Effect of flame temperature on structure and CO oxidation properties of Pt/CeO2 catalyst by flame-assisted spray pyrolysis

Naoya Minegishi , Peizhou Li , Tsuyoshi Nagasawa , Hidenori Kosaka
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Abstract

Flame synthesis offers the potential for the synthesis of structure-controlled catalysts. In this study, Pt/CeO2 nanoparticles were synthesized via flame-assisted spray pyrolysis (FASP) and used as CO oxidation catalysts. The catalysts were synthesized using a burner diffusion flame at three different flame temperatures (maximum flame temperatures, Tf = 1556, 1785, and 2026 K), and their particle structure and CO oxidation activity were evaluated. The synthesized Pt/CeO2 catalysts had a bimodal structure containing 100 nm-scale CeO2 loaded with 10 nm-scale Pt and fine CeO2 < 10 nm loaded with highly dispersed Pt (less than 1 nm). As the flame temperature increases from 1556 to 2026 K, the formation of fine CeO2 particles dominates, resulting in an increase in BET specific surface area from 7.97 to 112 m2/g and Pt dispersion from 4.67 to 20.6%. Insight into the particle formation routes that determine the catalyst structure is provided by numerical simulation of droplet evaporation in a burner flame. CO oxidation experiments showed that the temperature at which CO conversion reached 100% (T100) decreased from 513 to 378 K with increasing flame temperature in FASP. In addition, the thermal stability test showed that the Pt dispersion after thermal degradation was higher for Pt/CeO2 catalyst made by FASP at Tf = 2026 K than that prepared by the impregnation method, and the T100 for CO oxidation was lower by 20 K.

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火焰温度对火焰辅助喷雾热解 Pt/CeO2 催化剂结构和 CO 氧化性能的影响
火焰合成为合成结构可控的催化剂提供了可能。本研究通过火焰辅助喷雾热解(FASP)合成了 Pt/CeO2 纳米颗粒,并将其用作 CO 氧化催化剂。催化剂是在三种不同的火焰温度(最高火焰温度 Tf = 1556、1785 和 2026 K)下使用燃烧器扩散火焰合成的,并对其颗粒结构和 CO 氧化活性进行了评估。合成的 Pt/CeO2 催化剂具有双峰结构,其中 100 nm 级 CeO2 上负载有 10 nm 级 Pt,而细 CeO2 < 10 nm 上负载有高度分散的 Pt(小于 1 nm)。随着火焰温度从 1556 K 升至 2026 K,细小 CeO2 颗粒的形成占主导地位,导致 BET 比表面积从 7.97 m2/g 增至 112 m2/g,铂分散度从 4.67% 增至 20.6%。通过对燃烧器火焰中液滴蒸发的数值模拟,可以深入了解决定催化剂结构的颗粒形成途径。一氧化碳氧化实验表明,随着 FASP 中火焰温度的升高,一氧化碳转化率达到 100% 的温度(T100)从 513 K 降至 378 K。此外,热稳定性测试表明,在 Tf = 2026 K 时,FASP 制备的 Pt/CeO2 催化剂热降解后的铂分散度比浸渍法制备的催化剂高,CO 氧化的 T100 降低了 20 K。
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