Zihao Li, Zhisong Liu, Guanqun Gao, Weina Zhao, Yongjun Jiang, Xuan Tang, Sheng Dai*, Zan Qu, Naiqiang Yan and Lei Ma*,
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引用次数: 0
摘要
要满足有效消除汽车尾气中一氧化碳(CO)的日益严格的要求,提高 Pt/CeO2 催化剂的低温氧化活性是一项挑战。虽然还原活化是一种提高反应活性的简便策略,但以往的研究主要集中在使用 H2 作为还原剂,而忽略了汽车尾气中的主要成分 CO 本身的还原能力。本文制备了原子分散的 Pt/CeO2,并利用 CO 对其进行活化,从而将 90% 转化温度(T90)降低了 256 ℃,并在 200 ℃ 时将 CO 消耗率提高了 20 倍。活化后的 Pt/CeO2 催化剂在汽油或柴油废气的模拟工作条件下表现出优异的催化氧化活性和强大的水热稳定性。表征结果表明,CO 活化引发了大量 Pt0 梯度位点的形成,成为 CO 氧化的固有活性位点。此外,CO 活化削弱了 Pt-O-Ce 键的强度,从而产生了表面氧空位(Vo)。它可以作为氧气库,储存解离出的氧气,并将其转化为活性二氧中间体。相反,H2 的活化未能激发 Vo,而是引发了铂纳米团簇在氧气存在下向非活性 PtxOy 的失活转化。目前的研究工作为了解 CO 对 Pt/CeO2 的活化效应提供了一致的见解,旨在为提高消除汽车尾气中 CO、C3H6 和 NH3 的效率开辟一条宝贵的途径。
Enhanced Catalytic Oxidation Reactivity over Atomically Dispersed Pt/CeO2 Catalysts by CO Activation
The elevation of the low-temperature oxidation activity for Pt/CeO2 catalysts is challenging to meet the increasingly stringent requirements for effectively eliminating carbon monoxide (CO) from automobile exhaust. Although reducing activation is a facile strategy for boosting reactivity, past research has mainly concentrated on applying H2 as the reductant, ignoring the reduction capabilities of CO itself, a prevalent component of automobile exhaust. Herein, atomically dispersed Pt/CeO2 was fabricated and activated by CO, which could lower the 90% conversion temperature (T90) by 256 °C and achieve a 20-fold higher CO consumption rate at 200 °C. The activated Pt/CeO2 catalysts showed exceptional catalytic oxidation activity and robust hydrothermal stability under the simulated working conditions for gasoline or diesel exhausts. Characterization results illustrated that the CO activation triggered the formation of a large portion of Pt0 terrace sites, acting as inherent active sites for CO oxidation. Besides, CO activation weakened the Pt–O–Ce bond strength to generate a surface oxygen vacancy (Vo). It served as the oxygen reservoir to store the dissociated oxygen and convert it into active dioxygen intermediates. Conversely, H2 activation failed to stimulate Vo, but triggered a deactivating transformation of the Pt nanocluster into inactive PtxOy in the presence of oxygen. The present work offers coherent insight into the upsurging effect of CO activation on Pt/CeO2, aiming to set up a valuable avenue in elevating the efficiency of eliminating CO, C3H6, and NH3 from automobile exhaust.
期刊介绍:
Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences.
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