Efficient Pd on carbon catalyst for ammonium formate dehydrogenation: Effect of surface oxygen functional groups
Abstract
Formate solution is one of a kind promising liquid organic hydrogen carrier but suffers from kinetic challenges. This study investigates the kinetics of the surface functionalized Pd on carbon catalysts for formate dehydrogenation and the impact of O-functional groups. Here, the fraction of the distinguished O-functional groups was modulated by the different concentrated HNO3 solutions treatment or by H2 reduction. This study shows that the O-functional groups play critical roles in dispersing Pd nanoparticles and decreasing the activation energy for dehydrogenation. Density functional theory (DFT) calculation reveals that most O-functional groups enhance formate adsorption on the Pd active site. However, the existence of C=O groups consumes reducing agents and hinders the formation of metallic Pd. The electron transfer from Pd to oxygen functional groups is unfavorable to dehydrogenation. The as-prepared Pd5/re-ACA (reduced activated carbon washed by acid) exhibited significant activity with a higher turnover frequency of 13,511 h-1 than commercial Pd/C.
- Authors:
-
[3];
[3];
[1]
- Washington State Univ., Pullman, WA (United States)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office
- OSTI Identifier:
- 1924492
- Alternate Identifier(s):
- OSTI ID: 1959455
- Report Number(s):
- PNNL-SA-174225; LLNL-JRNL-834919
Journal ID: ISSN 0926-3373
- Grant/Contract Number:
- AC05-76RL01830; EE0008826; AC52-07NA27344
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Applied Catalysis. B, Environmental
- Additional Journal Information:
- Journal Volume: 321; Journal ID: ISSN 0926-3373
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; Ammonium formate; O-functional group; Dehydrogenation; LOHCs; Palladium; ammonium formate; dehydrogenation; palladium
Citation Formats
Dong, Zhun, Mukhtar, Ahmad, Ludwig, Thomas K., Akhade, Sneha A., Kang, Shinyoung, Wood, Brandon C., Grubel, Katarzyna, Engelhard, Mark H., Autrey, S. Thomas, and Lin, Hongfei. Efficient Pd on carbon catalyst for ammonium formate dehydrogenation: Effect of surface oxygen functional groups. United States: N. p., 2022.
Web. doi:10.1016/j.apcatb.2022.122015.
Dong, Zhun, Mukhtar, Ahmad, Ludwig, Thomas K., Akhade, Sneha A., Kang, Shinyoung, Wood, Brandon C., Grubel, Katarzyna, Engelhard, Mark H., Autrey, S. Thomas, & Lin, Hongfei. Efficient Pd on carbon catalyst for ammonium formate dehydrogenation: Effect of surface oxygen functional groups. United States. https://doi.org/10.1016/j.apcatb.2022.122015
Dong, Zhun, Mukhtar, Ahmad, Ludwig, Thomas K., Akhade, Sneha A., Kang, Shinyoung, Wood, Brandon C., Grubel, Katarzyna, Engelhard, Mark H., Autrey, S. Thomas, and Lin, Hongfei. Tue .
"Efficient Pd on carbon catalyst for ammonium formate dehydrogenation: Effect of surface oxygen functional groups". United States. https://doi.org/10.1016/j.apcatb.2022.122015. https://www.osti.gov/servlets/purl/1924492.
@article{osti_1924492,
title = {Efficient Pd on carbon catalyst for ammonium formate dehydrogenation: Effect of surface oxygen functional groups},
author = {Dong, Zhun and Mukhtar, Ahmad and Ludwig, Thomas K. and Akhade, Sneha A. and Kang, Shinyoung and Wood, Brandon C. and Grubel, Katarzyna and Engelhard, Mark H. and Autrey, S. Thomas and Lin, Hongfei},
abstractNote = {Formate solution is one of a kind promising liquid organic hydrogen carrier but suffers from kinetic challenges. This study investigates the kinetics of the surface functionalized Pd on carbon catalysts for formate dehydrogenation and the impact of O-functional groups. Here, the fraction of the distinguished O-functional groups was modulated by the different concentrated HNO3 solutions treatment or by H2 reduction. This study shows that the O-functional groups play critical roles in dispersing Pd nanoparticles and decreasing the activation energy for dehydrogenation. Density functional theory (DFT) calculation reveals that most O-functional groups enhance formate adsorption on the Pd active site. However, the existence of C=O groups consumes reducing agents and hinders the formation of metallic Pd. The electron transfer from Pd to oxygen functional groups is unfavorable to dehydrogenation. The as-prepared Pd5/re-ACA (reduced activated carbon washed by acid) exhibited significant activity with a higher turnover frequency of 13,511 h-1 than commercial Pd/C.},
doi = {10.1016/j.apcatb.2022.122015},
journal = {Applied Catalysis. B, Environmental},
number = ,
volume = 321,
place = {United States},
year = {Tue Sep 27 00:00:00 EDT 2022},
month = {Tue Sep 27 00:00:00 EDT 2022}
}
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Table 1: Thermodynamics of formic acid and formate solution up-taking and releasing H2.
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