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Han, Y. (2019). Biosensing platforms using graphene based bioreactive nanostructures with various dimensions. (Doctoral dissertation). Uppsala: Acta Universitatis Upsaliensis
Open this publication in new window or tab >>Biosensing platforms using graphene based bioreactive nanostructures with various dimensions
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Nanomaterials have brought new aspects and improvements to the biosensing field due to their unique physical and chemical properties that are not shown in the bulk state. This thesis focuses on concepting, developing and testing of biosensors where nanomaterials including graphene gold nanoparticles (AuNPs) and magnetic nanoparticles (MNPs) constitute the biosensors. The motivation is to improve the properties of biosensors for protein and nucleic acids by using the nanomaterials’ high surface volume ratio, their unique electrical properties, their good stability and biocompatibility.

The synthesis of well controlled hybrid materials was essential to obtain well performing nucleic acids sensors, whereas a protein sensor contained mainly graphene and organic molecules. The nanomechanical measurements were applied on pyrene-maltose functionalized graphene surfaces after incubating them with the protein. When the Concanavalin A was captured by the pyrene-maltose, the adhesion force of biosensor surface increased significantly. This detection principle was employed to quantify the Concanavalin A attachment to the surface sensitively.

In the development of the eletrocatalytic microRNA sensor, AuNPs were packaged into graphene oxide (GO) sheets to form three-dimensional network structures that both guide the electrical current and increase the surface area of the electrodes. Prior to the assembly of these GO-AuNPs hybrid materials, a duplex-specific nuclease-assisted target recycling reaction was employed for opening the surface of the DNA functionalized AuNPs. The electrocatalytical water splitting activity increased with the fraction of the AuNP surface and thus with the activity of the nuclease-assisted target recycling reaction.

Owing to the high shape anisotropy of graphene, a two-dimensional optomagnetic label GO-MNP nanohybrid was investigated for DNA detection. The DNA coils that were generated through rolling circle amplification absorbed on GO-MNP nanohybrid, leading to a hydrodynamic size increase or aggregation of the proposed nanolabels that can be detected by an optomagnetic sensor. An MNP assembly-based microRNA biosensing strategy is also included in the thesis. DNA scaffolds of the MNP assemblies contain DNAzyme substrate and thus can form cleavage catalytic structures in the presence of microRNA, leading to the disintegration of assemblies. The proposed nanomaterials based biosensing platforms show great potential in the clinical and biomedical applications.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2019. p. 55
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1779
Keywords
Graphene, nanoparticles, nanostructure, biosensors
National Category
Analytical Chemistry Engineering and Technology
Identifiers
urn:nbn:se:uu:diva-378561 (URN)978-91-513-0587-5 (ISBN)
Public defence
2019-04-25, Room 2005, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 13:15 (English)
Opponent
Supervisors
Available from: 2019-04-01 Created: 2019-03-06 Last updated: 2019-05-07
Han, Y., Li, H., Jafri, S. H., Ossipov, D. A., Hilborn, J. & LEIFER, K. (2019). Graphene Based Mechanical Biosensor by Employing Non-covalent Stacking Functionalization.
Open this publication in new window or tab >>Graphene Based Mechanical Biosensor by Employing Non-covalent Stacking Functionalization
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2019 (English)In: Article in journal, News item (Other academic) Submitted
Abstract [en]

Herein we demonstrate a novel methodology to achieve mechanical biosensor by employing the distinguished interaction forces between the atomic force microscope (AFM) probe and sensor surfaces as the response signal. This mechanical biosensor is fabricated by utilizing the non-covalent π-π stacking of pyrene-maltose onto graphene surfaces with Concanavalin A (Con A) as a target protein. The atomic resolution scanning tunneling microscopy (STM) images indicate the successful formation of the self-assembled and densely packed pyrene-maltose layer on the sensor surface, which gives distinct atomic lattice structure as compared to pristine graphene. This mechanical biosensor exhibits detection of Con A with the sensitivity down to nanomolar level. Therefore, this proposed mechanical biosensor has the potential to be employed in a variety of bio-sensing applications.

National Category
Nano Technology Analytical Chemistry
Identifiers
urn:nbn:se:uu:diva-378559 (URN)
Available from: 2019-03-06 Created: 2019-03-06 Last updated: 2020-01-08
Han, Y., Qiu, Z., Nawale, G. N., Varghese, O. P., Hilborn, J., Tian, B. & Leifer, K. (2019). MicroRNA detection based on duplex-specific nuclease-assisted target recycling and gold nanoparticle/graphene oxide nanocomposite-mediated electrocatalytic amplification. Biosensors & bioelectronics, 127, 188-193
Open this publication in new window or tab >>MicroRNA detection based on duplex-specific nuclease-assisted target recycling and gold nanoparticle/graphene oxide nanocomposite-mediated electrocatalytic amplification
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2019 (English)In: Biosensors & bioelectronics, ISSN 0956-5663, E-ISSN 1873-4235, Vol. 127, p. 188-193Article in journal (Refereed) Published
Abstract [en]

DNA technology based bio-responsive nanomaterials have been widely studied as promising tools for biomedical applications. Gold nanoparticles (AuNPs) and graphene oxide (GO) sheets are representative zero- and two-dimensional nanomaterials that have long been combined with DNA technology for point-of-care diagnostics. Herein, a cascade amplification system based on duplex-specific nuclease (DSN)-assisted target recycling and electrocatalytic water-splitting is demonstrated for the detection of microRNA. Target microRNAs can form DNA: RNA heteroduplexes with DNA probes on the surface of AuNPs, which can be hydrolyzed by DSN. MicroRNAs are preserved during the reaction and released into the suspension for the digestion of multiple DNA probes. After the DSN-based reaction, AuNPs are collected and mixed with GO to form AuNP/GO nanocomposite on an electrode for the following electrocatalytic amplification. The utilization of AuNP/GO nanocomposite offers large surface area, exceptional affinity to water molecules, and facilitated mass diffusion for the water-splitting reaction. For let-7b detection, the proposed biosensor achieved a limit detection of 1.5 fM in 80 min with a linear detection range of approximately four orders of magnitude. Moreover, it has the capability of discriminating non-target microRNAs containing even single-nucleotide mismatches, thus holding considerable potential for clinical diagnostics.

Keywords
Gold nanoparticles, Graphene oxide, MicroRNA detection, Electrocatalytic amplification, Duplex-specific nuclease
National Category
Analytical Chemistry Physical Chemistry
Identifiers
urn:nbn:se:uu:diva-377203 (URN)10.1016/j.bios.2018.12.027 (DOI)000457508800026 ()30611105 (PubMedID)
Funder
Swedish Research Council, 2016-05259Knut and Alice Wallenberg FoundationEU, Horizon 2020, 713683
Available from: 2019-02-25 Created: 2019-02-25 Last updated: 2019-04-24Bibliographically approved
Tian, B., Han, Y., Fock, J., Strömberg, M., Leifer, K. & Fougt Hansen, M. (2019). Self-Assembled Magnetic Nanoparticle−Graphene Oxide Nanotag for Optomagnetic Detection of DNA. Acs Applied Nano Materials, 2(3), pp. 1683-1690
Open this publication in new window or tab >>Self-Assembled Magnetic Nanoparticle−Graphene Oxide Nanotag for Optomagnetic Detection of DNA
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2019 (English)In: Acs Applied Nano Materials, ISSN 2574-0970, Vol. 2, no 3, p. 1683-1690Article in journal, News item (Refereed) Published
Abstract [en]

In this work, a two-dimensional self-assembled magnetic nanoparticle–graphene oxide (MNP-GO) nanocomposite is reported for the detection of DNA. Single-stranded DNA (ssDNA) coils, generated through a rolling circle amplification (RCA) reaction triggered by the hybridization of target oligos and padlock probes, have a strong interaction with MNP-GO nanotags through several mechanisms including π–π stacking, hydrogen bonding, van der Waals, electrostatic, and hydrophobic interactions. This interaction leads to a hydrodynamic size increase or aggregation of MNP-GO nanotags, which can be detected by a simple optomagnetic setup. Due to the high shape anisotropy, MNP-GO nanotags provide stronger optomagnetic signal than individual MNPs. Moreover, the avoidance of DNA probes (i.e., short ssDNA sequences as the biosensing receptor) provides easier material preparation and lower measurement cost. From real-time measurements of interactions between MNP-GO and RCA products amplified from a highly conserved Escherichia coli 16S rDNA sequence, a limit of detection of 2 pM was achieved with a total assay time of 90 min. Although the nonspecific binding force between GO and ssDNA is much weaker than the specific base-pairing force in a DNA duplex, the proposed method provides a detection limit similar to DNA probe-based magnetic biosensors, which can be ascribed to the abundant binding sites between GO and ssDNA. In addition, for target concentrations higher than 100 pM, the MNP-GO nanotags can be applied for a qualitative naked eye detection strategy based on nanotag–ssDNA flocculation.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2019
Keywords
Magnetic nanoparticles; graphene oxide; rolling circle amplification; single stranded DNA detection; optomagnetic sensing
National Category
Nano Technology Analytical Chemistry
Research subject
Analytical Chemistry
Identifiers
urn:nbn:se:uu:diva-378551 (URN)10.1021/acsanm.9b00127 (DOI)000462554000061 ()
Available from: 2019-03-06 Created: 2019-03-06 Last updated: 2019-04-24Bibliographically approved
Tian, B., Han, Y., Fock, J., Strömberg, M., Leifer, K. & Fougt Hansen, M. (2019). Self-Assembled Magnetic Nanoparticle−Graphene Oxide Nanotag for Optomagnetic Detection of DNA. Acs Applied Nano Materials, 2(3), 1683-1690
Open this publication in new window or tab >>Self-Assembled Magnetic Nanoparticle−Graphene Oxide Nanotag for Optomagnetic Detection of DNA
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2019 (English)In: Acs Applied Nano Materials, ISSN 2574-0970, Vol. 2, no 3, p. 1683-1690Article in journal (Refereed) Published
Abstract [en]

In this work, a two-dimensional self-assembled magnetic nanoparticle–graphene oxide (MNP-GO) nanocomposite is reported for the detection of DNA. Single-stranded DNA (ssDNA) coils, generated through a rolling circle amplification (RCA) reaction triggered by the hybridization of target oligos and padlock probes, have a strong interaction with MNP-GO nanotags through several mechanisms including π–π stacking, hydrogen bonding, van der Waals, electrostatic, and hydrophobic interactions. This interaction leads to a hydrodynamic size increase or aggregation of MNP-GO nanotags, which can be detected by a simple optomagnetic setup. Due to the high shape anisotropy, MNP-GO nanotags provide stronger optomagnetic signal than individual MNPs. Moreover, the avoidance of DNA probes (i.e., short ssDNA sequences as the biosensing receptor) provides easier material preparation and lower measurement cost. From real-time measurements of interactions between MNP-GO and RCA products amplified from a highly conserved Escherichia coli 16S rDNA sequence, a limit of detection of 2 pM was achieved with a total assay time of 90 min. Although the nonspecific binding force between GO and ssDNA is much weaker than the specific base-pairing force in a DNA duplex, the proposed method provides a detection limit similar to DNA probe-based magnetic biosensors, which can be ascribed to the abundant binding sites between GO and ssDNA. In addition, for target concentrations higher than 100 pM, the MNP-GO nanotags can be applied for a qualitative naked eye detection strategy based on nanotag–ssDNA flocculation.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2019
Keywords
Magnetic nanoparticles; graphene oxide; rolling circle amplification; single stranded DNA detection; optomagnetic sensing
National Category
Nano Technology Analytical Chemistry
Research subject
Analytical Chemistry
Identifiers
urn:nbn:se:uu:diva-378551 (URN)10.1021/acsanm.9b00127 (DOI)000462554000061 ()
Available from: 2019-03-06 Created: 2019-04-24 Last updated: 2019-04-24Bibliographically approved
Li, H., Han, Y., Duan, T. & Leifer, K. (2019). Size-dependent elasticity of gold nanoparticle measured by atomic force microscope based nanoindentation. Applied Physics Letters, 115(5), Article ID 053104.
Open this publication in new window or tab >>Size-dependent elasticity of gold nanoparticle measured by atomic force microscope based nanoindentation
2019 (English)In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 115, no 5, article id 053104Article in journal (Refereed) Published
Abstract [en]

The elasticity is one of the key properties in gold nanoparticles (AuNPs) and plays an essential role in the process design and applications. In this work, we have proposed an Argon plasma based technique to obtain well dispersed and neat AuNPs without surface functional groups. Our investigation on the size-dependent elasticity focused on the AuNPs with the size ranging from 2 nm to 12 nm by using atomic force microscope based nanoindentation technique under the peakforce quantitative nanomechanical mapping mode. The results show clearly that when the AuNPs are smaller than 6 nm, there is a significant increase in the elasticity as the smallest nanoparticles displacing an elastic modulus of ~140 GPa.  Our result provides important experimental evidence that contributes to a better understanding of the size-property relations as well as process design in AuNPs, and it also can be applied to measure the mechanical properties in a wide range of nano-objects.

National Category
Nano Technology
Identifiers
urn:nbn:se:uu:diva-378556 (URN)10.1063/1.5095182 (DOI)000478913700003 ()
Note

Hu Li and Yuanyuan Han contributed equally to this work.

Manuscript version in thesis list of papers did not include Tianbo Duan as author.

Available from: 2019-03-06 Created: 2019-03-06 Last updated: 2019-09-24Bibliographically approved
Yang, J., Han, Y., Luo, J., Liefer, K., Strömme, M. & Welch, K. (2019). Synthesis and Characterization of Amorphous Magnesium Carbonate Nanoparticles. Materials Chemistry and Physics, 224, 301-307
Open this publication in new window or tab >>Synthesis and Characterization of Amorphous Magnesium Carbonate Nanoparticles
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2019 (English)In: Materials Chemistry and Physics, ISSN 0254-0584, E-ISSN 1879-3312, Vol. 224, p. 301-307Article in journal (Refereed) Published
Abstract [en]

We report the template-free, low-temperature, environment-friendly synthesis of amorphous magnesium carbonate nanoparticles (AMN). Scanning electron microscopy and transmission electron microscopy show that AMN consist of small nanoparticles approximately 20-65 nm in diameter. Drying temperature and centrifugation are shown to affect the nanostructure and functional properties of the material. Aggregated AMN can be produced with a total pore volume up to 1.72 cm(3)/g and can absorb as much as 24 mmol/g water, substantially surpassing the pore volume and moisture-absorbing capacity of all previously described alkali earth metal carbonates. The nanoparticles are foreseen to be useful in applications such as water sorption, drug delivery and catalysis.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
Nanoparticle, Amorphous, Magnesium carbonate, Water sorption
National Category
Nano Technology
Identifiers
urn:nbn:se:uu:diva-354505 (URN)10.1016/j.matchemphys.2018.12.037 (DOI)000456750900036 ()
Funder
VINNOVA
Available from: 2018-06-20 Created: 2018-06-20 Last updated: 2019-04-24Bibliographically approved
Tian, B., Han, Y., Wetterskog, E., Donolato, M., Fougt Hansen, M., Svedlindh, P. & Strömberg, M. (2018). MicroRNA Detection through DNAzyme-Mediated Disintegration of Magnetic Nanoparticle Assemblies. ACS Sensors, 3, 1884-1891
Open this publication in new window or tab >>MicroRNA Detection through DNAzyme-Mediated Disintegration of Magnetic Nanoparticle Assemblies
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2018 (English)In: ACS Sensors, ISSN 2379-3694, Vol. 3, p. 1884-1891Article in journal (Refereed) Published
Abstract [en]

DNA-assembled nanoparticle superstructures offer numerous bioresponsive properties that can be utilized for point-of-care diagnostics. Functional DNA sequences such as deoxyribozymes (DNAzymes) provide novel bioresponsive strategies and further extend the application of DNA-assembled nanoparticle superstructures. In this work, we describe a microRNA detection biosensor that combines magnetic nanoparticle (MNP) assemblies with DNAzyme-assisted target recycling. The DNA scaffolds of the MNP assemblies contain substrate sequences for DNAzyme and can form cleavage catalytic structures in the presence of target DNA or RNA sequences, leading to rupture of the scaffolds and disintegration of the MNP assemblies. The target sequences are preserved during the cleavage reaction and release into the suspension to trigger the digestion of multiple DNA scaffolds. The high local concentration of substrate sequences in the MNP assemblies reduces the diffusion time for target recycling. The concentration of released MNPs, which is proportional to the concentration of the target, can be quantified by a 405 nm laser-based optomagnetic sensor. For the detection of let-7b in 10% serum, after 1 h of isothermal reaction at 50 degrees C, we found a linear detection range between 10 pM and 100 nM with a limit of detection of 6 pM. For the quantification of DNA target in buffer solution, a limit of detection of 1.5 pM was achieved. Compared to protein enzyme-based microRNA detection methods, the proposed DNAzyme-based biosensor has an increased stability, a reduced cost and a possibility to be used in living cells, all of which are valuable features for biosensing applications.

National Category
Analytical Chemistry Engineering and Technology
Research subject
Engineering Science with specialization in Solid State Physics
Identifiers
urn:nbn:se:uu:diva-363317 (URN)10.1021/acssensors.8b00850 (DOI)000446276300038 ()30188122 (PubMedID)
Funder
Swedish Research Council Formas, 221-2012-444Swedish Research Council Formas, 2011-1692EU, FP7, Seventh Framework Programme, 604448-NanoMag
Available from: 2018-10-16 Created: 2018-10-16 Last updated: 2019-04-24Bibliographically approved
Qin, T., Zhang, P., Wani, I. H., Han, Y., LEIFER, K., Nikolajeff, F. & Engqvist, H. (2017). A general strategy for template-free and low-cost synthesis of inorganic hollow spheres. Powder Technology, 319, 163-171
Open this publication in new window or tab >>A general strategy for template-free and low-cost synthesis of inorganic hollow spheres
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2017 (English)In: Powder Technology, ISSN 0032-5910, E-ISSN 1873-328X, Vol. 319, p. 163-171Article in journal (Refereed) Published
Abstract [en]

Inorganic hollow spheres have a great potential in many fields, such as calcium phosphate (Ca3(PO4)2) as carriers of active ingredients and local delivery. They are typically synthesized by the methods that reply on template-based strategies. However, the template residue and energy consumption during template removal are drawbacks. Currently developed template-free methods remain challenges such as time, cost and complicated procedures. In this paper, we introduce a general low-cost and template-free precipitation method with simple procedure. A series of inorganic hollow spheres, including calcium phosphate, calcium fluoride, strontium phosphate, strontium fluoride, barium phosphate and barium fluoride via magnesium were successfully synthesized, respectively. Based on these experimental results, a new model is proposed to explain the mechanism of the hollow inorganic spheres formation. This paper provides a general method to synthesize inorganic hollow spheres, which may have an important indication to other systems.

Keywords
Inorganic, Spheres, Hollow, Mechanism
National Category
Materials Engineering
Identifiers
urn:nbn:se:uu:diva-333956 (URN)10.1016/j.powtec.2017.06.051 (DOI)000407982600016 ()
Available from: 2017-12-13 Created: 2017-12-13 Last updated: 2019-04-24Bibliographically approved
Qin, T., Han, Y. & Zhang, P. (2017). A novel method to synthesize low-cost phosphate-based particles from natural water. Materials letters (General ed.), 206, 178-181
Open this publication in new window or tab >>A novel method to synthesize low-cost phosphate-based particles from natural water
2017 (English)In: Materials letters (General ed.), ISSN 0167-577X, E-ISSN 1873-4979, Vol. 206, p. 178-181Article in journal (Refereed) Published
Abstract [en]

Calcium phosphate (CaP) and magnesium phosphate (MgP) are widely used as biomaterials. A novel method for low-cost manufacturing of calcium phosphate spheres and magnesium phosphate micro particles was studied. The method focuses on novel strategies of utilizing seawater and lake water. In the natural water, the molar ratios of Mg/Ca are constant. The morphologies of the particles are determined by ratio of Ca/P. This simple method provides a prototype to synthesize low-cost inorganic spheres with natural water, which facilitate large-scale production.

Keywords
Phosphate-based, Spheres, Seawater, Lake water
National Category
Materials Engineering
Identifiers
urn:nbn:se:uu:diva-333736 (URN)10.1016/j.matlet.2017.07.017 (DOI)000407407300046 ()
Available from: 2017-11-20 Created: 2017-11-20 Last updated: 2019-04-24Bibliographically approved
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0001-7591-2969

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