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作 者:钟栎锭 吴玉瑾 王丽[1] 郭耘[1] ZHONG Liding;WU Yujin;WANG Li;GUO Yun(Institute of Industrial Catalysis,School of Chemistry and Molecular Engineering,East China University of Science and Technology,Shanghai 200237,China)
机构地区:[1]华东理工大学化学与分子工程学院,工业催化研究所,上海200237
出 处:《陕西师范大学学报(自然科学版)》2022年第2期67-76,F0002,共11页Journal of Shaanxi Normal University:Natural Science Edition
基 金:国家自然科学基金(21976057);上海市科委“科技创新行动计划”(19DZ1208000)。
摘 要:采用沉积沉淀法制备负载Pd催化剂,并以CO和C_(3)H_(8)氧化为模型反应,考察CoO_(x)的引入对Pd/Al_(2)O_(3)和Pd/CeO_(2)催化性能的影响。通过多种手段表征催化剂的物理结构、化学状态和氧化还原性能;并利用原位红外探讨CoO_(x)引入对氧化反应的促进机制。结果表明:Pd/CoO_(x)/CeO_(2)的C_(3)H_(8)氧化反应速率是Pd/CeO_(2)的2.7倍;Pd/CoO_(x)/Al_(2)O_(3)的CO氧化反应速率是Pd/Al_(2)O_(3)的2倍。CoO_(x)对氧化反应的促进作用与载体的氧化还原性和反应物密切相关,对不同载体和反应物的氧化促进机制不同。在CO氧化过程中,CoO_(x)的引入可以改变Pd的化学状态;而在C_(3)H_(8)氧化过程中,CoO_(x)的引入可以增强C_(3)H_(8)的吸附并影响其氧化中间物种在催化剂表面的稳定性。The Pd supported catalysts were prepared by the deposition precipitation method,and the oxidations of CO and C_(3)H_(8)were used as model reactions to investigate the influence of CoO_(x)introduction on the reaction performance of Pd/Al_(2)O_(3)and Pd/CeO_(2).The physical structure,chemical state and oxidation-reduction performance of the catalysts were characterized by a variety of characterization methods,and in situ DRIFTS was applied to explore the promotion mechanism of CoO_(x)introduction on the oxidation reaction.The results showed that the reaction rate of Pd/CoO_(x)/CeO_(2)to C_(3)H_(8)oxidation was 2.7 times that of Pd/CeO_(2),and the reaction rate of Pd/CoO_(x)/Al_(2)O_(3)to CO oxidation was 2 times that of Pd/Al_(2)O_(3).The promotion effects of CoO_(x)on oxidation reaction were closely related to the redox properties of the carriers and the reactants,and its promotion mechanisms for CO and C_(3)H_(8)oxidation were different.The introduction of CoO_(x)changed the chemical state of Pd during CO oxidation reaction,whereas enhanced the adsorption of C_(3)H_(8)and affected the stability of intermediate oxidation species on the catalyst surface during C_(3)H_(8)oxidation reaction.
关 键 词:PD CoO_(x) CO氧化 C_(3)H_(8)氧化
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