Ultrasensitive detection of toxic cations through changes in the tunnelling current across films of striped nanoparticles

Eun Seon Cho; Jiwon Kim; Baudilio Tejerina; Thomas M. Hermans; Hao Jiang; Hideyuki Nakanishi; Miao Yu; Alexander Z. Patashinski; Sharon C. Glotzer; Francesco Stellacci; Bartosz A. Grzybowski

doi:10.1038/nmat3406

Ultrasensitive detection of toxic cations through changes in the tunnelling current across films of striped nanoparticles

Eun Seon Cho, Jiwon Kim, Baudilio Tejerina, Thomas M. Hermans, Hao Jiang, Hideyuki Nakanishi, Miao Yu, Alexander Z. Patashinski, Sharon C. Glotzer, Francesco Stellacci, Bartosz A. Grzybowski

Integrated Sciences and Engineering Division

Research output: Contribution to journal › Article › peer-review

155 Citations (Scopus)

Abstract

Although multiple methods have been developed to detect metal cations, only a few offer sensitivities below 1â €‰pM, and many require complicated procedures and sophisticated equipment. Here, we describe a class of simple solid-state sensors for the ultrasensitive detection of heavy-metal cations (notably, an unprecedented attomolar limit for the detection of CH 3 Hg + in both standardized solutions and environmental samples) through changes in the tunnelling current across films of nanoparticles (NPs) protected with striped monolayers of organic ligands. The sensors are also highly selective because of the ligand-shell organization of the NPs. On binding of metal cations, the electronic structure of the molecular bridges between proximal NPs changes, the tunnelling current increases and highly conductive paths ultimately percolate the entire film. The nanoscale heterogeneity of the structure of the film broadens the range of the cation-binding constants, which leads to wide sensitivity ranges (remarkably, over 18 orders of magnitude in CH 3 Hg + concentration).

Original language	English
Pages (from-to)	978-985
Number of pages	8
Journal	Nature materials
Volume	11
Issue number	11
DOIs	https://doi.org/10.1038/nmat3406
Publication status	Published - 2012 Nov

Bibliographical note

Funding Information:
This work was supported by the Non-equilibrium Energy Research Center, which is an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under grant number DE-SC0000989. E.S.C. and F.S. acknowledge the support of ENI within the MIT Energy initiative for their work. E.S.C. is supported by a Samsung Scholarship from the Samsung Foundation of Culture. H.J., S.C.G. and F.S. acknowledge support from the Defense Threat Reduction Agency under Grant No. HDTRA1-09-1-0012. T.M.H. is financially supported by the Human Frontier Science Program. We acknowledge L. Meda for her X-ray photoelectron spectroscopy measurements, and R. Borrelli and P. Cesti for helpful discussions. We also thank the USGS for providing fish samples and for helpful discussions.

All Science Journal Classification (ASJC) codes

Chemistry(all)
Materials Science(all)
Condensed Matter Physics
Mechanics of Materials
Mechanical Engineering

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10.1038/nmat3406

Cite this

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title = "Ultrasensitive detection of toxic cations through changes in the tunnelling current across films of striped nanoparticles",

abstract = "Although multiple methods have been developed to detect metal cations, only a few offer sensitivities below 1{\^a} €‰pM, and many require complicated procedures and sophisticated equipment. Here, we describe a class of simple solid-state sensors for the ultrasensitive detection of heavy-metal cations (notably, an unprecedented attomolar limit for the detection of CH 3 Hg + in both standardized solutions and environmental samples) through changes in the tunnelling current across films of nanoparticles (NPs) protected with striped monolayers of organic ligands. The sensors are also highly selective because of the ligand-shell organization of the NPs. On binding of metal cations, the electronic structure of the molecular bridges between proximal NPs changes, the tunnelling current increases and highly conductive paths ultimately percolate the entire film. The nanoscale heterogeneity of the structure of the film broadens the range of the cation-binding constants, which leads to wide sensitivity ranges (remarkably, over 18 orders of magnitude in CH 3 Hg + concentration).",

author = "Cho, {Eun Seon} and Jiwon Kim and Baudilio Tejerina and Hermans, {Thomas M.} and Hao Jiang and Hideyuki Nakanishi and Miao Yu and Patashinski, {Alexander Z.} and Glotzer, {Sharon C.} and Francesco Stellacci and Grzybowski, {Bartosz A.}",

note = "Funding Information: This work was supported by the Non-equilibrium Energy Research Center, which is an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under grant number DE-SC0000989. E.S.C. and F.S. acknowledge the support of ENI within the MIT Energy initiative for their work. E.S.C. is supported by a Samsung Scholarship from the Samsung Foundation of Culture. H.J., S.C.G. and F.S. acknowledge support from the Defense Threat Reduction Agency under Grant No. HDTRA1-09-1-0012. T.M.H. is financially supported by the Human Frontier Science Program. We acknowledge L. Meda for her X-ray photoelectron spectroscopy measurements, and R. Borrelli and P. Cesti for helpful discussions. We also thank the USGS for providing fish samples and for helpful discussions.",

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AU - Grzybowski, Bartosz A.

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Ultrasensitive detection of toxic cations through changes in the tunnelling current across films of striped nanoparticles

Abstract

Bibliographical note

All Science Journal Classification (ASJC) codes

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