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Elucidation of the Active Sites in Single-Atom Pd1/CeO2 Catalysts for Low-Temperature CO Oxidation
ACS Catalysis ( IF 12.9 ) Pub Date : 2020-08-20 , DOI: 10.1021/acscatal.0c02480
Dong Jiang 1 , Gang Wan 2 , Carlos E. García-Vargas 1 , Linze Li 3 , Xavier Isidro Pereira-Hernández 1 , Chongmin Wang 3 , Yong Wang 1, 4
Affiliation  

Supported precious metals with atomic dispersion are of great interest in catalysis due to their potentials in achieving maximum atom efficiency and unique reactivities. Herein, the active sites for low-temperature CO oxidation are elucidated over single-atom Pd1/CeO2 catalysts prepared via high-temperature atom trapping (AT). The increased oxygen vacancies on CeO2 surface induced by 800 °C air calcination result in decreased Pd–CeO2 coordinations, i.e., the coordination-unsaturated Pd2+ on CeO2. Light-off and light-out measurements coupled with CO-DRIFTS and X-ray absorption characterization confirm that these coordination-unsaturated Pd2+ on CeO2 are much more reactive than the fully coordinated counterpart, evidenced by a decrease of T90 (temperature to achieve 90% conversion) by ∼100 °C in CO oxidation at a gas hourly space velocity of 300 L g–1 h–1.

中文翻译:

低温CO氧化单原子Pd 1 / CeO 2催化剂中活性位的阐明

具有原子分散性的负载型贵金属具有催化作用,因为它们具有实现最大原子效率和独特反应性的潜力。在此,在通过高温原子俘获(AT)制备的单原子Pd 1 / CeO 2催化剂上阐明了低温CO氧化的活性位点。上的CeO增加氧空位2通过800℃空气中煅烧结果诱导的表面下降的Pd-的CeO 2个配位,即,配位不饱和的Pd 2+上的CeO 2。起燃和熄灭测量与CO-DRIFTS和X射线吸收特征相结合证实了CeO上这些配位不饱和的Pd 2+2的反应性比完全协调的对应物要强得多,这在气体每小时空速300 L g –1 h –1的条件下在CO氧化中将T 90(达到90%转化的温度)降低了约100°C 。
更新日期:2020-10-02
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