Journal of Chemical Engineering of Japan, Vol. 37, No. 2, pp. 253–260, 2004 Research Paper
Copyright © 2004 The Society of Chemical Engineers, Japan 253
Sub-critical Water Hydrolysis Treatment for Waste Squid Entrails and
Production of Amino Acids, Organic Acids, and Fatty Acids
Hiroyuki YOSHIDA and Omid TAVAKOLI
Department of Chemical Engineering, College of Engineering,
Osaka Prefecture University, 1-1 Gakuen-cho, Sakai-shi,
Osaka 599-8531, Japan
Keywords: Sub-critical Water, Squid Wastes, Amino Acid, Organic Acid, Fatty Acid
The study presented in this paper is focused on processing squid wastes by using sub-critical water
extraction and hydrolysis to produce valuable substances. Using a small-scale batch reactor (9.0 cm
3
),
squid entrails were treated with sub- and supercritical water without oxidants. Reaction conditions in-
volved temperatures of 443–673 K, pressures 0.792–30.0 MPa, and reaction times 1–50 minutes. Fat and
oil were extracted into sub-critical water very efficiently, and soluble proteins, organic acids, and amino
acids were produced in the aqueous phase by a hydrolysis reaction. Even in the short reaction time
of 5 min, more than 99% of solid were converted to those products in the temperature, which was higher
than 550 K. Results showed a maximum total yield of sixteen amino acids of 0.1031 kg/kg dry en-
trails at 473 K (5 min), and a maximum total yield of seven organic acids of 0.055 kg/kg dry entrails at
553 K (40 min). Also the oil extracted with hexane included useful fatty acids. Our experimental results
indicated that the sub-critical water treatment method is very efficient for converting waste squid en-
trails to valuable materials as resources for many other industries.
Introduction
Seafood processing and related waste discharges
have become a serious problem since damping of those
kinds of wastes has been banned by the London treaty
of 1996. In Japan, about 1.3 million tons of seafood
wastes are produced a year. After the London treaty,
almost all those wastes have been incinerated and the
running cost of which is $500–800 per ton of wastes,
which is very expensive. Therefore an efficient process
for converting seafood wastes to useful materials is
strongly needed to achieve zero emissions. Yoshida et
al. (1999) showed that sub-critical water hydrolysis is
an efficient method for production of useful substances
such as amino acids, organic acids, fatty acids, oil, and
so on, from fish wastes. Kang et al. (2001) used sub-
and supercritical water to produce amino acid from fish
wastes. Other applications of sub- and supercritical
water treatment have also reported. Kabyemela et al .
(1999) decomposed glucose, fructose and cellobiose.
Sasaki et al. (2000) reported hydrolysis of cellulose,
and Taylor et al. (2001) investigated hydrolysis of
methyl t-butyl ether. Also some technologies of sub-
and supercritical water conditions with oxidants have
been reported, such as treatment of wastewaters con-
taining organic pollutants including hazardous organic
(Modell, 1989), pyridine (Crain et al., 1993), Azo dye
Received on December 18, 2002. Correspondence concerning
this article should be addressed to H. Yoshida (E-mail address:
yoshida@chemeng.osakafu-u.ac.jp).
(Donlagic and Levec, 1997), linear alkylbenzene
sulfonates (Mantzavinos et al., 2000), municipal sew-
age sludge (Goto et al ., 1999), phenol (Savage et al .,
1995; Portela et al ., 2001), and aqueous polyvinyl al-
cohol (Won et al., 2001).
There are three important reasons to use sub-criti-
cal water treatment. Firstly, the main aim in
supercritical water oxidation is that wastes must be
decomposed to CO
2
, N
2
, and water. On the other hand
the sub-critical water hydrolysis produces many use-
ful and valuable organic substances. This is because
the ion product of water shows maximum value around
520–550 K in the sub-critical region. Secondly, sub-
critical water acts as a powerful solvent and exhibits
important effects in its physical properties. This is be-
cause the dielectric constant decreases with increas-
ing temperature. Moreover, sub-critical water is an
excellent extraction solvent for polar and non-polar
organic substances, and a much broader range of
polarities can be achieved in this condition. Thirdly,
this process is more economic than, not only
supercritical water treatment, but also the incineration
processes. The supercritical water treatment process
is normally carried out at very high temperatures
(higher than 1000 K) and high pressures, and the ap-
paratus decays quickly by strong oxidation even if very
expensive Hastelloy is used. The incineration process
is also very expensive, as we already mentioned.
Since the squid entrails contain a lot of cadmium
and other harmful metal cations; their treatment has