Structural determination of Enzyme-Graphene Nanocomposite Sensor Material

Durgesh K. Rai; Manickam Gurusaran; Volker Urban; Kiana Aran; Lulu Ma; Pingzuo Li; Shuo Qian; Tharangattu N. Narayanan; Pulickel M. Ajayan; Dorian Liepmann; Kanagaraj Sekar; María Efigenia Álvarez-Cao; Juan José Escuder-Rodríguez; María Esperanza Cerdán; María Isabel González-Siso; Sowmya Viswanathan; Ramasamy Paulmurugan; Venkatesan Renugopalakrishnan

doi:10.1038/s41598-019-51882-7

Structural determination of Enzyme-Graphene Nanocomposite Sensor Material

Durgesh K. Rai, Manickam Gurusaran, Volker Urban, Kiana Aran, Lulu Ma, Pingzuo Li, Shuo Qian, Tharangattu N. Narayanan, Pulickel M. Ajayan, Dorian Liepmann, Kanagaraj Sekar, María Efigenia Álvarez-Cao, Juan José Escuder-Rodríguez, María Esperanza Cerdán, María Isabel González-Siso, Sowmya Viswanathan, Ramasamy Paulmurugan, Venkatesan Renugopalakrishnan

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3 Scopus citations

Abstract

State-of-the-art ultra-sensitive blood glucose-monitoring biosensors, based on glucose oxidase (GOx) covalently linked to a single layer graphene (SLG), will be a valuable next generation diagnostic tool for personal glycemic level management. We report here our observations of sensor matrix structure obtained using a multi-physics approach towards analysis of small-angle neutron scattering (SANS) on graphene-based biosensor functionalized with GOx under different pH conditions for various hierarchical GOx assemblies within SLG. We developed a methodology to separately extract the average shape of GOx molecules within the hierarchical assemblies. The modeling is able to resolve differences in the average GOx dimer structure and shows that treatment under different pH conditions lead to differences within the GOx at the dimer contact region with SLG. The coupling of different analysis methods and modeling approaches we developed in this study provides a universal approach to obtain detailed structural quantifications, for establishing robust structure-property relationships. This is an essential step to obtain an insight into the structure and function of the GOx-SLG interface for optimizing sensor performance.

Original language	English
Article number	15519
Journal	Scientific Reports
Volume	9
Issue number	1
DOIs	https://doi.org/10.1038/s41598-019-51882-7
State	Published - Dec 1 2019

Funding

This work was supported by the Laboratory Directed Research and Development program of Oak Ridge National Laboratory. Utilization of the Bio-SANS instrument of the Oak Ridge National Laboratory Center for Structural Molecular Biology (FWP ERKP291) is supported by the Office of Biological and Environmental Research of the US Department of Energy. Research at the High Flux Isotope Reactor and at the Spallation Neutron Source of Oak Ridge National Laboratory was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. VR and SV acknowledge the Rothschild Foundation, NIH, NSF, USAFOSR, and the Wallace H. Coulter Foundation for early support of research at Florida International University. Grupo EXPRELA was supported by Xunta de Galicia (Consolidación D.O.G. 10-10-2012. Contract no. 2012/118) cofinanced by FEDER. VR would like to dedicate this work to Varun. DKR would like to thank Leighton Coats, Venu Gopal Vandavasi and Sai Venkatesh Pingali for helpful discussions.VR would like to dedicate this work to Varun and acknowledge inspiration by Suraj.

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Rai, D. K., Gurusaran, M., Urban, V., Aran, K., Ma, L., Li, P., Qian, S., Narayanan, T. N., Ajayan, P. M., Liepmann, D., Sekar, K., Álvarez-Cao, M. E., Escuder-Rodríguez, J. J., Cerdán, M. E., González-Siso, M. I., Viswanathan, S., Paulmurugan, R., & Renugopalakrishnan, V. (2019). Structural determination of Enzyme-Graphene Nanocomposite Sensor Material. Scientific Reports, 9(1), Article 15519. https://doi.org/10.1038/s41598-019-51882-7

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abstract = "State-of-the-art ultra-sensitive blood glucose-monitoring biosensors, based on glucose oxidase (GOx) covalently linked to a single layer graphene (SLG), will be a valuable next generation diagnostic tool for personal glycemic level management. We report here our observations of sensor matrix structure obtained using a multi-physics approach towards analysis of small-angle neutron scattering (SANS) on graphene-based biosensor functionalized with GOx under different pH conditions for various hierarchical GOx assemblies within SLG. We developed a methodology to separately extract the average shape of GOx molecules within the hierarchical assemblies. The modeling is able to resolve differences in the average GOx dimer structure and shows that treatment under different pH conditions lead to differences within the GOx at the dimer contact region with SLG. The coupling of different analysis methods and modeling approaches we developed in this study provides a universal approach to obtain detailed structural quantifications, for establishing robust structure-property relationships. This is an essential step to obtain an insight into the structure and function of the GOx-SLG interface for optimizing sensor performance.",

author = "Rai, {Durgesh K.} and Manickam Gurusaran and Volker Urban and Kiana Aran and Lulu Ma and Pingzuo Li and Shuo Qian and Narayanan, {Tharangattu N.} and Ajayan, {Pulickel M.} and Dorian Liepmann and Kanagaraj Sekar and {\'A}lvarez-Cao, {Mar{\'i}a Efigenia} and Escuder-Rodr{\'i}guez, {Juan Jos{\'e}} and Cerd{\'a}n, {Mar{\'i}a Esperanza} and Gonz{\'a}lez-Siso, {Mar{\'i}a Isabel} and Sowmya Viswanathan and Ramasamy Paulmurugan and Venkatesan Renugopalakrishnan",

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Rai, DK, Gurusaran, M, Urban, V, Aran, K, Ma, L, Li, P, Qian, S, Narayanan, TN, Ajayan, PM, Liepmann, D, Sekar, K, Álvarez-Cao, ME, Escuder-Rodríguez, JJ, Cerdán, ME, González-Siso, MI, Viswanathan, S, Paulmurugan, R & Renugopalakrishnan, V 2019, 'Structural determination of Enzyme-Graphene Nanocomposite Sensor Material', Scientific Reports, vol. 9, no. 1, 15519. https://doi.org/10.1038/s41598-019-51882-7

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AU - Rai, Durgesh K.

AU - Gurusaran, Manickam

AU - Urban, Volker

AU - Aran, Kiana

AU - Ma, Lulu

AU - Li, Pingzuo

AU - Qian, Shuo

AU - Narayanan, Tharangattu N.

AU - Ajayan, Pulickel M.

AU - Liepmann, Dorian

AU - Sekar, Kanagaraj

AU - Álvarez-Cao, María Efigenia

AU - Escuder-Rodríguez, Juan José

AU - Cerdán, María Esperanza

AU - González-Siso, María Isabel

AU - Viswanathan, Sowmya

AU - Paulmurugan, Ramasamy

AU - Renugopalakrishnan, Venkatesan

PY - 2019/12/1

Y1 - 2019/12/1

N2 - State-of-the-art ultra-sensitive blood glucose-monitoring biosensors, based on glucose oxidase (GOx) covalently linked to a single layer graphene (SLG), will be a valuable next generation diagnostic tool for personal glycemic level management. We report here our observations of sensor matrix structure obtained using a multi-physics approach towards analysis of small-angle neutron scattering (SANS) on graphene-based biosensor functionalized with GOx under different pH conditions for various hierarchical GOx assemblies within SLG. We developed a methodology to separately extract the average shape of GOx molecules within the hierarchical assemblies. The modeling is able to resolve differences in the average GOx dimer structure and shows that treatment under different pH conditions lead to differences within the GOx at the dimer contact region with SLG. The coupling of different analysis methods and modeling approaches we developed in this study provides a universal approach to obtain detailed structural quantifications, for establishing robust structure-property relationships. This is an essential step to obtain an insight into the structure and function of the GOx-SLG interface for optimizing sensor performance.

AB - State-of-the-art ultra-sensitive blood glucose-monitoring biosensors, based on glucose oxidase (GOx) covalently linked to a single layer graphene (SLG), will be a valuable next generation diagnostic tool for personal glycemic level management. We report here our observations of sensor matrix structure obtained using a multi-physics approach towards analysis of small-angle neutron scattering (SANS) on graphene-based biosensor functionalized with GOx under different pH conditions for various hierarchical GOx assemblies within SLG. We developed a methodology to separately extract the average shape of GOx molecules within the hierarchical assemblies. The modeling is able to resolve differences in the average GOx dimer structure and shows that treatment under different pH conditions lead to differences within the GOx at the dimer contact region with SLG. The coupling of different analysis methods and modeling approaches we developed in this study provides a universal approach to obtain detailed structural quantifications, for establishing robust structure-property relationships. This is an essential step to obtain an insight into the structure and function of the GOx-SLG interface for optimizing sensor performance.

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VL - 9

JO - Scientific Reports

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ER -

Structural determination of Enzyme-Graphene Nanocomposite Sensor Material

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