Citation: Yanling Yang, Zhenfa Ding, Huimin Wang, Jianhui Li, Yanping Zheng, Hongquan Guo, Li Zhang, Bing Yang, Qingqing Gu, Haifeng Xiong, Yifei Sun. Dynamic tracking of exsolved PdPt alloy/perovskite catalyst for efficient lean methane oxidation[J]. Chinese Chemical Letters, ;2024, 35(4): 108585. doi: 10.1016/j.cclet.2023.108585 shu

Dynamic tracking of exsolved PdPt alloy/perovskite catalyst for efficient lean methane oxidation

Yanling Yang ^{a, b, 1} ,
Zhenfa Ding ^{a, 1} ,
Huimin Wang ^c ,
Jianhui Li ^c ,
Yanping Zheng ^{c, d} ,
Hongquan Guo ^a ,
Li Zhang ^b ,
Bing Yang ^e ,
Qingqing Gu ^e ,
Haifeng Xiong ^{c, d, f, *,} ,
Yifei Sun ^{a, d, *,}

a.
College of Energy, Xiamen University, Xiamen 361005, China
b.
School of Environment and Civil Engineering, Dongguan University of Technology, Dongguan 523808, China
c.
Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
d.
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
e.
CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
f.
Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen 361102, China

haifengxiong@xmu.edu.cn

yfsun@xmu.edu.cn

Received Date: 20 April 2023
Revised Date: 8 May 2023
Accepted Date: 17 May 2023
Available Online: 19 May 2023

Figures(4)

Supported Pd based catalysts are considered as the efficient candidates for low-carbon alkane oxidation for their outstanding capability to break C-H bond. Whereas, the irreversible deactivation of Pd based catalysts was still frequently observed. Herein, we reinforced the extruded Pd nanoparticles with quantitive Pt to assemble the evenly distributed PdPt nanoalloy onto ferrite perovskite (PdPt-LCF) matrix with strengthened robustness of metal/oxide support interface. We further co-achieved the enhanced performance, anti-overoxidation as well as resistance of vapor-poisoning in durability measurement. The operando X-ray photoelectron spectroscopy (O-XPS) combined with various morphology characterizations confirms that the accumulation of surface deep-oxidation species of Pd⁴⁺ is the culprit for fast activity loss in exsolved Pd system, especially at high temperature of 400 ℃. Conversely, it could be completely suppressed by in-situ alloying Pd with equal amount of Pt, which helps maintain the metastable Pd²⁺/Pd shell and metallic solid-solution core structure. The density function theory (DFT) calculations further buttress that the dissociation of CH was facilitated on alloy/perovskite interface which is, on the contrary, resistant toward O–H bond cleavage, as compared to Pd/perovskite. Our work suggests that the modification of exsolved metal/oxide catalytic interface could further enrich the toolkit of heterogeneous catalyst design.
- Exsolution,
- PdPt alloy,
- Operando characterization,
- Methane conversion,
- Deep-oxidation
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