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

Abstract

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 insightsmore » into the SMIC and SMSI in ferric oxide-supported Pd catalysts, which could guide the preparation of highly efficient supported catalysts for practical applications.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [5]; ORCiD logo [5];  [3];  [6];  [3]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [2];  [2]; ORCiD logo [7];  [2]; ORCiD logo [8]
  1. 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)
  2. China Univ. of Petroleum, Beijing (China). State Key Lab. of Heavy Oil, Beijing Key Lab. of Oil & Gas Pollution Control
  3. Univ. of Tennessee, Knoxville, TN (United States)
  4. Jiangsu Univ., Zhenjiang (China). Inst. for Energy Research
  5. Shanghai Jiao Tong Univ. (China)
  6. Brookhaven National Lab. (BNL), Upton, NY (United States)
  7. 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
  8. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1810000
Grant/Contract Number:  
AC05-00OR22725; 21673290; U1662103; 21776174; 21871007; 21801009
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 10; Journal Issue: 15; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; FeOx overlayers; Pd; interface; support-metal interface confinement; density functional theory

Citation Formats

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, and Dai, Sheng. Deep Understanding of Strong Metal Interface Confinement: A Journey of Pd/FeOx Catalysts. United States: N. p., 2020. Web. doi:10.1021/acscatal.0c01447.
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. Deep Understanding of Strong Metal Interface Confinement: A Journey of Pd/FeOx Catalysts. United States. https://doi.org/10.1021/acscatal.0c01447
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, and Dai, Sheng. Fri . "Deep Understanding of Strong Metal Interface Confinement: A Journey of Pd/FeOx Catalysts". United States. https://doi.org/10.1021/acscatal.0c01447. https://www.osti.gov/servlets/purl/1810000.
@article{osti_1810000,
title = {Deep Understanding of Strong Metal Interface Confinement: A Journey of Pd/FeOx Catalysts},
author = {Liu, Jixing and Wang, Lu and Okejiri, Francis and Luo, Jing and Zhao, Jiahua and Zhang, Pengfei and Liu, Miaomiao and Yang, Shize and Zhang, Zihao and Song, Weiyu and Zhu, Wenshuai and Liu, Jian and Zhao, Zhen and Feng, Guodong and Xu, Chunming and Dai, Sheng},
abstractNote = {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.},
doi = {10.1021/acscatal.0c01447},
journal = {ACS Catalysis},
number = 15,
volume = 10,
place = {United States},
year = {Fri Jul 17 00:00:00 EDT 2020},
month = {Fri Jul 17 00:00:00 EDT 2020}
}

Works referenced in this record:

Electronic metal-support interactions in Pt/FeO nanospheres for CO oxidation
journal, September 2020


Interfacial Effects of CeO 2 -Supported Pd Nanorod in Catalytic CO Oxidation: A Theoretical Study
journal, May 2015


A Theory/Experience Description of Support Effects in Carbon-Supported Catalysts
journal, October 2019


Taming the stability of Pd active phases through a compartmentalizing strategy toward nanostructured catalyst supports
journal, April 2019


Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts
journal, September 2016

  • Matsubu, John C.; Zhang, Shuyi; DeRita, Leo
  • Nature Chemistry, Vol. 9, Issue 2
  • DOI: 10.1038/nchem.2607

Tuning the Reactivity of Ultrathin Oxides: NO Adsorption on Monolayer FeO(111)
journal, June 2016

  • Merte, Lindsay R.; Heard, Christopher J.; Zhang, Feng
  • Angewandte Chemie International Edition, Vol. 55, Issue 32
  • DOI: 10.1002/anie.201601647

Ultrastable Gold Nanocatalyst Supported by Nanosized Non-Oxide Substrate
journal, May 2006

  • Yan, Wenfu; Brown, Suree; Pan, Zhengwei
  • Angewandte Chemie International Edition, Vol. 45, Issue 22
  • DOI: 10.1002/anie.200503808

Structure of the catalytically active copper–ceria interfacial perimeter
journal, February 2019


Taming interfacial electronic properties of platinum nanoparticles on vacancy-abundant boron nitride nanosheets for enhanced catalysis
journal, June 2017

  • Zhu, Wenshuai; Wu, Zili; Foo, Guo Shiou
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15291

First-principles extrapolation method for accurate CO adsorption energies on metal surfaces
journal, April 2004


Interface-Confined Ferrous Centers for Catalytic Oxidation
journal, May 2010


Interface-Confined Oxide Nanostructures for Catalytic Oxidation Reactions
journal, March 2013

  • Fu, Qiang; Yang, Fan; Bao, Xinhe
  • Accounts of Chemical Research, Vol. 46, Issue 8
  • DOI: 10.1021/ar300249b

A Sacrificial Coating Strategy Toward Enhancement of Metal–Support Interaction for Ultrastable Au Nanocatalysts
journal, December 2016

  • Zhan, Wangcheng; He, Qian; Liu, Xiaofei
  • Journal of the American Chemical Society, Vol. 138, Issue 49
  • DOI: 10.1021/jacs.6b10472

High Catalytic Activity and Chemoselectivity of Sub-nanometric Pd Clusters on Porous Nanorods of CeO 2 for Hydrogenation of Nitroarenes
journal, February 2016

  • Zhang, Sai; Chang, Chun-Ran; Huang, Zheng-Qing
  • Journal of the American Chemical Society, Vol. 138, Issue 8
  • DOI: 10.1021/jacs.5b11413

Interfacial Effects in Iron-Nickel Hydroxide-Platinum Nanoparticles Enhance Catalytic Oxidation
journal, May 2014


High-Temperature-Stable Catalysts by Hollow Sphere Encapsulation
journal, December 2006

  • Arnal, Pablo M.; Comotti, Massimiliano; Schüth, Ferdi
  • Angewandte Chemie International Edition, Vol. 45, Issue 48
  • DOI: 10.1002/anie.200603507

Carbide-Supported Au Catalysts for Water–Gas Shift Reactions: A New Territory for the Strong Metal–Support Interaction Effect
journal, September 2018

  • Dong, Jinhu; Fu, Qiang; Jiang, Zheng
  • Journal of the American Chemical Society, Vol. 140, Issue 42
  • DOI: 10.1021/jacs.8b08246

Facile Synthesis of Highly Porous Metal Oxides by Mechanochemical Nanocasting
journal, April 2018


Synergistic Effects of Au and FeO x Nanocomposites in Catalytic NO Reduction with CO
journal, October 2016


An atomic-scale view of single-site Pt catalysis for low-temperature CO oxidation
journal, March 2018

  • Therrien, Andrew J.; Hensley, Alyssa J. R.; Marcinkowski, Matthew D.
  • Nature Catalysis, Vol. 1, Issue 3
  • DOI: 10.1038/s41929-018-0028-2

Elucidating the Nanoparticle–Metal Organic Framework Interface of Pt@ZIF-8 Catalysts
journal, November 2017

  • Whitford, Cassandra L.; Stephenson, Casey J.; Gómez-Gualdrón, Diego A.
  • The Journal of Physical Chemistry C, Vol. 121, Issue 45
  • DOI: 10.1021/acs.jpcc.7b06773

Control of metal-support interactions in heterogeneous catalysts to enhance activity and selectivity
journal, November 2019

  • van Deelen, Tom W.; Hernández Mejía, Carlos; de Jong, Krijn P.
  • Nature Catalysis, Vol. 2, Issue 11
  • DOI: 10.1038/s41929-019-0364-x

Strong Metal–Support Interactions between Gold Nanoparticles and ZnO Nanorods in CO Oxidation
journal, June 2012

  • Liu, Xiaoyan; Liu, Ming-Han; Luo, Yi-Chia
  • Journal of the American Chemical Society, Vol. 134, Issue 24
  • DOI: 10.1021/ja3033235

Interface-Confined FeO x Adlayers Induced by Metal Support Interaction in Pt/FeO x Catalysts
journal, September 2017


Electronic properties and charge transfer phenomena in Pt nanoparticles on γ-Al2O3: size, shape, support, and adsorbate effects
journal, January 2012

  • Behafarid, F.; Ono, L. K.; Mostafa, S.
  • Physical Chemistry Chemical Physics, Vol. 14, Issue 33
  • DOI: 10.1039/c2cp41928a

Approaches for Understanding and Controlling Interfacial Effects in Oxide-Supported Metal Catalysts
journal, July 2018


Bimetallic synergy in cobalt–palladium nanocatalysts for CO oxidation
journal, December 2018


Microkinetics of alcohol reforming for H2 production from a FAIR density functional theory database
journal, February 2018


A New Type of Strong Metal–Support Interaction and the Production of H 2 through the Transformation of Water on Pt/CeO 2 (111) and Pt/CeO x /TiO 2 (110) Catalysts
journal, May 2012

  • Bruix, Albert; Rodriguez, José A.; Ramírez, Pedro J.
  • Journal of the American Chemical Society, Vol. 134, Issue 21
  • DOI: 10.1021/ja302070k

Polymorphous Transformations of Nanometric Iron(III) Oxide: A Review
journal, July 2011

  • Machala, Libor; Tuček, Jiří; Zbořil, Radek
  • Chemistry of Materials, Vol. 23, Issue 14
  • DOI: 10.1021/cm200397g

New Strategies for the Preparation of Sinter‐Resistant Metal‐Nanoparticle‐Based Catalysts
journal, July 2019

  • Wang, Lingxiang; Wang, Liang; Meng, Xiangju
  • Advanced Materials, Vol. 31, Issue 50
  • DOI: 10.1002/adma.201901905

Strong metal-support interactions. Group 8 noble metals supported on titanium dioxide
journal, January 1978

  • Tauster, S. J.; Fung, S. C.; Garten, R. L.
  • Journal of the American Chemical Society, Vol. 100, Issue 1
  • DOI: 10.1021/ja00469a029

Contribution of physical blocking and electronic effect to establishment of strong metal-support interaction in rhodium/titanium dioxide catalysts
journal, August 1992

  • Belzunegui, Juan P.; Sanz, Jesus; Rojo, Jose M.
  • Journal of the American Chemical Society, Vol. 114, Issue 17
  • DOI: 10.1021/ja00043a019

Adsorption kinetics and isotopic equilibration of oxygen adsorbed on the Pd(111) surface
journal, May 1989

  • Guo, Xingcai; Hoffman, Alon; Yates, John T.
  • The Journal of Chemical Physics, Vol. 90, Issue 10
  • DOI: 10.1063/1.456386

Classical strong metal–support interactions between gold nanoparticles and titanium dioxide
journal, October 2017


Tuning of catalytic sites in Pt/TiO2 catalysts for the chemoselective hydrogenation of 3-nitrostyrene
journal, September 2019

  • Macino, Margherita; Barnes, Alexandra J.; Althahban, Sultan M.
  • Nature Catalysis, Vol. 2, Issue 10
  • DOI: 10.1038/s41929-019-0334-3

Tuning Pt-CeO2 interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen
journal, March 2019

  • Pereira-Hernández, Xavier Isidro; DeLaRiva, Andrew; Muravev, Valery
  • Nature Communications, Vol. 10, Issue 1
  • DOI: 10.1038/s41467-019-09308-5

Structural evolution of atomically dispersed Pt catalysts dictates reactivity
journal, April 2019


Aluminum hydroxide-mediated synthesis of mesoporous metal oxides by a mechanochemical nanocasting strategy
journal, January 2019

  • Liu, Jixing; Cheng, Huifang; Bao, Jiafeng
  • Journal of Materials Chemistry A, Vol. 7, Issue 40
  • DOI: 10.1039/c9ta06727b

Wet-Chemistry Strong Metal–Support Interactions in Titania-Supported Au Catalysts
journal, January 2019

  • Zhang, Jian; Wang, Hai; Wang, Liang
  • Journal of the American Chemical Society, Vol. 141, Issue 7
  • DOI: 10.1021/jacs.8b10864

In Situ and Theoretical Studies for the Dissociation of Water on an Active Ni/CeO 2 Catalyst: Importance of Strong Metal-Support Interactions for the Cleavage of O-H Bonds
journal, February 2015

  • Carrasco, Javier; López-Durán, David; Liu, Zongyuan
  • Angewandte Chemie International Edition, Vol. 54, Issue 13
  • DOI: 10.1002/anie.201410697

A Linear Scaling Relation for CO Oxidation on CeO 2 -Supported Pd
journal, March 2018

  • Liu, Jin-Xun; Su, Yaqiong; Filot, Ivo A. W.
  • Journal of the American Chemical Society, Vol. 140, Issue 13
  • DOI: 10.1021/jacs.7b13624