Controlling the rate of change of Ni dispersion in commercial catalyst by ALD overcoat during dry reforming of methane

Shaik Afzal; Anuj V. Prakash; Patrick Littlewood; Tobin J. Marks; Eric Weitz; Peter C. Stair; Nimir O. Elbashir

doi:10.1016/j.ijhydene.2020.03.008

Controlling the rate of change of Ni dispersion in commercial catalyst by ALD overcoat during dry reforming of methane

Shaik Afzal, Anuj V. Prakash, Patrick Littlewood, Tobin J. Marks, Eric Weitz, Peter C. Stair, Nimir O. Elbashir

Northwestern University

Research output: Contribution to journal › Article › peer-review

2 Citations (Scopus)

Abstract

This study investigates changes in dispersion with time-on-stream of a Ni catalyst coated with alumina by Atomic Layer Deposition (ALD) in Dry Reforming of Methane (DRM) conditions. A 20 wt% commercial Ni catalyst is coated with 5, 10, and 20 ALD cycles and tested for DRM at 650 °C, 1 atm for 40 h. Using an in-situ H₂–CO pulse chemisorption technique, it is found that the rate of decline in catalyst dispersion is more rapid in the uncoated catalyst (~0.11%h⁻¹) than 5-ALD catalyst (~0.025%h⁻¹). TEM images before and after reaction show that the average particle size for the uncoated catalyst increases from 8.5 nm to 24.5 nm, indicating sintering, whereas the 5-ALD catalyst retained the initial particle size. The reduced particle size also explains the 50% reduction in carbon formation-rate in the 5-ALD catalyst. The developed sequential H₂–CO chemisorption technique reliably measures in-situ dispersion in uncoated and ALD coated catalysts with exposed active sites.

Original language	English
Pages (from-to)	12835-12848
Number of pages	14
Journal	International Journal of Hydrogen Energy
Volume	45
Issue number	23
DOIs	https://doi.org/10.1016/j.ijhydene.2020.03.008
Publication status	Published - Apr 28 2020

Keywords

Atomic layer deposition (ALD)
Chemisorption
Dispersion
Methane dry reforming (DRM)
Ni catalyst

ASJC Scopus subject areas

Renewable Energy, Sustainability and the Environment
Fuel Technology
Condensed Matter Physics
Energy Engineering and Power Technology

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Controlling the rate of change of Ni dispersion in commercial catalyst by ALD overcoat during dry reforming of methane. / Afzal, Shaik; Prakash, Anuj V.; Littlewood, Patrick; Marks, Tobin J.; Weitz, Eric; Stair, Peter C.; Elbashir, Nimir O.

In: International Journal of Hydrogen Energy, Vol. 45, No. 23, 28.04.2020, p. 12835-12848.

Research output: Contribution to journal › Article › peer-review

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title = "Controlling the rate of change of Ni dispersion in commercial catalyst by ALD overcoat during dry reforming of methane",

abstract = "This study investigates changes in dispersion with time-on-stream of a Ni catalyst coated with alumina by Atomic Layer Deposition (ALD) in Dry Reforming of Methane (DRM) conditions. A 20 wt% commercial Ni catalyst is coated with 5, 10, and 20 ALD cycles and tested for DRM at 650 °C, 1 atm for 40 h. Using an in-situ H2–CO pulse chemisorption technique, it is found that the rate of decline in catalyst dispersion is more rapid in the uncoated catalyst (~0.11%h−1) than 5-ALD catalyst (~0.025%h−1). TEM images before and after reaction show that the average particle size for the uncoated catalyst increases from 8.5 nm to 24.5 nm, indicating sintering, whereas the 5-ALD catalyst retained the initial particle size. The reduced particle size also explains the 50% reduction in carbon formation-rate in the 5-ALD catalyst. The developed sequential H2–CO chemisorption technique reliably measures in-situ dispersion in uncoated and ALD coated catalysts with exposed active sites.",

keywords = "Atomic layer deposition (ALD), Chemisorption, Dispersion, Methane dry reforming (DRM), Ni catalyst",

author = "Shaik Afzal and Prakash, {Anuj V.} and Patrick Littlewood and Marks, {Tobin J.} and Eric Weitz and Stair, {Peter C.} and Elbashir, {Nimir O.}",

note = "Funding Information: This work was supported by Qatar National Research Fund (QNRF) , member of Qatar Foundation (NPRP X - 100 - 2 - 024). The statements made herein are solely the responsibility of the authors. The authors would also like to acknowledge Dr. Said Mansour from Qatar Environment and Energy Research Institute (QEERI) and Dr. Kim Hansoo from Microscopy Imaging Center (MIC) , Texas A&M University for their support in obtaining TEM images. ",

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AU - Afzal, Shaik

AU - Prakash, Anuj V.

AU - Littlewood, Patrick

AU - Marks, Tobin J.

AU - Weitz, Eric

AU - Stair, Peter C.

AU - Elbashir, Nimir O.

N1 - Funding Information: This work was supported by Qatar National Research Fund (QNRF) , member of Qatar Foundation (NPRP X - 100 - 2 - 024). The statements made herein are solely the responsibility of the authors. The authors would also like to acknowledge Dr. Said Mansour from Qatar Environment and Energy Research Institute (QEERI) and Dr. Kim Hansoo from Microscopy Imaging Center (MIC) , Texas A&M University for their support in obtaining TEM images.

PY - 2020/4/28

Y1 - 2020/4/28

N2 - This study investigates changes in dispersion with time-on-stream of a Ni catalyst coated with alumina by Atomic Layer Deposition (ALD) in Dry Reforming of Methane (DRM) conditions. A 20 wt% commercial Ni catalyst is coated with 5, 10, and 20 ALD cycles and tested for DRM at 650 °C, 1 atm for 40 h. Using an in-situ H2–CO pulse chemisorption technique, it is found that the rate of decline in catalyst dispersion is more rapid in the uncoated catalyst (~0.11%h−1) than 5-ALD catalyst (~0.025%h−1). TEM images before and after reaction show that the average particle size for the uncoated catalyst increases from 8.5 nm to 24.5 nm, indicating sintering, whereas the 5-ALD catalyst retained the initial particle size. The reduced particle size also explains the 50% reduction in carbon formation-rate in the 5-ALD catalyst. The developed sequential H2–CO chemisorption technique reliably measures in-situ dispersion in uncoated and ALD coated catalysts with exposed active sites.

AB - This study investigates changes in dispersion with time-on-stream of a Ni catalyst coated with alumina by Atomic Layer Deposition (ALD) in Dry Reforming of Methane (DRM) conditions. A 20 wt% commercial Ni catalyst is coated with 5, 10, and 20 ALD cycles and tested for DRM at 650 °C, 1 atm for 40 h. Using an in-situ H2–CO pulse chemisorption technique, it is found that the rate of decline in catalyst dispersion is more rapid in the uncoated catalyst (~0.11%h−1) than 5-ALD catalyst (~0.025%h−1). TEM images before and after reaction show that the average particle size for the uncoated catalyst increases from 8.5 nm to 24.5 nm, indicating sintering, whereas the 5-ALD catalyst retained the initial particle size. The reduced particle size also explains the 50% reduction in carbon formation-rate in the 5-ALD catalyst. The developed sequential H2–CO chemisorption technique reliably measures in-situ dispersion in uncoated and ALD coated catalysts with exposed active sites.

KW - Atomic layer deposition (ALD)

KW - Chemisorption

KW - Dispersion

KW - Methane dry reforming (DRM)

KW - Ni catalyst

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