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

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外文摘要：Supported Pd based catalysts are considered as the efficient candidates for low-carbon alkane oxida-tion 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)ma-trix 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 C-H was facilitated on alloy/perovskite interface which is,on the con-trary,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.

外文关键词：

ExsolutionPdPt alloyOperando characterizationMethane conversionDeep-oxidation

作者：

Yanling Yang、Zhenfa Ding、Huimin Wang、Jianhui Li、Yanping Zheng、Hongquan Guo、Li Zhang、Bing Yang、Qingqing Gu、Haifeng Xiong、Yifei Sun

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作者单位：

College of Energy,Xiamen University,Xiamen 361005,China

School of Environment and Civil Engineering,Dongguan University of Technology,Dongguan 523808,China

Department of Chemistry,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China

State Key Laboratory of Physical Chemistry of Solid Surfaces,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China

CAS Key Laboratory of Science and Technology on Applied Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China

Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM),Xiamen 361102,China

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基金：

国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金中央高校基本科研业务费专项福建省科技计划Guangdong Basic and Applied Basic Research FundScience and Technology Projects of Inno-vation Laboratory for Sciences and Technologies of Energy Ma-terials of Fujian Province(中央高校基本科研业务费专项

项目编号：

2227213622202041221021352220216322172129207202201192022L30772022A1515110239HRTP-[2022]-320720220008

出版年：

2024

DOI：

10.1016/j.cclet.2023.108585

中国化学快报(英文版)

中国化学会

中国化学快报(英文版)

CSTPCD

影响因子：0.771

ISSN：1001-8417

年,卷(期)：2024.35(4)

参考文献量32