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UNIVERSITY OF MILAN – CATHOLIC UNIVERSITY OF BRESCIA. Sub- ppm ammonia detection in urban environments with carbon nanotubes gas sensors: possible strategies to enhance the sensitivity. Rigoni Federica 1° year Phd student [email protected] Carbon nanotubes.

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Rigoni federica 1 year phd student federicarigoni gmail

UNIVERSITY OF MILAN – CATHOLIC UNIVERSITY OF BRESCIA

Sub-ppm ammonia detection in urban environments with carbon nanotubes gas sensors:possible strategies to enhance the sensitivity.

Rigoni Federica

1° yearPhdstudent

[email protected]


Carbon nanotubes

Carbonnanotubes

  • Severalallotropicformofcarbon, depending on itshybridization (diamond, graphite, graphene, fullerene, carbonnanotube …)

  • Manyscientificpapers start citing

    “Carbonnanotubes, discoveredby

    Iijima in 1991 …”

  • Iijimaproduced a newallotropicform

    ofcarbon (thathecalledmicrotubules

    ofgraphiticcarbon), usinganarc-discharge

    evaporationmethodsimilartothat

    usedfor fullerene (C60) synthesis.

Tetrahedral (3D)

Trigonal (2D)

Linear (1D)

sp3

sp2

sp

d = 3 nm

S. Iijima, Nature354 (1991) 56


What are carbon nanotubes

What are carbonnanotubes?

Roll-up

GRAPHENE SHEET

CARBON NANOTUBE

C hybridization sp2


Rigoni federica 1 year phd student federicarigoni gmail

Single-wallcarbonnanotubeSWNTdiameter 1-3 nm

Multi-wallcarbonnanotube MWNT diameter up to 100 nm

diameter ≈ nm

length ≈ µm

1D crystal

Chiralindexes (n,m)

(17,0)

zig-zag

(10,10)

armchair

(12,8)

chiral

Different chiralities: different characteristics

Ifn-m = multiple of 3

metallic tube

otherwise

semiconductive tube


Electronic properties of swnt

Electronic propertiesof SWNT

Single wallcarbonnanotubehasdiameter ≈ nm and length ≈ µm,

We can consideritas a one-dimensionalcrystal.

Density OfStates in a 1D crystal

Van Hovesingularities

KATAURA PLOT

The KATAURA PLOT relatesthe energy of the band gaps in a carbon nanotube and its diameter (in the first-order tight binding approximation).

Katauraetal.SyntheticMetals103 (1999) 2555


Carbon nanotubes as gas sensors

Carbonnanotubesas gas sensors

  • CNTs are appealing systems for extremely sensitive gas sensors for at least two reasons:

  • their one-dimensional nature makes them very sensitive to tiny external perturbations

  • huge surface-to-volume ratio

NO2: OXIDIZING MOLECULE

BASIC IDEA:

The interactionresulting in a charge transfer between the gas molecule and the carbonnanotubecauses a variation in the electrical conductance (or resistance) of the tube, detectable with an electronic system.

NH3: REDUCING MOLECULE

Kong et al. Science, 287 (2000) 622


Why monitoring ammonia gas

Whymonitoringammonia gas?

ppm (parts per million)

Hazardoussubstances, explosive, …

Environmentalmonitoring

ppb (parts per billion)

NH3

In urbanenvironment:

lessthan 50 ppb

NH3isoneof the mainprecursorsofsecondary fine particulate (PM10, PM2.5)

Our goal: toenhance the sensitivityofcarbonnanotubesbased gas sensors in ordertodetectsub-ppmconcentrationsof NH3.

Ammoniaconcentrationsoverone week

in Milan (data source: ARPA Lombardia)


Chemiresistor gas sensor

Chemiresistor gas sensor

SWNT dispersed in a solutionof water, NaOH, SodiumLaurylSulfate

InterdigitatedPtelectrodes

Electricalcircuit

SWNT bridgesbetweenelectrodes

Alumina (ceramic)substrate

Methodsofpreparation

Drop-casting

method

Dielectrophoresis

method

1 μl

1 μl

Alternate Currentappliedduring the deposition

(V = 5 V ; f = 1 MHz)


Strategies to enhance the sensitivity of a swnt based chemiresistor

Strategiestoenhance the sensitivityof a SWNT basedchemiresistor

  • Sonicationof the sample (in ultrasound bath) to reduce the film thickness

    thinner the film on the substrate, betteris the charge transfer from the gas moleculeto the electricalcontacts.

  • Dielectrophoresismethodtoalign the SWNT

    a methodtobetterdistribute the SWNT on the substrateistoapplyan alternate currentbetween the electrodes, during the deposition. In this way SWNTstendstobealigned

  • Functionalization

  • Otherarchitectures

    (e.g. chem-FET)

Moscatello et al. MRS, 1057 (2008)


Response variation of the resistance

Response: variationof the resistance

SENSITIVITY:

sub-

ppm


Dielectrophoresis method to align the cnt

Dielectrophoresismethodtoalign the CNT

Drop-castingmethod

Dielectrophoresismethod

1 μl

1 μl

SEM

images


Rigoni federica 1 year phd student federicarigoni gmail

(a) ,(b) SWNT on ceramic ID substrate


In literature

In literature…

There are manyworkson carbonnanotubesasammonia gas sensors, butveryfewofthemreport the detection ofconcentrationsbelow the ppm level.

FunctionalizationwithPolyaniline

(PANI, a conductivepolymer)

Functionalizationwith metal nanoparticles

High temperature

Penzaet al. Sens. And Act. B, 135(2008) 289

Zhanget al. Electroanalysis, 18 (2006) 1153


Future steps

Future steps

  • Functionalization

  • Differentdeviceconcepts, e.g. chemicalFieldEffect Transistor (chem-FET)

CNTs

Drain

Source

S

D

SiO2

The gateallowstochange the voltage (gatevoltageVg).

GATE: p-doped Si


Chemical field effect transistor fet

ChemicalFieldEffect Transistor (FET)

Vgate = 0

Vgate > 0

more electrons

Vgate < 0

more holes

K. Uchida et al., Phys. Rev. B 79, 85402 (2009)


Thanks for the attention questions

Thanksfor the attention!QUESTIONS?


Chemical field effect transistor fet1

ChemicalFieldEffect Transistor (FET)


Chemical field effect transistor fet2

ChemicalFieldEffect Transistor (FET)

SWNTs

S

D

GATE: p-doped Si

Vgate < 0

Vgate = 0

Vgate> 0


Experimental set up

Experimental set-up

Commercial sensor

Based on metal oxides

Temperature sensor

Chem FET

Chemiresistor:

SWNT on interdigitatedelectrodes

Humiditysensor


Electrical circuit

Electricalcircuit

  • Chemiresistor

  • Chem-FET


Raman

Raman


Raman spectrum of swnt

Ramanspectrumof SWNT

Ramanspectrumgivesusmany information about the vibrationalmodesofcarbonnanotubes.

  • Principalpeaks:

  • RBM: RadialBreathing Mode

  • (150 - 350 cm¯¹)

  • D-band: Disorderinduced band

  • (1350 cm¯¹)

  • G-band: tangential (derived from the graphite like in-plane) mode

  • (1560 – 1600 cm¯¹)

  • G’-band: overtoneofD-band

G-band

Intensity

RBM

G’-band

D-band

Ramanshift (cm¯¹)

R. Graupner J. RamanSpectrosc. 38, 673 (2007)


Metallic vs semiconductive swnts

Metallic vs SemiconductiveSWNTs

RamanspectraofSWNTs in bundlesusing different excitation energy (2.54, 2.41 and 1.92 eV).

The metallic or semiconductingcharacter of the tubes is definitely confirmed by the line-shapeof the TM (G-band).

Lorentianprofile

RBM

G-band

semicond.

Lorentianprofile

semicond.

S

M

Breit-Wigner-Fano

profile

S

metallic

S

L. Alvarez et al.Chem. Phys. Lett. 316, 186 (2000)


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