Details

Autor(en) / Beteiligte

• Jiang, Yuheng
• Fan, Yingying
• Liu, Xiaolong
• Xie, Jun
• Li, Siyang
• Huang, Kefu
• Fan, Xiaoyu
• Long, Chang
• Zuo, Lulu
• Zhao, Wenshi
• Zhang, Xu
• Sun, Juehan
• Xu, Peng
• Li, Jiong
• Dong, Fan
• Tan, Ting
• Tang, Zhiyong

Titel

Steering Photooxidation of Methane to Formic Acid over A Priori Screened Supported Catalysts

Ist Teil von

• Journal of the American Chemical Society, 2024-06, Vol.146 (23), p.16039-16051

Ort / Verlag

American Chemical Society

Erscheinungsjahr

2024

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Efficient methane photooxidation to formic acid (HCOOH) has emerged as a sustainable approach to simultaneously generate value-added chemicals and harness renewable energy. However, the persistent challenge lies in achieving a high yield and selectivity for HCOOH formation, primarily due to the complexities associated with modulating intermediate conversion and desorption after methane activation. In this study, we employ first-principles calculations as a comprehensive guiding tool and discover that by precisely controlling the O2 activation process on noble metal cocatalysts and the adsorption strength of carbon-containing intermediates on metal oxide supports, one can finely tune the selectivity of methane photooxidation products. Specifically, a bifunctional catalyst comprising Pd nanoparticles and monoclinic WO3 (Pd/WO3) would possess optimal O2 activation kinetics and an intermediate oxidation/desorption barrier, thereby promoting HCOOH formation. As evidenced by experiments, the Pd/WO3 catalyst achieves an exceptional HCOOH yield of 4.67 mmol gcat –1 h–1 with a high selectivity of 62% under full-spectrum light irradiation at room temperature using molecular O2. Notably, these results significantly outperform the state-of-the-art photocatalytic systems operated under identical condition.