Silver-decorated palladium on carbon catalyst for enhanced ammonium formate dehydrogenation
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- Washington State University, Pullman, WA (United States)
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Washington State University, Pullman, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Energy and Environment Division, Pacific Northwest National Laboratory (PNNL), Richland, WA 99352, USA
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Palladium (Pd)-based catalysts efficiently convert ammonium formate solution to hydrogen at low temperatures (<100 °C), but they tend to deactivate quickly during stability testing. This manuscript presents a systematic investigation into the catalytic properties of Pd–Ag bimetallic catalysts, focusing on their surface compositions and exploring the mechanisms behind the deactivation of Pd/Ag-based catalysts. Here this study reports a carbon-supported Pd–Ag bimetallic nanoparticle (NP) catalyst obtained through a galvanic replacement method, which showed enhanced formate dehydrogenation performance. The best catalyst, Pd3Ag10/ACA-G (Pd–Ag bimetallic NPs with a 3 : 10 mass ratio loaded on acid-washed activated carbon, prepared by the galvanic replacement method), presents the highest activity with a TOF of 5202 h-1 (~2.6-fold of commercial Pd/C). The enhanced electron density of Pd–Ag bimetallic nanoparticles, coupled with the advantages of a smaller nanoparticle size, and the modulation of hydrogen adsorption energy through the Ag/Pd surface alloy on the Ag/Pd(111) facet, collectively resulted in experimentally higher turnover rates of hydrogen production. The changes on the catalyst surface, including surface Ag fraction decrease, NP size growth, and O-containing species (carboxylate, etc.) adsorption, gradually resulted in catalyst deactivation.
- Research Organization:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Environmental Molecular Sciences Laboratory (EMSL), Richland, WA (United States)
- Sponsoring Organization:
- USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Biological and Environmental Research (BER)
- Grant/Contract Number:
- AC52-07NA27344; EE0008826; AC05-76RL01830
- OSTI ID:
- 2283283
- Alternate ID(s):
- OSTI ID: 2248118; OSTI ID: 2337499
- Report Number(s):
- LLNL-JRNL-848105; PNNL-SA-193833; 1072752; TRN: US2408593
- Journal Information:
- Catalysis Science and Technology, Vol. 14, Issue 2; ISSN 2044-4753
- Publisher:
- Royal Society of ChemistryCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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