Electrospinning of Heated Gelatin-Sodium
Alginate-Water Solutions
SungCheal Moon, Richard J. Farris
Polymer Science and Engineering Department, Silvio O. Conte National Center for Polymer Research,
University of Massachusetts Amherst, Amherst, Massachusetts 01003
Most polymers that are electrospun are dissolved in a
solvent and are spun at ambient temperature. Gelatin,
a natural polymer, has excellent potential in medical
applications as a biodegradable polymer, especially
when combined with sodium alginate. Unfortunately,
gelatin/water or gelatin/sodium alginate/water solu-
tions cannot be electrospun at ambient temperature
without the incorporation of substances that are con-
sidered potentially toxic to the human body, such as
acetic acid. In this study, gelatin/water solutions with
and without sodium alginate were successfully electro-
spun without the use of additional solvents by using
heated water solutions. The effect of electrospinning
parameters such as solution concentration and applied
voltage on the nanofiber morphology of these solutions
was studied. These nanofibers from heated gelatin/
water solutions exhibited good morphology with an av-
erage size of 291 ± 67 nm at 18% concentration to
414 ± 52 nm at 20% concentration. Similar sizes were
observed when sodium alginate was incorporated into
the gelatin/water solutions, although the relationship
was dependent upon the amount of sodium alginate in
the solution as well as the total concentration. Typi-
cally, these nanofibers containing sodium alginate
were produced at a lower gelatin concentration com-
pared with the gelatin/water nanofibers because of the
increase of viscosity and conductivity of the solutions
due to the addition of the highly viscous and conduc-
tivity sodium alginate. POLYM. ENG. SCI., 49:1616–1620,
2009. ª 2009 Society of Plastics Engineers
INTRODUCTION
Electrospinning was introduced in early 1930s [1, 2]
and has been recognized as an efficient processing method
to manufacture nanoscale fibrous structures for many
applications [3–5]. The technique can apply to not only
synthetic polymers but also natural polymers. Many stud-
ies have been reported on electrospun poly(vinyl alcohol)
(PVA), poly(ethylene oxide) (PEO), nylon, collagen, silk
fibroin, and alginate [3, 5–13].
Correspondence to: Richard J. Farris; e-mail: rjfarris@polysci.umass.edu
DOI 10.1002/pen.21355
Published online in Wiley InterScience (www.interscience.wiley.com).
C 2009 Society of Plastics Engineers
V ers by electrospinning is difficult [22]. This is because of
Electrospun nanofibers have been considered in bioma-
terials as a high performance filter, wound-dressing, drug
delivery system, and cell-growth scaffold due to its high
surface to volume ratio [4, 12–17]. In particular, the elec-
trospinning of natural polymers has been increasingly
studied because of the increased interest in bioengineering
[5]. For many biomedical applications, the most important
characteristics that are targeted include biocompatibility
and mechanical performance. In comparison with their
synthetic counterparts, natural biopolymers generally have
better biocompatibility and hence are more suitable for
human body [3]. However, although natural polymers
have many of the desired characteristics required for bio-
medical engineering applications, most natural polymers
have limited applications because of the difficulty of
handling.
Among the natural polymers, gelatin, which can be
obtained by denaturing collagen, is a very conventional
one. Gelatin is known to have biocompatibility and biode-
gradability similar to collagen. Furthermore, it can be eas-
ily obtained by extraction from animal tissue such as skin,
muscle, and bone. Gelatin also has an important merit in
that it is an inexpensive biopolymer. For these reasons,
there are many studies related to the usage of gelatin in
various forms for many different applications [3, 5, 18–
21]. However, there are few attempts to form nanofibrous
gelatin by electrospinning, and when it is done, the solu-
tions used included solvents that are highly toxic, such as
1,1,1,3,3,3-hexafluoro-2-propanol, trifluoroacetic acid, and
2,2,2-trifluoroethanol as well as slightly to moderately
toxic solvent such as acetic acid for easy dissolution and
the prevention of gelation at room temperature [3, 5, 22].
Unfortunately, gelatin/water solutions cannot be processed
via electrospinning at room temperature. Moreover, when
dissolved in water at a temperature around or above
378C, gelatin becomes a kind of a colloidal sol [3, 5].
Alginate, a biodegradable polymer derived from ma-
rine brown algae, bears structural resemblance to glycos-
aminoglycan (GAG), one of the major components of nat-
ural extracellular matrices (ECMs) found in human tissue
[23]. It is also known that fabrication of alginate nanofib-
POLYMER ENGINEERING AND SCIENCE—-2009
the gelation of alginate solutions at very low polymer a grounded target. The polymer solution is loaded into the
concentrations (e.g., ca. 2 wt% for alginate in deionized syringe and an electrode is clipped onto the needle. The
water) and their high viscosity at higher polymer concen- needle, electrode, and grounded target are all enclosed in
trations. One way to solve this problem is to incorporate a chamber to reduce the influence of air currents on the
a fraction of copolymer and to apply surfactants or/and trajectory of the electrospun jet. The syringe was heated
cosolvents to the alginate solution. For example, electro- by a heat gun to reduce/prevent gelation in the syringe
spinning of alginate from blends with PEO has been during electrospinning. The solutions are typically electro-
reported [12, 23, 24]. spun between 8 and 15 kV horizontally onto a grounded
In this study, electrospun gelatin nanofibers using gelatin/ stationary target. The grounded target is
12 cm from the
sodium alginate/water solutions were investigated. Heated charged capillary tip.
solutions were used to prevent rapid gelation of the gel-
atin/sodium alginate/water solutions at room tempera-
ture during electrospinning. The effect of electrospin- Characterization
ning parameters such as solution concentration and Morphologies such as diameter and diameter distribu-
applied voltage on the resulting fiber morphology was tion of the electrospun nanofibers were observed by field
investigated. emission scanning electron microscopy (FE-SEM). Sam-
ples were mounted onto SEM plates, sputter coated with
gold, and examined using a JOEL JSM 6320FXV electron
EXPERIMENTAL
microscope to determine fiber diameters and their
distribution. The average diameter of the electrospun
Materials and Electrospinning nanofibers was determined by measuring the diameters of
nanofibers at 100 different points on a SEM image
Gelatin (Class98) was received from the Eastman
(20,000–30,0003) using the annotation and measurement
Kodak Company. Sodium alginate (NaAlg), derived from
tool on the JEOL program. The diameters are presented
seaweed, was received from the Chosun University
as the average 6 standard deviation.
(Republic of Korea). Distilled water and acetic acid were
used for solvents. The composition of the solutions stud-
ied is shown in Table 1. All solutions except for the two RESULTS AND DISCUSSION
that combined acetic acid were prepared at 458C under
The goal of this study was to produce electrospun
constant stirring. The two solutions with acetic acid,
nanofibers from gelatin/sodium alginate/water solutions
which is considered a slightly to moderately toxic solvent,
without the use of toxic solvents. The method chosen was
were prepared and spun at ambient temperature to com-
to electrospin above room temperature using a heat gun
pare with heated gelatin/water solutions. Also, gelatin sol-
to prevent the gelation of the solutions during electrospin-
utions containing sodium alginate, an antifungal agent,
ning. The effect of electrospinning parameters such as so-
were prepared.
lution concentration and applied voltage on the generated
The electrospinning apparatus consists of a heat gun, a
fiber morphology was observed.
high voltage power supply, a syringe infusion pump, and
The solutions of gelatin/water/acetic acid studied and
the method used are shown in Table 1. The 11 and 12%
TABLE 1. Composition of the gelatin solutions for electrospinning.
gelatin nanofibers using acetic acid in combination with
water as the solvent showed good morphology in the
Composition (wt%) range of applied voltage of 8–9 kV, a needle to target dis-
Polymer Solvent
tance of 12 cm, and solvent concentration ratio of dis-
Item (unit) tilled water:acetic acid ¼ 1:9 (w/w) (Table 2). The aver-
Sample Sodium Distilled Acetic age diameters of those were
135 6 23, 163 6 33 nm,
name Gelatin alginate water acid
respectively.
11GWAA 11.0 — 8.9 80.1 When only water was used as the solvent and the solu-
12GWAA 12.0 — 8.8 79.2 tions were heated to prevent gelation during electrospin-
10GW 10.0 — 90.0 — ning, gelatin nanofibers with good morphology and aver-
15GW 15.0 — 85.0 — age diameters ranging from 291 6 67 to 414 6 52 nm
18GW 18.0 — 82.0 —
20GW 20.0 — 80.0 —
were obtained using 18 and 20% gelatin concentration
10G1SAW 10.0 1.0 89.0 — (Table 2 and Fig. 1). Reports of electrospun gelatin nano-
15G0.1SAW 15.0 0.1 84.9 — fibers from gelatin/water solution without the addition of
15G0.5SAW 15.0 0.5 84.5 — toxic solvents have not been found [3, 5, 17–21]. The
15G1SAW 15.0 1.0 84.0 — average diameters of these nanofibers made from heated
15G2SAW 15.0 2.0 83.0 —
18G0.1SAW 18.0 0.1 81.9 —
solutions increased with increasing applied voltage for a
gelatin concentration of 18%, but decreased for the 20%
G, gelatin; W, distilled water; SA, sodium alginate; AA, acetic acid. gelatin concentration. There was no difficulty in producing

DOI 10.1002/pen POLYMER ENGINEERING AND SCIENCE—-2009 1617

 TABLE 2. Morphology and diameter of the electrospun gelatin nanofibers by FE-SEM.

Item (unit) Composition (wt%) Electrospinning parameter

Sample name G/SA/W/AA Applied voltage (kV) Average diameter (nm) Morphology

11GWAA 11.0/0.0/8.9/80.1 8 137 6 37 No beads

9 135 6 23 No beads
12GWAA 12.0/0.0/8.8/79.2 8 152 6 34 No beads
9 163 6 33 No beads
10GW 10.0/0.0/90.0/0.0 12 169 6 30 Many beads
15GW 15.0/0.0/85.0/0.0 12 277 6 51 few beads
15 290 6 65 few beads
18GW 18.0/0.0/82.0/0.0 12 291 6 67 No beads
15 353 6 111 No beads
20GW 20.0/0.0/80.0/0.0 12 414 6 52 No beads
15 338 6 41 No beads
10G1SAW 10.0/1.0/89.0/0.0 12 161 6 39 Few beads
15 122 6 32 Few beads
15G0.1SAW 15.0/0.1/84.9/0.0 12 238 6 76 Few beads
15 246 6 60 Few beads
15G0.5SAW 15.0/0.5/84.5/0.0 12 241 6 96 Few beads
15 268 6 109 Few beads
15G1SAW 15.0/1.0/84.0/0.0 12 343 6 109 No beads
15 330 6 140 No beads
15G2SAW 15.0/2.0/83.0/0.0 12 347 6 74 No beads
15 337 6 80 No beads
18G0.1SAW 18.0/0.1/81.9/0.0 12 252 6 102 No beads
15 273 6 99 No beads

G, gelatin; W, distilled water; SA, sodium alginate; AA, acetic acid.

high quality nanofibers from gelatin/water solutions when
heated solutions were used providing a temperature of at
least
458C was used.
The electrospun gelatin/sodium alginate nanofibers,
from heated gelatin/sodium alginate/water solutions with-
out toxic solvents such as acetic acid, also had good mor-
phology without beads above 15 wt% gelatin content and
1 wt% sodium alginate content (Table 2). The morphol-
ogy of 10–18% gelatin/sodium alginate/water nanofibers,
made at an applied voltage of 12 kV, are shown in Fig. 2.
The electrospun gelatin/sodium alginate/water nanofibers
with good morphology were produced at lower gelatin
concentration compared with the gelatin/water nanofibers
because of the increase of viscosity and conductivity of
solutions using high viscosity and conductivity sodium al-
ginate. As shown in Fig. 3, the average diameters of 15
and 18% gelatin/sodium alginate/water nanofibers without
beads were 252 6 102 and 347 6 74 nm. Also, the aver-
age diameters of these nanofibers decreased with increas-
ing an applied voltage above 1 wt% sodium alginate con-
tent due to the increase of pulling force at higher applied
voltage for the highly viscous solutions (Table 2). For exam-
ple, the average diameter of electrospun gelatin nanofibers
from a solution of gelatin/sodium alginate/water ¼

FIG. 1. SEM photomicrographs of the electrospun gelatin nanofibers from 18% gelatin/water solutions with-
out acetic acid at applied voltage of 12 kV.

1618 POLYMER ENGINEERING AND SCIENCE—-2009 DOI 10.1002/pen

 FIG. 2. SEM photomicrographs of the electrospun gelatin nanofibers from solutions of gelatin/sodium algi-
nate/water at applied voltage of 12 kV.
FIG. 3. Average diameter vs. sodium alginate content of the electro-
spun 15% gelatin nanofibers from solutions of gelatin/sodium alginate/
water.
DOI 10.1002/pen
15.0/1.0/84.0 (w/w/w) was decreased from 343 6 109 nm
to 330 6 140 nm by increasing the applied voltage from
12 to 15 kV (Table 2).
CONCLUSIONS
In this study, nanofibers were produced via electrospin-
ning gelatin/sodium alginate/water solutions without the
use of additional solvents, such as acetic acid, by using a
heat gun to prevent solution gelation during electrospin-
ning. The effect of electrospinning parameters such as so-
lution concentration and applied voltage on the resulting
fiber morphologies was investigated. Quality fibers with
excellent appearing morphology were produced using
these methods providing the solution temperatures were at
least 458C. Gelatin/water solutions incorporating sodium
alginate as an antifungal agent will hopefully find applica-
tions in the biomedical field.
POLYMER ENGINEERING AND SCIENCE—-2009 1619
REFERENCES
1. A. Formhals, U.S. Patent 1,975,504 (1934).
2. A. Formhals, U.S. Patent 2,160,962 (1939).
3. Z.M. Huang, Y.Z. Zhang, S. Ramakrishna, and C.T. Lim,
Polymer, 45, 5361 (2004).
4. Z.M. Huang, Y.Z. Zhang, M. Kotaki, and S. Ramakrishna,
Compos. Sci. Technol., 63, 2223 (2003).
5. C.S. Ki, D.H. Back, K.D. Gang, K.H. Lee, I.C. Um, and
Y.H. Park, Polymer, 46, 5094 (2005).
6. B. Ding, H.Y. Kim, S.C. Lee, C.L. Shao, D.R. Lee, S.J.
Park, G.B. Kwag, and K.J. Choi, J. Polym. Sci. Part B:
Polym. Phys., 40, 1261 (2002).
7. J.M. Deitzel, J.D. Kleinmeyer, J.K. Hirvonen, and N.C.
Beck Tan, Polymer, 42, 8163 (2001).
8. H. Fong, W. Liu, C.S. Wang, and R.A. Vaia, Polymer, 43,
775 (2002).
9. J.A. Matthews, G.E. Wnek, D.G. Simpson, and G.L. Bowlin,
Biomacromolecules, 3, 232 (2002).
10. H.J. Jin, S.V. Fridrikh, G.C. Rutledge, and D.L. Kaplan,
Biomacromolecules, 3, 1233 (2002).
11. H. Liu and Y.L. Hsieh, J. Polym. Sci. Part B: Polym. Phys.,
40, 2119 (2002).
12. S. Safi, M. Morshed, S.A.H. Ravandi, and M. Ghiaci,
J. Appl. Polym. Sci., 104, 3245 (2007).
1620 POLYMER ENGINEERING AND SCIENCE—-2009
13. S.C. Moon, B.Y. Ryu, J.K. Choi, B.W. Jo, and R.J. Farris,
Polym. Eng. Sci., 49, 52 (2008).
14. S. Sukigara, M. Gandhi, J. Ayutsede, M. Micklus, and F.
Ko, Polymer, 44, 5721 (2003).
15. J. Zeng, X. Xu, X. Chen, Q. Liang, X. Bian, L. Yang, and
X. Jing, J. Control. Release, 92, 227 (2003).
16. S.R. Bhattarai, N. Bhattarai, H.K. Yi, P.H. Hwang, D.I.
Cha, and H.Y. Kim, Biomaterials, 25, 2595 (2004).
17. W.J. Li, C.T. Laurencin, E.J. Caterson, R.S. Tuan, and F.K.
Ko, J. Biomed. Mater. Res., 60, 613 (2002).
18. Y. Tabata and Y. Ikada, Adv. Drug Deliv. Rev., 31, 287
(1998).
19. N.W. Fadnavis, G. Sheelu, B.M. Kumar, M.U. Bha-
lerao, and A.A. Deshpande, Biotechnol. Prog., 19, 557
(2003).
20. M.C. Chang, C.C. Ko, and W.H. Douglas, Biomaterials, 24,
3087 (2003).
21. R. Cortesi, C. Nastruzzi, and S.S. Davis, Biomaterials, 19,
1641 (1998).
22. J.H. Song, H.E. Kim, and H.W. Kim, J. Mater. Sci.: Mater.
Med., 19, 95 (2008).
23. N. Bhattarai, Z.S. Li, D. Edmondson, and M.Q. Zhang, Adv.
Mater., 18, 1463 (2006).
24. J.W. Lu, Y.L. Zhu, Z.X. Guo, P. Hu, and J. Yu, Polymer,
47, 8026 (2006).
DOI 10.1002/pen