanism between Pd and H 2 -reduced ZrO 2, which not only facilitates CO 2 adsorption and activation owing to generating more oxygen vacancies (Ov) but also promotes CH 4 activation owing to resulting larger-sized metallic Pd particles. DFT calculations demonstrate that the C–C coupling between CH 3 * and COOH* exhibits a lower barrier, which favors acetic acid formation.