TY - JOUR
T1 - Single-atom doping of MoS2with manganese enables ultrasensitive detection of dopamine
T2 - Experimental and computational approach
AU - Lei, Yu
AU - Butler, Derrick
AU - Lucking, Michael C.
AU - Zhang, Fu
AU - Xia, Tunan
AU - Fujisawa, Kazunori
AU - Granzier-Nakajima, Tomotaroh
AU - Cruz-Silva, Rodolfo
AU - Endo, Morinobu
AU - Terrones, Humberto
AU - Terrones, Mauricio
AU - Ebrahimi, Aida
N1 - Funding Information:
We would like to thank the Materials Research Institute at the Pennsylvania State University and their staff for their assistance with the material characterization. We also acknowledge S. Subramanian for help in the first XPS measurement. Y.L., D.B., M.T., and A.E. would like to acknowledge the NSF:I/UCRC ATOMIC program for support (award #1540018). A.E. also acknowledges the Start-up Fund from the Pennsylvania State University. M.C.L. and H.T. are grateful to the NSF (EFRI-1433311). The supercomputer time was provided by the Center for Computational Innovations (CCI) at Rensselaer Polytechnic Institute and the Extreme Science and Engineering Discovery Environment (XSEDE; project TG-DMR17008), which is supported by NSF grant number ACI-1053575.
Publisher Copyright:
© 2020 The Authors.
PY - 2020/8
Y1 - 2020/8
N2 - Two-dimensional transition metal dichalcogenides (TMDs) emerged as a promising platform to construct sensitive biosensors. We report an ultrasensitive electrochemical dopamine sensor based on manganese-doped MoS2 synthesized via a scalable two-step approach (with Mn ∼2.15 atomic %). Selective dopamine detection is achieved with a detection limit of 50 pM in buffer solution, 5 nM in 10% serum, and 50 nM in artificial sweat. Density functional theory calculations and scanning transmission electron microscopy show that two types of Mn defects are dominant: Mn on top of a Mo atom (MntopMo) and Mn substituting a Mo atom (MnMo). At low dopamine concentrations, physisorption on MnMo dominates. At higher concentrations, dopamine chemisorbs on MntopMo, which is consistent with calculations of the dopamine binding energy (2.91 eV for MntopMo versus 0.65 eV for MnMo). Our results demonstrate that metal-doped layered materials, such as TMDs, constitute an emergent platform to construct ultrasensitive and tunable biosensors.
AB - Two-dimensional transition metal dichalcogenides (TMDs) emerged as a promising platform to construct sensitive biosensors. We report an ultrasensitive electrochemical dopamine sensor based on manganese-doped MoS2 synthesized via a scalable two-step approach (with Mn ∼2.15 atomic %). Selective dopamine detection is achieved with a detection limit of 50 pM in buffer solution, 5 nM in 10% serum, and 50 nM in artificial sweat. Density functional theory calculations and scanning transmission electron microscopy show that two types of Mn defects are dominant: Mn on top of a Mo atom (MntopMo) and Mn substituting a Mo atom (MnMo). At low dopamine concentrations, physisorption on MnMo dominates. At higher concentrations, dopamine chemisorbs on MntopMo, which is consistent with calculations of the dopamine binding energy (2.91 eV for MntopMo versus 0.65 eV for MnMo). Our results demonstrate that metal-doped layered materials, such as TMDs, constitute an emergent platform to construct ultrasensitive and tunable biosensors.
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U2 - 10.1126/sciadv.abc4250
DO - 10.1126/sciadv.abc4250
M3 - Article
C2 - 32821846
AN - SCOPUS:85089811384
SN - 2375-2548
VL - 6
JO - Science Advances
JF - Science Advances
IS - 32
M1 - abc4250
ER -