化学
甲酸
甲烷
催化作用
选择性
产量(工程)
解吸
光化学
化学工程
有机化学
热力学
吸附
物理
工程类
作者
Yuheng Jiang,Yingying Fan,Xiaolong Liu,Jun Xie,Siyang Li,Kefu Huang,Xiaoyu Fan,Chang Long,Lulu Zuo,Wenshi Zhao,Xu Zhang,Juehan Sun,Peng Xu,Jiong Li,Fan Dong,Ting Tan,Zhiyong Tang
摘要
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.
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