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Visualizing zeptomole (electro)catalysis at single nanoparticles within an ensemble

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Lai, Stanley Chi Shing, Dudin, Petr V., Macpherson, Julie V. and Unwin, Patrick R.. (2011) Visualizing zeptomole (electro)catalysis at single nanoparticles within an ensemble. Journal of the American Chemical Society, Volume 133 (Number 28). pp. 10744-10747. ISSN 0002-7863

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Official URL: http://dx.doi.org/10.1021/ja203955b

Abstract

The relationship between the structural properties, such as the size and the shape, of a catalytic nanoparticle and its reactivity is a key concept in (electro) catalysis. Current understanding of this relationship is mainly derived from studies involving large ensembles of nanoparticles (NPs). However, the results necessarily reflect the average catalytic behavior of an ensemble, even though the properties of individual particles may vary widely. Here, we demonstrate a novel approach using scanning electrochemical cell microscopy (SECCM) to locate and map the reactivity of individual NPs within an electrocatalytic ensemble, consisting of platinum NPs supported on a single carbon nanotube. Significantly, our studies show that subtle variations in the morphology of NPs lead to dramatic changes in (potential-dependent) reactivity, which has important implications for the design and assessment of NP catalysts. The instrumental approach described is general and opens up new avenues of research in functional imaging, nanoscale electron transfer, and catalysis.

Item Type:	Journal Article
Subjects:	Q Science > QD Chemistry T Technology > TP Chemical technology
Divisions:	Faculty of Science > Chemistry
Library of Congress Subject Headings (LCSH):	Electrochemistry, Electrocatalysis, Nanoparticles, Scanning electrochemical microscopy
Journal or Publication Title:	Journal of the American Chemical Society
Publisher:	American Chemical Society
ISSN:	0002-7863
Date:	20 July 2011
Volume:	Volume 133
Number:	Number 28
Page Range:	pp. 10744-10747
Identification Number:	10.1021/ja203955b
Status:	Peer Reviewed
Publication Status:	Published
Access rights to Published version:	Restricted or Subscription Access
Funder:	Engineering and Physical Sciences Research Council (EPSRC) , European Research Council (ERC)
References:	(1) Somorjai, G. A. Science 1985, 227, 902. (2) Daniel, M.-C.; Astruc, D. Chem. Rev. 2003, 104, 293. (3) Chen, A.; Holt-Hindle, P. Chem. Rev. 2010, 110, 3767. (4) Xu, W. L.; Shen, H.; Liu, G. K.; Chen, P. Nano Res. 2009, 2, 911. (5) Xu, Z.; Xiao, F. S.; Purnell, S. K.; Alexeev, O.; Kawi, S.; Deutsch, S. E.; Gates, B. C. Nature 1994, 372, 346. (6) S nche -S nche , C. M. Solla- ull n, . Vidal-Iglesias, F. J.; Aldaz, A.; Montiel, V.; Herrero, E. J. Am. Chem. Soc. 2010, 132, 5622. (7) Tian, N.; Zhou, Z. Y.; Sun, S. G.; Ding, Y.; Wang, Z. L. Science 2007, 316, 732. (8) Ahmadi, T. S.; Wang, Z. L.; Green, T. C.; Henglein, A.; ElSayed, M. A. Science 1996, 272, 1924. (9) Sun, Y. G.; Xia, Y. N. Science 2002, 298, 2176. (10) Burda, C.; Chen, X.; Narayanan, R.; El-Sayed, M. A. Chem. Rev. 2005, 105, 1025. (11) Ortalan, V.; Uzun, A.; Gates, B. C.; Browning, N. D. Na-ture Nanotech. 2010, 5, 843. (12) Vajda, S.; Pellin, M. J.; Greeley, J. P.; Marshall, C. L.; Curtiss, L. A.; Ballentine, G. A.; Elam, J. W.; Catillon-Mucherie, S.; Redfern, P. C.; Mehmood, F.; Zapol, P. Nature Mater. 2009, 8, 213. (13) Greeley, J.; Rossmeisl, J.; Hellmann, A.; Nørskov, J. K. Z. Phys. Chem. 2007, 221, 1209. (14) Hashmi, A. S. K.; Hutchings, G. J. Angew. Chem. Int. Ed. 2006, 45, 7896. (15) Krapf, D.; Wu, M.-Y.; Smeets, R. M. M.; Zandbergen, H. W.; Dekker, C.; Lemay, S. G. Nano Lett. 2005, 6, 105. (16) Chen, S.; Kucernak, A. J. Phys. Chem. B 2003, 107, 8392. (17) Xiao, X. Y.; Bard, A. J. J. Am. Chem. Soc. 2007, 129, 9610. (18) Tel-Vered, R.; Bard, A. J. J. Phys. Chem. B 2006, 110, 25279. (19) Meier, J.; Friedrich, K. A.; Stimming, U. Faraday Discuss. 2002, 121, 365. (20) Chen, S.; Kucernak, A. J. Phys. Chem. B 2004, 108, 3262. (21) Bard, A. J. J. Am. Chem. Soc. 2010, 132, 7559. (22) Ebejer, N.; Schnippering, M.; Colburn, A. W.; Edwards, M. A.; Unwin, P. R. Anal. Chem. 2010, 82, 9141. (23) Quinn, B. M.; Dekker, C.; Lemay, S. G. J. Am. Chem. Soc. 2005, 127, 6146. (24) Day, T. M.; Unwin, P. R.; Wilson, N. R.; Macpherson, J. V. J. Am. Chem. Soc. 2005, 127, 10639. (25) Penner, R. M. J. Phys. Chem. B 2002, 106, 3339. (26) Bayati, M.; Abad, J. M.; Nichols, R. J.; Schiffrin, D. J. J. Phys. Chem. C 2010, 114, 18439. (27) Jeon, H.; Joo, J.; Kwon, Y.; Uhm, S.; Lee, J. J. Power Sources 2010, 195, 5929. (28) Wilson, M. S.; Garzon, F. H.; Sickafus, K. E.; Gottesfeld, S. J. Electrochem. Soc. 1993, 140, 2872. (29) Mamat, M. S.; Grigoriev, S. A.; Dzhus, K. A.; Grant, D. M.; Walker, G. S. Int. J. Hydrogen Energy 2010, 35, 7580. (30) Komanicky, V.; Menzel, A.; You, H. J. Phys. Chem. B 2005, 109, 23550. (31) Devred, F.; Gieske, A. H.; Adkins, N.; Dahlborg, U.; Bao, C. M.; Calvo-Dahlborg, M.; Bakker, J. W.; Nieuwenhuys, B. E. Appl. Catal. A: General 2009, 356, 154. (32) Schlogl, R. Angew. Chem.-Int. Edit. 2003, 42, 2004. (33) Erisman, J. W.; Sutton, M. A.; Galloway, J.; Klimont, Z.; Winiwarter, W. Nat. Geosci. 2008, 1, 636. (34) Huber, G. W.; Iborra, S.; Corma, A. Chem. Rev. 2006, 106, 4044. (35) Vasile, M. J.; Enke, C. G. J. Electrochem. Soc. 1965, 112, 865. (36) Gewirth, A. A.; Thorum, M. S. Inorg. Chem. 2010, 49, 3557. (37) Basame, S. B.; White, H. S. Anal. Chem. 1999, 71, 3166.
URI:	http://wrap.warwick.ac.uk/id/eprint/38596