skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Nano-Array Integrated Structured Catalysts: A New Paradigm upon Conventional Wash-Coated Monolithic Catalysts?

Abstract

The monolithic catalyst, namely the structured catalyst, is one of the important categories of catalysts used in various fields, especially in catalytic exhaust after-treatment. Despite its successful application in conventional wash-coated catalysts in both mobile and stationary catalytic converters, washcoat-based technologies are facing multi-fold challenges, including: (1) high Pt-group metals (PGM) material loading being required, driving the market prices; (2) less-than ideal distribution of washcoats in typically square-shaped channels associated with pressure drop sacrifice; and (3) far from clear correlations between macroscopic washcoat structures and their catalytic performance. To tackle these challenges, the well-defined nanostructure array (nano-array)-integrated structured catalysts which we invented and developed recently have been proven to be a promising class of cost-effective and efficient devices that may complement or substitute wash-coated catalysts. This new type of structured catalysts is composed of honeycomb-structured monoliths, whose channel surfaces are grown in situ with a nano-array forest made of traditional binary transition metal oxide support such as Al 2O 3, CeO 2, Co 3O 4, MnO 2, TiO 2, and ZnO, or newer support materials including perovskite-type ABO3 structures, for example LaMnO 3, LaCoO 3, LaNiO, and LaFeO 3. The integration strategy parts from the traditional washcoat technique. Instead, anmore » in situ nanomaterial assembly method is utilized, such as a hydro (solva-) thermal synthesis approach, in order to create sound structure robustness, and increase ease and complex-shaped substrate adaptability. Specifically, the critical fabrication procedures for nano-array structured catalysts include deposition of seeding layer, in situ growth of nano-array, and loading of catalytic materials. The generic methodology utilization in both the magnetic stirring batch process and continuous flow reactor synthesis offers the nano-array catalysts with great potential to be scaled up readily and cost-effectively. The tunability of the structure and catalytic performance could be achieved through morphology and geometry adjustment and guest atoms and defect manipulation, as well as composite nano-array catalyst manufacture. Excellent stabilities under various conditions were also present compared to conventional wash-coated catalysts.« less

Authors:
 [1];  [1];  [1]
  1. Univ. of Connecticut, Storrs, CT (United States)
Publication Date:
Research Org.:
Univ. of Connecticut, Storrs, CT (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1425390
Alternate Identifier(s):
OSTI ID: 1430256
Grant/Contract Number:  
EE0006854; EE0000210
Resource Type:
Accepted Manuscript
Journal Name:
Catalysts
Additional Journal Information:
Journal Volume: 7; Journal Issue: 12; Journal ID: ISSN 2073-4344
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; nanostructures; nano-array structured catalysts; wash-coat structured catalysts; wet chemical synthesis; tunable structure and performance; stability

Citation Formats

Weng, Junfei, Lu, Xingxu, and Gao, Pu-Xian. Nano-Array Integrated Structured Catalysts: A New Paradigm upon Conventional Wash-Coated Monolithic Catalysts?. United States: N. p., 2017. Web. doi:10.3390/catal7090253.
Weng, Junfei, Lu, Xingxu, & Gao, Pu-Xian. Nano-Array Integrated Structured Catalysts: A New Paradigm upon Conventional Wash-Coated Monolithic Catalysts?. United States. doi:10.3390/catal7090253.
Weng, Junfei, Lu, Xingxu, and Gao, Pu-Xian. Mon . "Nano-Array Integrated Structured Catalysts: A New Paradigm upon Conventional Wash-Coated Monolithic Catalysts?". United States. doi:10.3390/catal7090253. https://www.osti.gov/servlets/purl/1425390.
@article{osti_1425390,
title = {Nano-Array Integrated Structured Catalysts: A New Paradigm upon Conventional Wash-Coated Monolithic Catalysts?},
author = {Weng, Junfei and Lu, Xingxu and Gao, Pu-Xian},
abstractNote = {The monolithic catalyst, namely the structured catalyst, is one of the important categories of catalysts used in various fields, especially in catalytic exhaust after-treatment. Despite its successful application in conventional wash-coated catalysts in both mobile and stationary catalytic converters, washcoat-based technologies are facing multi-fold challenges, including: (1) high Pt-group metals (PGM) material loading being required, driving the market prices; (2) less-than ideal distribution of washcoats in typically square-shaped channels associated with pressure drop sacrifice; and (3) far from clear correlations between macroscopic washcoat structures and their catalytic performance. To tackle these challenges, the well-defined nanostructure array (nano-array)-integrated structured catalysts which we invented and developed recently have been proven to be a promising class of cost-effective and efficient devices that may complement or substitute wash-coated catalysts. This new type of structured catalysts is composed of honeycomb-structured monoliths, whose channel surfaces are grown in situ with a nano-array forest made of traditional binary transition metal oxide support such as Al2O3, CeO2, Co3O4, MnO2, TiO2, and ZnO, or newer support materials including perovskite-type ABO3 structures, for example LaMnO3, LaCoO3, LaNiO, and LaFeO3. The integration strategy parts from the traditional washcoat technique. Instead, an in situ nanomaterial assembly method is utilized, such as a hydro (solva-) thermal synthesis approach, in order to create sound structure robustness, and increase ease and complex-shaped substrate adaptability. Specifically, the critical fabrication procedures for nano-array structured catalysts include deposition of seeding layer, in situ growth of nano-array, and loading of catalytic materials. The generic methodology utilization in both the magnetic stirring batch process and continuous flow reactor synthesis offers the nano-array catalysts with great potential to be scaled up readily and cost-effectively. The tunability of the structure and catalytic performance could be achieved through morphology and geometry adjustment and guest atoms and defect manipulation, as well as composite nano-array catalyst manufacture. Excellent stabilities under various conditions were also present compared to conventional wash-coated catalysts.},
doi = {10.3390/catal7090253},
journal = {Catalysts},
number = 12,
volume = 7,
place = {United States},
year = {2017},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 3 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Monolithic reactors for environmental applications
journal, May 2005

  • Avila, Pedro; Montes, Mario; Miró, Eduardo E.
  • Chemical Engineering Journal, Vol. 109, Issue 1-3
  • DOI: 10.1016/j.cej.2005.02.025

Exceptional high-temperature stability through distillation-like self-stabilization in bimetallic nanoparticles
journal, November 2009

  • Cao, Anmin; Veser, Götz
  • Nature Materials, Vol. 9, Issue 1
  • DOI: 10.1038/nmat2584

In situ TPR removal: a generic method for fabricating tubular array devices with mechanical and structural soundness, and functional robustness on various substrates
journal, January 2012

  • Zhang, Zhonghua; Gao, Haiyong; Cai, Wenjie
  • Journal of Materials Chemistry, Vol. 22, Issue 43, p. 23098-23105
  • DOI: 10.1039/c2jm34606k

Oxidation reactions on neutral cobalt oxideclusters: experimental and theoretical studies
journal, January 2010

  • Xie, Yan; Dong, Feng; Heinbuch, Scott
  • Phys. Chem. Chem. Phys., Vol. 12, Issue 4
  • DOI: 10.1039/B915590B

Mechanical Stability of Monolithic Catalysts: Scattering of Washcoat Adhesion and Failure Mechanism of Active Material
journal, October 2013

  • Wu, Dongfang; Zhang, Hua
  • Industrial & Engineering Chemistry Research, Vol. 52, Issue 41
  • DOI: 10.1021/ie402546q

DOC modeling combining kinetics and mass transfer using inert washcoat layers
journal, August 2016


Mechanistic Studies of the Oxygen Evolution Reaction by a Cobalt-Phosphate Catalyst at Neutral pH
journal, November 2010

  • Surendranath, Yogesh; Kanan, Matthew W.; Nocera, Daniel G.
  • Journal of the American Chemical Society, Vol. 132, Issue 46
  • DOI: 10.1021/ja106102b

Synthesis, characterization and CO oxidation of TiO2/(La,Sr)MnO3 composite nanorod array
journal, April 2012


Manganese Oxide Nanoarray-Based Monolithic Catalysts: Tunable Morphology and High Efficiency for CO Oxidation
journal, March 2016

  • Chen, Sheng-Yu; Song, Wenqiao; Lin, Hui-Jan
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 12
  • DOI: 10.1021/acsami.6b00578

Nonprecious catalytic honeycombs structured with three dimensional hierarchical Co3O4 nano-arrays for high performance nitric oxide oxidation
journal, January 2013

  • Ren, Zheng; Guo, Yanbing; Zhang, Zhonghua
  • Journal of Materials Chemistry A, Vol. 1, Issue 34
  • DOI: 10.1039/c3ta11156c

Hierarchically nanostructured materials for sustainable environmental applications
journal, January 2013


Monolith structures, materials, properties and uses
journal, September 2001


Origin of the High Activity and Stability of Co3O4 in Low-temperature CO Oxidation
journal, June 2008


Automotive exhaust catalysis
journal, May 2003


One-dimensional ZnO nanostructures: Solution growth and functional properties
journal, August 2011


Alkaline doped TiO2 sol–gel catalysts: Effect of sintering on catalyst activity and selectivity for acetone condensation
journal, August 2006


Synthesis of High Surface Area ZnO(0001) Plates as Novel Oxide Supports for Heterogeneous Catalysts
journal, July 2010

  • Burton, Patrick D.; Peterson, Eric J.; Boyle, Timothy J.
  • Catalysis Letters, Vol. 139, Issue 1-2
  • DOI: 10.1007/s10562-010-0405-1

Low-temperature oxidation of CO catalysed by Co3O4 nanorods
journal, April 2009

  • Xie, Xiaowei; Li, Yong; Liu, Zhi-Quan
  • Nature, Vol. 458, Issue 7239, p. 746-749
  • DOI: 10.1038/nature07877

Combined (S)TEM-FIB Insight into the Influence of the Preparation Method on the Final Surface Structure of a Co 3 O 4 /La-Modified-CeO 2 Washcoated Monolithic Catalyst
journal, June 2013

  • Hernández-Garrido, Juan C.; Gómez, Diana M.; Gaona, Diana
  • The Journal of Physical Chemistry C, Vol. 117, Issue 25
  • DOI: 10.1021/jp400151y

Preparation of monolithic catalysts
journal, November 2001

  • Nijhuis, T. Alexander; Beers, Annemarie E. W.; Vergunst, Theo
  • Catalysis Reviews, Vol. 43, Issue 4
  • DOI: 10.1081/CR-120001807

Mechanical-Agitation-Assisted Growth of Large-Scale and Uniform ZnO Nanorod Arrays within 3D Multichannel Monolithic Substrates
journal, July 2013

  • Xiao, Wen; Guo, Yanbing; Ren, Zheng
  • Crystal Growth & Design, Vol. 13, Issue 8
  • DOI: 10.1021/cg400672z

Comparative study of the catalytic performance and final surface structure of Co3O4/La-CeO2 washcoated ceramic and metallic honeycomb monoliths
journal, September 2015


Mechanical stability of monolithic catalysts: Factors affecting washcoat adhesion and cohesion during preparation
journal, May 2014

  • Wu, Dongfang; Kong, Shangshang; Zhang, Hua
  • AIChE Journal, Vol. 60, Issue 8
  • DOI: 10.1002/aic.14480

Selective Synthesis of Co 3 O 4 Nanocrystal with Different Shape and Crystal Plane Effect on Catalytic Property for Methane Combustion
journal, December 2008

  • Hu, Linhua; Peng, Qing; Li, Yadong
  • Journal of the American Chemical Society, Vol. 130, Issue 48
  • DOI: 10.1021/ja806400e

Monolith-Like TiO 2 Nanotube Array Supported Pt Catalyst for HCHO Removal under Mild Conditions
journal, April 2014

  • Chen, Huayao; Rui, Zebao; Ji, Hongbing
  • Industrial & Engineering Chemistry Research, Vol. 53, Issue 18
  • DOI: 10.1021/ie5004009

Low temperature propane oxidation over Co3O4 based nano-array catalysts: Ni dopant effect, reaction mechanism and structural stability
journal, January 2016


The significance of vehicle emissions standards for levels of exhaust pollution from light vehicles in an urban area
journal, June 2011


Surface active sites on Co3O4 nanobelt and nanocube model catalysts for CO oxidation
journal, April 2010


Nano-array based monolithic catalysts: Concept, rational materials design and tunable catalytic performance
journal, December 2015