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新規分析ストラテジーによる海藻由来ハロゲン系抗菌成分の探索とヒト曝露評価

Research Project

Project/Area Number 21K12262
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Review Section Basic Section 63030:Chemical substance influence on environment-related
Research InstitutionDaiichi University, College of Pharmaceutical Sciences

Principal Investigator

藤井 由希子  第一薬科大学, 薬学部, 准教授 (80733542)

Co-Investigator(Kenkyū-buntansha) 原口 浩一  第一薬科大学, 薬学部, 特別研究員 (00258500)
小林 果  三重大学, 医学系研究科, 講師 (70542091)
原田 浩二  京都大学, 医学研究科, 准教授 (80452340)
小川 和加野  第一薬科大学, 薬学部, 教授 (90397878)
Project Period (FY) 2021-04-01 – 2025-03-31
Project Status Granted (Fiscal Year 2023)
Budget Amount *help
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2023: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
Fiscal Year 2022: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
Fiscal Year 2021: ¥1,560,000 (Direct Cost: ¥1,200,000、Indirect Cost: ¥360,000)
Keywords天然由来ハロゲン系化合物 / ハロゲン / 塩素 / 臭素 / Halogenated Compounds / 残留性有機化学物質 / フェノール性化合物 / ヒト曝露 / Naturally-occurring / 天然由来 / NHCs / 残留性有機化合物 / 環境保健 / 衛生化学 / 分析化学 / 曝露評価
Outline of Research at the Start

食用海藻が生産する抗菌性ハロゲン化合物について、ノンターゲット分析を用いた網羅的探索、ヒトへの曝露量の解明、抗菌作用評価と腸内細菌叢との関連性の検討を行う。

Outline of Annual Research Achievements

海洋生態系によって生産される有機化合物には、陸生生態系が生産するものとは異なり、ハロゲンである塩素原子や臭素原子を豊富に含む化合物群がある。これらは天然由来ハロゲン系化合物(NHCs; Naturally-occurring Halogenated Compounds)と呼ばれている。その一部は人工の環境汚染物質(PCB類や臭素系難燃剤等)やその代謝物(hydroxy-PCBやhydroxy-PBDE等)、人工の抗菌剤(トリクロサン等)に類似したあるいは同一の構造を有している。このことからNHCsによるヒトへの健康影響が考えられるが、その詳細な生理活性やヒトへの曝露実態は明らかではない。さらに未同定のNHCsも環境中に存在すると考えられている。NHCsには、メトキシ基をもつ無極性NHCsと一つ以上のヒドロキシ基を持つフェノール性NHCsが存在する。本研究ではいまだ情報の少ないフェノール性NHCsを中心に新規化合物の探索、その生理活性の解明、食用海藻や海洋生態系での生物濃縮を通じたヒトへの曝露実態の把握を行うことを目的としている。
1年目の2021年度は海産物(海藻、海綿、貝類等)を対象にハロゲン固有のスペクトルパターンを用いたノンターゲットスクリーニングを行ったところ、新規フェノール性NHCsとして7および8臭素化体のbrominated dihydroxylated diphenoxybenzenes (diOH-BDPBs)を発見した(Environmental pollution 2021, 289, 117933)。2年目の2022年度はNHCsのヒト曝露実態を明らかにするために、食事中のNHCsとヒト血清中のNHCsの測定を行った。日本人の食事中にはNHCが検出され、食用魚介類由来であると考えられた。また血清中にもNHCsは検出された。3年目の2023年度は2年目の結果(食事中のNHCs)の論文報告(Exposure Health 2023. https://doi.org/10.1007/s12403-023-00604-6)を行うとともに、次年度に行う抗菌活性スクリーニングの準備を行った。

Current Status of Research Progress
Current Status of Research Progress

3: Progress in research has been slightly delayed.

Reason

2021年度は海綿から新規のフェノール性NHCsを見出すことができた(Environmental pollution 2021, 289, 117933)。2年目の2022年度はNHCsのヒト曝露実態を明らかにするために、食事中のNHCsとヒト血清中のNHCsの測定を行った。3年目の2023年度は2年目の結果(食事中のNHCs)の論文報告(Exposure Health 2023. https://doi.org/10.1007/s12403-023-00604-6)を行うとともに、抗菌活性スクリーニングの準備を行った。

Strategy for Future Research Activity

2023年度は食事中のNHCsの論文報告(Exposure Health 2023. https://doi.org/10.1007/s12403-023-00604-6)を行うとともに、次年度に行う抗菌活性スクリーニングの準備を行った。2024年度はそれぞれ検出された物質の抗菌活性の評価を行う。

Report

(3 results)
  • 2023 Research-status Report
  • 2022 Research-status Report
  • 2021 Research-status Report
  • Research Products

    (39 results)

All 2024 2023 2022 2021 Other

All Int'l Joint Research (3 results) Journal Article (25 results) (of which Int'l Joint Research: 12 results,  Peer Reviewed: 25 results,  Open Access: 11 results) Presentation (11 results) (of which Int'l Joint Research: 2 results,  Invited: 2 results)

  • [Int'l Joint Research] アントワープ大学(ベルギー)

    • Related Report
      2023 Research-status Report
  • [Int'l Joint Research] アントワープ大学(ベルギー)

    • Related Report
      2022 Research-status Report
  • [Int'l Joint Research] アントワープ大学(ベルギー)

    • Related Report
      2021 Research-status Report
  • [Journal Article] Temporal trends in exposure to parabens, benzophenones, triclosan, and triclocarban in adult females in Kyoto, Japan, from 1993 to 20162024

    • Author(s)
      Yoshida Nao、Lyu Zhaoqing、Kim Sungmin、Park Nayoun、Hitomi Toshiaki、Fujii Yukiko、Kho Younglim、Choi Kyungho、Harada Kouji H.
    • Journal Title

      Environmental Science and Pollution Research

      Volume: - Issue: 25 Pages: 37050-37059

    • DOI

      10.1007/s11356-024-33627-w

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Levels and spatial profile of per- and polyfluoroalkyl substances in edible shrimp products from Japan and neighboring countries; a potential source of dietary exposure to humans2024

    • Author(s)
      Fujii Yukiko、Kato Yoshihisa、Miyatake Masayuki、Akeda Syunpei、Nagata Sigeru、Ando Junpei、Kido Katsumi、Ohta Chiho、Koga Nobuyuki、Harada Kouji H.、Haraguchi Koichi
    • Journal Title

      Environment International

      Volume: - Pages: 108685-108685

    • DOI

      10.1016/j.envint.2024.108685

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Changes in Carbon, Nitrogen, and Oxygen Stable Isotope Ratios and Mercury Concentrations in Killer Whales (Orcinus orca) during and after Lactation2024

    • Author(s)
      Endo Tetsuya、Kimura Osamu、Terasaki Masaru、Kato Yoshihisa、Fujii Yukiko、Haraguchi Koichi
    • Journal Title

      Journal of Marine Science and Engineering

      Volume: 12 Issue: 4 Pages: 623-623

    • DOI

      10.3390/jmse12040623

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Detection of Bromochloro Alkanes in Indoor Dust Using a Novel CP-Seeker Data Integration Tool2024

    • Author(s)
      McGrath Thomas J.、Saint-Vanne Julien、Hutinet S?bastien、Vetter Walter、Poma Giulia、Fujii Yukiko、Dodson Robin E.、Johnson-Restrepo Boris、Muenhor Dudsadee、Le Bizec Bruno、Dervilly Gaud、Covaci Adrian、Cariou Ronan
    • Journal Title

      Analytical Chemistry

      Volume: 96 Issue: 12 Pages: 4942-4951

    • DOI

      10.1021/acs.analchem.3c05800

    • Related Report
      2023 Research-status Report
    • Peer Reviewed
  • [Journal Article] Bioaccumulation and biotransformation of plasticisers diisononyl phthalate and di(2-ethylhexyl) terephthalate in black soldier fly larvae reared on (micro)plastic-contaminated food waste2024

    • Author(s)
      Lievens Siebe、Yin Shanshan、Belova Lidia、Fujii Yukiko、Bombeke Jasper、Smet Jeroen De、Borght Mik Van Der、Covaci Adrian、Poma Giulia
    • Journal Title

      Journal of Environmental Exposure Assessment

      Volume: 3 Issue: 1

    • DOI

      10.20517/jeea.2023.46

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Dietary Exposure to Dicofol, Endosulfan, and Naturally Produced Halogenated Bipyrroles: 24-hr Food Duplicate Surveys from Five Prefectures in Japan2023

    • Author(s)
      Fujii Yukiko、Harada Kouji H.、Kato Yoshihisa、Kimura Osamu、Endo Tetsuya、Haraguchi Koichi
    • Journal Title

      Exposure and Health

      Volume: Oct 17 Issue: 4 Pages: 989-999

    • DOI

      10.1007/s12403-023-00604-6

    • Related Report
      2023 Research-status Report
    • Peer Reviewed
  • [Journal Article] An international investigation of chlorinated paraffin concentrations and homologue distributions in indoor dust2023

    • Author(s)
      McGrath Thomas J.、Poma Giulia、Hutinet S?bastien、Fujii Yukiko、Dodson Robin E.、Johnson-Restrepo Boris、Muenhor Dudsadee、Dervilly Gaud、Cariou Ronan、Covaci Adrian
    • Journal Title

      Environmental Pollution

      Volume: 333 Pages: 121994-121994

    • DOI

      10.1016/j.envpol.2023.121994

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Carbon, nitrogen, and oxygen stable isotope ratios of striped dolphins and short-finned pilot whales stranded in Hokkaido, northern Japan, compared with those of other cetaceans stranded and hunted in Japan2023

    • Author(s)
      Endo Tetsuya, Kimura Osamu、Terasaki Masaru、Nakagun Shotaro、Kato Yoshihisa、Fujii Yukiko、Haraguchi Koichi、Baker C. Scott
    • Journal Title

      Isotopes in Environmental and Health Studies

      Volume: 59 Issue: 3 Pages: 230-247

    • DOI

      10.1080/10256016.2023.2234590

    • Related Report
      2023 Research-status Report
    • Peer Reviewed
  • [Journal Article] Profiles and determinants of dicofol, endosulfans, mirex, and toxaphenes in breast milk samples from 10 prefectures in Japan2023

    • Author(s)
      Fujii Yukiko、Harada Kouji H.、Ito Yoshiko、Yoshitake Miho、Matsunobu Chiharu、Kato Yoshihisa、Ohta Chiho、Koga Nobuyuki、Kimura Osamu、Endo Tetsuya、Koizumi Akio、Haraguchi Koichi
    • Journal Title

      Chemosphere

      Volume: 311 Pages: 137002-137002

    • DOI

      10.1016/j.chemosphere.2022.137002

    • Related Report
      2022 Research-status Report
    • Peer Reviewed
  • [Journal Article] Temporal trends in bisphenol exposures and associated health risk among Japanese women living in the Kyoto area from 1993 to 20162023

    • Author(s)
      Lyu Zhaoqing、Harada Kouji H.、Kim Sungmin、Fujitani Tomoko、Hitomi Toshiaki、Pan Rui、Park Nayoun、Fujii Yukiko、Kho Younglim、Choi Kyungho
    • Journal Title

      Chemosphere

      Volume: 316 Pages: 137867-137867

    • DOI

      10.1016/j.chemosphere.2023.137867

    • Related Report
      2022 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Chlorinated persistent organic pollutants in human breast milk in the Miyagi Prefecture disaster-affected area 1 year after the Great East Japan Earthquake of 20112023

    • Author(s)
      Choi Jungmi、Fujii Yukiko、Lyu Zhaoqing、Kobayashi Hatasu、Fujitani Tomoko、Harada Kouji H.
    • Journal Title

      Environmental Health and Preventive Medicine

      Volume: 28 Issue: 0 Pages: 27-27

    • DOI

      10.1265/ehpm.22-00260

    • ISSN
      1342-078X, 1347-4715
    • Related Report
      2022 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] チャイニーズハムスター肝ミクロゾームによるTetrachlorobiphenylの代謝2023

    • Author(s)
      太田千穂;加藤善久;原口浩一;藤井由希子;木村治;古賀信幸
    • Journal Title

      福岡医学雑誌

      Volume: 114

    • Related Report
      2022 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] 2,2′,3,4′,5′,6-六塩素化ビフェニル(CB149)のラット,ハムスター, モルモットおよびヒトにおける in vitro 代謝の比較研究2023

    • Author(s)
      太田千穂;原口浩一;加藤善久;藤井由希子;木村治;古賀信幸
    • Journal Title

      福岡医学雑誌

      Volume: 114

    • Related Report
      2022 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Occurrence and contamination profile of legacy and emerging per- and polyfluoroalkyl substances (PFAS) in Belgian wastewater using target, suspect and non-target screening approaches2022

    • Author(s)
      Jeong Yunsun、Da Silva Katyeny Manuela、Iturrospe Elias、Fuiji Yukiko、Boogaerts Tim、van Nuijs Alexander L.N.、Koelmel Jeremy、Covaci Adrian
    • Journal Title

      Journal of Hazardous Materials

      Volume: 437 Pages: 129378-129378

    • DOI

      10.1016/j.jhazmat.2022.129378

    • Related Report
      2022 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Levels of Short- and Medium-Chain Chlorinated Paraffins in Edible Insects and Implications for Human Exposure2022

    • Author(s)
      McGrath Thomas J.、Fujii Yukiko、Jeong Yunsun、Bombeke Jasper、Covaci Adrian、Poma Giulia
    • Journal Title

      Environmental Science & Technology

      Volume: 56 Issue: 18 Pages: 13212-13221

    • DOI

      10.1021/acs.est.2c03255

    • Related Report
      2022 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Exposure to phthalate esters in Japanese females in Kyoto, Japan from 1993 to 2016: Temporal trends and associated health risks2022

    • Author(s)
      Lyu Zhaoqing、Harada Kouji H.、Kim Sungmin、Fujitani Tomoko、Cao Yang、Hitomi Toshiaki、Fujii Yukiko、Kho Younglim、Choi Kyungho
    • Journal Title

      Environment International

      Volume: 165 Pages: 107288-107288

    • DOI

      10.1016/j.envint.2022.107288

    • Related Report
      2022 Research-status Report 2021 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Letter to the editor on “Global performance and trends of research on per- and polyfluoroalkyl substances (PFASs) between 2001 and 2018 using bibliometric analysis”: How can we identify PFAS studies?2022

    • Author(s)
      Fujii Yukiko、Fujitani Tomoko、Zou Xiaoli、Harada Kouji H.
    • Journal Title

      Chemosphere

      Volume: 306 Pages: 135130-135130

    • DOI

      10.1016/j.chemosphere.2022.135130

    • Related Report
      2022 Research-status Report
    • Peer Reviewed
  • [Journal Article] Comment on “Associations of Prenatal Exposure to Per- and Polyfluoroalkyl Substances with the Neonatal Birth Size and Hormones in the Growth Hormone/Insulin-Like Growth Factor Axis”: What Is the Origin of PFHxS Found in the Human Body?2022

    • Author(s)
      Fujii Yukiko、Harada Kouji H.、Trzcinski Antoine P.
    • Journal Title

      Environmental Science & Technology

      Volume: 56 Issue: 8 Pages: 5283-5284

    • DOI

      10.1021/acs.est.1c08190

    • Related Report
      2022 Research-status Report 2021 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Metabolism of 2,2ʼ,4,4ʼ,6,6ʼ-Hexachlorobiphenyl (PCB155) by Rat, Guinea Pig and Human Liver Microsomes and Human Cytochrome P450s2021

    • Author(s)
      太田 千穂, 加藤 善久, 藤井 由希子, 原口 浩一, 木村 治, 古賀 信幸.
    • Journal Title

      福岡醫學雜誌

      Volume: 112 Issue: 2 Pages: 127-135

    • DOI

      10.15017/4483198

    • NAID

      120007124568

    • ISSN
      0016-254X
    • Year and Date
      2021-06-25
    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Identification of novel halogenated naturally occurring compounds in marine biota by high-resolution mass spectrometry and combined screening approaches.2021

    • Author(s)
      Belova L, Fujii Y, Cleys P, Smielowska M, Haraguchi K, Covaci A
    • Journal Title

      Environmental Pollution

      Volume: 289 Pages: 117933-117933

    • DOI

      10.1016/j.envpol.2021.117933

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Urinary equol levels are positively associated with urinary estradiol excretion in women2021

    • Author(s)
      Fujitani Tomoko、Fujii Yukiko、Lyu Zhaoqing、Harada Sassa Mariko、Harada Kouji H.
    • Journal Title

      Scientific Reports

      Volume: 11 Issue: 1 Pages: 19532-19532

    • DOI

      10.1038/s41598-021-98872-2

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Journal Article] Occurrence, patterns, and sources of hazardous organic chemicals in edible insects and insect-based food from the Japanese market2021

    • Author(s)
      Poma Giulia、Fujii Yukiko、Lievens Siebe、Bombeke Jasper、Gao Beibei、Jeong Yunsun、McGrath Thomas Jacob、Covaci Adrian
    • Journal Title

      Food and Chemical Toxicology

      Volume: 154 Pages: 112311-112311

    • DOI

      10.1016/j.fct.2021.112311

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Absence of Detectable Radionuclides in Breast Milk in Sendai, Japan in 2012 Even by High-Sensitivity Determination: Estimated Dose among Infants after the Fukushima Nuclear Disaster2021

    • Author(s)
      Lyu Zhaoqing、Soleman Sani Rachman、Fujitani Tomoko、Fujii Yukiko、Mahmoud Manal A. M.、Harada Kouji H.
    • Journal Title

      International Journal of Environmental Research and Public Health

      Volume: 18 Issue: 11 Pages: 1-8

    • DOI

      10.3390/ijerph18115825

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Systematic Review Protocol for the Current State of Chemical Exposure in Infants via Breast Milk, Artificial Milk and Dairy Products2021

    • Author(s)
      Mahmoud Manal A. M.、Abdel-Mohsein Hosnia、Mahmoud Usama、Lyu Zhaoqing、Soleman Sani Rachman、Li Meng、Fujitani Tomoko、Harada Sassa Mariko、Fujii Yukiko、Cao Yang、Hitomi Toshiaki、Harada Kouji H.
    • Journal Title

      International Journal of Environmental Research and Public Health

      Volume: 18 Issue: 9 Pages: 4436-4436

    • DOI

      10.3390/ijerph18094436

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Estimation of dietary intake and sources of organohalogenated contaminants among infants: 24-h duplicate diet survey in Fukuoka, Japan2021

    • Author(s)
      Fujii Y, Poma G, Malarvannan G, Soeda F, Toda A, Haraguchi K, Covaci A.
    • Journal Title

      Environmental Research

      Volume: 195 Pages: 110745-110745

    • DOI

      10.1016/j.envres.2021.110745

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] ラット肝ミクロゾームによるPCB138とPCB140の代謝比較2024

    • Author(s)
      太田千穂, 加藤善久, 藤井由希子, 原口浩一, 木村治, 古賀信幸
    • Organizer
      日本薬学会第144年会
    • Related Report
      2023 Research-status Report
  • [Presentation] Metabolism of 2,2',4,4',6,6'-Hexachlorobiphebnyl by Rat, Guinea Pig and Human Liver Microsomes and Human Cytochrome P4502023

    • Author(s)
      Chiho Ohta, Yoshihisa Kato, Yukiko Fujii, Koichi Haraguchi, Osamu Kimura, Nobuyuki Koga
    • Organizer
      Dioxin 2023
    • Related Report
      2023 Research-status Report
    • Int'l Joint Research
  • [Presentation] 天然由来の臭素系有機化合物6-OH-BDE47のヒト曝露と血中濃度2023

    • Author(s)
      藤井由希子, 原田浩二, 原口浩一, 小泉昭夫
    • Organizer
      第93回日本衛生学会学術総会
    • Related Report
      2022 Research-status Report
  • [Presentation] 日本および周辺国沿岸部のエビ可食部中の有機フッ素化合物濃度2023

    • Author(s)
      加藤善久, 藤井由希子, 宮城香寛, 岩村 昇, 跡部一孝, 原口浩一
    • Organizer
      第31回環境化学討論会(第2回環境化学物質3学会合同大会)
    • Related Report
      2022 Research-status Report
  • [Presentation] Caco-2細胞における排出トランスポーターの発現と輸送能に及ぼす 5,7-ジメトキシフラボンの影響2023

    • Author(s)
      木村 治, 町田 拓自, 柳 圭鉉, 足達 令昴, 太田 千穂, 古賀 信幸, 加藤 善久, 藤井 由希子, 原口 浩一, 遠藤 哲也, 飯塚 健治, 遠藤 泰
    • Organizer
      日本薬学会第143年会
    • Related Report
      2022 Research-status Report
  • [Presentation] 2,4,6-三塩素置換PCB異性体PCB168のラット肝ミクロゾームによる代謝2023

    • Author(s)
      太田 千穂, 加藤 善久, 藤井 由希子, 原口 浩一, 木村 治, 古賀 信幸
    • Organizer
      日本薬学会第143年会
    • Related Report
      2022 Research-status Report
  • [Presentation] 人工・天然の残留性有機ハロゲン化合物のヒト曝露の解明2023

    • Author(s)
      藤井由希子
    • Organizer
      第93回日本衛生学会学術総会
    • Related Report
      2022 Research-status Report
    • Invited
  • [Presentation] Identification of novel halogenated naturally occurring compounds in sea sponge by high-resolution mass spectrometry and combined screening approaches2022

    • Author(s)
      Belova Lidia, Fujii Yukiko, Cleys Paulien, Haraguchi Koichi, Covaci Adrian
    • Organizer
      17th International Symposium on Hyphenated Techniques in Chromatography and Separation Technology
    • Related Report
      2022 Research-status Report 2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] 2,2',4,4',5,6'-六塩素化ビフェニル(PCB154)のラット肝ミクロゾームによる代謝2022

    • Author(s)
      太田 千穂, 藤井 由希子, 原口 浩一, 加藤 善久, 木村 治, 古賀 信幸
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      藤井由希子
    • Organizer
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    • Invited
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Published: 2021-04-28   Modified: 2024-12-25  

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