化学
纳米棒
甲烷
脱氢
催化作用
产量(工程)
选择性
光催化
吸附
光化学
异质结
化学工程
无机化学
有机化学
物理化学
冶金
光电子学
工程类
材料科学
作者
Yufei Cui,Hui Yang,Wenhao Zhou,Yongqing Ma,Ganhong Zheng,Bin Chen,Chuhong Zhu,Meiling Wang
标识
DOI:10.1016/j.jcat.2024.115546
摘要
Selective CH4 upgrading to C1 products and avoiding over oxidation remains a key challenge. Here, we develop a highly efficient Ni/CeO2 nanorods containing both uniformly dispersed Ni-single-site and NiOx/CeO2 heterojunction for 100 % selectively CH4 conversion to C1 products (CH3OH, HCHO, CH3OOH and HCOOH). Under optimized photocatalytic experimental conditions, a high C1 product yield of 5.6 mmol g-1h−1 was obtained with 100 % selectivity with presence of H2O2. Mechanism study showed that the Ni-single-site together with formed oxygen vacancy (Ov) facilitated CH4 adsorption and activation. The terminal O atom of adsorbed ·OOH can fill the Ov, with the remaining *OH initiating *CH3 dehydrogenation and forming *CH2OH, which further reacts with ·OH to generate the main product HCHO. During the whole photocatalytic process, the formed NiOx/CeO2 heterojunction promoted carrier separation and enhanced catalytic performance.
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