Dry Reforming of Methane on Single-Site Ni/MgO Catalysts: Importance of Site Confinement
Abstract
Single-site catalysts (SSCs) have drawn considerable attention, because of their superior behaviors in catalysis. However, the origin of promoting the effect of a single site is not well understood. Here in this paper, we take the single-atom Ni1/Mg(100) and single-site Ni4/Mg(100) catalysts as a case study to elucidate their behaviors under the complex dry reforming of methane (DRM, CO2 + CH4→ 2CO + 2H2) reaction by combining theoretical modeling (density functional theory and kinetic Monte Carlo simulation) and experimental studies. The synergy between single Ni atom and MgO is found to improve the binding property of MgO; yet, it is not enough to dissociate CO2 and CH4. It can be achieved by the single-site Ni4/MgO(100) catalyst, enabling the formations of CO, H2, and H2O under the DRM conditions. During this process, coking, as observed for bulklike Ni particles, is eliminated. By confining the reaction to occur at the isolated Ni sites in the SSC, the Ni4/MgO(100) catalyst is able to balance the CO2 and CH4 activations, which is identified as the key for tuning the DRM activity and selectivity of Ni/MgO catalysts. The theory-identified promotion introduced by increasing the size of MgO-supported Ni clusters from Ni1 to Ni4 and themore »
- Authors:
-
- Taiyuan Univ. of Technology, Taiyua, Shanxi (China). Key Lab. of Coal Science and Technology of Ministry of Education and Shanxi Province
- State Univ. of New York (SUNY), Stony Brook, NY (United States). Chemistry Dept.
- Univ. of Sydney, NSW (Australia). Lab. for Catalysis Engineering, School of Chemical and Biomolecular Engineering
- Yangzhou Univ.,Yangzhou, Jiangsu (China). Mechanical Engineering College
- Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1473658
- Report Number(s):
- BNL-209070-2018-JAAM
Journal ID: ISSN 2155-5435
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 8; 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; DFT; dry reforming of methane; KMC; Ni/MgO; single-site catalyst; site confinement; TEM
Citation Formats
Zuo, Zhijun, Liu, Shizhong, Wang, Zichun, Liu, Cheng, Huang, Wei, Huang, Jun, and Liu, Ping. Dry Reforming of Methane on Single-Site Ni/MgO Catalysts: Importance of Site Confinement. United States: N. p., 2018.
Web. doi:10.1021/acscatal.8b02277.
Zuo, Zhijun, Liu, Shizhong, Wang, Zichun, Liu, Cheng, Huang, Wei, Huang, Jun, & Liu, Ping. Dry Reforming of Methane on Single-Site Ni/MgO Catalysts: Importance of Site Confinement. United States. https://doi.org/10.1021/acscatal.8b02277
Zuo, Zhijun, Liu, Shizhong, Wang, Zichun, Liu, Cheng, Huang, Wei, Huang, Jun, and Liu, Ping. Wed .
"Dry Reforming of Methane on Single-Site Ni/MgO Catalysts: Importance of Site Confinement". United States. https://doi.org/10.1021/acscatal.8b02277. https://www.osti.gov/servlets/purl/1473658.
@article{osti_1473658,
title = {Dry Reforming of Methane on Single-Site Ni/MgO Catalysts: Importance of Site Confinement},
author = {Zuo, Zhijun and Liu, Shizhong and Wang, Zichun and Liu, Cheng and Huang, Wei and Huang, Jun and Liu, Ping},
abstractNote = {Single-site catalysts (SSCs) have drawn considerable attention, because of their superior behaviors in catalysis. However, the origin of promoting the effect of a single site is not well understood. Here in this paper, we take the single-atom Ni1/Mg(100) and single-site Ni4/Mg(100) catalysts as a case study to elucidate their behaviors under the complex dry reforming of methane (DRM, CO2 + CH4→ 2CO + 2H2) reaction by combining theoretical modeling (density functional theory and kinetic Monte Carlo simulation) and experimental studies. The synergy between single Ni atom and MgO is found to improve the binding property of MgO; yet, it is not enough to dissociate CO2 and CH4. It can be achieved by the single-site Ni4/MgO(100) catalyst, enabling the formations of CO, H2, and H2O under the DRM conditions. During this process, coking, as observed for bulklike Ni particles, is eliminated. By confining the reaction to occur at the isolated Ni sites in the SSC, the Ni4/MgO(100) catalyst is able to balance the CO2 and CH4 activations, which is identified as the key for tuning the DRM activity and selectivity of Ni/MgO catalysts. The theory-identified promotion introduced by increasing the size of MgO-supported Ni clusters from Ni1 to Ni4 and the MgO-introduced site confinement of single-site catalysts are verified by corresponding experimental studies, highlighting the essential roles of confined sites in tuning the performance of SSCs during complex catalytic processes.},
doi = {10.1021/acscatal.8b02277},
journal = {ACS Catalysis},
number = ,
volume = 8,
place = {United States},
year = {Wed Sep 26 00:00:00 EDT 2018},
month = {Wed Sep 26 00:00:00 EDT 2018}
}
Web of Science
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