Composition and Structure of Fluorescent Graphene Quantum Dots Generated by Enzymatic Degradation of Graphene Oxide

He, Xiaoyun; Sorescu, Dan C.; Star, Alexander

doi:10.1021/acs.jpcc.1c01564

Title: Composition and Structure of Fluorescent Graphene Quantum Dots Generated by Enzymatic Degradation of Graphene Oxide

Journal Article · Tue Jun 15 00:00:00 EDT 2021 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.1c01564· OSTI ID:1836782

He, Xiaoyun ^[1]; Sorescu, Dan C. ^[2];

^[1]

Univ. of Pittsburgh, PA (United States)
National Energy Technology Lab. (NETL), Pittsburgh, PA (United States); Univ. of Pittsburgh, PA (United States)

The broad applications of carbon nanomaterials (CNMs) in both materials and life sciences necessitate investigation of their metabolites due to the inevitable contact of CNMs and biological systems. Graphene oxide (GO), along with other types of CNMs, can be enzymatically degraded by myeloperoxidase (MPO), an enzyme released during the innate immune response. However, the enzymatic degradation products are neither well-defined nor well-understood. Some products generated during MPO-catalyzed degradation of GO could emit blue photoluminescence (PL) and were simply dubbed graphene quantum dots (GQDs) without further elucidating their structures. In this work, we use liquid chromatography-mass spectrometry (LC-MS) to isolate and elucidate chemical structures of the MPO-catalyzed degradation products. A general chemical formula screening workflow was developed for the GQDs, which are in the form of polyaromatic hydrocarbons (PAHs), obtained in the degradation products. Structures of the PAHs responsible for the blue PL were further proposed using density functional theory (DFT) calculations. Our results indicated that structures with several conjugated benzene rings are likely to generate the observed PL. This work provides insights into the mechanism of enzymatic degradation and open opportunities for fluorescence imaging of GO in biological systems.

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Research Organization:: National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE)

Grant/Contract Number:: 2003302

OSTI ID:: 1836782

Journal Information:: Journal of Physical Chemistry. C, Vol. 125, Issue 24; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Composition and Structure of Fluorescent Graphene Quantum Dots Generated by Enzymatic Degradation of Graphene Oxide

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