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  Stabilization of Single Metal Atoms on Graphitic Carbon Nitride

Chen, Z., Mitchell, S., Vorobyeva, E., Leary, R. K., Hauert, R., Furnival, T., et al. (2017). Stabilization of Single Metal Atoms on Graphitic Carbon Nitride. Advanced Functional Materials, 27(8): 1605785. doi:10.1002/adfm.201605785.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002C-428B-2 Version Permalink: http://hdl.handle.net/21.11116/0000-0001-1E85-8
Genre: Journal Article

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2383090.pdf (Publisher version), 5MB
 
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 Creators:
Chen, Zupeng, Author
Mitchell, Sharon, Author
Vorobyeva, Evgeniya, Author
Leary, Rowan K., Author
Hauert, Roland, Author
Furnival, Tom, Author
Ramasse, Quentin M., Author
Thomas, John M., Author
Midgley, Paul A., Author
Dontsova, Dariya1, Author              
Antonietti, Markus2, Author              
Pogodin, Sergey, Author
López, Núria, Author
Pérez-Ramírez, Javier, Author
Affiliations:
1Dariya Dontsova, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1933288              
2Markus Antonietti, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863321              

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Free keywords: aberration-corrected scanning transmission electron microscopy, carbon nitride, density functional theory, kinetic Monte Carlo simulations, single-atom heterogeneous catalysts
 Abstract: Graphitic carbon nitride (g-C3N4) exhibits unique properties as a support for single-atom heterogeneous catalysts (SAHCs). Understanding how the synthesis method, carrier properties, and metal identity impact the isolation of metal centers is essential to guide their design. This study compares the effectiveness of direct and postsynthetic routes to prepare SAHCs by incorporating palladium, silver, iridium, platinum, or gold in g-C3N4 of distinct morphology (bulk, mesoporous and exfoliated). The speciation (single atoms, dimers, clusters, or nanoparticles), distribution, and oxidation state of the supported metals are characterized by multiple techniques including extensive use of aberration-corrected electron microscopy. SAHCs are most readily attained via direct approaches applying copolymerizable metal precursors and employing high surface area carriers. In contrast, although post-synthetic routes enable improved control over the metal loading, nanoparticle formation is more prevalent. Comparison of the carrier morphologies also points toward the involvement of defects in stabilizing single atoms. The distinct metal dispersions are rationalized by density functional theory and kinetic Monte Carlo simulations, highlighting the interplay between the adsorption energetics and diffusion kinetics. Evaluation in the continuous three-phase semihydrogenation of 1-hexyne identifies controlling the metal–carrier interaction and exposing the metal sites at the surface layer as key challenges in designing efficient SAHCs.

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 Dates: 2017-01-132017
 Publication Status: Published in print
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 Identifiers: DOI: 10.1002/adfm.201605785
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Title: Advanced Functional Materials
  Other : Adv. Funct. Mater.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: 12 Volume / Issue: 27 (8) Sequence Number: 1605785 Start / End Page: - Identifier: ISSN: 1616-301X