Observation of Oscillatory Surface Reactions of Riboflavin, Trolox, and Singlet Oxygen Using Single Carbon Nanotube Fluorescence Spectroscopy

2012-12-01
Sen, Fatih
Boghossian, Ardemis A.
Sen, Selda
Ulissi, Zachary W.
Zhang, Jingqing
Strano, Michael S.
Single-molecule fluorescent microscopy allows semiconducting single-walled carbon nanotubes (SWCNTs) to detect the adsorption and desorption of single adsorbate molecules as a stochastic modulation of emission intensity. In this study, we identify and assign the signature of the complex decomposition and reaction pathways of riboflavin in the presence of the free radical scavenger Trolox using DNA-wrapped SWCNT sensors dispersed onto an aminopropyltriethoxysilane (APTES) coated surface. SWCNT emission is quenched by riboflavin-induced reactive oxygen species (ROS), but increases upon the adsorption of Trolox, which functions as a reductive brightening agent. Riboflavin has two parallel reaction pathways, a Trolox oxidizer and a photosensitizer for singlet oxygen and superoxide generation. The resulting reaction network can be detected in real time in the vicinity of a single SWCNT and can be completely described using elementary reactions and kinetic rate constants measured independently. The reaction mechanism results in an oscillatory fluorescence response from each SWCNT, allowing for the simultaneous detection of multiple reactants. A series-parallel kinetic model is shown to describe the critical points of these oscillations, with partition coefficients on the order of 10(6) - 10(4) for the reactive oxygen and excited state species. These results highlight the potential for SWCNTs to characterize complex reaction networks at the nanometer scale.
ACS NANO

Suggestions

Observation of long-range, near-side angular correlations in pPb collisions at the LHC
Chatrchyan, S.; et. al. (Elsevier BV, 2013-01-01)
Results on two-particle angular correlations for charged particles emitted in pPb collisions at a nucleon-nucleon center-of-mass energy of 5.02 TeV are presented. The analysis uses two million collisions collected with the CMS detector at the LHC. The correlations are studied over a broad range of pseudorapidity, eta, and full azimuth, phi, as a function of charged particle multiplicity and particle transverse momentum, p(T). In high-multiplicity events, a long-range (2 < vertical bar Delta eta vertical bar...
Preparation and thermal characterization of poly(2-vinylpyridine) copolymers coordinated to Cr nanoparticles
Öztürk, Yurdagül; Kayran, Ceyhan; Hacaloğlu, Jale (2015-06-01)
In this study, polystyrene-block-poly(2-vinylpyridine), PS-b-P2VP, polyisoprene-block-poly(2-vinylpyridne), PI-b-P2VP and poly(methyl metacrylate)-block-poly(2-vinylpyridine), PMMA-b-P2VP, coordinated to Cr metal were synthesized and characterized by Fourier transform infrared, transmission electron microscopy and direct pyrolysis mass spectrometry techniques. Both thermal degradation mechanism and thermal stability of P2VP blocks were affected by the coordination of Cr nanoparticles to nitrogen of pyridine...
Analysis of vibrational spectra in relation to the thermodynamic quantities close to the phase transitions in ammonium halides (NH4F and NH4I)
Tari, O.; Yurtseven, Hasan Hamit (2017-01-01)
The pressure dependences of the vibrational frequencies of the TO and L modes are analyzed from the literature data and the thermodynamic quantities such as isothermal compressibility K gamma, thermal expansion alpha p and the specific heat C-p - C-v are calculated through the mode Grilneisen parameters of those modes in ammonium halides (NH4F and NH4I). For this calculation, the observed frequencies of the TO mode (238 cm(-1) at 1 bar) and the L mode (74.7 meV at 1.9 GPa) are used for the phases of I, II a...
Investigation of glucose electrooxidation mechanism over N-modified metal-doped graphene electrode by density functional theory approach
Duzenli, Derya; Önal, Işık; Tezsevin, Ilker (2022-10-01)
In this work, various precious and non-precious metals reported in the literature as the most effective catalysts for glucose electrooxidation reaction were investigated by the density functional theory (DFT) approach in order to reveal the mechanisms taking place over the catalysts in the fuel cell. The use of a single-atom catalyst model was adopted by insertion of one Au, Cu, Ni, Pd, Pt, and Zn metal atom on the pyridinic N atoms doped graphene surface (NG). beta form of d-glucose in alkaline solution wa...
Development of view factor correlations for modeling thermal radiation in solid particle solar receivers using CFD-DEM
Johnson, Evan; Baker, Derek Keıth; Tarı, İlker (null; 2018-10-05)
Radiation heat transfer must be modeled when designing any high temperature solid particle solar receiver or particle-fluid heat exchanger, but computationally efficient radiation models are not currently available in coupled Computational Fluid Dynamics - Discrete Element Method (CFD-DEM) codes, which is the focus of this work. Monte Carlo ray tracing simulations were run to find view factors between particles in packed beds, and correlations were found to estimate both particle-particle and particle-wall ...
Citation Formats
F. Sen, A. A. Boghossian, S. Sen, Z. W. Ulissi, J. Zhang, and M. S. Strano, “Observation of Oscillatory Surface Reactions of Riboflavin, Trolox, and Singlet Oxygen Using Single Carbon Nanotube Fluorescence Spectroscopy,” ACS NANO, pp. 10632–10645, 2012, Accessed: 00, 2020. [Online]. Available: https://hdl.handle.net/11511/68240.