Abstract:
Electrocatalytic proton reduction leading to the formation of adsorbed molecular hydrogen on gold nanoparticles of 1-3 and 14-16 nm diameter stabilized by 1-mercapto-undecane-11-tetra(ethyleneglycol) has been demonstrated by cyclic voltammetry using a hanging mercury drop electrode. The nanoparticles were adsorbed to the electrode from aqueous dispersion and formed robust surface layers transferrable to fresh base electrolyte solutions. Unique electrocatalytic proton redox chemistry was observed that has no comparable counterpart in the electrochemistry of bulk gold electrodes. Depending on size, the nanoparticles have a discrete number of electrocatalytically active sites for the two-electron/two-proton reduction process. The adsorbed hydrogen formed is oxidized with the reverse potential sweep. These findings represent a new example of qualitative different behavior of nanoparticles in comparison with the corresponding bulk material. © 2012 American Chemical Society.
Registro:
Documento: |
Artículo
|
Título: | Electrocatalytic hydrogen redox chemistry on gold nanoparticles |
Autor: | Brust, M.; Gordillo, G.J. |
Filiación: | Department of Chemistry, University of Liverpool, Crown Street, Liverpool L69 7ZD, United Kingdom Departamento de Química Inorgánica, Analítica y Química Física, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, (1428), Buenos Aires, Argentina
|
Palabras clave: | Active site; Adsorbed hydrogen; Aqueous dispersions; Base electrolytes; Bulk materials; Discrete numbers; Electrocatalytic; Gold electrodes; Gold Nanoparticles; Hanging mercury drop electrodes; Molecular hydrogen; Potential sweep; Proton reduction; Redox chemistry; Reduction process; Surface layers; Cyclic voltammetry; Electrocatalysis; Gold; Hydrogen; Mercury (metal); Protons; Reduction; Nanoparticles; 1 mercapto undecane 11 tetra(ethyleneglycol); electrolyte; ethylene glycol; gold nanoparticle; hydrogen; unclassified drug; article; catalyst; cyclic potentiometry; electrochemistry; electrode; oxidation reduction reaction |
Año: | 2012
|
Volumen: | 134
|
Número: | 7
|
Página de inicio: | 3318
|
Página de fin: | 3321
|
DOI: |
http://dx.doi.org/10.1021/ja2096514 |
Título revista: | Journal of the American Chemical Society
|
Título revista abreviado: | J. Am. Chem. Soc.
|
ISSN: | 00027863
|
CODEN: | JACSA
|
CAS: | ethylene glycol, 107-21-1; hydrogen, 12385-13-6, 1333-74-0
|
Registro: | https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00027863_v134_n7_p3318_Brust |
Referencias:
- Astruc, D., (2004) Chem. Rev., 104, pp. 293-346
- Hutchings, G.J., Brust, M., Schmidbaur, H., (2008) Chem. Soc. Rev., 37, pp. 1759-1765
- Myroshnychenko, V., Rodríguez-Fernández, J., Pastoriza-Santos, I., Funston, A.M., Novo, C., Mulvaney, P., Liz-Marzán, L.M., García De Abajo, F.J., (2008) Chem. Soc. Rev., 37, pp. 1792-1805
- Herzing, A.A., Kiely, C.J., Carley, A.F., Landon, P., Hutchings, G.J., (2008) Science, 321, pp. 1331-1335
- Haruta, M., Kobayashi, T., Sano, H., Yamada, N., (1987) Chem. Lett., pp. 405-408
- Haruta, M., Yamada, N., Kobayashi, T., Iijima, S., (1989) J. Catal., 115, pp. 301-309
- Haruta, M., (1997) Catal. Today, 36, pp. 153-166
- Ingram, R.S., Hostetler, M.J., Murray, R.W., Schaaff, T.G., Khoury, J.T., Whetten, R.L., Bigioni, T.P., First, P.N., (1997) J. Am. Chem. Soc., 119, pp. 9279-9280
- Chen, S., Ingram, R.S., Hostetler, M.J., Pietron, J.J., Murray, R.W., Schaaff, T.G., Khoury, J.T., Whetten, R.L., (1998) Science, 280, pp. 2098-2101
- Chen, S., Murray, R.W., Feldberg, S.W., (1998) J. Phys. Chem. B, 102, pp. 9898-9907
- Murray, R.W., (2008) Chem. Rev., 108, pp. 2688-2720
- Tsunoyama, H., Ichikuni, N., Sakurai, H., Tsukuda, T., (2009) J. Am. Chem. Soc., 131, pp. 7086-7093
- Tsukuda, T., Tsunoyama, H., Sakurai, H., (2011) Chem.-Asian J., 6, pp. 736-748
- Mirkhalaf, F., Schiffrin, D.J., (2010) Langmuir, 26, pp. 14995-15001
- Claus, P., (2005) Appl. Catal., A, 291, pp. 222-229
- Kartusch, C., Van Bokhoven, J.A., (2009) Gold Bull., 42, pp. 343-348
- Barrio, L., Liu, P., Rodríguez, J.A., Campos-Martín, J.M., Fierro, J.L.G., (2006) J. Chem. Phys., 125, p. 164715
- Brug, G.J., Sluyters-Rehbach, M., Sluyters, J.H., (1984) J. Electroanal. Chem., 181, pp. 245-266
- Hamelin, A., Weaver, M.J., (1987) J. Electroanal. Chem., 223, pp. 171-184
- Vetter, K.J., (1967) Electrochemical Kinetics, , Academic Press: New York
- Hasan, M., Bethell, D., Brust, M., (2002) J. Am. Chem. Soc., 124, pp. 1132-1133
- Bethell, D., Brust, M., Schiffrin, D.J., Kiely, C.J., (1996) J. Electroanal. Chem., 409, pp. 137-143
- Brust, M., Bethell, D., Kiely, C.J., Schiffrin, D.J., (1998) Langmuir, 14, pp. 5425-5429
Citas:
---------- APA ----------
Brust, M. & Gordillo, G.J.
(2012)
. Electrocatalytic hydrogen redox chemistry on gold nanoparticles. Journal of the American Chemical Society, 134(7), 3318-3321.
http://dx.doi.org/10.1021/ja2096514---------- CHICAGO ----------
Brust, M., Gordillo, G.J.
"Electrocatalytic hydrogen redox chemistry on gold nanoparticles"
. Journal of the American Chemical Society 134, no. 7
(2012) : 3318-3321.
http://dx.doi.org/10.1021/ja2096514---------- MLA ----------
Brust, M., Gordillo, G.J.
"Electrocatalytic hydrogen redox chemistry on gold nanoparticles"
. Journal of the American Chemical Society, vol. 134, no. 7, 2012, pp. 3318-3321.
http://dx.doi.org/10.1021/ja2096514---------- VANCOUVER ----------
Brust, M., Gordillo, G.J. Electrocatalytic hydrogen redox chemistry on gold nanoparticles. J. Am. Chem. Soc. 2012;134(7):3318-3321.
http://dx.doi.org/10.1021/ja2096514