Deep Understanding of Strong Metal Interface Confinement: A Journey of Pd/FeOx Catalysts

Liu, Jixing; Wang, Lu; Okejiri, Francis; Luo, Jing; Zhao, Jiahua; Zhang, Pengfei; Liu, Miaomiao; Yang, Shize; Zhang, Zihao; Song, Weiyu; Zhu, Wenshuai; Liu, Jian; Zhao, Zhen; Feng, Guodong; Xu, Chunming; Dai, Sheng

doi:10.1021/acscatal.0c01447

Title: Deep Understanding of Strong Metal Interface Confinement: A Journey of Pd/FeO_x Catalysts

Journal Article · Fri Jul 17 00:00:00 UTC 2020 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.0c01447 · OSTI ID:1810000

^[1]; Wang, Lu ^[2]; Okejiri, Francis ^[3]; Luo, Jing ^[4]; Zhao, Jiahua ^[5];

^[5]; Liu, Miaomiao ^[3]; Yang, Shize ^[6]; Zhang, Zihao ^[3];

^[2];

^[4];

^[2]; Zhao, Zhen ^[2];

^[7]; Xu, Chunming ^[2];

^[8]

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 FeO_x 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 FeO_x 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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Natural Science Foundation of China (NSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1810000

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 15 Vol. 10; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
FeOx overlayers
Pd
density functional theory
interface
support-metal interface confinement

Title: Deep Understanding of Strong Metal Interface Confinement: A Journey of Pd/FeOx Catalysts

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Title: Deep Understanding of Strong Metal Interface Confinement: A Journey of Pd/FeO_x Catalysts