microparticles and electroconductive … · 932 i. bica, m. balasoiu, m. bunoiu, l. iordaconiu 7...

MICROPARTICLES AND ELECTROCONDUCTIVE

MAGNETORHEOLOGICAL SUSPENSIONS

I. BICA1, M. BALASOIU2,3, M. BUNOIU1, L. IORDACONIU1

1West University of Timişoara, Faculty of Physics, Bd. V. Pârvan, No. 4, 300223 Timişoara, România

Email: [email protected]; [email protected]; [email protected] 2National Institute for Nuclear Physics and Engineering, P.O. Box MG-6, RO-077125 Bucharest-

Magurele, Romania, E-mail: [email protected] 3Joint Institute for Nuclear Research, Dubna, 141980, Moscow Region, Russian Federation

E-mail: [email protected]

Received September 22, 2015

Magnetorheological and electroconductive magnetorheological suspensions are of

great interest for both: scientific and applicative research. In the present paper, the

production methods of microparticles and electroconductive magnetorheological

suspensions, together with the involved electroconductive mechanisms are reviewed.

Key words: microparticles, magnetorheological suspension, electro conductivity,

magnetic field, electrical resistance.

1. INTRODUCTION

Magnetorheological suspensions (MRSs), ever since they were discovered

[1, 2] and respectively, ever since the mechanisms [3–10] which endow them with

inciting physical properties were defined, have attracted alongside with

electrorheological fluids (ERF) [11–17] great interest in both their scientific study

and their application.

The scientific interest relates to the mechanisms that determine the

modifications of the rheological properties of MRS in magnetic field [18–25]. The

interest in their application relates to the devising of different devices or/and

subassemblies for: deadening vibrations [26–37], building clutches [38–42],

producing of revolving tightening [43], devising of solid materials with elasticity

constants pre-established by means of an applied magnetic field variation [44–47],

for utilization in cancer therapies [48–52], in building orthopedic prostheses [53],

finishing solid surfaces [53–56], etc.

The electroconductive MRSs are of recent date [57, 58]. They can be used in

the production of giant magnetoresistors [57, 58], in the manufacture of sensors for

the detection of fringe fields in magnetic heads [59] as well as warfare agents [60]

and also in the devising of magnetoresistances in narrow stripes [61] etc.

Rom. Journ. Phys., Vol. 61, Nos. 5–6, P. 926–945, Bucharest, 2016

mailto:[email protected]





2 Microparticles and electroconductive magnetorheological suspensions 927

The production methods of microparticles and electroconductive

magnetorheological suspensions, together with the involved electroconductive

mechanisms are reviewed in the present paper.

2. PRODUCTION OF ELECTROCONDUCTIVE MAGNETORHEOLOGICAL

SUSPENSIONS

MRSs are polyphasic fluids [65–70]. In the liquid phase (nonpolar liquids,

polar liquids, water and others [10, 57, 58, 62]), mixtures of particles (magnetic

and non-magnetic [57, 58]) and additives are introduced [65–70]. The magnetic

particles can have micrometric [62] or/and milimetric dimensions [57, 63].

The additives used in the production of electroconductive MRSs can be of

the graphite powder type [57, 58], fumed silicon, carbon fibers [67–70], stearic

acid [58] and others. Their role is to keep the magnetic particles at a distance

or/and to modify some of the transport properties of MRSs [57].

The magnetic nanoparticles, stabilized in the carrier liquid [9, 71, 72] are

magnetic monodomains [9, 73]. In the case of mixing them with magnetic

microparticles in a carrier liquid, they form aggregates surrounding the

microparticles. Thus, their role is to ensure stability to MRS [64, 65].

Electroconductive MRSs have as fluid phase a liquid with remarkable

dielectric properties [57], mineral oil [58, 74, 75] and others. The solid phase of

electroconductive MRSs, consists of milimetric particles of silicon steel [57], iron

microparticles [58, 74, 75] etc.

The graphite microparticles [57, 58], the stearic acid [58, 74, 75], the carbon

fibers [67–70], also have the role of keeping the suspension stable and of providing

it with qualities which are of interest for applications [57, 58, 74, 75].

The solid phase production for electroconductive MRS is achieved with high

productivity by plasma and electric arc methods. Thus, in the electric arc plasma

[76–83], by modification of the main technological parameters, iron microparticles

and microspheres [76–78] (Fig. 1), iron microtubes [79] (Fig. 2), octopus-shaped

microparticles [80] (Fig. 3), SiO2 microtubes [81] (Fig. 4), pore macrospheres [82]

(Fig. 5) and SiO2 microparticles [83] (Fig. 6), are obtained.

Fe nitride nanoparticles are obtained by thermal decomposition of Fe(CO)5

in the Ar-N2 capacitive plasma [84]. By thermal decomposition of Fe(CO)5 in the

argon plasma jet [85], iron atoms and CO molecules result. Fe atoms condense on

the gas particles. Depending on the plasma jet velocity and on the quantity of

toluene +10% Fe(CO)5 mixture, iron carbide microparticles of pre-established

dimensions result (Fig. 7).

928 I. Bica, M. Balasoiu, M. Bunoiu, L. Iordaconiu 3

a b

Fig. 1 – Iron particles obtained by plasma procedures [76–78]; (a) microparticles;

(b) pore microspheres.

a b

c d

Fig. 2


e f

Fig. 2 (continued) – Cylinder-shaped micro-particles [79]: (a), (b) and (c): micro-tubes; (d): branching

micro-tubes with semitransparent walls; (e): branching micro-cylinders; (f): micro-tube with one

closed end. The ratio length – micro-tube diameter is, for: (a) 52; (b) 19.38; (c) 29 and (f) 27.35.

Work regime: tension on arc: U = 40Vdc; current intensity: I = 175 Adc; argon flow:

D = 0.7510-3 m3s-1; nozzle diameter: d = 210-3m; nozzle – rod distance = 6 10-3 m;

rod advance speed: v = 1.15 10-3 ms-1; rod diameter: de = 310-3 m; material: carbon steel.

Fig. 3 – Octopus forms micro-particles: nucleus diameter: 20 m; ligaments length:

max. 160 m; ligaments thickness: 8 m (at the base), and 4 m (at the top) [80].

Fig. 4 – Cross section of SiO2 microtubes [81].


Fig. 5 – Iron macro-spheres obtained in the plasma arc (voltage on the arc: 160 Vdc, current intensity:

250 Adc, nozzle diameter: 3.5 10-3 m) transferred upon a carbon steel plate (thickness: 15 10-3 m)

in argon (flow rate: 1.8 10-3 m3s-1); width of the cut: 4 10-3 m; material advance velocity:

0.023 10-3 ms-1 10% [82].

Fig. 6 – SiO2 micro-particles obtained by spheroidising of the glass powder in revolving electric arc

(voltage on the arc: 50 Vdc, current intensity: 100 Adc, argon flow: 1.6 10-5 m3/s; glass powder

granulation ranging between 150 m and 530 m; powder flow: 2 10-6 kg/s; arc revolution:

800 rev/s) [83].


Fig. 7 – Iron microparticles and iron carbide, with mean diameter of 12.1 nm [85].

By using the procedure described in Ref. [85], graphite nanoparticles with a

mean diameter of 11.6 nm are obtained from iron-2 etylhexamaleat. The existence

of definite flaws, under the form of iron oxides [76, 80] leads, by mechanisms

described in Ref. [88], to the diminution of saturation magnetization of the iron

microparticles.

This drawback can be removed, according to Ref. [89] by thermal

decomposition of Fe2(CO)9 in mineral oil with stearic acid, under the protection of

Ar+6% H2.

Fig. 8 – Forms and dimensions of iron microparticles obtained

by the in situ thermal decomposition of Fe2(CO)9 [88].

At 358 K, thermal decomposition of Fe2(CO)9 occurs and nuclei of iron

atoms [88] are formed in the carrier liquid. These iron nuclei become stable when


their size is at least 3.8 nm [85]. By adjusting the undercooling of the system

composed from iron atoms, the dimensional control of the magnetic particles [89]

is achieved. From TEM and SANS measurements it is found that the obtained

particles (Fig. 8) have a mean radius of about 2 m [87]. XRD analysis has shown

that the particles do not present traces of oxides [58], and are formed mainly from

Fe of BCC type lattice structure with possible very small amount of austenite FCC

type structure [87].

2.1. MAGNETIZATION CURVES OF ELECTROCONDUCTIVE MAGNETORHEOLOGICAL

SUSPENSIONS

The magnetic particles in the electroconductive MRS in magnetic field

become magnetic dipoles [9, 10].

For the case of the magnetic fields of low intensities, as compared with

those corresponding to the saturation magnetization, MRS magnetization can be [9]

approximated by the relation:

)(* LmnM (1)

where *n is the density of the magnetic dipoles, m is the dipolar moment and )(L

is Langmuir’s function. is a dimensionless value, equal to the relation between

the maximum magnetic energy and the thermal energy:

kT

Hm

0 (2)

where 0 is the magnetic permeability of the vacuum, H

is the magnetic field

intensity vector, k is the Boltzmann constant and T is the temperature.

For

1

1)( ,1 L

and

11

11 *

sMmnM .

If H

, then sMM , where sM is the saturation magnetization.

The existence in the solid phase of non-magnetic additives diminishes the

saturation magnetization, as shown in Fig. 9.


Fig. 9 – Magnetization M of MRSs and EMRS obtained with type VSM880 vibration magnetometer.

MRSs and EMRSs are composed from 48.77% massive iron particles with mean diameter of 3,75 m,

dispersed in mineral oil with stearic acid and, respectively, 43.54% massive iron particles with mean

diameter 3.75 m, dispersed in mineral oil with stearic acid and graphite powder of granulation ranging

between 2 m and 32 m [58].

The aria of the MRS hysteresis curve (Fig. 10), based on 2.10 m diameter

iron microparticles is null.

Fig. 10 – Magnetization M as a function of the effective intensity effH of the alternative magnetic

field for various value of the volume fraction of electroconductive MRSs [88].


2.2. RHEOLOGY OF ELECTROCONDUCTIVE MAGNETORHEOLOGICAL SUSPENSIONS

Like ERF [89–91], MRSs drastically modify their rheological properties. If

the former do that in electrical field, the latter do it in magnetic field (Fig. 11).

a b

Fig. 11 – Magnetorheological data: (a) the variation of the viscosity as a function of the intensity H

of the magnetic field; (b) the variation of the shear stress as a function of the intensity H of the

magnetic field.

In both cases, the j’s stand for parameters [58].

Here:

MRS is magnetorheological suspension based on mineral oil and iron

microparticles with the mean diameter 3.75 m;

EMRS are formed from MRS + graphite microparticles with the

granulation ranging between 2 m and 32 m.

Naturally, there are various approaches to the dependence of on H. In

some on them [62, 92–95], the shear stress is proportional to H, while in other

approaches [95], is independent of H.

For the case of electroconductive MRSs where the motion velocities of the

magnetic dipoles are low (Fig. 12), the shear stresses can be approximated by

means of the following relation [96]:

HH 2 (3)

where and are fitting parameters.

The viscosity (Fig. 13) of electroconductive MRSs is quasi-linear with H

for volume fraction and shear velocities as parameter [74].


Fig. 12 – Migration velocity v of the iron microparticles of the intensity I of the electric current through

the coil of the electromagnet (Fig. 14a) for various values of [74].

a b

Fig. 13 – Variation of MRS viscosity as a function of the intensity I of the electric current through

the coil of the electromagnet (Fig. 14a) for: (a) = 0.27, and (b) = 0.60 [74].

2.3. MAGNETORESISTORS AND ELECTRICAL RESISTANCES

The device, consisting of a tube made of a dielectric material, filled with

electroconductive MRS and provided with two electrodes at its ends, is called

magnetoresistor [58].

The magnetoresistor is placed between the poles of an electromagnet, as

shown in Fig. 14.

For H = 0, the electrical resistance R of the magnetoresistor is infinite. In an

applied magnetic field, the iron microparticles become magnetic dipoles, with

identical [74] and equal [96] magnetic moments:


Ham

3

40

3

(4)

where “a” is the mean radius and is the magnetic susceptivity.

The magnetic dipoles m

are aligned with the magnetic field lines as shown

in Fig. 14b. The initial mean distance between dipoles m

is xmax.

Because of the dipolar interaction [9, 74], the dipoles attract each other. At a

given moment t (t > 0), the distance between the dipole is x (x < xmax).

The vacancies in the chains of dipoles are taken, by diffusion [9], by the free

magnetic particles in MRSs.

a b

Fig. 14 – Experimental assembly (a): 1 – magnetic core; 2 – coil; 3 – non-magnetic electrode;

4 – glass tube; 5 – electroconductive MRS, A – ampermeter; S – adjustable current source, – digital

ohmmeter [74]. The iron microparticles, aligned at the initial moment with the direction of the

magnetic field lines (b). H

– magnetic field intensity;

– magnetic field gradient;

m

– dipolar magnetic moment.

The thermal energy kT of the particles does not undo the dipolar ties when

the condition [97, 98] takes place:

kTHa 2230

9

(5)

Each chain of magnetic dipoles has equivalent electrical resistance [74]:

2

11

2

a

xnR m

, (6)

where m is the electrical resistivity of the carrier liquid and 1n is the number of

dipoles in the chain.


If the inner diameter of the magnetoresistor is equal to the length l of the

body consisting of MRS, then:

a

ln

21 (7)

The

2

28

3

a

ln dipole chains represent the equivalent of the electrical

resistance of the magnetoresistor [74], which is:

3

2

2

1

la

x

n

RR m (8)

The motion law, x = x(t) of the dipoles in the chain results from the motion

equation of the dipoles [9, 74] and, for the case studied by us [74], it assumes the

form:

taHl

Mxx s

18

20max

(9)

then from the Eq. (8), one obtains:

taH

l

Mx

laR sm

18

3

2 20max

(10)

Indeed, from the determinations performed by means of the assembly in

Fig. 14a and represented graphically (Figs. 15 and 16), it results that the model

released describes, with good approximations the dependence of R on t and h for

fixed a, l, m and [74].

The viscosity of the mineral oil (carrier liquid) decreases with the

temperature T increase (Fig. 17). According to the model (Eq. 10), R decreases

monotonously by T and it depends considerably on H (Fig. 18).

In longitudinal alternative magnetic field ( OxHeff ||

– Fig. 14a), the mean

value of the movement of the magnetic dipoles is null and electrical conduction

does not set in MRS [88]. For transversal magnetic fields ( OxHeff

– Fig. 14a),

following the distortion of the body consisting of MRS, the microparticles get close

together, create contact along the direction Ox in Fig. 14a, and the electrical

conduction occurs in MRS.


a b

c

Fig. 15 – Variation of R by time t, for = 0.27 [72].

(a) H = 30 kA/m;

(b) H = 40 kA/m;

(c) H = 60 kA/m; H = 70 kA/m; H = 80 kA/m.

a b

Fig. 16


c

Fig. 16 (continued) – Variation of R by time t, for = 0.60 [72].

(a) H = 30 kA/m;

(b) H = 40 kA/m;

(c) H = 60 kA/m; H = 70 kA/m; H = 80 kA/m.

280 300 320 340 360 380 4000.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

1.6

1.8

2.0

2.2

(P

a s

)

T(K)

Fig. 17 – Temperature T dependence of the mineral oil viscosity .


Fig. 18 – Temperature T dependence of the resistance R [74].

For T = const., R depends considerably on effH for fixed (Fig. 19).

Due to the introduction of solid phases in the suspension, the viscosity [99,

100] modifies incrementally. Indeed, according to the devised model (Eq. 10), R

can be pre-established from the MRS composition, as shown in Fig. 20.

Interactions occur between the magnetic dipole chains, which, for properly

chosen values of the time-constant magnetic field, are of attractive type [101–105].

The intensity of the magnetic interaction between the magnetic dipole chains

is much lower than the intensity of the interactions between the magnetic dipoles in

the chain [9, 106, 107]. For this reason, the resistance R of MRSs is much higher

for the case of the transversal magnetic field than the electrical resistance of MRSs

for the case of the longitudinal electrical conduction (Fig. 21).

a b

Fig. 19 – Variation of R by time t and effH , for: (a) 1 0.30; (b) 2 0.06 [88].


Fig. 20 – The electrical resistance R of the magnetoresistor as a function of time (t) for various

compositions of MRS, for H = 43, 75 kA/m.

0 40 80 120 160 200

0

2

4

6

8

10

12

14

longitudinal magnetic field

transversal magnetic field

H=78kA/m

R(k

)

t(s)

Fig. 21 – The electrical resistance R of the magnetoresistor in MRS based on mineral oil with stearic

acid in mixture with iron microparticles and graphite powder [58] for the case of transversal conduction

and for the case of longitudinal conduction, respectively, at the same value of the external magnetic

field intensity (H = 78 kA/m). Here: 12 0015.0 mm (where: 1m is mass of the MRS [58] and 2m

is mass of the graphite microparticles).

3. CONCLUSIONS

The electroconductive MRS is a quasi-homogeneous mixture, consisting of a

carrier liquid having good dielectric properties, mixed with magnetic and/or non-

magnetic particles.


The solid phase of electroconductive MRSs is obtained, with high

productivity, by plasma and arc procedures. The dimension and the shape of the

particles can be pre-established by adjusting the technological parameters of the

plasma. By in situ decomposition of Fe2(CO)9, iron microparticles with no traces of

oxides are obtained. The dimension of the iron microparticles can be pre-

established by adjusting the undercooling of the system formed by the iron atoms

and the carrier liquid mixed with the protection gas (Ar+6%N2).

The electroconductive MRSs are soft magnetic materials. The saturation

magnetization and the magnetization curve slope depend on the density of the

magnetic dipoles in the carrier liquid.

The rheological properties of the electroconductive MRSs are determined by

the magnetic properties of the particles, by their volume fraction and by their shear

velocity, for fixed densities of the external magnetic field. The electrical resistance

and, implicitly, the electrical conductivity of MRSs is established in only in the

presence of the magnetic field. The electrical conduction of MRSs is of

longitudinal or/and transversal type in time-constant magnetic field. It is of

transversal type only in alternative magnetic field. The electrical conductivity

depends on the composition of MRS. It can be fixed in time, it can be changed in

time and it is strongly influenced by the intensity of the external magnetic field for

the fixed and T values.

Acknowledgements. The finance support from the Romania-JINR Cooperation Programme on

2014–2015 and Grants of Romanian Governmental Plenipotentiary Representative at JINR Dubna for

2015 is acknowledged.

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