TY - JOUR
T1 - Aerosol-Jet-Printed Graphene Immunosensor for Label-Free Cytokine Monitoring in Serum
AU - Parate, Kshama
AU - Rangnekar, Sonal V.
AU - Jing, Dapeng
AU - Mendivelso-Perez, Deyny L.
AU - Ding, Shaowei
AU - Secor, Ethan B.
AU - Smith, Emily A.
AU - Hostetter, Jesse M.
AU - Hersam, Mark C.
AU - Claussen, Jonathan C.
N1 - Funding Information:
J.C.C. gratefully acknowledges funding support for this work from the National Science Foundation under award number CBET-1706994 and ECCS-1841649 as well as from the U.S. Department of Agriculture, under award number 2016-67021-25038. J.M.H. acknowledges funding support from the Iowa Veterinary Medical Association and Iowa Livestock Health Advisory Council. E.B.S. was supported by the Air Force Research Laboratory under agreement number FA8650-15-2-5518. S.V.R. was supported by the U.S. Department of Commerce, National Institute of Standards and Technology (Award 70NANB19H005) as part of the Center for Hierarchical Materials Design (CHiMaD). This work made use of the EPIC Facility of Northwestern University’s NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the MRSEC program (NSF DMR-1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN. The U.S. Government is authorized to reproduce and distribute reprints for Governmental purposes notwithstanding any copyright notation thereon. The views and conclusions contained herein are those of the authors and should not be interpreted as necessarily representing the official policies or endorsements, either expressed or implied, of the sponsors.
PY - 2020/2/19
Y1 - 2020/2/19
N2 - Graphene-based inks are becoming increasingly attractive for printing low-cost and flexible electrical circuits due to their high electrical conductivity, biocompatibility, and manufacturing scalability. Conventional graphene printing techniques, such as screen and inkjet printing, are limited by stringent ink viscosity requirements properties and large as-printed line width that impedes the performance of printed biosensors. Here, we report an aerosol-jet-printed (AJP) graphene-based immunosensor capable of monitoring two distinct cytokines: interferon gamma (IFN-γ) and interleukin 10 (IL-10). Interdigitated electrodes (IDEs) with 40 μm finger widths were printed from graphene-nitrocellulose ink on a polyimide substrate. The IDEs were annealed in CO2 to introduce reactive oxygen species on the graphene surface that act as chemical handles to covalently link IFN-γand IL-10 antibodies to the graphene surfaces. The resultant AJP electrochemical immunosensors are capable of monitoring cytokines in serum with wide sensing range (IFN-γ: 0.1-5 ng/mL; IL-10: 0.1-2 ng/mL), low detection limit (IFN-γ: 25 pg/ml and IL-10: 46 pg/ml) and high selectivity (antibodies exhibited minimal cross-reactivity with each other and IL-6) without the need for sample prelabeling or preconcentration. Moreover, these biosensors are mechanically flexible with minimal change in signal output after 250 bending cycles over a high curvature (φ = 5 mm). Hence, this technology could be applied to numerous electrochemical applications that require low-cost electroactive circuits that are disposable and/or flexible.
AB - Graphene-based inks are becoming increasingly attractive for printing low-cost and flexible electrical circuits due to their high electrical conductivity, biocompatibility, and manufacturing scalability. Conventional graphene printing techniques, such as screen and inkjet printing, are limited by stringent ink viscosity requirements properties and large as-printed line width that impedes the performance of printed biosensors. Here, we report an aerosol-jet-printed (AJP) graphene-based immunosensor capable of monitoring two distinct cytokines: interferon gamma (IFN-γ) and interleukin 10 (IL-10). Interdigitated electrodes (IDEs) with 40 μm finger widths were printed from graphene-nitrocellulose ink on a polyimide substrate. The IDEs were annealed in CO2 to introduce reactive oxygen species on the graphene surface that act as chemical handles to covalently link IFN-γand IL-10 antibodies to the graphene surfaces. The resultant AJP electrochemical immunosensors are capable of monitoring cytokines in serum with wide sensing range (IFN-γ: 0.1-5 ng/mL; IL-10: 0.1-2 ng/mL), low detection limit (IFN-γ: 25 pg/ml and IL-10: 46 pg/ml) and high selectivity (antibodies exhibited minimal cross-reactivity with each other and IL-6) without the need for sample prelabeling or preconcentration. Moreover, these biosensors are mechanically flexible with minimal change in signal output after 250 bending cycles over a high curvature (φ = 5 mm). Hence, this technology could be applied to numerous electrochemical applications that require low-cost electroactive circuits that are disposable and/or flexible.
KW - aerosol jet printing
KW - cytokines
KW - electrochemical biosensor
KW - graphene
KW - interdigitated electrode
KW - printed electronics
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U2 - 10.1021/acsami.9b22183
DO - 10.1021/acsami.9b22183
M3 - Article
C2 - 32040290
AN - SCOPUS:85080841694
VL - 12
SP - 8592
EP - 8603
JO - ACS applied materials & interfaces
JF - ACS applied materials & interfaces
SN - 1944-8244
IS - 7
ER -