Synergetic Effect of K Sites and Pt Nanoclusters in an Ordered Hierarchical Porous Pt-KMnOx/Ce0.25Zr0.75O2 Catalyst for Boosting Soot Oxidation

被引:59
作者
Xiong, Jing [3 ]
Wei, Yuechang [3 ,4 ]
Zhang, Yilin [3 ]
Zhang, Peng [3 ]
Yu, Qi [3 ]
Mei, Xuelei [3 ]
Liu, Xi [1 ,2 ]
Zhao, Zhen [3 ]
Liu, Jian [3 ,4 ]
机构
[1] Shanghai Jiao Tong Univ, In Situ Ctr Phys Sci, Sch Chem & Chem, Shanghai 200240, Peoples R China
[2] SynfuelsChina Co Ltd, Syncat Beijing, Beijing 101407, Peoples R China
[3] China Univ Petr, Coll Sci, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
[4] China Univ Petr, Beijing Key Lab Opt Detect Technol Oil & Gas, Beijing 102249, Peoples R China
来源
ACS CATALYSIS | 2020年 / 10卷 / 13期
基金
中国国家自然科学基金; 北京市自然科学基金;
关键词
hierarchical porous catalyst; OMMM; ultrafine nanoclusters; synergetic effect; soot oxidation; CORE-SHELL NANOPARTICLES; HIGHLY-ACTIVE CATALYSTS; GOLD NANOPARTICLES; SOLID-SOLUTIONS; METAL-OXIDES; DIESEL SOOT; COMBUSTION; EMISSION; PERFORMANCE; CERIA;
D O I
10.1021/acscatal.0c01911
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We have designed and elaborately fabricated the ordered hierarchical macro-meso-microporous catalysts of Ce0.25Zr0.75O2-supported Pt-embedded KMnOx nanoparticles (OMMM Pt-KMnOx/Ce0.25Zr0.75O2). Three dimensionally ordered macro-mesoporous (3DOMM) Ce0.25Zr0.75O2 oxide was synthesized by the combined methods of evaporation-induced interfacial self-assembly (EISA) and colloidal crystal templates (CCT). KMnOx nanoparticles (NPs) possess the natural microporous nanostructure of an octahedral molecular sieve (OMS) with an average size of 0.46 nm. Pt nanoclusters were anchored in situ at the microporous structure of KMnOx NPs and formed Pt-KMnOx active sites. For the OMMM Pt-Pt-KMnOx/Ce0.25Zr0.75O2 catalyst, a 3D ordered macroporous (250 nm) structure can enhance contact efficiency between soot and catalysts, and a high specific surface area with contributions from ordered mesopores (5 nm) is beneficial for dispersion of KMnOx NPs and activation of gaseous reactants (O-2 and NO). Meanwhile, a microporous (0.46 nm) structure can anchor K sites and ultrafine Pt nanoclusters. The synergetic effect of ternary K-Mn-Pt components can transform gas reactants to the effective intermediate species and thereafter oxidize the well-dispersed soot particles. The OMMM Pt-KMnOx/Ce0.25Zr0.75O2 catalyst possesses high catalytic activity and stability for soot oxidation under the conditions of loose contact: i.e., its TOF value is 2.10 h(-1) at 290 degrees C, which is more than a 4-fold increase over the 3DOMM Ce0.25Zr0.75O2 support (0.47 h(-1)). The architected hierarchical porous structure rationalizes an alternative protocol to improve solid-solid contact and the resulting activity, which can be further applied to other catalysis systems with different catalysts and reactants.
引用
收藏
页码:7123 / 7135
页数:13
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