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PII: S0144-8617(17)31354-1
DOI: https://doi.org/10.1016/j.carbpol.2017.11.067
Reference: CARP 13018
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Please cite this article as: Li, Guantian., & Zhu, Fan., Quinoa
starch: Structures, properties, and applications.Carbohydrate Polymers
https://doi.org/10.1016/j.carbpol.2017.11.067
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Quinoa starch: Structures, properties, and applications
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School of Chemical Sciences, University of Auckland, Private Bag 92019, Auckland
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1142, New Zealand
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* Correspondence, email: fzhu5@yahoo.com
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Highlights
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Quinoa starch granules are very small (1 to 3 m) with low amylose contents
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Quinoa starch modification has great potential for Pickering emulsion application
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Comparative analysis between quinoa starch and other starch sources conducted
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Abstract
Quinoa (Chenopodium quinoa Willd.) has gained popularity worldwide due to the
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attractive nutritional profile. It also has much potential for food security due to the
great genetic diversity. Starch is the main component of quinoa grain and makes up to
70% of the dry matter. The starch plays a crucial role in the functional properties of
quinoa and related food products. The starch granules are rather small (~13 m) with
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relatively low amylose contents as compared with most of the other starches. Quinoa
amylopectin has a significant amount of short chains and super-long chains. These
unique features have generated research interest in using the starch for food and other
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physicochemical properties, modifications, and applications of quinoa starch. It
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becomes obvious that this starch has great potential for food and nonfood
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applications.
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Keywords: Chenopodium quinoa; small granule; pseudocereal; starch modification;
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Pickering emulsion; starch digestion
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1. Introduction
Quinoa (Chenopodium quinoa Willd.) of the Chenopodiceae family is native to the
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Andes, and has been cultivated in the Andean Region for several thousand years
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(Taylor & Parker, 2002; Fleming & Galwey, 1995). Before the Spanish colonization
of South America, quinoa had been widely grown as a staple grain crop for its edible
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experience a renaissance within South America, not only for domestic consumption
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but also for export (Fleming & Galwey, 1995). Quinoa cultivation is in the process of
rapid expansion outside its traditional cultivated areas with good yields (FAOSTAT,
2017; Wang & Zhu, 2016). World production of quinoa has kept increasing in the
period of 19922014, exceeding 192 thousand metric tons in 2014 (FAOSTAT, 2017).
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Quinoa plays a significant role in food security for its broad genetic diversity and an
It can grow from sea level to 4000 meters above sea level, at humidity ranging from
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environments with low input costs (Jacobsen, 2003). The above-mentioned
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characteristics make quinoa a strategic crop for providing nutrition and food security
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in the face of climate change (Ruiz et al., 2013). The genome of quinoa has been
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recently sequenced, providing the genetic basis for the improvements in agricultural
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traits and food processing properties of this crop (Jarvis et al., 2017). Quinoa seeds
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come in a variety of colors ranging from white to red and black (Vega-Galvez et al.,
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In recent years, there has been renewed interest in quinoa due to its attractive
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nutritional features. The seed is a source of starch, protein, dietary fiber, fat, minerals,
Valencia, & Nair, 1993; Vega-Galvez et al., 2010). It contains no gluten and can be a
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gluten-free alternative for persons with celiac disease (Alvarez-Jubete, Arendt, &
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Gallagher, 2010).
The major component of quinoa seed is starch, which varies from ~30 to 70% of the
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dry matter (Supplementary Table 1). The quality of quinoa food products can be much
affected by the properties of the starch (Wang, Opassathavorn, & Zhu, 2015b). Recent
research has shown that quinoa starch can be an ingredient for food and non-food
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applications (Wang et al., 2015b; Wang & Zhu, 2016). Compared with other starches
from maize, potato, and wheat, there is a lack of systematic knowledge of quinoa
starch. This limits the further development of this crop and the utilization of the
starch. This review summarizes the present knowledge of the isolation, composition,
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uses of quinoa starch. Suggestions for the direction to improve the understanding and
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utilization of this starch are provided.
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2. Isolation of quinoa starch
Various milling and soaking approaches have been applied to remove the non-starch
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components. The seeds were washed and steeped in water or alkaline solutions before
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homogenizing in a blender (Araujo-Farro, Podadera, Sobral, & Menegalli, 2010;
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Wright, Huber, Fairbanks, & Huber, 2002). Alternatively, the seeds were dry-milled
into flour before soaking in solutions (Li, Wang, & Zhu, 2016; Mundigler, 1998;
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Watanabe, Peng, Tang, & Mitsunaga, 2007). It should be noted that too harsh dry-
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milling conditions may induce damages to starch granules (Li & Zhu, 2017c; Qian &
Kuhn, 1999). The solution used to soak the seeds or flour could be deionized water or
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(SDS), or sodium acetate to remove the other components such as protein, lipid,
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saponins, and fibers (Atwell, Patrick, Johnson, & Glass, 1983; Li et al., 2016;
effective in starch purification but the cost is high, which may not be suitable for large
sample preparation. The soaking time varied from 5 min to 1 week among different
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studies (Atwell et al., 1983; Steffolani, Len, & Prez, 2013). Long soaking may give
rise to microbial issues, whereas the altered pH may induce damage to starch granules
After soaking, the suspension was filtered and the starch in filtrate was recovered by
centrifuge. High centrifugation speed (> 2000 g) was applied to increase the
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recovery of starch due to the small granule size (Li et al., 2016; Lindeboom, Chang,
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Falk, & Tyler, 2005b; Steffolani et al., 2013).
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The starch cake was re-suspended in water to further remove the non-starch
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components and chemical reagents added. It should be noted that residue of the
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reagents, if not washed off probably, may affect the physicochemical properties of
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starch such as enzyme susceptibility (Zhang & Hamaker, 1999).
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The starch yield was in range of 3053.3% (Jan, Panesar, Rana, & Singh, 2017;
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Wright et al., 2002). The purity was from 93% to 99% (Jan et al., 2017; Mundigler,
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1998; Srichuwong et al., 2017). The quinoa starch isolations were mainly carried out
starch.
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Starch is mainly composed of two kinds of biopolymers: the linear amylose and the
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branched amylopectin (Prez & Bertoft, 2010). The amylose contents of quinoa starch
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exclusion chromatography (SEC) (Table 1). Amylose content estimated by iodine
binding-based methods ranged from 0.3% to 27.7% (Table 1). It is notable that the
significantly lower (7.1%) than that calculated from the whole starch (25.4%) (Tang,
Watanabe, & Mitsunaga, 2002). Such a difference could be due to the long-chain
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fraction of quinoa amylopectin also complex with iodine, causing an overestimation
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of amylose content (Tang et al., 2002; Vilaplana, Hasjim, & Gilbert, 2012). The lipids
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of starch granules may affect the amylose content measured by iodine-binding based
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method by forming amylose-lipid inclusion complexes (Srichuwong & Jane, 2007).
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Thus, the iodine binding method should be with other method for the estimation of
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amylose content in quinoa starch.
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The amylose contents estimated from SEC of whole starch were 410.9% (Table 1).
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The values seem to be lower than those estimated by SEC of debranched whole starch
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which ranged from 3.5 to 27.0% (Table 1). The presence of long unit chains of
amylopectin may affect the amylose content estimated from debranched whole starch
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The Con A binding based method has been also used for quantifying the amylose
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content of quinoa starch (Gibson, Solah, & McCleary, 1997). Only the branched
Merrick, 1965). Apart from amylopectin, branched amylose may also get precipitated
in this process. Although the amylose content estimated by this method has been
reported as high as 19.7%, the majority of the studies reported a value of less than
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10% (Table 1). The lower amylose content estimated by this method may due to the
over-estimation in the value from the iodine binding and SEC of debranched whole
precipitation.
The isolated starch contains minor components such as protein, lipid, ash, and fiber
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(Table 1). The majorities of the studies reported the values of the minor components
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being less than 0.5% (Table 1). High contents of minor components suggest an
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insufficient purification of starch. It should be borne in mind that these minor
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components, though small in quantity, may have effects on the functional properties
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Table 1. Chemical composition of quinoa starch
Amylose content Ash Lipid Fiber
No. Method A
Protein (%) Reference
(%) (%) (%) (%)
18 Iodine-SP 14.3327.66 de Briceo & Briceo, 1980
1 Iodine-SP 11 0.11 0.04 Atwell et al., 1983
Iodine-SP &
1 20 B, 4 C Praznik et al., 1999
SEC
19.820.6 D,
2 Iodine-SP Wright et al., 2002
20.621.0 E
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1 Iodine-SP 25.4 F, 7.1 G Tang et al., 2002
Ando et al., 2002; Tari et al.,
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1H Iodine-SP 11.123.9
2003; Araujo-Farro et al., 2010a
8 Iodine-SP 0.312.1 Lindeboom et al., 2005b
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26 Iodine-SP 7.725.7 Li et al., 2016
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2 Iodine-SP 9.4612.1 0.890.95 0.180.22 0.320.40 0.100.13 Jan et al., 2017
1 Iodine-PT 9.28 0.91 0.11 Lorenz, 1990
Qian & Kuhn, 1999; Linsberger-
1 H
Con A 8.2512.2
A: concanavalin A precipitation based method; A: amylose content (%) is based on starch content; B:
amylose content determined calorimetrically by whole starch solution; C: amylose content determined
by SEC method; D: un-defatted starch sample; E: defatted starch sample; F: amylose content calculated
by: 100%BV(whole starch)/BV(amylose); G: amylose content calculated by: 100% [BV(starch)
BV(amylopectin)]/[BV(amylose)BV(amylopectin)]; H: Number of samples applied for each literature
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4. Structure of quinoa starch
4.1.Morphology
(SEM), transmission electron microscopy (TEM), Coulter Counter (CC), and laser
light diffraction (LLD) have been employed to study the morphology of quinoa starch
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granules (Supplementary Table 2). The individual starch granules could be released
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during the isolation process (Atwell et al., 1983; Qian & Kuhn, 1999). The size of
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quinoa granule was mostly in the range of 0.42.0 m, which was smaller than that of
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most starches from other botanical origins (Supplementary Table 2). The shape of
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quinoa starch was polygonal, angular, and irregular. The diversities in both the shape
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and size of single quinoa starch granule is relatively small (Lindeboom, Chang, &
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Tyler, 2004; Li & Zhu, 2017a). Light microscopy, limited in the resolution capacity,
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should not be used to study the details of quinoa starch granules. TEM analysis
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showed that quinoa starch granule had a homogeneous outer layer with high density
and a hilum with low density (Supplementary Fig. 2) (Tang et al., 2002).
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Quinoa starch may present as aggregations (Supplementary Table 2). These spherical
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single starch granules (Fig. 1) (Ando et al., 2002; Lorenz, 1990; Ruales & Nair, 1994;
Srichuwong et al., 2017). It should be noted that these aggregates may give rise to the
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artefacts of granule size distribution data. The formation of these aggregates may be
largely due to the presence of protein as adding pepsin facilitated their dissolution
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A B
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Figure 1. SEM photos showing aggregates (A) and starch granules (B) in quinoa
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perisperms (A: Magnification: 5,000, sample from Peru; B: Magnification:
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30,000, sample from South America) (Srichuwong et al., 2017; Li & Zhu, 2017a)
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E PT
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4.2. Crystallinity
Quinoa starch has an A-type polymorph (Supplementary Table 3). The degree of
The value from peak fitting method (the area ratio between crystalline peak and total
peak) appeared to be higher than those calculated from the ratio of crystalline area
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(separated by a smooth line in spectrum) and total areas. The degree of crystallinity of
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quinoa starch has been reported to be lower than amaranth, garden orache, and normal
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maize starches and higher than barley, adzuki, and kaiwa starches (Qian & Kuhn,
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1999; Steffolani et al., 2013; Tang et al., 2002; Wright et al., 2002). Such differences
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may be due to the differences in the chemical structure and composition of starches
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(Prez & Bertoft, 2010). The quinoa starch has been reported to have a significant
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amount of Afp-chains which could contribute to the defects in crystalline lamella and
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contribute to the low crystallinity in quinoa starch. The peak around 0.44 nm (d-
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This peak is not significant for quinoa starch, indicating quinoa starch had a low level
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The nature of quinoa starch crystallinity can be probed by techniques other than XRD,
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Table 2. Chemical structure of quinoa starch, amylose, and amylopectin
Sample type No. max (nm) BV DP CL NC Molecular mass Analytical method Reference
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Whole starch 1 27 Debranched whole starch on GPC (Bio-Gel P-10) Atwell et al., 1983
AM: 595604,
A
Whole starch 1 Whole starch on GPC (Sepharose CL-2B) Ruales & Nair, 1994
AP:575
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Whole starch 4 587596 0.320.41 Iodine absorption spectrum Inouchi et al., 1999
4,600
Iodine absorption spectrum; whole starch on SEC
Whole starch 1 161,000, Mw: 1.13107 Praznik et al., 1999
ED system
DPw: 70,000
0.287 Tang et al., 2002; Ando
Whole starch 1A 602609 Iodine absorption spectrum
0.305 et al., 2002
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AM:601621, Whole starch on GPC (Sepharose CL-2B);
Whole starch 9 Li & Zhu, 2017b
AP:581608 debranched whole starch on GPC (Sepharose CL-6B)
Amylopectin 4 Debranched AP analyzed by HPAEC-PAD Inouchi et al., 1999
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No.: number of samples studied; max: the wavelength with the maximum absorbance; BV: blue value; DP: degree of polymerization; DPw: weight-average degree of
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polymerization; DPn: number-average degree of polymerization; CL: average chain length; NC: number of chains per molecule; Mw: weight-average molecular mass; Mn:
number-average molecular mass; AM: amylose fraction; AP: amylopectin fraction; GPC: gel-permeation chromatography; SEC: size-exclusion chromatography; HPAEC-
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PAD: high-performance anion-exchange chromatography with pulsed amperometric detection; FACE: fluorophore-assisted capillary electrophoresis; A: Number of samples
applied for each literature.
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E PT
CC
A
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4.3.Chemical structure
4.3.1. Starch
researchers (Table 2). Blue value (BV) is defined as the absorption value of a light
with the wavelength of 680 nm when passing through a cell containing a mixture of
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starch (Bourne, Haworth, Macey, & Peat, 1948). Both BV and max of a starch
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solution increase with increasing degree of polymerization (DP) of the linear glucan
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molecules (Bailey & Whelan, 1961). Among different reports, max and BV of quinoa
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starch have been reported in the range of 578609 nm and 0.2870.41, respectively
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(Table 2). However, the approach appeared to be spurious as the starch is a mixture of
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amylose and amylopectin.
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4.3.2. Amylose
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Iodine absorption spectrum (IBS) and SEC have been used to study the structure of
quinoa amylose (Table 2). BV and max of isolated quinoa amylose ranged from
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0.9981.101 and 648663 nm, respectively (Tang et al., 2002; Watanabe et al., 2007).
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max has been also estimated in the amylose fraction from the SEC of quinoa starch,
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which ranged from 595621 nm (Li & Zhu, 2017b; Ruales & Nair, 1994). A
comparative study showed that BV of quinoa amylose was significantly lower than
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that of barley and adzuki starch, which could be due to their differences in the
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Quinoa amylose had lower number-based degree of polymerization (DPnAM) and
average chain length (CLAM) than barley and adzuki amyloses and more number of
chains per amylose molecule (NCAM) than barley and adzuki amyloses (Tang et al.,
2002; Watanabe et al., 2007). A SEC study revealed a lower ratio of long-chain
amylose to short-chain amylose of quinoa starch than normal maize starch (Li & Zhu;
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2017b). Quinoa amylose appeared to be smaller with more branches, which explained
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its lower BV value (Tang et al., 2002; Watanabe et al., 2007).
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A
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E PT
CC
A
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A B
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10 6
Weight-based carbohydrate content
A
Molar-based carbohydrate content
5 Weight-based carbohydrate content
8 Molar-based carbohydrate content
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4
Carbohydrate content (%)
4
ED 2
2 1
PT
0
0
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-1
0 10 20 30 40 50 60 70 80 90 0 10 20 30 40 50 60 70 80 90
CC
Figure 2. Weight- and molar-based unit chain length distributions of typical quinoa amylopectin (A) and the ,-LDs (B) (sample S21). The
carbohydrate content (%) is calculated based on the total weight of carbohydrate (weight-based carbohydrate content, empty dots) or total molar
amount (molar-based carbohydrate content, solid dots) (Li & Zhu, 2017b).
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4.3.3. Amylopectin
Both the max and BV of quinoa amylopectin were significantly higher than those of
barley and adzuki amylopectins (Tang et al., 2002). DPnAP, CLAP, and NCAP of quinoa
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amylopectin appeared to be between those of barley and adzuki amylopectins (Tang et
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al., 2002).
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Super-long unit chains have been observed in quinoa amylopectin through SEC of the
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debranched amylopectin with contents between 13 and 19% (Tang et al., 2002;
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Watanabe et al., 2007). The high amount of these super-long chains may explain the
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high max and BV values of quinoa amylopectin. It may also explain the great
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starch based methods and those by Con A or SEC of whole starch based method as
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discussed above. The structure and function of these large-amount super-long chains
assisted capillary electrophoresis (FACE) (Fig. 2) (Li & Zhu, 2017b; Srichuwong et
al., 2017; Zhu, Corke, & Bertoft, 2011). A large amount of short unit chains with DP <
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12 and a shoulder of the HPAEC chromatogram at around DP 1820 were recorded
(Li & Zhu, 2017b; Srichuwong et al., 2017). Quinoa amylopectin had higher amounts
of short unit chains with DP < 12 and lower amounts of chains with DP of 1335 than
waxy maize starch (Inouchi et al., 1999). The ratio between short and long chains of
quinoa amylopectin tended to be higher than those of amylopectins from other sources
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(Bertoft, Piyachomkwan, Chatakanonda, & Sriroth, 2008; Li & Zhu, 2017b).
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The average chain length of quinoa amylopectins (CLAP) (9 varieties) estimated by
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HPAEC-PAD ranged from 1617 glucosyl residues, which were shorter than those
SC
quantified by using SEC (1821 glucosyl residues) (Li & Zhu, 2017b; Tang et al.,
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2002; Watanabe et al., 2007). Such a difference could be readily attributed to the
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different analytical methods used in different studies. Quinoa CLAP was shorter than
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that of most of the amylopectins from other sources except for oat amylopectin as
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estimated by the same analytical method (Bertoft et al., 2008; Li & Zhu, 2017b).
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,-LDs) (Bertoft, 2004). The amount of carbohydrate removed during the enzymatic
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hydrolysis is termed -limit value or ,-limit value (Bertoft, 2004). The -limit value
CC
of quinoa amylopectin (1 variety) has been reported to be 59% (Ando et al., 2002).
Another study showed that ,-limit values for quinoa amylopectins were between
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52.7 to 56.4% (Li & Zhu, 2017b). The varieties could coming from different
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length profile of quinoa amylopectin had a shoulder at DP 57 and two peaks at DP
External chain length (ECL) and internal chain length (ICL) of quinoa amylopectins
were shorter than those of amylopectins from several of A-type starches (e.g., waxy
maize starch) and most of B- and C-type starches (e.g., potato starch) (Bertoft et al.,
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2008; Li & Zhu, 2017b). Bertoft et al. (2008) categoried amylopectins into 4 groups
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based on the internal unit chain profiles. Group 1 amylopectins had the highest
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amount of short internal unit chains and the lowest amount of long internal unit
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chains. Group 4 amylopectins had just the opposite compositional pattern. Group 2
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and 3 amylopectins were intermediate between group 1 and 4 samples (Bertoft et al.,
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2008). Quinoa amylopectin shared a lot of similarities with both the group 1 and
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group 2 amylopectins, though it did not strictly fit into any group (Bertoft et al.,
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2008).
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The unit chains in amylopectin could be classified as A-chains which do not carry
other chains, B-chains which carry other chains, and C-chain which has the sole
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reducing end (Peat, Whelan, & Thomas, 1952). The amount of A-chains can be
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accurately evaluated from the ,-LDs where all the A-chains are maltose stubs
CC
ranged between 46.4 to 50.1% (Li & Zhu, 2017b). A portion of A-chains (DP 68) is
A
(Bertoft, 2004). The molar percentages of Afp in quinoa amylopectins has been found
to be higher than that of most of other amylopectins estimated by Bertoft et al. (2008).
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Therefore, the unit chain profile of quinoa amylopectin appeared to be rather unique
the molar ratio between the short and long unit chains, which ranged between 10 to
16.6 (Li & Zhu, 2017b; Tang et al., 2002; Watanabe et al., 2007). However, the
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accurate cluster structure could only be estimated from the isolated clusters which
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were well illustrated in many occasions by Bertoft and co-workers (Bertoft, 2013).
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The future work would be to apply this analytical approach to include quinoa
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amylopectin.
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Table 3. Gelatinization properties of quinoa starch
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Starch Scanning rate Scanning
No. Instrument To (oC) Tp (oC) Tc (oC) H (J/g) A Reference
concentration (oC/min) range (oC)
N
Atwell et al., 1983; Tang et
10.316.7
1 DSC 3240% (w/w) 5 50.654.5 60.662.6 66.071.3 al., 2002; Srichuwong et al.,
A
J/g
2017
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1 DSC 21% (w/w) 10 30120 59.9 64.5 71 1.66 Qian & Kuhn, 1999
4 DSC 33% (w/w) 52.257.4 54.261.9 67.668.5 7.310.5 Inouchi et al., 1999
2 DSC
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21% (w/w) 10 20120 51.451.8 55.756.1 64.364.5 12.6 Wright et al., 2002
3 DSC 25% (w/w) 10 25120 54.2555.72 61.6663.01 8.459.00 Steffolani et al., 2013
26 DSC 25% (w/w) 10 2590 50.158.3 56.265.0 65.874.9 10.814.4 Li et al., 2016
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2 DSC 30% (w/w) 10 10120 64.3266.61 69.3671.56 75.7876.98 4.345.10 Jan et al., 2017
CC
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A
CC
EPT
ED
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A
N
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SC
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5.1.Gelatinization measured by DSC and microscopy
Kofler hot-stage setting) were used to study the gelatinization properties of quinoa
DSC (e.g., starch concentration and heating rate) make the results among different
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studies difficult for comparison (Zhu, 2015). Variations in gelatinization properties
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were observed within the same study (Inouchi et al., 1999; Jan et al., 2017; Li et al.,
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2016; Lindeboom et al., 2005b). For example, Li et al. (2016) revealed that Tp and H
SC
of 26 quinoa starch samples ranged from 56.265.0 oC and 10.814.4 J/g,
respectively.
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Comparative studies showed that the gelatinization temperatures of quinoa starch
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were lower than those of amaranth, maize, garden orach, adzuki, kaiwa, sorghum,
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millet, and wheat starches, and were similar to those of barley starch. H of quinoa
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starch was lower than that of amaranth, maize, and adzuki starches, were similar to
that of garden orach, kaiwa, and sorghum starches, and were higher than that of
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barley and wheat starches (Inouchi et al., 1999; Qian & Kuhn, 1999; Srichuwong et
E
al., 2017; Steffolani et al., 2013; Tang et al., 2002; Wright et al., 2002). Such
CC
the differences in starch composition and structure (Srichuwong & Jane, 2007;
A
Correlation analysis shows that the gelatinization temperatures and H were closely
correlated with the fine structure of amylopectin (Li & Zhu, 2017a; Srichuwong et al.,
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2017). For example, the high amount of short unit chains, especially the Afp-chains,
and low amounts of long unit chains in quinoa amylopectin may provide an
explanation for the low gelatinization temperatures of quinoa starch (Li & Zhu,
2017a).
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endothermic process occurring around 100 oC. Tang et al. (2002) showed that the H
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for amylose-lipid inclusion complexes in quinoa starch was lower than that in barley
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and adzuki starches. Wright et al. (2002) found no endothermic process for the
SC
amylose-lipid complexes of quinoa starch. These reports suggested that the level of
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amylose-lipid complex in quinoa starch was quite low, which agreed with the XRD
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results (Section 4.2).
A
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During starch gelatinization process, the extents of granule swelling and the release of
soluble material are usually monitored by the swelling and solubility tests. The
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starches are heated at various temperatures. The solubilized and undissolved materials
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are separated and weighted, from which the swelling power (SP), water solubility
CC
index (WSI), and swelling factor (SF) could be calculated (Supplementary Table 4).
The increasing SP toward high temperature suggested that quinoa starch granules
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could better maintain their integrity under heating than some other starches such as
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condition, stirring, and separation method could impact on the results, which makes
The SP and WSI of quinoa starch were negatively correlated with the amylose
content, suggesting amylose could restrict the swelling of starch granules (Li et al.,
2016; Lindeboom et al., 2005b). The SP at low temperatures (i.e., 55 oC) was
T
correlated with the amylopectin structural parameters such as Afp and the ratio of
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short-to-long chains, whereas the SP and WSI at higher temperatures (e.g., 95 oC) and
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AML was more related to the internal structure of quinoa amylopectins such as the
SC
molar amounts of B-chain categories (Li & Zhu, 2017a). These results suggested the
U
roles of diverse chain categories in the swelling properties of starch as reviewed
N
previously (Srichuwong & Jane, 2007; Vamadevan & Bertoft, 2015).
A
M
5.3.Rheological properties
ED
5.3.1. Pasting
(RVA), Brabender viscograph (BV), and rheometer equipped with a starch cell
E
(Supplementary Table 5). Within the same study, great variations in pasting properties
CC
were observed among different quinoa samples (Supplementary Table 5). This could
due to the high diversities in composition as well as the molecular and granular
A
structure of quinoa starch. In comparative studies, the PV of quinoa starch was higher
than that of most other starches such as waxy maize, wheat, millet, buckwheat, garden
orach, kaiwa, white sorghum, amaranth, and red sorghum starch (Praznik et al.,
25
1999; Qian & Kuhn, 1999; Srichuwong et al., 2017; Steffolani et al., 2013; Wright et
al., 2002). The high PV of quinoa starch corresponded well with the high SP as
described in Section 5.2. PV has been found positively correlated with the amounts of
amylose and long chain fraction of amylopectin. This may be due to the long glucan
chains restricting the swelling and improving the ability for granules to maintain their
T
structure (Li et al., 2016; Li & Zhu, 2017b). In contrast, opposite correlation pattern
IP
between PV and amylose was also reported (Lindeboom et al., 2005b). Another study
R
revealed a parabolic relationship between PV and amylose content (Srichuwong et al.,
SC
2017). These conflicting results indicated the relationship between PV and amylose
U
content is complicated. Other factors such as granule size, super-long chains in
N
amylopectin, and the presence of ghost structure may also contribute to the high PV
A
Small deformation oscillatory and shear-stability tests were applied on quinoa starch
(Jan et al., 2017; Lindeboom et al., 2005b; Praznik et al., 1999). The shear-stability of
PT
quinoa starch was higher than that of amaranth, waxy maize, millet, and buckwheat
E
starches, and was similar to that of wheat starch (Praznik et al., 1999). The high shear-
CC
stability of quinoa starch gel agreed with previous discussions on SP and pasting
behaviors. The shear-stability of quinoa starch was positively correlated with amylose
A
26
5.4. Retrogradation
The retrogradation of quinoa starch has been monitored by several approaches (DSC,
6 & 7).
T
5.4.1. Amylopectin re-crystallization measured by DSC
IP
The amylopectin re-crystallization was monitored by DSC (Supplementary Table 6).
R
The starch retrogradation is significantly affected by the water content and storage
SC
conditions. The comparison of results of different studies may be meaningless (Wang,
U
Li, Copeland, Niu, & Wang, 2015a). The retrogradation percentage (R%, the
N
percentage ratio between the enthalpy change of retrogradation and gelatinization) of
A
quinoa starch was lower than that of kaiwa, sorghum, millet, maize, and wheat
M
starches, and was higher than that of amaranth starch (Srichuwong et al., 2017;
ED
correlated with long unit chains of DP 1324 (Srichuwong et al., 2017). The possible
E
reason for the low R% in quinoa starch could be due to the short ECL of quinoa
CC
amylopectin retarding the formation of double helical structure (Li & Zhu, 2017b).
A
Texture profile analysis (TPA) has been used to study the retrogradation of quinoa
starch (Supplementary Table 7). Hardness (HD) of quinoa starch was much lower than
27
that of kaiwa starch under the same conditions (Steffolani et al., 2013). Positive
correlations between amylose content and HD of quinoa starch gel have been
observed (Li et al., 2016; Steffolani et al., 2013). These confirm the central role of
amylose in starch gelation. Quinoa amylose is short in average chain length and
highly branched as discussed above, which could have impacts on the gel texture. The
T
texture properties of quinoa starch may also be affected by the amylopectin internal
IP
structure. For example, the ratio between short and long B-chains of ,-LDs of
R
quinoa amylopectins (9 samples) was negatively correlated with HD and positively
SC
correlated with adhesiveness (AD) (Li & Zhu, 2017a). As discussed above, the quinoa
U
amylopectin has a significant amount of super-long chains. These super-long chains
N
may also contribute to the starch gel texture (Tang et al., 2002; Watanabe et al., 2007).
A
M
5.4.3. Turbidity
ED
The changes in turbidity or clarity of starch gel could be used to reflect the
retrogradation process. The quinoa starch gel with less amylose showed lower
PT
turbidity (Jan et al., 2017). Like the other aspects of retrogradation, the turbidity can
E
amylopectin, and minor components which could mask the inherent turbidity of starch
A
28
As retrogradation progresses, water is expelled from starch gel due to recrystallization
water separated from storing the gel at low temperature (e.g., 4 oC) or from the freeze-
thaw process. The gel concentration, thermal history, and centrifugation settings could
significantly impact on the syneresis of starch gel (Zhu, 2015). Lindeboom et al.
T
(2005b) found diversities in freeze-thaw stability of 8 quinoa starch with the syneresis
IP
after the first cycle ranging from 035%. Therefore, good freeze-thaw stability of
R
quinoa starch gel can be achieved by selecting suitable quinoa variety. No correlations
SC
have been found between the freeze-thaw stability and amylose content of quinoa
U
starch, while the correlations between the syneresis or freezethaw stability and
N
amylopectin structure are yet to be studied (Ahamed, Singhal, Kulkarni, & Pal,
A
5.5.Enzyme susceptibility
Different studies used various approaches (source and category of enzyme, buffer
PT
quinoa starch (Supplementary Table 8). Quinoa starch appeared to have higher
CC
enzyme susceptibility than most of the other starches such as barley, adzuki, maize,
millet, wheat, and sorghum starches (Inouchi et al., 1999; Srichuwong et al., 2017;
A
The high specific surface area of quinoa starch has been suggested as the main reason
for the high enzyme susceptibility (Inouchi et al., 1999; Li et al., 2016; Srichuwong et
29
al., 2017; Tang et al., 2002). Lorenz (1990) suggested that the enzyme susceptibility
of quinoa starch was negatively correlated with the amylose content. Thus the
amylose may reduce the enzyme susceptibility at an earlier stage of hydrolysis. The
T
negatively correlated with CLAP (Li & Zhu, 2017a). This is due to the short unit
IP
chains of amylopectin such as Afp-chains are too short to form double helices and
R
cause defects in the crystalline structure, making it more susceptible to the enzyme
SC
attack (Vamadevan & Bertoft, 2015). The hydrolysis extent of quinoa starch after 24 h
U
was positively correlated with the molar amount of A-chains which are assumed to
N
forming the crystalline lamellae (Acrystal) (Li & Zhu, 2017a). This might suggest that the
A
the digestible starch is more related to the amount of chains forming crystalline
ED
region.
PT
In recent years, there has been increased interest in quinoa starch for various food
CC
applications (Supplementary Table 9). Both native and modified starches were used
described below.
30
6.1.1. Film
The native quinoa starch was blended with low-density polyethylene (LDPE) as
biodegradable fillers (Ahamed, Singhal, Kulkarni, Kale, & Pal, 1996a). Quinoa starch
based films were prepared with glycerolat various pH and drying conditions (Araujo-
Farro et al., 2010). The optimized conditions for film preparation were obtained as
T
21.2% of glycerol, pH 10.7, and drying at 36 oC for 14 h (Araujo-Farro et al., 2010).
IP
The film was colorless and had better mechanical properties and barrier properties
R
than the films made from maize starch, yam starch, and amaranth flour (Araujo-Farro
SC
et al., 2010).
U
Quinoa starch was also used to manufacture active biofilms with gold nanoparticles
N
(AuNPs) (Pagno et al., 2015). The addition of AuNPs increased the tensile strength
A
and UV absorption while decreasing the solubility of the resulting films, which is
M
desired for food packaging and coating. Moreover, the biofilms have been found
ED
having a good thermal stability and antimicrobial activity with great potential for
Starch based films and coatings have attracted much attentions in food industry for
E
the environmental compatibility (Jimnez, Fabra, Talens, & Chiralt, 2012). The
CC
31
Food ingredients can be encapsulated by various starch based systems at micro- or
nano-scales for controlled delivery (Zhu, 2017). The native quinoa starch granules
have been used as wall material to entrap vanillin (Tari, Annapure, Singhal, &
Kulkarni, 2003; Tari & Singhal, 2002). It seemed that the amylose content was
positively correlated with the encapsulation capacity of the starches, though the exact
T
reasons remain to the analysed (Tari & Singhal, 2002; Tari et al., 2003).
IP
6.2. Chemically-modified starch
R
Quinoa starch has been modified by octenyl succinic anhydride (OSA) to various
SC
degrees of substitution for stabilizing Pickering emulsions (Supplementary Table 9).
U
N
6.2.1. Preparation of OSA-modified starch
A
The preparation and functional properties of OSA-modified starches have been well
M
reviewed previously (Sweedman Tizzotti, Schfer, & Gilbert, 2013). Briefly, native
ED
quinoa starch was suspended in water with the addition of certain amounts of OSA.
The pH of solution was maintained at 7.47.9 and the reaction was completed when
PT
the pH reached a constant value (Rayner, Sj, Timgren, & Dejmek, 2012a; Timgren,
E
Rayner, Dejmek, Marku, & Sj, 2013). The OSA-modified quinoa starch was
CC
32
The OSA-modified quinoa starch has increased hydrophobicity, which is suitable for
mixed thoroughly with water phase and oil phase. The mixture was emulsified in a
high-shear mixer (Matos, Timgren, Sj, Dejmek, & Rayner, 2013; Timgren et al.,
2013).
T
Matos et al. (2013) prepared a Pickering double emulsion (W1/O/W2) stabilized by
IP
OSA-modified quinoa starch granules. A water-in-oil emulsion (W1/O) was prepared
R
first and then emulsified with W2 phase in the presence of OSA-modified quinoa
SC
starch (Matos et al., 2013).
U
N
6.2.3. Characteristics of Pickering emulsions stablished by OSA-modified starch
A
The particle size of Pickering emulsions decreased with increasing amounts of added
M
starch (Rayner, Timgren, Sj, & Dejmek, 2012b). Rheological analysis showed that
ED
the linear viscoelastic region of emulsion was in a short range of 0.0001 to 0.002,
which suggests low shear resistance (Rayner et al., 2012b). The degree of OSA
PT
2012a). High ionic strength of buffer could narrow the size distribution of emulsions
CC
(Rayner et al., 2012a; Timgren et al., (2013). The Pickering emulsion formed by
For the Pickering double emulsions, the average size of inner particles was 3.1 m,
whereas the size of the droplets stabilized by starch granules showed a mean diameter
33
of 33 m (Matos et al., 2013). The majority of the encapsulated oils (90%) remained
Both the Pickering emulsion and Pickering double emulsion systems were employed
to produce powders with high oil contents (> 70%) through freeze-drying (Marefati,
Rayner, Timgren, Dejmek, & Sj, 2013; Marefati, Sj, Timgren, Dejmek, &
T
Rayner, 2015).
IP
The oil properties, especially the melting temperature, may impact on the stability of
R
emulsions during freeze-drying (Marefati et al., 2015). The partially-gelatinized OSA-
SC
modified quinoa starch gave the emulsion higher stability against the freeze-thaw
U
process than the non-heat treated starch (Marefati et al., 2013; Marefati et al., 2015).
N
The dual modification of H2SO4 and OSA increased the emulsion capacity of quinoa
A
starch (Saari, Heravifar, Rayner, Wahlgren, and Sj, 2016). Matos, Marefati,
M
Gutirrez, Wahlgren, & Rayner (2016) showed that the emulsion formed by OSA-
ED
modified quinoa starch in non-granular form was less stable than that by OSA-
34
T
R IP
SC
U
N
A
M
ED
E PT
CC
without (a, c, e) and with heat treatment (b, d, f) as observed by light microscopy
A
(ad) and SEM (e, f) (Marefati, Bertrand, Sj, Dejmek, & Rayner, 2017)
35
OSA-modified starches have been commonly used for the encapsulation of functional
food ingredients (Zhu, 2017). Curcumin has been encapsulated by a heated emulsion
successful delivery of this bioactive to the large intestine (Fig. 3) (Marefati et al.,
T
2017). Overall, the Pickering emulsions stabilized by OSA-modified quinoa starch
IP
granules appeared to have potential in novel formulations of food products,
R
pharmaceutical drugs, and cosmetics (Rayner 2012a; Marefati et al., 2013).
SC
6.3. Physically-modified starch
U
N
Dry-heating was used to modify the hydrophobicity of quinoa starch (Rayner et al.,
A
2012a; Timgren et al., 2013) (Supplementary Table 9). However, the emulsion
M
capacity of heat-treated starch was less efficient than OSA-modified quinoa starch
ED
Quinoa starch was modified by high hydrostatic pressure (HHP) up to 600 MPa at
PT
different conditions (Li & Zhu, 2018; Linsberger-Martin et al., 2012). The quinoa
E
starch has been found to be more sensitive to HHP treatment than maize starch (Li &
CC
Zhu, 2018). Resistant starch (RS) content of HHP-treated quinoa starch was increased
choosing correct processing techniques and conditions may improve the quality of
36
7. Conclusions
Quinoa starch is small in granule size (~12 m) with A-type polymorph. The
T
short chains and branches. Apart from the genetics, the amylose content of quinoa
IP
starch can be affected by the presence of super-long chains in amylopectin. Quinoa
R
amylopectin is abundant in short unit chains (e.g., Afp-chains) and lack of long chains
SC
as compared with other kinds of amylopectins. The amylopectin structure gives
U
quinoa starch several special physicochemical properties such as low gelatinization
N
temperatures and slow retrogradation. The quinoa starch showed high SP and PV
A
during pasting event with a degree of resistance to shearing. There has been
M
increasing interest in using quinoa starch for food and nonfood applications. Native
ED
quinoa starch has been used in biofilm production and in microencapsulation of food
ingredients (e.g., oils) for its small granule size. The OSA-modified quinoa starch was
PT
showed several promising properties such as high emulsifying efficiency and stability.
CC
Physical modifications such as HHP has been applied on quinoa starch to obtain
Compared with the starches isolated from major crops such as maize and potato,
research on both structure and applications of quinoa starch is still limited. Quinoa has
37
diversity. The diversity in starch properties remains to be studied by assessing the
the cluster structure of quinoa amylopectin are still unknown. Although many studies
reported the quinoa starch properties, the different experimental settings used by
T
the methods can improve this common issue that existed in our starch research
IP
community. The modifications and uses of quinoa starch remain much less
R
investigated. Several commonly used modifications such as ultrasound, annealing,
SC
cross-linking, and dual modifications could be applied on quinoa starch in the future.
U
Native and modified quinoa starches with promising properties could have application
N
potential such as fat replacement, novel food additives, pharmaceuticals, cosmetics,
A
Acknowledgments
supported this research. The figures are reprinted with permissions from the
E
publishers.
CC
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