Accepted Manuscript

Floral origin markers for authenticating Lavandin honey (Lavandula angustifolia x

latifolia). Discrimination from Lavender honey (Lavandula latifolia)
L. Castro-Vzquez, V. Leon-Ruiz, M.E. Alaon, M.S. Prez-Coello, A.V. GonzlezPorto
PII:

S0956-7135(13)00438-6

DOI:

10.1016/j.foodcont.2013.09.003

Reference:

JFCO 3445

To appear in:

Food Control

Received Date: 7 May 2013

Revised Date:

31 August 2013

Accepted Date: 2 September 2013

Please cite this article as: Castro-VzquezL., Leon-RuizV., AlaonM.E., Prez-CoelloM.S. & GonzlezPortoA.V., Floral origin markers for authenticating Lavandin honey (Lavandula angustifolia x latifolia).
Discrimination from Lavender honey (Lavandula latifolia), Food Control (2013), doi: 10.1016/
j.foodcont.2013.09.003.
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Floral origin markers for authenticating Lavandin honey (Lavandula angustifolia x

latifolia). Discrimination from Lavender honey (Lavandula latifolia)

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L. Castro-Vzquez a , V. Leon-Ruiz b, M. E. Alaon c, M. S. Prez-Coello c, A.V.

Gonzlez-Porto b

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Food Technology Area, Faculty of Pharmacy, University of Castilla-La Mancha,

Campus Universitario, Albacete, Spain

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Marchamalo. Guadalajara, Spain.

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Beekeeping Research Centre of Marchamalo, Camino San Martn s/n. 19180.

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Campus Universitario Ciudad Real, Spain

Food Technology Area, Faculty of Chemistry, University of Castilla-La Mancha,

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AUTHOR INFORMATION

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* Corresponding author. Tel.: +34-926-295300, Fax: +34-926-295318.

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E-mail: LuciaIsabel.Castro@uclm.es

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ABSTRACT
The aim of this study was to identify the botanical origin of lavandin honey, a

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monofloral product of recent proliferation obtained from a hybrid of the species

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Lavandula angustifolia and L. latifolia. Lavandin was authenticated here in chemical,

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palynological and sensory terms, and discriminated from the more common Lavender

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honey (L. latifolia).

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A total of 14 physicochemical parameters, 26 pollen types, 13 sensory attributes

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and 80 volatile compounds were identified and/or quantified for this purpose.
High concentrations of -nonalactone, farnesol and acetovanillone, which were for

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the first time identified as components of honey aroma in this study, together with

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several lactones, dehydrovomifoliol, 4-methoxyacetophenone and decanal are proposed

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as chemical markers for authenticating lavandin monofloral honey. In sensory terms,

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increased scores for caramel and peach compote sensations, together with an also

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increased Rubus pollen content, provide additional useful information for the accurate

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authentication of lavandin honey and its discrimination from lavender honey (L.

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latifolia).

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Results showed enough floral markers to authenticate the botanical origin of

Lavandin honey allowing its marketing as monofloral rather than generic honey.

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Keywords:

Lavandin-honey;

palynological-analysis, sensory-profile.

volatile-markers,

physicochemical-parameters,

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1. Introduction
Lavender is a popular aromatic mediterranean herb belonging to Lamiaceae

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family. The genus Lavandula contains several species, although the more common

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species that is believed to have aromatherapy and pharmaceutical values are Lavandula

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dentata (French lavender), Lavandula angustifolia, Lavandula latifolia, Lavandula

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stoechas and Lavandula hybrida.

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In the beekeeping context, honey from Lavender (Lavandula latifolia), commonly

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known as spike Lavender, is currently among the most appreciated high-quality

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honeys by virtue of its pleasant aroma and taste. Although, in recent years cultivation

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of the hybrid Lavender species known as Lavandin, which is a cross between Lavandula

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angustifolia and Lavandula latifolia, has proliferated widely at the expense of Lavender

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because it has major advantages for flavouring industries (Paschalina & Apostolos,

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2003). This has been especially so in Spain, where large cropping areas of Lavandin (L.

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angustifolia x L. latifolia) have be established lately.

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When Lavender honey is commercialized, no distinction between species

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(Lavender or Lavandin) is made, however honey producers know that honey from L.

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latifolia exhibits substantial sensory differences from Lavandin honey. For this reason,

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the Spanish beekeeping industry, which is concentrated in the Alcarria region (central

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Spain), is highly interested in finding ways to differentiate these species with a view to

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characterizing and marketing Lavandin honey as a monofloral product with its own,

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identifiable features.

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The traditional approach to identifying the botanical origin of honey relies on

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examination of its pollen (Anklam, 1998; Louveaux, Maurizio, & Vorwohl, 1978;

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Soria, Gonzlez, de Lorenzo, Martnez-Castro, & Sanz, 2004). This analysis requires a

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high skill and does not ensure reliable identification if the honey concerned contains

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little or no pollen. The minimum proportion of L. latifolia pollen needed to characterize

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Lavender honey as monofloral is about 15% (La Serna Ramos, 2007; Sanz, Prada,

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Gmez-Ferreras, Lorenzo, & Jrez, 1980), which is the typical proportion for all other

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species of the family Labiatae. In honey from Lavandin, which contains few pollen

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grains, this botanical analysis is of little use. Therefore, authenticating Lavandin honey

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entails using additional analytical and physicochemical markers not identified to date.

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Since the chief factor in honey characterization is its aroma, the analysis of

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volatile components is a useful tool to authenticate unifloral honeys. Lavender honey

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has so far been characterized in terms of its hexanal, heptanal, nerolidol oxide and

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coumarin contents (Bouseta, Collins, & Dufour, 1992; Bouseta, Scheirman, & Collin,

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1996; Castro-Vzquez, Daz-Maroto, Gonzalez-Vias, & Prez-Coello 2009; Guyot-

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Declerck, Renson, Bouseta, & Collin, 2002; Radovic, Careri, Mangia, Musci, Gerboles,

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& Ankla, 2001; Shimoda, Wu, & Osajima, 1996). However, little is known about

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Lavandin hybrid honey (Lavandula angustifolia x latifolia) volatile composition.

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Although phenylacetaldehyde and heptanoic acid contents allowed Lavandin honey to

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be distinguished from Lavender honey in a previous study (Guyot-Declerck et al.,

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2002), the Lavender samples used were from L. angustifolia, which is less frequently

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used for honey production. Therefore, the contents in the previous compounds by

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themselves are seemingly inadequate to characterize Lavandin honey.

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Based on the foregoing, and on the increasing demand for products with specific

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characteristics and an identifiable geographical origin, the ability to authenticate

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Lavandin honey may be extremely useful for the beekeeping sector in the protected

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designation of origin (PDO) La Alcarria (central Spain). Therefore, the purposes of this

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study were as follows: (a) to identify volatile components in Lavandin honey

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(Lavandula angustifolia x latifolia) with a view to its authentication and discrimination

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from lavender honey (L. latifolia); (b) to evaluate physicochemical parameters and

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pollen types associated with Lavandin honey; and (c) to elucidate the sensory profile of

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Lavandin honey in order to facilitate its authentication.

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2.Material and methods

2.1. Samples

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All honeys were collected from La Alcarria (Spanish north-central area) sheltered

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by the Origin Denomination and had not been industrially processed. Samples belong to

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several beehives, corresponding with the beekeepers cropping areas.

Ten Lavender honeys (Lavandula latifolia) and ten Lavandin honeys (Lavandula

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angustifolia x latifolia) were analysed just after harvest by professional beekeepers. The

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samples were stored at 4 C until analysis.

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2.2. Isolation and analysis of volatile compounds

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The isolation of the volatile compounds was done on the styrene-divinylbenzene

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cartridges (Lichrolut EN, Merck, 0.5 g of phase), previously conditioned with 10 ml of

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dichloromethane, 5 ml of methanol and 10 ml of ethanol/distilled water (10%) at a flow

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rate of 2 mL/minute. Ten grams of each honey were dissolved in 50 mL of distilled

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water and 25 L of 2-pentanol (1g/L) was added as internal standard. Theses solutions

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were passed through cartridges. Then, sugars were eluted with 25 mL of distilled water,

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in order to eliminate artefacts. Volatile compounds were eluted with 30mL of

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dichloromethane at a flow rate of 2 ml/minute. The organic phase collected was

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concentrated in a Vigreux column and analysed by GC/MS Castro-Vzquez, Daz-

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Maroto, Guchu, & Prez-Coello, 2006.

An Agilent 6890 N gas chromatograph, coupled to a 5973 Inert mass selective

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detector was used. Two microliters of extracts were injected in splitless mode (0.6 min)

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on a polyethylene glycol capillary column BP-21 (50 m x 0.32 mm x 0.25 m of film

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thickness). The oven temperature was programmed to remain at 60 C for 3 min and

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then increase 2 C/min to 200 C and held for 30 min. Helium was used as carrier gas at

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a flow rate of 0.8 mL/min-1. Injector and transfer line temperatures were 250 C and

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280 C, respectively. Mass detector conditions were: electronic impact (EI) mode at 70

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eV; scan mass acquisition range: 40-450 amu.

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Peak identifications were based on comparison of their mass spectra with the

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corresponding commercial pure standards purchase from Sigma-Aldrich with a

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chemical purity between 85-99 %, and/or with those reported by the NBS75K and

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Wiley A commercial libraries. The quantitative analysis by total ion was performed

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using 2-pentanol such as internal standard. Further, individual response factors, ranged

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between 0-1, were taken into account. Response factors for each compound were

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calculated in water solution with 350 and 448 g/L of glucose and fructose, respectively,

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like a model honey. For compounds which commercial standards was not available, the

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response factors of compounds with similar chemical structures were used. All the

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samples were injected in duplicate.

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2.3. Melissopalynological analysis

Pollen analysis was carried out using the method established by the International

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Commission of Bee Botany described by Louveaux et al., (1978). The study of the

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sediment pollen spectrum was performed by microscopic analysis. Ten grams of honey

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was used for concentrating and counting all the pollen and spores particles. At least 300

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grains of pollen from each honey preparation were counted per slide.

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2.4. Physicochemical and Colour Analysis

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Physicochemical parameters were analysed following the specifications of the

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International Honey Commission and Spanish legislation (Bogdanov, Lullmann, Martin,

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Ohe, Russmann, & Vorwohl, 2000; B.O.E., 1986).

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determined using an ABBE refractometer model NAR-1T. Free acidity was analysed by

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potentiometric titration, and pH using pH-meter model Eutech Systems XS PC510.

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Hydroxymethylfurfural content was determined based on the method of White, 1979

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using a Hitachi U-1100 Spectrophotometer. Conductivity was measured with a

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Radiometer CDM-83 conductivimeter.

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Color parameters were established in the CIELAB system by reflection method

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(measuring geometry d/8, illuminant D65, range 380 to 780 nm, observer 10) using a

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Hitachi model U-1100 spectrophotometer (CIE 1986). Colour was also determined

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using a Pfund colour grader Lovibond Visual Comparator 2000 Series.

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2.5. Descriptive Sensory Analysis

Lavender (L. latifolia) and Lavandin honeys were evaluated according to

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quantitative descriptive analysis (QDA), where each honey was individually evaluated

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using a list with previously defined descriptors. The panel was formed by eight

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assessors, members of Food Technology Department (UCLM) and beekeeping research

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centre (Marchamalo) with aged ranging from 28 to 45 years. Sessions were performed

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in a tasting room with individual chambers that were separated of the area where the

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samples were prepared (ISO 8589, 1998). During the evaluation, room temperature was

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21C and 70% humidity. Three different coded samples were presented in random order

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to each assessor in 40-mL glass vials sealed with a twist-off cap and at room

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temperature. Mineral water was provided for the assessors mouth-rinsing between

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samples. Sessions were carried out between 11:00 and 13:00.

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The screening of assessors was carried out in previous studies to determine

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sensory profiles of unifloral honeys (Castro-Vazquez et al., 2009; Castro-Vzquez,

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Daz-Maroto, de Torres, & Prez-Coello 2010) All of them had prior experience in

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discrimination and descriptive sensory test.

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Despite that, a training of judges was done during six sessions. In the first one,

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aqueous standards solutions of linalool, -decalactone, and benzaldehyde (50 ppb), and

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eugenol, 1,8-cineol, (15ppb) were used to identify floral, fresh fruit, bitter

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almond, spice and balsamic notes. Those levels were chosen based on their

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proximity to their respective odour detection thresholds in air. Each panellist correctly

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described the standards and then knowing their identities.

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To complete the training period, the judges evaluated sixteen lavender (L.

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latifolia) and lavandin honeys during four sessions. In each session, the subjects

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received four honey samples and individually described the flavour and taste sensory

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attributes with their own terminology. The judges generated a total of ten olfactory and

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eight gustatory descriptors.

A new session was carried out in order to discuss the terms generated by each

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individual, and, with the supervision of a panel leader, they consensually defined the

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terms that adequately described the aroma and taste sensory similarities and differences

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among the evaluated honeys. Finally, seven olfactory and six flavour attributes were

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considered among the best at describing the sensory characteristics of lavender (L.

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latifolia) and lavandin honeys and the main differences between them. The aim of judge

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training was twofold: reaching a consensus about the meaning of each attribute and

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achieving intensity rating in a reliable way.

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The formal evaluation of honeys consisted in ten sessions realized in different

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days. The panellist used a 10 cm non-structured scale, from 0 to 10, to rate the intensity

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of each attribute, previously selected. Scales were delimited at the ends by the terms

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"weak" and "strong. Two replications of all sample assessments were performed.

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2.6. Statistical Analysis

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The statistical methods used for data analysis was a Student T-test for independent

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samples, to determine significant differences between volatile composition of honeys,

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and among sensory profiles of honey types. Step-way Discriminant analysis to select the

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aroma compounds most useful in differentiating the two honey sources was performed.

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One way ANOVA was used to check differences among physicochemical values.

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Statistical processing was carried out by using the SPSS 17.0 statistical software

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package for Windows.

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3. Results and discussion

3.1. Identification of honey volatile markers
A total of eighty volatile organic compounds (VOCs) were quantified in Lavandin

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(Lavandula angustifolia x latifolia) and Lavender (Lavandula latifolia) honeys.

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Although most are present in both types of honey, the two honey types can be

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differentiated in terms of their concentrations.

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Table 1 shows the volatile fingerprints off the two types of honey as obtained by

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SPE/GCMS analysis. Students t-test for independent samples was used to identify

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significant differences according to monofloral origin. As can be seen, there were

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marked differences between the two types of honey. There were none, however, in

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hexanal or phenylacetaldehyde levels, which, according to Guyot-Declerck et al., can be

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used to differentiate Lavender and Lavandin honeys. This was probably a result of the

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particular honey species investigated by these authors being L. angustifolia rather than

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L. latifolia.

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The most interesting finding of this study was that lactones are the volatile

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compounds most markedly contributing to distinguishing Lavandin honey from

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Lavender honey (L. latifolia). Thus, the mean contents in -butyrolactone, pantolactone

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and -nonalactone of Lavandin honey were 57.4% higher than those of Lavender honey.

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-Nonalactone was especially relevant in this respect, as it was identified as a

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component of honey aroma for the first time in this work. This lactone was present at

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significantly higher concentrations in Lavandin honey, which contained it at levels

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above its odour threshold (Table 2). Therefore, -nonalactone can be an effective

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volatile marker for authenticating Lavandin honey. Figure 1 shows a typical

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chromatogram for Lavandin honey with its peaks clearly identified and numbered.
One other outstanding compound quantified in Lavandin honey was decanal. This

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compound was recently reported to occur in similar amounts in chestnut and acacia

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honeys (Castro-Vazquez et al.,2010; Plutowska, Chmiel, Dymerski, & Wardencki,

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2011; Radovic et al., 1996). The mean concentration of decanal can also be used to

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authenticate Lavandin honey since, as found in this study, it was twice higher in it than

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in Lavender honey.

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Worth special note are the statistical differences in farnesol mean levels between

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honeys from L. latifolia and L. angustifolia x latifolia cultivated in the Alcarria region

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(Spain). Thus, the farnesol contents of Lavandin honey were 8 times higher than those

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found in Lavender honey. The fact that this compound was never previously identified

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in honey warrants its use as a floral marker for authenticating Lavandin honey.

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One other interesting result was the presence of acetovanillone in substantial

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amounts in Lavandin honey (27 g/kg vs only 2.7 g/kg in Lavender honey). Such a

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large difference can also be useful with a view to differentiating honeys by botanical

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origin. Acetovanillone has a flavour threshold of 100 ppb (Campo, Ferreira, Escudero,

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Marques, & Cacho, 2005), so it can hardly contribute to Lavandin honey aroma;

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however, the high levels found in Lavandin (L. angustifolia x latifolia) honey can be of

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help for its authentication and differentiation from Lavender honey.

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The

honeys were also found to contain substantial amounts of 4-

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methoxyacetophenone, a compound involved in the shikimic acid conversion pathway.

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The differences in 4-methoxyacetophenone contents between Lavandin and Lavender

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(L. latifolia) honeys can also be used to discriminate between the two. The sweet aroma

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of 4-metohoxyacetophenone may influence the sensory profile of Lavandin honey.

Dehydrovomifoliol levels in the studied honeys were similar to or greater than

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those in honeys from other blossom sources, particularly eucalyptus eucalyptus (Castro-

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Vzquez et al. 2006; DArcy, Rintoul, Rowland & Blackman, 1997; Guyot,

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Scheirmann, & Collin, 1999; Piasenzotto, Gracco, & Conte, 2003). In any case, such

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levels were significantly higher in Lavandin honey than in Lavender honey.

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Finally, several compounds involved in plant metabolism such as linalool,

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hotrienol, camphor, p-cymen-8-ol and 1,8-cineole (isomer I) were all absent or present

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at low levels in Lavandin honey relative to Lavender honey (L. latifolia).

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The previous results constitute a breakthrough towards authenticating Lavandin

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honey and can therefore be highly interesting for the beekeeping industry in the Alcarria

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region, which has long sought effective ways to differentiate these two types of

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monofloral honeys.

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The chemical data were subjected to stepwise discriminant analysis in order to

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confirm the two groups of honeys on the basis of volatile compounds. Using the data for

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all VOCs and their standard deviations afforded considerable data simplification. Two

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different independent discriminant functions were computed. Table 3 shows the

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individual variables most markedly contributing to discrimination between Lavender (L.

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latifolia) and Lavandin (L. angustifolia x latifolia) honeys, and their coefficients. Cross-

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validation afforded 100% correct assignment of the honey samples.

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3.2. Palynological profile

Several pollen types were found in Lavander and Lavandin honeys, although only
those whose taxa appear in at least 50% of the samples have been represented (Fig. 2).
In Lavender honeys, the most frequent species associated to Lavandula latifolia

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pollen were Leguminosae, Lonicera, Satureja, Cichorioideae, Asteroideae, Lamiun,

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Plantago and Rosaceae. From a botanical point of view, these species are related to

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wild vegetation.

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On the other hand, in Lavandin honeys (L. latifolia), Rubus was the most

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characteristic pollen since it was present in all samples, although Retama,

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Scrophulariaceae, Brassica, Crataegus, Cytisus, Prunus, Rosmarinus officinalis, Salix,

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Trifolium and Thymus pollens were also frequently found. The three first species seem

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to be a reflection of the cropping areas.

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The exclusive presence of pollen from Conium and Heliotropium-europaeum in

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Lavandin honeys, and Boraginaceae in Lavender ones (Figure 1) cant be used as

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markers of the type of honey since their presence didnt occur in all the honey samples.

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Despite that, the presence of the cited pollens can be considered an extra tool for honeys

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differentiation.

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Although palynologycal data were not enough to differentiate these honey types,

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the joint information of pollen composition with other physico-chemical, volatile and

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sensory markers seem to be a better way to distinguish Lavander (L. latifolia) and

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Lavandin honeys.

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3.3. Physicochemical and colour parameters

The physico-chemical parameters of Lavender (Lavandula latifolia) and Lavandin

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(Lavandula angustifolia x latifolia) honeys are shown in Table 4. The mean value,

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standard deviation and maximum and minimum values were shown.

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Water content of these honeys was below 20%, not exceeding the maximum limit

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established by the European Honey Directive., 2001. The same occurs with HMF

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content, which only reflects honey freshness, regardless its botanical origin. The results

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obtained for the studied honeys were below the legal limit established as 40 mg/kg.

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After the application of the One-Way ANOVA test to the studied parameters, only

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electrical conductivity and moisture showed significantly statistical differences (p<

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0.05) between Lavender and Lavandin honeys, while free acidity, pH and colour did not

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show any difference at that significance level.

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Differences in moisture could be due to different harvesting time between the two

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types of honey. Lavandin samples were collected between July and August, dry and hot

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climatic period in Central Spain; while Lavender honeys were harvested in September,

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usually a rainy month, thus the moisture level of Lavender honeys are higher.

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On the other hand, electrical conductivity values, which are closely related to the

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concentration of mineral salts from soil and plants, are higher in Lavandin honeys; this

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fact could be due to the fertilizer that is added to the soil in the growing areas.

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With regard to colour, value obtained by Pfund and CIElab methods was similar.

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According to Pfund scale, usually used in the honey industry, the colour of Lavender

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and Lavandin honeys is extra light amber with an average values slightly higher in

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Lavandin honeys (45 mm) than in Lavender samples (40 mm).

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3.4. Sensory Differentiation between Lavender and Lavandin Honeys

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Lavender (L. latifolia) and Lavandin honeys were compared in sensory terms for

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the first time in this study. A comprehensive sensory description was obtained from

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their aroma and flavour profiles. Figure 3 shows a spiderweb diagram displaying the

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average intensity scores for the different attributes.

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The data set was subjected to Students t-test in order to identify significant

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differences between the two types of honey. All sensory impressions except aftertaste

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intensity and quality exhibited significant differences at the p < 0.05 level.

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The most relevant differences noted by the judges in Lavandin honey were much

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less strong (p > 0.05) in balsamic, fresh, citric, lavender and floral aromas

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and tastes, in comparison with Lavender honey. The lower concentrations of hotrienol

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and linalool in Lavandin honey (Table 1) account for the significantly lower scores

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given to lavender and floral flavours in Lavandin samples. On the other hand, the

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decreased levels of p-cymen-8-ol and 1,8-cineole which confer fresh, citric and

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balsamic aromas (Amoore and & Venstrom, 1966; http://www.flavornet.org) in

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Lavandin honey may also be associated to its characteristic sensory profile.

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Caramel and jam/peach compote were the specific attributes receiving the

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highest scores in Lavandin honey relative to Lavender honey (L. latifolia). The

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increased caramel scores for Lavandin honey are consistent with its also increased

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amounts of 4-methoxyacetophenone and, mainly, lactones, which are largely associated

374

to this attribute (http://www.flavornet.org). In fact, the mean sensory scores confirm that

ACCEPTED MANUSCRIPT

375

lactone levels largely account for and influence the typical caramel notes of Lavandin

376

honey.

377
Moreover, the presence of -nonalactone, which occurs naturally in peaches and

379

apricots (Cullere, Escudero, Cacho, & Ferreira, 2004; Sevenants & Jennings, 1996), is

380

consistent with the jam/peach compote aroma and flavour notes best reflecting the

381

distinguishing features identified by the assessors in Lavandin floral honey.

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378

382

The higher intensities of caramel and jam/peach compote notes appear to be

384

an unequivocal support for Lavandin honeys authentication from a sensory point of

385

view.

M
AN
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383

386
387

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D

388
389
390

393
394
395
396
397
398
399

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C

392

EP

391

ACCEPTED MANUSCRIPT

4. Conclusions

401

The results of this study reveal that the volatile composition and sensory profile of

402

Lavandin honey (L. angustifolia x latifolia), and its palynological characteristics last

403

one with smaller contribution, are specific enough to allow its floral source to be

404

identified and certified. Also, the previous factors afford discriminating between honeys

405

from Lavandin and Lavender (L. latifolia), which is a breakthrough for the honey

406

research and beekeeping sectors.

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SPE/GC-MS determinations revealed marked differences in volatile profile

408

between the two monofloral types of honey. The increased levels of -nonalactone,

409

farnesol and acetovanillone, which were for the first time identified in honey here, are

410

proposed as Lavandin floral markers. These compounds, together with 1-heptanol,

411

decanal, 4-methoxyacetophenone and dehydrovomifoliol, allow Lavandin honey to be

412

accurately discriminated from Lavender honey (L. latifolia) in terms of volatile

413

composition.

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407

Although pollen profiles are inadequate to differentiate Lavender (L. latifolia) and

415

Lavandin honey, the joint use of palynological data and physicochemical markers may

416

be useful to distinguish them.

EP

414

Lavandin (L. angustifolia x latifolia) honey and Lavender (L. latifolia) honey are

418

also distinguishable in sensory terms. Thus, quince compote and caramel

419

sensations, which are closely associated to the volatile composition of Lavandin honey,

420

are its key sensory descriptors.

421

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C

417

The proposed volatile and sensory markers provide a powerful authentication tool

422

for Lavandin (L. angustifolia x latifolia) honey and a self-obvious marketing advantage

423

for the beekeeping sector since it can enable its marketing as monofloral honey with a

424

characteristic profile different from that of Lavender honey (L. latifolia).

ACCEPTED MANUSCRIPT

425

AUTHOR INFORMATION

426

Corresponding Author

427
Phone:

+34-926-295300, Fax: +34-926-295318.

429

E-mail: LuciaIsabel.Castro@uclm.es

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430

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Funding Sources

433

The authors wish to thank the professional beekeeper for supplying the samples. This

434

study was supported by the Junta de Comunidades de Castilla-La Mancha (05-299/IA-

435

47, PAI09-0018-9267), INIA-FEDER funds (RTA2007-00072-C03 and Support

436

through Researcher Contract INIA-CCAA).

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437

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438
439
440

443
444
445
446
447
448
449

AC
C

442

EP

441

ACCEPTED MANUSCRIPT

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Sevenants, M.R., & Jennings, W.G. (1996). Volatile compounts of peach. Journal of the

566

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567

Shimoda, M., Wu, Y., & Osajima, Y., (1996). Aroma Compounds from Aqueous

569

Solution of Haze (Rhus succedanea) Honey Determined by Adsorptive Column

570

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568

571

Soria, A.C., Gonzalez, M., de Lorenzo, C., Martinez-Castro, I., & Sanz, J. (2004).

573

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575

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572

577

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578

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579
580
581
582

ACCEPTED MANUSCRIPT

TABLE CAPTIONS

Table 1. Minimum, maximum, and average concentrations (g/Kg) of volatile

RI
PT

compounds determined in Lavender and Lavandin honeys from La Alcarria area.

Table 2. Aroma descriptors and Olfactive perception threshold (ppb) of some

SC

compounds that statistically differentiate Lavender and Lavandin honeys

Table 3. Standard Canonical Discriminant Functions coefficients of Lavender

M
AN
U

(Lavandula latifolia) and Lavandin (Lavandula angustifolia x latifolia) honeys

cultivated in La Alcarria, according to their volatile composition.

Table 4. Physicochemical and colour parameters in the honey types studied, including

AC
C

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D

the results of the One-Way ANOVA test applied to the mean values.

ACCEPTED MANUSCRIPT

Table 1. Minimum, maximum, and average concentrations (g/Kg) of volatile

compounds determined in Lavender and Lavandin honeys from La Alcarria area.
Lavender honeys
(L.latifolia)
COMPOUNDS

RI

Min

Max

Mean

SD

Min

Max

Mean

SD

RI
PT

Lavandin honeys
(L. angustifolia x latifolia)

Hexanal

1044

15.12

26.04

20.18

4.43

6.88

51.74

27.41

15.22

3-Penten-2-ol

1136

21.15

102.14

46.46

27.51

19.85

177.74

73.54

50.99

Heptanal

1168

1.60

7.52

4.01

2.00

1.94

7.47

4.03

1.67

1214

2.89

24.25

11.82

6.85

6.22

25.84

14.05

6.21

3-Methyl-1-butanol
2-Methyl-3-(2H)
dihydrofuranone*

1245

1.68

14.29

4.39

3.90

tr

14.51

8.98

4.26

3-Methyl-3-buten-1-ol

1252

9.37

46.95

23.03

12.37

11.18

47.96

29.22

13.55

SC

3-Methoxy-1-butanol*

1260

tr

15.86

4.40

5.92

3-Hydroxy-2-butanone

1289

7.26

34.32

13.88

8.04

2-Hexanol

1293

1.74

56.35

18.77

10

2-Methyl-2-buten-1-ol

1313

8.10

36.77

11

1-Hexanol

1352

20.93

118.54

12

1-Hydroxy-2-butanone

1363

0.48

13

Nonanal

1388

14

2-Butoxyethanol

1391

15

Ethyl octanoate

16
17
18

Acetic acid

1450

3.52

20.99

8.32

5.33

2.46

14.97

8.22

3.94

19

(E)-Linalool oxide

1459

3.30

31.95

8.70

9.20

2.30

38.18

9.74

11.10

20

Furfural

1470

1.48

20.82

8.16

6.94

3.37

22.77

12.49

6.09

21

2-Ethyl-1-hexanol

1478

3.83

31.21

11.57

8.55

4.07

17.94

10.22

5.04

22

-Campholene aldehyde*

1483

1.40

5.74

2.40

1.33

1.48

4.48

2.97

1.06

19.91

7.78

7.72

56.55

17.55

18.20

19.76

2.13

72.39

28.02

25.43

16.16

8.41

9.35

54.20

29.17

16.17

65.31

37.43

2.25

325.91

131.65

112.03

13.31

3.96

3.77

tr

9.29

3.76

3.39

9.68

67.38

26.10

19.41

7.40

33.26

21.66

8.39

tr

28.52

9.71

9.26

tr

16.16

8.89

6.39

1430

tr

10.38

3.10

3.56

tr

8.32

2.72

2.81

(Z)-Linalool oxide

1438

10.10

52.40

20.44

13.22

4.20

27.40

11.93

1-Heptanol

1445

2.31

10.14

6.99

3.12

9.25

34.85

21.63

24

1-(2-Furanyl)ethanone

25

Camphor

26

Benzaldehyde

27

Propanoic acid

TE
D

Decanal

1489

AC
C

4.19

12.57

29.51

6.92

2.43

5.82

3.81

0.58

n.d.

n.d.

n.d.

17.61

7.58
11.80

5.19

13.28

1508

2.05

23.90

5.91

1517

tr

1.51

0.85

1532

7.30

50.51

21.95

12.86

9.62

45.88

26.05

9.47

1544

3.39

12.07

6.37

2.63

1.12

12.46

6.23

3.70

1553

11.01

28.23

8.17

2.90

EP

23

M
AN
U

tr

3.01

17.54

0.94

28

Linalool

29

Octanol

1564

1.91

10.90

4.74

3.19

3.67

10.61

6.49

2.48

30

2-Methylpropanoic acid

1576

3.83

26.02

9.05

6.75

5.82

21.82

11.19

5.32

31

Hotrienol *

1616

27.96

219.87 113.31

66.61

7.28

111.56

53.57

32

-Valerolactone

1621

3.55

18.32

7.69

4.29

2.19

28.15

7.63

7.61

33

Butanoic acid

1627

4.84

133.18

31.58

39.43

10.50

197.41

74.66

78.19

34

Ethyl decanoate

1632

n.d.

436.45

59.47

143.04

n.d.

9.11

2.57

3.52

35

-Butyrolactone

1646

2.36

12.55

9.11

3.65

13.57

36.04

19.29

36

Phenylacetaldehyde

1661

19.53

142.58

85.74

48.68

51.26

243.72

107.68

78.82

37

1-Nonanol

1670

2.79

32.69

7.79

9.43

n.d.

12.09

3.45

4.53

5.80

0.87

15.15

7.05

4.33

34.96

7.28

ACCEPTED MANUSCRIPT

Table 1. (Continued)
Lavender honeys
(L.latifolia)
COMPOUNDS

RI

Min

Max

Mean

Lavandin honeys
(L. angustifolia x latifolia)
SD

Min

Max

Mean

SD

Furfuryl alcohol

1679

10.03

27.61

21.71

12.48

2.33

44.20

17.83

13.90

39

3-Methylbutanoic acid

1682

7.91

71.92

20.71

19.70

11.16

41.96

25.86

10.98

40

Ketoisophorone

1686

2.34

12.75

6.17

3.77

1.68

41

-Terpineol

1691

0.45

10.19

2.95

2.88

n.d.

2.87

1.13

1.01

42

Epoxylinalool (isomer I) *

1732

2.15

26.09

13.27

10.92

4.02

86.99

28.62

26.49

43

Epoxylinalool (isomer II) *

1745

0.73

15.02

5.63

5.51

2.55

57.12

17.07

44

Myrtenol *

1796

0.39

15.96

2.96

4.96

n.d.

14.16

3.37

4.21

45

Hexanoic acid

1857

15.13

97.25

52.42

29.02

32.27

126.50

81.08

31.15

46

p-Cymen-8-ol *

1878

0.85

12.40

4.79

47

2-Hydroxycineole *

1882

0.75

12.71

4.52

48

Mequinol *

1891

n.d.

11.37

4.20

3.14

1.54

26.51

6.92

7.28

49

Benzylalcohol

1903

11.47

186.83

51.78

53.79

143.74

58.55

44.31

50

Nonadecane

1921

n.d.

n.d.

n.d.

n.d.

16.88

4.65

6.68

n.d.

4.29

0.73

3.86

n.d.

5.23

2.16

3.92

n.d.

n.d.

n.d.

104.65

19.29

268.57

79.12

71.46

1382.46

526.33

381.17

53.63

758.65

390.36

245.57

21.07

10.48

6.13

2.76

27.20

16.61

9.10

26.29

35.83

4.24

49.81

19.81

15.41

59.31

119.14

4.45

48.53

12.03

12.95

443.10

138.01

17.45

54.58

31.15

10.74

36.68

53
54

Heptanoic acid

1972

55

(E)-3-Hexenoic acid

1981

n.d.

116.10

56

6-Methyl-2-methoxypyrazine

1996

6.08

375.54

57

Methylfurancarboxylate

2027

17.43

77.00

TE
D

58

Pantolactone

2031

11.98

33.92

24.57

59

Methylfurancarboxylate

2036

tr

tr

tr

60

-Nonalactone

2041

7.23

16.30

12.33

61

Octanoic acid

2051

20.22

52.30

29.13

11.34

62

p-Cresol

2068

1.95

9.88

4.51

2.31

63

p-Mentha-1(7),2-dien-8-ol *

2071

n.d.

4.92

1.34

64

Nonanoic acid

2154

9.87

170.87

65

Eugenol

2144

4.07

44.67

EP

AC
C

1.84

107.83

tr

1940

62.40

50.07

n.d.

38.23

10.16

30.06

63.28

38.97

16.00

68.45

36.48

16.70

1.75

5.64

3.30

1.37

1.77

n.d.

9.47

2.94

3.67

45.29

54.32

10.51

53.21

33.19

14.00

12.63

12.28

2.57

12.46

8.49

3.43

4-Methoxyacetophenone *

2168

17.05

36.25

27.57

67

8-Nonen-2-one

2183

tr

19.22

8.66

68

1,8-Cineole (isomer II)

2228

18.22

35.66

69

1-Hydroxylinalool *

2269

20.23

148.90

70

trans-Sobrerol *

2276

11.02

2283
> 2280

7.52

34.87

66

1.53

10.27

1929

4.29

19.01

18.16

1,8-Cineole (isomer I)
2-Phenylethanol
2,6-Dimethyl-3,7-octadien-2,6diol *

4.54

2.48

374.94

51

189.46

4.61

12.01

52

1968

SC

9.45

M
AN
U

RI
PT

38

3.20

8.81
14.52
10.51

5.99

40.20

109.30

64.85

25.07

5.95

7.22

34.73

16.48

25.04

5.76

16.29

40.28

25.17

7.94

57.00

41.26

17.05

106.33

58.64

32.80

102.30

40.79

41.34

4.02

139.52

42.03

46.35

127.02

2489.44

634.44

730.32

150.82

1653.92

643.02

483.03

n.d.

1120.68

263.08

345.09

62.46

337.43

175.23

104.39

481.18

128.91

138.10

42.75

477.24

192.18

160.59

12.67

71

Triethylenglycol

72

Hexadecanoic acid

73

Benzoic acid

36.25

74

Coumarin

23.82

355.02

142.14

103.59

n.d.

230.06

100.35

79.72

75

Pentacosane

n.d.

110.60

12.29

36.87

n.d.

174.68

23.85

56.66

ACCEPTED MANUSCRIPT

Table 1. (Continued)

Lavender honeys
(L.latifolia)

76

Hydroxymethylfurfural

77

Farnesol *

78

Benzenacetic acid

Min

Max

Mean

SD

Min

Max

Mean

SD

> 2280

n.d.

3713.08

618.59

1181.38

34.34

246.69

149.29

78.21

8.22

3.05

71.71

214.20

126.27

n.d.

Dehydrovomifoliol *

n.d.

6.21
66.01

2.76

40.00

3.25

9.33

44.92

63.69

2.81
16.75

10.02
72.55

59.01

24.83

16.77

332.41

154.51

78.42

19.60

73.22

145.28

SC

21.30

27.09

113.23

29.60

TE
D

M
AN
U

RI: Retention indices based on polyethylene glycol capillary column BP-21 (50 m x
0.32 mm x 0.25 mm of film thickness
* Compounds tentatively identified using Wiley and NBS75K Libraries
Tr: Traces; n.d.: not detected compounds
a,b: Different letters in the same row indicate statistical differences (P< 0.05) according
to the Student-Newman-Keuls test.

Compounds reported for the first time as honey constituents.

EP

80

Acetovanillone

AC
C

79

RI

RI
PT

COMPOUNDS

Lavandin honeys
(L. angustifolia x latifolia)

ACCEPTED MANUSCRIPT

Table 2. Aroma descriptors and Olfactive perception threshold (ppb) of some

compounds that statistically differentiate Lavender and Lavandin honeys

Decanal

AB

Camphor

AB

Linalool

AB

Hotrienol

threshold

Aroma des
a
Identification criptors

(ppb)

soap, orange peel, tallow(1)

Camphor

floral, fruity

unknown

(1)

floral, fresh, fruity

110

(2)

p-Cymen-8-ol

AB

Musty

AB

eucalyptus, fresh, balsamic(3)

AB

(1)

cotton candy

coconut, candy, peach

(4)

4-Methoxyacetophenone

sweet, anisic, coumarin, fruity

Farnesol

flower, oil

(1)

(7)

8.17

17.61

0.85

n.d.

17.54

7.05

113.31

53.57

4.79

0.73

12(8)

10.27

n.d.

unknown

24.53

50.07

12.33

38.97

(4)

30

(1)

Lavandin
honeys
Mean Con.
(ppb)

unknown

M
AN
U

-Nonalactone

AB

(6)

25
(1)

1,8-Cineole
Pantolactone

3(5)

(1)

SC

Compounds

Lavender
honeys
Mean Con.
(ppb)

RI
PT

Olfactive
perception

unknown
20

(9)

27.57

64.85

3.05

24.83

The identification of the volatile compounds is indicated by the following:

TE
D

A: mass spectrum and retention time consistent with those of an authentic standard;
B structural proposals are given on the basis of mass spectral data (NBS75K and Wiley A )

The reference from which the olfactive perception threshold has been taken is taken is given in
parentheses: (1) http://www.flavornet.org; (2) Quian &Wang, 2005; (3) Faria, Boido, Carrau,

EP

Versini, & Dellacassa, 2005; (4)Ferreira, Lopez, & Cacho, 2000; (5) Ahmed, Dennison,

Dougherty, & Shaw 1978; (6) Aznar, Lpez, Cacho, & Ferreira, 2003; (7) Riberau-Gayon,

AC
C

Glories, Maujean, &Dubourdieu, 2000; (8) Amoore and & Venstrom, 1966; (9) Ohloff, 1978.

ACCEPTED MANUSCRIPT

Table 3.

Standard Canonical Discriminant Functions coefficients of Lavender

(Lavandula latifolia) and Lavandin (Lavandula angustifolia x latifolia) honeys

Hexanoic acid

Coefficients
attached to
Function 1
1.853

Coefficients
attached to
Function 2
-3.714

-0.135

0.388

p-Cymen-8-ol

1.156

-Nonalactone

-0.453

Dehydrovomifoliol

AC
C

EP

TE
D

(Constant)

0.661

-2.667
1.604

-3.486

M
AN
U

p-Mentha-1(7),2-dien-8-ol

SC

Linalool

RI
PT

cultivated in La Alcarria, according to their volatile composition.

-0.058

0.555

-12.563

-59.795

ACCEPTED MANUSCRIPT

Table 4. Physicochemical and colour parameters in the honey types studied, including
the results of the One-Way ANOVA test applied to the mean values.

Electrical conductivity (mS/cm)

Mean SD
(min - max)

16.62 1.60
(14.53 - 19.40)

15.43 0.67
(14.45 - 16.25)

4.60 4.97
(0.15 - 16.02)

2.28 2.69
(0.15 - 9.28)

0.22 0.07
(0.13 - 0.32)

0.29 0.05
(0.21 - 0.39)

3.88 0.25
(3.64 - 4.46)

4.02 0.13
(3.91 - 4.26)

M
AN
U

pH

Mean SD
(min - max)

RI
PT

HMF (mg/kg)

Lavandin honeys
(L. angustifolia x latifolia)

SC

Moisture (%)*

Lavender honeys
(L.latifolia)

Free acidity (meq/kg)

19.34 4.17
(14.40 - 25.80)

20.73 3.25
(15.25 - 25.00)

Pfund colour (mm of Pfund)

40.06 12.91
(24.21 61.48)

45.41 15.48
(19.22 67.84)

X10

0.42 0.03
(0.38 - 0.47)

0.43 0.04
(0.37 - 0.48)

Y10

0.43 0.02
(0.40 - 0.47)

0.44 0.04
(0.39 - 0.54)

0.15 0.05
(0.06 - 0.22)

0.14 0.06
(0.06 - 0.25)

2.08 3.37
(-2.03 - 7.28)

4.59 3.48
(-0.17 - 12.22)

52.75 14.30
(36.83 - 80.53)

54.33 14.95
(27.90 - 70.34)

52.86 14.40
(36.88 - 80.85)

54.58 15.09
(27.90 - 70.53)

hab.10 (hue angle)

88.45 3.29
(84.83 - 93.15)

85.70 3.16
(79.02 - 90.32)

L*10 (lightness)

80.93 4.99
(74.70 - 88.96)

77.39 8.49
(56.94 - 87.84)

Z10

a*10
(chromaticity + red / green)

AC
C

C*ab (chroma)

EP

b*10
(chromaticity + yellow / blue)

TE
D

C.I.E. L a*b* colour

* Significant difference between groups p < 0.05

SD: standard deviation.

ACCEPTED MANUSCRIPT

FIGURE CAPTIONS
Figure 1. Typical chromatogram obtained from Lavandin honey samples by GC-MS

RI
PT

Figure 2. Comparison between percentage of pollen of the more abundant botanical

species that occur in lavender and Lavandin honeys

AC
C

EP

TE
D

M
AN
U

scores of eight judges (two replicates) are shown.

SC

Figure 3. Descriptive Sensory Analysis of Lavandin and Lavender honeys. Mean

ACCEPTED MANUSCRIPT

53

RI
PT

71

49

66

31

61

45

11

2: 3-Penten-2-ol
6: 3-Methyl-3-buten-1-ol
8: 3-Hydroxy-2-butanone
9: 2-Hexanol
10: 2-Methyl-2-buten-1-ol
11: 1-Hexanol
13: Nonanal
17: 1-Heptanol
21: 2-Ethyl-1-hexanol

21 2326
28

42

52

58

43

23: Decanal
26: Benzaldehyde
28: Linalool
31: Hotrienol
35: -Butyrolactone
38: Furfuryl alcohol
42: Epoxylinalool (isomer I)
43: Epoxylinalool (isomer II)
45: Hexanoic acid

70
73

78

69

68

60

TE
D

35 38
13
17

EP

9
6 8 10

AC
C

M
AN
U

SC

IS

74

79
77

80

65

49: Benzylalcohol
52: 2-Phenylethanol
53: 2,6-Dimethyl-3,7-octadien-2,6-diol
58: Pantolactone
60: -Nonalactone
61: Octanoic acid
65: Eugenol
66: 4-Methoxyacetophenone
68: 1,8-Cineole (isomer II)

69: 1-Hydroxylinalool
71: Triethylenglycol
73: Benzoic acid
74: Coumarin
77:Farnesol
78: Benzenacetic acid
79: Acetovanillone
80: Dehydrovomifoliol

Fig. 1.Typical chromatogram obtained from Spanish Lavandin honey samples (Lavandula angustifolia x latifolia) by GC-MS

AC
C
EP

species that occur in Lavender and Lavandin honeys

TE
D

Fig. 2. Comparison between percentage of pollen of the more abundant botanical

Echium spp.

Cytisus t.

Cruciferae

Crataegus t.

Brassica sp.

SC

0
Thymus

Trifolium t.

Salix spp.

Rosmarinus officinalis L.

Rosaceae

RI
PT

50

Prunus t.

Plantago spp.

Lotus t.

Lamium

Heliotropium europaeum

M
AN
U

Lavender honeys (L.latifolia)

Boraginaceae

Asteroidae

Conium

Scrophulariaceae

Retama spp.

Rubus

Satureja spp.

Cichorioideae

Lonicera

Leguminosae

Lavandula latifolia Medik.

ACCEPTED MANUSCRIPT

100

Lavandin honeys (L. angustifolia-L.latifolia)

ACCEPTED MANUSCRIPT

Odor Evaluation

Balsamic
7,0

5,0

Caramel

Fresh

4,0
3,0
2,0
1,0
0,0

Floral

Jam/Peach compote

M
AN
U

Citric

SC

Lavander

RI
PT

6,0

Flavor evaluation

Sweet taste

TE
D

10,0
8,0

Floral taste

6,0

Citric taste

4,0
2,0

EP

0,0

AC
C

Jam/Peach compote taste

Caramel taste

Balsamic taste

Lavender honey (Lavandula latifolia)

Lavandin honey (L. angustifolia-L. latifolia)

Fig. 3. Descriptive Sensory Analysis of Lavandin and Lavender honeys. Mean scores
of eight judges (two replicates) are shown.

ACCEPTED MANUSCRIPT

Highlights
- Lavandin honey (Lavandula angustifolia x latifolia) had been characterized for the first

RI
PT

time.

- Lavandin monofloral honeys showed botanical markers that allow typify this floral

SC

origin.

- -Nonalactone, farnesol and acetovanillone are proposed as volatile markers for

- The

M
AN
U

Lavandin honey authentication.

sensory profile of Lavandin honey was characterized by intensities of caramel and

TE
D

peach compote notes.

AC
C

EP

- Results provide a complete differentiation between Lavender and Lavandin honeys.