Single-Molecule Fluorescence Imaging of. Nanocatalytic Processes

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1 Single-Molecule Fluorescence Imaging of Nanocatalytic Processes Da Huang Catalyst is a substance that could change the rate of a chemical reaction and it plays important roles in daily lives, such as in the field of chemical synthesis industry, environmental control and energy generation etc. 1 Usually, catalysts are classified into three different types, herterogeneous catalyst, homogenneous catalyst and enzyemes. The nanocatalysts, which is one kind of heterogeneous catalyst, keeps attracting many researchers, such as gold nanoparticles. The increased surface-tovolume ratio and new electronic properties from quantum confinement make them much better compared to their corresponding bulk materials. 1-3 With advanced transmission electron microscopy 4,5, scanning-probe microscopies 6,7, and crystallography, structures of nanoparticles can be studied at the single-particle level down to atomic resolution. What about the catalytic properties? They have mainly been studied at the ensemble level, obtaining their averaged properties. 7,9 While for nanoparticles like gold nanoparticles, their size and structure is variable, which inevitably lead to different properties for individual particles. How different are they? Are the differences significant? In order to address these questions, one needs to study nanoparticle catalysis at the single-particle level. Several research groups have carried out electrochemical measurements on single nanoparticle by detecting electrical current to reveal their catalystic properties While Novo et al. observed redox catalysis by single AuNP by utilizing surface plasmon spectroscopy. 16 However, for fluorescence technique, which has the advantage such as high sensitivity down to even single molecule level compared to those methods as well as those properties such as chemical specificity, real time, tens of nanometer in spatial precision and the ability to be coupled to other techniques, it should play a role in revealing the catalytic properties of those nanocatalysts. 1

2 fig. 1 The catalysis process of Cholesterol Oxidase In 1998, there was a science paper published by Dr. Xie, which studied the enzyme dynamics of cholesterol oxidase by fluorescence technique, which is shown in fig.1. Cholesterol oxidase (COx) catalyzes the oxidation of cholesterol by oxygen. The active site of the enzyme (E) involves a flavin adenine dinucleotide (FAD) cofactor, which is naturally fluorescent in its oxidized form but not in its reduced form. In a full cycle of the catalytic process, The FAD is first reduced by a cholesterol molecule to FADH 2, and is then oxidized by O 2, yielding H 2 O 2. Thus, Enzymatic turnovers of single cholesterol oxidase molecules could be observed in real time by monitoring the emission from flavin adenine dinucleotide (FAD). 17 The dynamic and static disorder of Cholesterol Oxidase could then be determined separately, which is essentially indistinguishable in ensemble measurements. Based on Xie s idea, Chen in Cornell studied the catalytic process of those nanocatalysts, such as catalysis of gold nanoparticles and electrocatalysis by carbon nano tubes. A detailed example on gold nano particles will be shown to illustrate how this method works and what kind of information could be generated. 2

3 fig. 2 The set up for gold nanoparticle catalysis study With the help of the fluoregenic reaction from Resazurin to Resorufin, which could be catalyzed by AuNPs, the monitoring of catalysis processes on single AuNPs could be achieved. The set up is shown in fig.2. And a typical turnover trajectory for a single AuNP could be obtained as in fig fig. 3 The turnover trajectory of a single AuNP With the help of the kinetic model in fig.4, the kinetic parameters, which describe each AuNP catalysis step, could be solved. They help to determine and understand the catalytic properties of AuNPs in it whole catalysis process. After that, it is able to determine the heterogeneity of the catalytic properties among different AuNPs, the heterogeneity of the catalytic properties of one single AuNP during its catalytic process and the heterogeneity of the surface sites of AuNPs. 19 3

4 fig. 4 The theoretical kinetic model of AuNPs catalysis process It is true, as illustrated by the AuNPs study, that the single-molecule fluorescence approach offers rich insights into nanoscale catalysis process and helps to overcome the heterogeneity among different AuNPs. Coupled to the other techniques, such as Surface Plasmon, more information on nanocatalysts could then be obtained. However, this method also has its intrinsic limitation, which requires the fluoregenic reaction and limits its application on certain nanocatalysts. Also, this method gives no information on molecular mechanisms. Reference: 1. Somorjai, G.A.; Contreras, A.M.; Montano, M.; Rioux, R.M. Proc. Natl. Acad. Sci. U. S. A. 2006, 103, Abbet, S.; Heiz, U. Chem. Nanomater. 2004, 2, Gai, P.L.; Roper, R.; White, M. G. Curr. Opin. Solid State Mater. Sci. 2002, 6, Burda, C.; Chen, X.; Narayanan, R.; El-Sayed, M.A. Chem. Rev. 2005, 105, Sun, Y.; Xia, Y. Science 2002, 298, Chen, M.; Goodman, D.W. Acc. Chem. Res. 2006, 39,

5 7. Jaramillo, T.F.; Jorgensen, K.P.; Bonde, J.; Nielson, J.H.; Horch, S.; Chorkendorff, I. Science 2007, 317, Jadzinsky, P.D.; Calero, G. et. al. Science 2007, 318: Haruta, M., Yamada, N., Kobayashi, T.; Iijima, S.J. Catal. 1989, 115, Fan, F.-R.F.; Kwak, J.; Bard, A.J. J. Am. Chem. Soc. 1996, 118, Fan, F.-R.F.; Bard, A.J. Science 1997, 277, Meier, J.; Friedrich, K.A.; Stimming, U. Faraday Discuss. 2002, 121, Meier, J.; Schiotz, J.; Liu, P.; Norskov, J. K.; Stimming, U. Chem. Phys. Lett. 2004, 390, Chen, S. L.; Kucernak, A. J. Phys. Chem. B 2004, 108, Krapf, D.; Wu, M.-Y.; Smeets, R.M.M.; Zandbergen, H.W.; Dekker, C.; Lemay, S.G. Nano Lett. 2006, 6, Novo, C.; Funston, A.M.; Mulvaney, P. Nat. Nanotechnol. 2008, 3, Lu, H.P.; Xun, L.Y.; Xie, X.S. Science 1998, 282, Xu, W.; Kong, J.S.; Yeh, Y.-T.E.; Chen, P. Nat. Mater. 2008, 7, Xu, W.; Kong, J.S. and Chen, P. Phys. Chem. Chem. Phy. 2009, 11,

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