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Rate Inhibition and Enhancement on Ceria-Promoted Pd Monolith Catalysts: Oxidation of Acetylene, Ethylene, and Propylene and Their Mixtures
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2019-04-15 , DOI: 10.1021/acs.iecr.9b00978 Wendy Lang 1 , Michael P. Harold 1
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2019-04-15 , DOI: 10.1021/acs.iecr.9b00978 Wendy Lang 1 , Michael P. Harold 1
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The catalytic oxidations of acetylene, ethylene, and propylene under transient and steady-state conditions were studied using model Pd/Al2O3 and Pd/CeO2–ZrO2 monolith catalysts. Kinetics and light-off measurements highlight the differences between the oxidation of each hydrocarbon. Acetylene is strongly self-inhibiting and −1 order while the reaction order with respect to ethylene is +1, both at temperatures below light-off. Ethylene oxidation is moderately inhibited by oxygen at low temperatures and ethylene at high temperatures. Mixture light-off experiments reveal acetylene inhibits the oxidations of ethylene, propylene, and CO. Light-off of the other species follow acetylene oxidation, which is nearly unaffected by the other species. The Pd/CeO2–ZrO2 catalyst gives consistently higher conversion compared with Pd/Al2O3 at the same Pd loading for each of the individual oxidation reactions, although the negative-order kinetics of acetylene is sustained. Oxidation of acetylene and mixtures containing acetylene are enhanced with Pd/CeO2–ZrO2 compared to Pd/Al2O3. The effects of oxidative or reductive pretreatment of the catalysts on species oxidations are also evaluated. Mechanistic implications for the reactions are described to guide kinetic model development. The findings highlight and clarify inhibition effects during single and co-oxidation and offer insights into optimizing the catalyst composition and its operation.
中文翻译：
二氧化铈促进的Pd整体催化剂的速率抑制和增强：乙炔，乙烯和丙烯及其混合物的氧化
使用Pd / Al 2 O 3模型和Pd / CeO 2 -ZrO 2模型研究了瞬态和稳态条件下乙炔，乙烯和丙烯的催化氧化。整体催化剂。动力学和起燃测量结果突出了每种烃的氧化之间的差异。乙炔在低于起燃温度下都具有很强的自抑制性，并且相对于乙烯的反应阶数为+1，而乙烯的反应阶数为+1。低温下的氧气和高温下的乙烯会适度抑制乙烯的氧化。混合起燃实验表明乙炔可抑制乙烯，丙烯和CO的氧化。其他物种的起燃遵循乙炔氧化，几乎不受其他物种的影响。与Pd / Al 2 O 3相比，Pd / CeO 2 -ZrO 2催化剂的转化率始终较高。对于每个单独的氧化反应，在相同的Pd负载下，尽管乙炔的负序动力学得以维持。与Pd / Al 2 O 3相比，Pd / CeO 2 -ZrO 2增强了乙炔和含有乙炔的混合物的氧化。还评估了催化剂的氧化或还原预处理对物质氧化的影响。描述了反应的机理含义，以指导动力学模型的发展。这些发现突出并阐明了单氧化和共氧化过程中的抑制作用，并为优化催化剂组成及其操作提供了见识。
更新日期：2019-04-15
中文翻译：
二氧化铈促进的Pd整体催化剂的速率抑制和增强：乙炔，乙烯和丙烯及其混合物的氧化
使用Pd / Al 2 O 3模型和Pd / CeO 2 -ZrO 2模型研究了瞬态和稳态条件下乙炔，乙烯和丙烯的催化氧化。整体催化剂。动力学和起燃测量结果突出了每种烃的氧化之间的差异。乙炔在低于起燃温度下都具有很强的自抑制性，并且相对于乙烯的反应阶数为+1，而乙烯的反应阶数为+1。低温下的氧气和高温下的乙烯会适度抑制乙烯的氧化。混合起燃实验表明乙炔可抑制乙烯，丙烯和CO的氧化。其他物种的起燃遵循乙炔氧化，几乎不受其他物种的影响。与Pd / Al 2 O 3相比，Pd / CeO 2 -ZrO 2催化剂的转化率始终较高。对于每个单独的氧化反应，在相同的Pd负载下，尽管乙炔的负序动力学得以维持。与Pd / Al 2 O 3相比，Pd / CeO 2 -ZrO 2增强了乙炔和含有乙炔的混合物的氧化。还评估了催化剂的氧化或还原预处理对物质氧化的影响。描述了反应的机理含义，以指导动力学模型的发展。这些发现突出并阐明了单氧化和共氧化过程中的抑制作用，并为优化催化剂组成及其操作提供了见识。
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