posted on 2023-12-22, 11:14authored byJianghao Zhang, Chuo Du, Shuchao Ge, Yifan Jin, Shuo Hu, Hongfei Xiao, Xiaoxiao Qin, Kunlin Li, Xueyan Chen, Min Chen, Jinhou Fang, Changbin Zhang
The catalytic oxidation of carbon
monoxide (CO) under ambient conditions
plays a crucial role in the abatement of indoor CO, which poses risks
to human health. Despite the notable activity exhibited by Pt-based
catalysts in CO oxidation, their efficacy is usually diminished by
the CO self-poisoning issue. In this work, three different Pt/CeO2-based catalysts, which have distinct coordinative environments
of Pt but an identical Pt/CeO2 substrate structure, were
synthesized by activating the catalyst with CO using different temperatures
and durations. Compared with clean and graphite-covered Pt on CeO2, the one modified by epoxy carbon showed higher activity
and stability. The combination of characterizations and density functional
theory modeling demonstrated that the clean Pt on CeO2 rapidly
deactivated due to the CO self-poisoning albeit high initial activity,
and conversely, low initial activity was observed for the more stable
graphite-covered catalyst due to the obstruction of the Pt site. In
contrast, epoxy carbon species on Pt shifted the d-band of Pt to lower
energy, weakening the Pt–CO binding strength. Such a modification
mitigated the self-poisoning effect while maintaining ample active
sites and enabling the complete oxidative removal of CO under ambient
conditions. This work may provide a general approach to tackling the
self-poisoning issue.