Engineering multicomponent metal-oxide units for efficient methane combustion over palladium-based catalysts,Catalysis Science & Technology

当前位置： X-MOL 学术 › Catal. Sci. Technol. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Engineering multicomponent metal-oxide units for efficient methane combustion over palladium-based catalysts
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020-10-30 , DOI: 10.1039/d0cy01742f
Yelin Chen _{1,

2,

3,

4,

5} , Jia Lin _{1,

2,

3,

4,

5} , Xiaohua Chen _{1,

2,

3,

4,

5} , Siqin Fan _{1,

2,

3,

4,

5} , Ying Zheng _{1,

2,

3,

4,

5}

Affiliation

Multicomponent catalysts have been long known for their potential to improve catalytic performance, whereas rational design proposes profound challenges. Herein, we present a strategy for engineering metal oxide units to realize efficient methane combustion through incorporating Mg into Pd/Ce_xZr_1−xO₂–Al₂O₃ catalysts. Catalysts are facilely obtained through a sol–gel method and incipient wetness impregnation process; meanwhile, the surface and structural properties are tuned via Mg modification. The doped Mg component enters the CZ lattice, inducing numerous oxygen vacancies and favourable oxygen migration due to the structural and electronic mismatch between Mg²⁺ and Ce⁴⁺ (or Zr⁴⁺). The generated MgAl₂O₄ spinel and oxygen vacancies conjointly result in weaker Pd–O bonds and improved reducibility. Meanwhile, the efficient oxygen transfer between the metal and support contributes to the reformation of bulk PdO. Consequently, the smooth conversion of Pd ↔ PdO is realized, which is beneficial for methane oxidation. Moreover, the catalytic activity of Pd/5CZA-yM varies with the particle size of palladium species. The as-prepared Pd/5CZA-5M with a moderate Pd particle size demonstrates significantly boosted catalytic activity and long-term stability compared to the unmodified one.

中文翻译：

工程多组分金属氧化物单元，可在钯基催化剂上高效甲烷燃烧

多组分催化剂因其提高催化性能的潜力而久负盛名，而合理的设计则提出了严峻的挑战。本文中，我们提出了一种工程化金属氧化物单元的策略，该策略是通过将Mg掺入Pd / Ce _x Zr _{1- x} O ₂ -Al ₂ O ₃催化剂中来实现有效的甲烷燃烧。催化剂是通过溶胶-凝胶法和初期湿润浸渍法轻松获得的。同时，通过对镁的改性来调节其表面和结构性能。掺杂的Mg组分进入CZ晶格，由于Mg之间的结构和电子失配，导致许多氧空位和有利的氧迁移²⁺和Ce⁴⁺（或Zr⁴⁺）。生成的MgAl₂ O₄尖晶石和氧空位共同导致Pd-O键变弱，还原性提高。同时，金属与载体之间的有效氧转移有助于重整PdO。因此，实现了Pd↔PdO的平滑转化，这对于甲烷氧化是有利的。此外，Pd / 5CZA- y M的催化活性随钯物质的粒径而变化。与未改性的Pd / 5CZA-5M相比，Pd粒度适中的Pd / 5CZA-5M具有明显的催化活性和长期稳定性。

更新日期：2020-11-13

点击分享查看原文

点击收藏

阅读更多本刊最新论文本刊介绍/投稿指南11