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Trivalent Iron Is Responsible for the Yellow Color Development in the Nacre of Akoya Pearl Oyster Shells

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Abstract

The gold and cream colors of cultured Akoya pearls, as well as natural yellow nacre of pearl oyster shells, are thought to arise from intrinsic yellow pigments. While the isolation of the yellow pigments has been attempted using a large amount of gold pearls, the substance concerned is still unknown. We report here on the purification and characterization of yellow pigments from the nacre of Akoya pearl oyster shells. Two yellow components, YC1 and YC2, were isolated from the HCl-methanol (HCl-MeOH) extract from nacreous organic matrices obtained by decalcification of the shells with ethylenediaminetetraacetic acid (EDTA). Energy-dispersive X-ray and infrared spectroscopy analyses suggested that YC1 and YC2 precipitated under basic conditions are composed of Fe-containing inorganic and polyamide-containing organic compounds, respectively. YC1 solubilized under acidic conditions exhibited positive reactions to KSCN and K4[Fe(CN)6] reagents, showing the same ultraviolet-visible absorption spectrum as those of Fe(III)-containing compounds. In addition, X-ray absorption fine structure analysis supported the compound in the form of Fe(III). The total amount of Fe was approximately 2.6 times higher in the yellow than white nacre, and most Fe was fractionated into the EDTA-decalcifying and HCl-MeOH extracts. These results suggest that Fe(III) coordinated to EDTA-soluble and insoluble matrix compounds are mainly associated with yellow color development not only in the Akoya pearl oyster shells but also in the cultured Akoya pearls.

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Acknowledgments

We thank the staffs of the Mikimoto Pearl Farms in Tatoku and Hakata, Japan, for their help with selection and cleaning of Akoya pearl oyster shells. We also thank Dr. D.A. Coury (Western Governors University, USA) for the helpful suggestions regarding the manuscript.

Funding

This study was partially supported by Grant-in-Aid for Challenging Exploratory Research (JSPS KAKENHI grant numbers JP23658169 to MA and JP17K19282 to SK), Grant-in-Aid for Scientific Research (B) (JP26292108 to MA), and Grant-in-Aid for Scientific Research on Innovative Areas IBmS (JP19H05771 to MS).

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Authors and Affiliations

  1. Graduate School of Bioresources, Mie University, 1577 Kurima-machiya, Tsu, Mie, 514-8507, Japan

    Makoto Kakinuma, Chiaki Kasugai, Mirai Koide & Kayo Mitani

  2. School of Marine Biosciences, Kitasato University, 1-15-1 Kitasato, Minami, Sagamihara, Kanagawa, 252-0373, Japan

    Ko Yasumoto, Kaho Shidoji & Shugo Watabe

  3. Graduate School of Agricultural and Life Sciences, The University of Tokyo, 1-1-1 Yayoi, Bunkyo, Tokyo, 113-8657, Japan

    Michio Suzuki & Shigeharu Kinoshita

  4. Research and Development Department, Mikimoto Pharmaceutical Co., Ltd., 1425 Kurose, Ise, Mie, 516-8581, Japan

    Fumihiro Hattori & Kaoru Maeyama

  5. National Research Institute of Aquaculture, Japan Fisheries Research and Education Agency, 422-1 Nakatsuhamaura, Minami-ise, Mie, 516-0193, Japan

    Masahiko Awaji

  6. Pearl Research Laboratory, Mikimoto Co., Ltd., 923 Hazako-osaki, Hamajima, Shima, Mie, 517-0403, Japan

    Kiyohito Nagai

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  1. Makoto Kakinuma
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Correspondence to Makoto Kakinuma.

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Supplementary Fig. 1

UV-VIS spectra of the various extracts obtained from the YN powder. The EDTA and HCl-MeOH extracts were directly subjected to UV-VIS spectral analysis. On the other hand, the acetone extract was dissolved in MeOH (1.0 mg/mL) after evaporation, and the SDS-DTT extract was diluted 10 times with H2O, and then used for UV-VIS spectral analysis. Numbers shown in the spectra indicate absorption maxima (λmax). (PPTX 104 kb)

Supplementary Fig. 2

TLC chromatogram of acetone extract obtained from YN powder. The acetone extract dissolved in MeOH (1.0 mg/mL) after evaporation was applied to a TLC glass plate RP-18 F254s (5 x 10 cm, No. 1.15685.0001, Merck Millipore) and developed with a mixed solvent of MeOH-acetone [8 : 2 (v/v)]. After development, the TLC plate was observed under visible light (VIS) and ultraviolet light at 365/254 nm (UV365/UV254). Arrows and arrowheads indicate weakly colored components fluoresce red and not, respectively, under UV light. (PPTX 8904 kb)

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Kakinuma, M., Yasumoto, K., Suzuki, M. et al. Trivalent Iron Is Responsible for the Yellow Color Development in the Nacre of Akoya Pearl Oyster Shells. Mar Biotechnol 22, 19–30 (2020). https://doi.org/10.1007/s10126-019-09927-5

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