在二氧化铈负载的钯纳米催化剂中掺杂镨作为减少甲烷氧化过程中水抑制作用的有效策略,Applied Catalysis B: Environment and Energy

在二氧化铈负载的钯纳米催化剂中掺杂镨作为减少甲烷氧化过程中水抑制作用的有效策略

Applied Catalysis B: Environment and Energy

(

IF

20.2

)

Pub Date : 2022-08-26

, DOI:

10.1016/j.apcatb.2022.121898

Sabrina Ballauri

,

Enrico Sartoretti

,

Min Hu

,

Carmine D’Agostino

,

Zijuan Ge

,

Liang Wu

,

Chiara Novara

,

Fabrizio Giorgis

,

Marco Piumetti

,

Debora Fino

,

Nunzio Russo

,

Samir Bensaid

本研究报告了 Pd/Ce-Pr 催化剂的改进设计。对具有不同成分的 Pd 浸渍纳米结构二氧化铈-镨催化剂进行了综合表征和干法和湿法甲烷氧化测试。通过 XRD、TPR/TPO、拉曼和 HRTEM 分析检测到的强 PdO-PrO x相互作用将 Pd 主要以其氧化形式保留在具有高镨含量的材料中，从而导致较低的活性。相反，在二氧化铈中引入有限量的 Pr 可以获得比典型的 Pd/CeO 2更具活性的催化剂（2% 的 Pd 负载在具有 10% Pr 的混合氧化物上）系统。因此，同时存在还原和氧化形式的 Pd 是高活性的关键因素。此外，通过 NMR 和原位FTIR 研究，该样品的较高疏水性显着降低了 Pd 基材料典型的 H 2 O 抑制效应，为在实际应用中使用该系统铺平了道路。

"点击查看英文标题和摘要"

Praseodymium doping in ceria-supported palladium nanocatalysts as an effective strategy to minimize the inhibiting effects of water during methane oxidation

The present study reports an improved design for Pd/Ce-Pr catalysts. Pd-impregnated nanostructured ceria-praseodymia catalysts with different compositions were comprehensively characterized and tested for dry and wet methane oxidation. The strong PdO-PrOx interaction, detected via XRD, TPR/TPO, Raman and HRTEM analyses, retains Pd mainly in its oxidized form in the materials with high praseodymium content, thus resulting in a lower activity. Conversely, the introduction of a limited amount of Pr in ceria allows to obtain a more active catalyst (2% of Pd supported on a mixed oxide with 10% of Pr) than the typical Pd/CeO2 systems. Hence, the simultaneous presence of Pd in its reduced and oxidized forms results to be a key factor for high activity. Additionally, the higher hydrophobicity of this sample, investigated through NMR and in situ FTIR, markedly reduces the H2O inhibition effect typical of Pd-based materials, paving the way for using this system in real applications.

更新日期：2022-08-26