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Interfacing nanomaterials for bioelectronic applications
Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The integration of nanomaterials between biological and electronic world has revolutionized the way of understanding how to generate functional bioelectronic device and open a new horizon for the future of bioelectronics. The use of nanomaterials as a versatile interface in the area of bioelectronics offers many practical solutions and recently outshines as an alternative method to overcome technical challenges to control and regulate the mean of communication between biological and electronics systems. Therefore, the interfacing nanomaterials yields broad platform of functional units for the integration as bioelectronic interfaces and starts to have a great importance to many fields within the life science.

In parallel with the advancements for the successful combination of biological and electronic worlds using nanotechnology in a conventional way, a new branch of switchable bioelectronics based on signal-responsive materials and related interfaces have been emerged. The switchable bioelectronics consists of functional interfaces equipped with molecular cue that able to mimic and adapt their natural environment and change physical and chemical properties on demand. These switchable interfaces are essential to develop a range of technologies to understand function and properties of biological systems such as bio-catalysis, control of ion transfer and molecular recognition used in bioelectronics systems.

This thesis focuses on both the integration of functional nanomaterials to improve electrical interfacing between biological system and electronics and also the generation of a dynamic interface having ability to respond real-life physical and chemical changes. The developing of such a dynamic interface allows one to understand how do living system probe and respond their changing environment and also help control and modulate bio-molecular interactions in a confined space using external physical and chemical stimuli. First, the integration of various nanomaterials is described to understand the effect of different surface modifications and morphologies using different materials on the basis of enzyme-based electrochemical sensing of biological analytes. Then, various switchable interfaces including temperature, light and pH, consist of graphene-enzyme and responsive polymer, are developed to control and regulate enzymebased biomolecular reactions. Finally, physically controlled programmable bio-interface which is described by “AND” and “OR” Boolean logic operations using two different stimuli on one electrode, is introduced. Together, the findings presented in this thesis lay the groundwork for the establishment switchable and programmable bioelectronics. The both approaches are promising candidates to provide key building blocks for future practical systems, as well as model systems for fundamental research.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2015. , 76 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1684
National Category
Biochemistry and Molecular Biology Biochemistry and Molecular Biology
Identifiers
URN: urn:nbn:se:liu:diva-120990DOI: 10.3384/diss.diva-120990ISBN: 978-91-7519-028-0 (print)OAI: oai:DiVA.org:liu-120990DiVA: diva2:850438
Public defence
2015-09-07, Planck, Fysikhuset, Campus Valla, Linköping, 13:15 (English)
Opponent
Supervisors
Available from: 2015-09-01 Created: 2015-09-01 Last updated: 2016-06-07Bibliographically approved
List of papers
1. Template-Directed Hierarchical Self-Assembly of Graphene Based Hybrid Structure for Electrochemical Biosensing
Open this publication in new window or tab >>Template-Directed Hierarchical Self-Assembly of Graphene Based Hybrid Structure for Electrochemical Biosensing
2013 (English)In: Biosensors & bioelectronics, ISSN 0956-5663, E-ISSN 1873-4235, Vol. 49, 53-62 p.Article in journal (Refereed) Published
Abstract [en]

A template-directed self-assembly approach, using functionalised graphene as a fundamental building block to obtain a hierarchically ordered graphene-enzyme-nanoparticle bioelectrode for electrochemical biosensing, is reported. An anionic surfactant was used to prepare a responsive, functional interface and direct the assembly on the surface of the graphene template. The surfactant molecules altered the electrostatic charges of graphene, thereby providing a convenient template-directed assembly approach to a free-standing planar sheet of sp(2) carbons. Cholesterol oxidase and cholesterol esterase were assembled on the surface of graphene by intermolecular attractive forces while gold nanoparticles are incorporated into the hetero-assembly to enhance the electro-bio-catalytic activity. Hydrogen peroxide and cholesterol were used as two representative analytes to demonstrate the electrochemical sensing performance of the graphene-based hybrid structure. The bioelectrode exhibited a linear response to H2O2 from 0.01 to 14 mM, with a detection limit of 25 nM (S/N=3). The amperometric response with cholesterol had a linear range from 0.05 to 0.35 mM, sensitivity of 3.14 mu A/mu M/cm(2) and a detection limit of 0.05 mu M. The apparent Michaelis-Menten constant (K-m(app)) was calculated to be 1.22 mM. This promising approach provides a novel methodology for template-directed bio-self-assembly over planar sp(2) carbons of a graphene sheet and furnishes the basis for fabrication of ultra-sensitive and efficient electrochemical biosensors.

Place, publisher, year, edition, pages
Elsevier, 2013
National Category
Medical Laboratory and Measurements Technologies
Identifiers
urn:nbn:se:liu:diva-91866 (URN)10.1016/j.bios.2013.04.004 (DOI)000323396700009 ()
Projects
Hierarchicalself-assembly, Templatedirected hybridnanomaterial, Graphene Nano-biointerface, Biosensor
Funder
Swedish Research Council, VR- 2011-6058357EU, FP7, Seventh Framework Programme, PIIF-GA-2009-254955
Available from: 2013-05-03 Created: 2013-05-03 Last updated: 2017-12-06
2. Two-dimensional gold-tungsten disulphide bio-interface for high-throughput electrocatalytic nano-bioreactors
Open this publication in new window or tab >>Two-dimensional gold-tungsten disulphide bio-interface for high-throughput electrocatalytic nano-bioreactors
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2014 (English)In: Advanced Materials Interfaces, ISSN 2196-7350, Vol. 1, no 6, 1400136- p.Article in journal (Refereed) Published
Abstract [en]

A high-throughput electrocatalytic nano-bioreactor on tungsten disulphide nanosheets is demonstrated for the first time. The fundamental goal of this research is to develop a higher surface area, resulting in a greater enzyme loading and thereby increasing bio-catalytic activity within a nano-confined volume. As a result, the nanobio-system is capable of highly specific recognition of target bioanalytes, therefore, showing significant potentials in a range of bioreactor applications.

Place, publisher, year, edition, pages
Wiley-VCH Verlagsgesellschaft, 2014
Keyword
Nanobioreactor, electrocatalysis, bioelectronics, self-assembly, WS2 nanosheet
National Category
Nano Technology
Identifiers
urn:nbn:se:liu:diva-107975 (URN)10.1002/admi.201400136 (DOI)000348284500012 ()
Projects
Swedish Research Council, VRFP7, European Commission
Funder
Swedish Research Council, VR-2011-6058357EU, FP7, Seventh Framework Programme, PIIF-GA-2009-254955
Available from: 2014-06-24 Created: 2014-06-24 Last updated: 2015-09-01Bibliographically approved
3. Probing electrocatalytic properties of aerographite for the design of flexible bio-electrode
Open this publication in new window or tab >>Probing electrocatalytic properties of aerographite for the design of flexible bio-electrode
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(English)Manuscript (preprint) (Other academic)
Keyword
Aerographite, electrocatalytic bio-electrode, bioelectrocatalysis, density functional theory
National Category
Chemical Sciences
Identifiers
urn:nbn:se:liu:diva-120980 (URN)
Available from: 2015-09-01 Created: 2015-09-01 Last updated: 2015-09-01Bibliographically approved
4. Switchable bioelectronics
Open this publication in new window or tab >>Switchable bioelectronics
2016 (English)In: Biosensors & bioelectronics, ISSN 0956-5663, E-ISSN 1873-4235, Vol. 76, 251-265 p.Article in journal (Refereed) Published
Abstract [en]

We review the rapidly emerging field of switchable interfaces and its implications for bioelectronics. We seek to piece together early breakthroughs and key developments, and highlight and discuss the future of switchable bioelectronics by focusing on bio-electrochemical processes based on mimicking and controlling biological environments with external stimuli. All these studies strive to answer a fundamental question: “how do living systems probe and respond to their surroundings? And, following on from that: “how one can transform these concepts to serve the practical world of bioelectronics?” The central obstacle to this vision is the absence of versatile interfaces that are able to control and regulate the means of communication between biological and electronic systems. Here, we review the overall progress made to date in building such interfaces at the level of individual biomolecules and focus on the latest efforts to generate device platforms that integrate bio-interfaces with electronics.

Place, publisher, year, edition, pages
Elsevier, 2016
Keyword
Switchable bioelectronics, Stimuli-responsive bio-interface, Controllable catalysis
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-120983 (URN)10.1016/j.bios.2015.06.023 (DOI)000364895000020 ()26139319 (PubMedID)
Available from: 2015-09-01 Created: 2015-09-01 Last updated: 2017-12-04Bibliographically approved
5. On/off-switchable zipper-like bioelectronics on a graphene interface.
Open this publication in new window or tab >>On/off-switchable zipper-like bioelectronics on a graphene interface.
2014 (English)In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 26, no 3, 482-486 p.Article in journal (Refereed) Published
Abstract [en]

An on/off-switchable graphene based zipper-like interface is architectured for efficient bioelectrocatalysis. The graphene interface transduces a temperature input signal into structural changes of the membrane, resulting in the amplification of electrochemical signals and their transformation into the gated transport of molecules through the membrane.

Place, publisher, year, edition, pages
Weinheim, Germany: Wiley-VCH Verlagsgesellschaft, 2014
National Category
Chemical Sciences
Identifiers
urn:nbn:se:liu:diva-102942 (URN)10.1002/adma.201303075 (DOI)000334289300015 ()
Projects
VR
Funder
Swedish Research Council
Available from: 2014-01-08 Created: 2014-01-08 Last updated: 2017-12-06Bibliographically approved
6. pH-induced on/off-switchable graphene bioelectronics
Open this publication in new window or tab >>pH-induced on/off-switchable graphene bioelectronics
2015 (English)In: Journal of materials chemistry. B, ISSN 2050-750X, E-ISSN 2050-7518, Vol. 3, no 37, 7434-7439 p.Article in journal (Refereed) Published
Abstract [en]

Switchable interfaces can deliver functionally reversible reactivity with their corresponding analytes, which thus allows one to positively respond the activity of biological elements, including enzymes and other biomolecules, through an encoded stimulus. We have realised this by the design of stimuli-responsive graphene interfaces for pH-encoded operation of bioelectronics. In this study, we have demonstrated stimuli-responsive graphene interfaces for pH-encoded operation of bioelectronics. The resulting switchable interfaces are capable of highly specific, on-demand operation of biosensors, which has significant potential in a wide range of analytical applications.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY, 2015
Keyword
Switchable bioelectronics, smart interfaces, graphene oxide, glucose oxidase
National Category
Chemical Sciences
Identifiers
urn:nbn:se:liu:diva-120986 (URN)10.1039/c5tb01355k (DOI)000361554100014 ()
Note

Funding: Swedish Research Council [VR-2011-6058357]

Available from: 2015-09-01 Created: 2015-09-01 Last updated: 2017-12-04Bibliographically approved
7. Light-triggered on/off-switchable graphene-based bioelectronics
Open this publication in new window or tab >>Light-triggered on/off-switchable graphene-based bioelectronics
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(English)Manuscript (preprint) (Other academic)
Keyword
Self-controlled bio-devices, stimuli-encoded bioelectronics, smart graphene, light-switchable bioelectrocatalysis
National Category
Physical Chemistry Biochemistry and Molecular Biology
Identifiers
urn:nbn:se:liu:diva-120987 (URN)
Available from: 2015-09-01 Created: 2015-09-01 Last updated: 2017-01-11Bibliographically approved
8. Programmable bioelectronics in a stimuli-encoded 3D graphene
Open this publication in new window or tab >>Programmable bioelectronics in a stimuli-encoded 3D graphene
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(English)Manuscript (preprint) (Other academic)
Keyword
Programmable bioelectronics; stimuli-encoded graphene; switchable electrode; smart logic gates
National Category
Physical Chemistry Biochemistry and Molecular Biology
Identifiers
urn:nbn:se:liu:diva-120989 (URN)
Available from: 2015-09-01 Created: 2015-09-01 Last updated: 2015-09-01Bibliographically approved

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