cs9b00107_si_001.pdf (1.05 MB)
Interaction-Induced Self-Assembly of Au@La2O3 Core–Shell Nanoparticles on La2O2CO3 Nanorods with Enhanced Catalytic Activity and Stability for Soot Oxidation
journal contribution
posted on 2019-03-18, 00:00 authored by Qiangqiang Wu, Jing Xiong, Yilin Zhang, Xuelei Mei, Yuechang Wei, Zhen Zhao, Jian Liu, Jianmei LiThe
sintering resistance of supported Au nanoparticle (NP) catalysts
is crucial to their practical application in heterogeneous catalysis
reactions. Herein, a series of Au@La2O3 core–shell
nanoparticle catalysts supported on the surfaces of La2O2CO3 nanorods (Aun@La2O3/LOC-R) were successfully synthesized
via the method of interaction-induced self-assembly. Supported Au
NPs with uniform size are deposited on the surfaces of La2O2CO3 nanorods by the gas bubbling-assisted
membrane reduction (GBMR) method. La2O3 shell
layers spontaneously formed and then partially coated the surface
of Au NPs for interaction-induced self-assembly of Au@La2O3 core–shell NPs during the process of calcination
at 600 °C. The strong interaction between Au NPs and La2O3 oxides increases the density of active sites (oxygen
vacancies) for enhancing the adsorption–activation properties
of O2. Aun@La2O3/LOC-R catalysts show high catalytic activity and stability
for soot oxidation under the conditions of loose contact between soot
and catalyst. The catalytic activities (T50, TOF) of Au4@La2O3/LOC-R catalyst
for soot oxidation are 375 °C and 1.15 × 10–3 s–1, respectively. On the basis of the results
of various physicochemical characterizations, the strong metal (Au)–oxide
(La2O3) interactions and the increase in active
oxygen species of Aun@La2O3/LOC-R catalysts are responsible for enhancing the catalytic
activity of soot oxidation. The Au@La2O3 core–shell
nanostructure can improve catalytic stability and suppress sintering
of supported Au NPs during catalytic soot oxidation. The catalytic
mechanism of soot oxidation is proposed and discussed, in which the
catalytic oxidation of NO to NO2 over Au@La2O3 core–shell NPs is the key step for catalytic
soot oxidation; the active sites at the interface of the Au core and
La2O3 shell can promote catalytic NO oxidation.
Aun@La2O3/LOC-R
catalysts show promise in practical applications for diesel soot oxidation.