Keys Unlocking Redispersion of Reactive PdOx Nanoclusters on Ce-Functionalized Perovskite Oxides for Methane Activation

Yang, Yanling, Zhang, Li, Guo, Hongquan, Ding, Zhenfa, Wang, Weitao, Li, Jianhui, Zhou, Liujiang, Tu, Xin ORCID: 0000-0002-6376-0897, Qiu, Yongfu, Chen, Gui
et al (show 1 more authors) (2022) Keys Unlocking Redispersion of Reactive PdOx Nanoclusters on Ce-Functionalized Perovskite Oxides for Methane Activation. ACS APPLIED MATERIALS & INTERFACES, 14 (27). pp. 30704-30713.

[img] Text
ACS AMI.pdf - Author Accepted Manuscript

Download (2MB) | Preview


Nowadays, trace CH<sub>4</sub> emitted from vehicle exhausts severely threaten the balance of the ecology system of our earth. Thereby, the development of active and stable catalysts capable of methane conversion under mild conditions is critical. Here, we present a convenient method to redisperse catalytically inert PdO nanoparticles (NPs) (>10 nm) into reactive PdO<sub><i>x</i></sub> nanoclusters (∼2 nm) anchored on a Ce-doped LaFeO<sub>3</sub> parent. Isothermally activated in an N<sub>2</sub> flow, the redispersed catalyst achieved a CH<sub>4</sub> conversion of 90% at 400 °C, which is significantly higher than the fresh and H<sub>2</sub>- and O<sub>2</sub>-treated counterparts (625, 616, and 641 °C, respectively), indicating the importance of the gas atmosphere in the redispersion of PdO NPs. In addition, the comprehensive catalyst characterizations demonstrated that the isolated Ce ions in the perovskite lattice play an irreplaceable role in the redispersion of reactive sites and the reduction of the energy barrier for C-H scission. More importantly, the Ce additive helps to stabilize the PdO<sub><i>x</i></sub> species by reducing overoxidation, resulting in significant lifetime extension. Through a thorough understanding of structural manipulation, this study sheds light on the design of highly performing supported catalysts for methane oxidation.

Item Type: Article
Uncontrolled Keywords: CH4 oxidation, perovskite oxides, Ce doping, redispersion, PdOx nanoclusters
Divisions: Faculty of Science and Engineering > School of Electrical Engineering, Electronics and Computer Science
Depositing User: Symplectic Admin
Date Deposited: 12 Jul 2022 08:55
Last Modified: 28 Jun 2023 01:30
DOI: 10.1021/acsami.2c04442
Related URLs: