Patched bimetallic surfaces are active catalysts for ammonia decomposition
Abstract
In this study, ammonia decomposition is often used as an archetypical reaction for predicting new catalytic materials and understanding the very reason of why some reactions are sensitive on material’s structure. Core–shell or surface-segregated bimetallic nanoparticles expose outstanding activity for many heterogeneously catalysed reactions but the reasons remain elusive owing to the difficulties in experimentally characterizing active sites. Here by performing multiscale simulations in ammonia decomposition on various nickel loadings on platinum (111), we show that the very high activity of core–shell structures requires patches of the guest metal to create and sustain dual active sites: nickel terraces catalyse N-H bond breaking and nickel edge sites drive atomic nitrogen association. The structure sensitivity on these active catalysts depends profoundly on reaction conditions due to kinetically competing relevant elementary reaction steps. We expose a remarkable difference in active sites between transient and steady-state studies and provide insights into optimal material design.
- Authors:
-
- Univ. of Delaware, Newark, DE (United States); Beijing Institute of Technology, Beijing (China); Chinese Academy of Sciences (CAS), Beijing (China)
- Univ. of Delaware, Newark, DE (United States)
- Publication Date:
- Research Org.:
- Univ. of Delaware, Newark, DE (United States); Energy Frontier Research Centers (EFRC) (United States). Catalysis Center for Energy Innovation (CCEI)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1239294
- Grant/Contract Number:
- AC02-98CH10886; SC0001004
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 6; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; chemical sciences; catalysis; materials science; nanotechnology
Citation Formats
Guo, Wei, and Vlachos, Dionisios G. Patched bimetallic surfaces are active catalysts for ammonia decomposition. United States: N. p., 2015.
Web. doi:10.1038/ncomms9619.
Guo, Wei, & Vlachos, Dionisios G. Patched bimetallic surfaces are active catalysts for ammonia decomposition. United States. https://doi.org/10.1038/ncomms9619
Guo, Wei, and Vlachos, Dionisios G. Wed .
"Patched bimetallic surfaces are active catalysts for ammonia decomposition". United States. https://doi.org/10.1038/ncomms9619. https://www.osti.gov/servlets/purl/1239294.
@article{osti_1239294,
title = {Patched bimetallic surfaces are active catalysts for ammonia decomposition},
author = {Guo, Wei and Vlachos, Dionisios G.},
abstractNote = {In this study, ammonia decomposition is often used as an archetypical reaction for predicting new catalytic materials and understanding the very reason of why some reactions are sensitive on material’s structure. Core–shell or surface-segregated bimetallic nanoparticles expose outstanding activity for many heterogeneously catalysed reactions but the reasons remain elusive owing to the difficulties in experimentally characterizing active sites. Here by performing multiscale simulations in ammonia decomposition on various nickel loadings on platinum (111), we show that the very high activity of core–shell structures requires patches of the guest metal to create and sustain dual active sites: nickel terraces catalyse N-H bond breaking and nickel edge sites drive atomic nitrogen association. The structure sensitivity on these active catalysts depends profoundly on reaction conditions due to kinetically competing relevant elementary reaction steps. We expose a remarkable difference in active sites between transient and steady-state studies and provide insights into optimal material design.},
doi = {10.1038/ncomms9619},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {Wed Oct 07 00:00:00 EDT 2015},
month = {Wed Oct 07 00:00:00 EDT 2015}
}
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