Deep Understanding of Strong Metal Interface Confinement: A Journey of Pd/FeOx Catalysts
- Jiangsu Univ., Zhenjiang (China). Inst. for Energy Research; China Univ. of Petroleum, Beijing (China). State Key Lab. of Heavy Oil, Beijing Key Lab. of Oil & Gas Pollution Control; Univ. of Tennessee, Knoxville, TN (United States)
- China Univ. of Petroleum, Beijing (China). State Key Lab. of Heavy Oil, Beijing Key Lab. of Oil & Gas Pollution Control
- Univ. of Tennessee, Knoxville, TN (United States)
- Jiangsu Univ., Zhenjiang (China). Inst. for Energy Research
- Shanghai Jiao Tong Univ. (China)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Univ. of Tennessee, Knoxville, TN (United States); Chinese Academy of Sciences (CAS), Ningbo (China). Ningbo Inst. of Materials Technology and Engineering; Baoji Univ. of Arts and Sciences (China). Key Lab. of Advanced Molecular Engineering Materials
- Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Tuning the atomic interface configuration of noble metals (NMs) and transition-metal oxides is an effective straightforward yet challenging strategy to modulate the activity and stability of heterogeneous catalysts. Herein, Pd supported on mesoporous Fe2O3 with a high specific surface area was rationally designed and chosen to construct the Pd/iron oxide interface. As a versatile model, the physicochemical environments of Pd nanoparticles (NPs) could be precisely controlled by taming the reduction temperature. The experimental and density functional theory calculation results unveiled that the catalyst in the support–metal interface confinement (SMIC) state showed significantly enhanced catalytic activity and sintering resistance for CO oxidation. The constructed Fe sites at the interfaces between FeOx overlayers and Pd NPs not only provided additional coordinative unsaturated ferrous sites for the adsorption and activation of O2, thereby facilitating the activation efficiency of O2, but also impressively changed the reaction pathway of CO oxidation. As a result, the catalyst followed the Pd/Fe dual-site mechanism instead of the classical Mars–van Krevelen mechanism. For the catalyst in the strong metal–support interaction (SMSI) state, its catalytic activity was seriously suppressed because of the excessive encapsulation of the active Pd sites by FeOx overlayers. Thus, the present study therefore provides detailed insights into the SMIC and SMSI in ferric oxide-supported Pd catalysts, which could guide the preparation of highly efficient supported catalysts for practical applications.
- Research Organization:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Natural Science Foundation of China (NSFC)
- Grant/Contract Number:
- AC05-00OR22725; 21673290; U1662103; 21776174; 21871007; 21801009
- OSTI ID:
- 1810000
- Journal Information:
- ACS Catalysis, Vol. 10, Issue 15; ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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