journal article·2011-05

Hydrogen production from formic acid decomposition at room temperature using a Ag–Pd core–shell nanocatalyst

Karaked Tedsree, Tong Li, Simon Jones, Chun Wong Aaron Chan, Kai Man Kerry Yu, Paul A. J. Bagot, Emmanuelle A. Marquis, George D. W. Smith, Shik Chi Edman Tsang

Nature Nanotechnology· Volume 6· Issue 5
Publisher page

Abstract

Formic acid (HCOOH) has great potential as an in situ source of hydrogen for fuel cells, because it offers high energy density, is non-toxic and can be safely handled in aqueous solution. So far, there has been a lack of solid catalysts that are sufficiently active and/or selective for hydrogen production from formic acid at room temperature. Here, we report that Ag nanoparticles coated with a thin layer of Pd atoms can significantly enhance the production of H₂ from formic acid at ambient temperature. Atom probe tomography confirmed that the nanoparticles have a core-shell configuration, with the shell containing between 1 and 10 layers of Pd atoms. The Pd shell contains terrace sites and is electronically promoted by the Ag core, leading to significantly enhanced catalytic properties. Our nanocatalysts could be used in the development of micro polymer electrolyte membrane fuel cells for portable devices and could also be applied in the promotion of other catalytic reactions under mild conditions.
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Research context

OpenAlex topics: Carbon dioxide utilization in catalysis · CO2 Reduction Techniques and Catalysts · Electrocatalysts for Energy Conversion

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (29)

Show source-provided references
1. Zhao, T. S. Microfuel Cells: Principles and Applications (Elsevier, 2009).
2. Van den Berg, A. W. C. & Arean, C. O. Materials for hydrogen storage: current research trends and perspectives. Chem. Commun. 668–681 (2008).10.1039/B712576N ↗
3. Springer, T. E., Rockward, T., Zawodzinski, T. A. & Gottesfeld, S. Model for polymer electrolyte fuel cell operation on reformate feed–effects of CO, H2 dilution, and high fuel utilization. J. Electrochem. Soc. 148, A11–A23 (2001).10.1149/1.1344516 ↗
4. Loges, B., Boddien, A., Gartner, F., Junge, H. & Beller, M. Catalytic generation of hydrogen from formic acid and its derivatives: useful hydrogen storage materials. Top. Catal. 53, 902–914 (2010).10.1007/s11244-010-9522-8 ↗
5. Loges, B., Boddien, A., Junge, H. & Beller, M. Controlled generation of hydrogen from formic acid amine adducts at room temperature and application in H2/O2 fuel cells. Angew. Chem. Int. Ed. 47, 3962–3965 (2008).10.1002/anie.200705972 ↗
6. Fellay, C., Yan, N., Dyson, P. J. & Laurenczy, G. Selective formic acid decomposition for high-pressure hydrogen: a mechanistic study. Chem-Eur. J. 15, 3752–3760 (2009).10.1002/chem.200801824 ↗
7. Li, X. L., Ma, X. Y., Shi, F. & Deng, Y. Q. Hydrogen generation from formic acid decomposition with a ruthenium catalyst promoted by functionalized ionic liquids. ChemSusChem 3, 71–74 (2010).10.1002/cssc.200900218 ↗
8. Ruthven, D. M. & Upadhye, R. S. Catalytic decomposition of aqueous formic acid over suspended palladium catalysts. J. Catal. 21, 39–47 (1971).10.1016/0021-9517(71)90118-7 ↗
9. Ojeda, M. & Iglesia, E. Formic acid dehydrogenation on Au-based catalysts at near-ambient temperatures. Angew. Chem. Int. Ed. 48, 4800–4803 (2009).10.1002/anie.200805723 ↗
10. Zhou, X. C. et al. High-quality hydrogen from the catalyzed decomposition of formic acid by Pd–Au/C and Pd–Ag/C. Chem. Commun. 3540–3542 (2008).10.1039/b803661f ↗
11. Huang, Y., Zhou, X., Yin, M., Liu, C. & Xing, W. Novel PdAu@Au/C core–shell catalyst: superior activity and selectivity in formic acid decomposition for hydrogen generation, Chem. Mater. 22, 5122–5128 (2010).10.1021/cm101285f ↗
12. Ruban, A., Hammer, B., Stoltze, P., Skriver, H. L. & Norskov, J. K. Surface electronic structure and reactivity of transition noble metals. J. Mol. Catal. A 115, 421–429 (1997).10.1016/S1381-1169(96)00348-2 ↗
13. Larsen, R., Ha, S., Zakzeski, J. & Masel, R. I. Unusually active palladium-based catalysts for the electrooxidation of formic acid. J. Power Sources 157, 78–84 (2006).10.1016/j.jpowsour.2005.07.066 ↗
14. Borodko, Y. et al. Probing the interaction of poly(vinylpyrrolidone) with platinum nanocrystals by UV–Raman and FTIR. J. Phys. Chem. B 110, 023052 (2006).10.1021/jp063338+ ↗
15. Tao, F. et al. Reaction-driven restructuring of Rh–Pd and Pt–Pd core–shell nanoparticles. Science 322, 932–934 (2008).10.1126/science.1164170 ↗
16. Kobayashi, H. et al. Hydrogen absorption in the core/shell interface of Pd/Pt nanoparticles. J. Am. Chem. Soc. 130, 1818–1819 (2008).10.1021/ja078126k ↗
17. Zhong, C. et al. Nanostructured catalysts in fuel cells. Nanotechnology 21, 1–20 (2010).10.1088/0957-4484/21/6/062001 ↗
18. Mazumder, V., Chi, M., More, K. L. & Sun, S. Core/shell Pd/FePt nanoparticles as an active and durable catalyst for the oxygen reduction reaction. J. Am. Chem. Soc. 132, 7848–7849 (2010).10.1021/ja1024436 ↗
19. Kitchin, J. R., Norskov, J. K., Barteau, M. A. & Chen, J. G. Role of strain and ligand effects in the modification of the electronic and chemical properties of bimetallic surfaces. Phys. Rev. Lett. 93, 156801 (2004).10.1103/PhysRevLett.93.156801 ↗
20. Tang, W. & Henkelman, G. Charge redistribution in core–shell nanoparticles to promote oxygen reduction. J. Chem. Phys. 130, 194504 (2009).10.1063/1.3134684 ↗
21. Lossack, A. M., Bartels, D. M. & Roduner, E. Rate constants and kinetic isotope effects in hydrogen abstractions by H from formic acid. Res. Chem. Intermed. 27, 475–483 (2001).10.1163/156856701104202129 ↗
22. Himeda, Y., Onozawa-Komatsuzaki, M., Sugihara, H. & Kasuga, K. Simultaneous tuning of activity and water solubility of complex catalysts by acid–base equilibrium of ligands for conversion of carbon dioxide. Organometallics 26, 702–712 (2007).10.1021/om060899e ↗
23. Toshima, N. & Yonezawa, T. Bimetallic nanoparticles—novel materials for chemical and physical applications. New J. Chem. 22, 1179–1201 (1998).10.1039/a805753b ↗
24. Bagot, P. A. J., de Bocarmé, T. V., Cerezo, A. & Smith, G. D. W. 3D atom probe study of gas adsorption and reaction on alloy catalyst surfaces I: instrumentation. Surf. Sci. 600, 3028–3035 (2006).10.1016/j.susc.2006.05.026 ↗
25. Bagot, P. A. J., Cerezo, A. & Smith, G. D. W. 3D atom probe of gaseous adsorption on alloy catalyst surfaces III: ternary alloys—NO on Pt–Rh–Ru and Pt–Rh–Ir. Surf. Sci. 602, 1381–1391 (2008).10.1016/j.susc.2008.01.041 ↗
26. Yeung, C. M. Y. et al. Engineering Pt in ceria for a maximum metal-support interaction in catalysis. J. Am. Chem. Soc. 127, 18010–18011 (2005).10.1021/ja056102c ↗
27. Tedsree, K., Kong, A. T. S. & Tsang, S. C. Formate as a surface probe for ruthenium nanoparticles in solution 13C NMR spectroscopy. Angew. Chem. Int. Ed. 48, 1443–1446 (2009).10.1002/anie.200805240 ↗
28. Kim, K. S. & Barteau, M. A. Structural dependence of the selectivity of formic-acid decomposition on faceted TiO2 (001) surfaces. Langmuir 6, 1485–1488 (1990).10.1021/la00099a009 ↗
29. Hoshi, N., Nakamura, M. & Kida, K. Structural effects on the oxidation of formic acid on the high index planes of palladium. Electrochem. Commun. 9, 279–282 (2007).10.1016/j.elecom.2006.09.023 ↗