Light-driven Lytic Polysaccharide Monooxygenase Catalysis Mediated by Type I Photosensitizers

IF 2.6 4区 生物学 Q3 BIOCHEMISTRY & MOLECULAR BIOLOGY
ChemBioChem Pub Date : 2024-10-24 DOI:10.1002/cbic.202400486
Ana Gabriela Veiga Sepulchro, Milena Moreira Vacilotto, Lucas D. Dias, Vanessa O. A. Pellegrini, Josman Velasco., Natalia M. Inada, Fernando Segato, Igor Polikarpov
{"title":"Light-driven Lytic Polysaccharide Monooxygenase Catalysis Mediated by Type I Photosensitizers","authors":"Ana Gabriela Veiga Sepulchro,&nbsp;Milena Moreira Vacilotto,&nbsp;Lucas D. Dias,&nbsp;Vanessa O. A. Pellegrini,&nbsp;Josman Velasco.,&nbsp;Natalia M. Inada,&nbsp;Fernando Segato,&nbsp;Igor Polikarpov","doi":"10.1002/cbic.202400486","DOIUrl":null,"url":null,"abstract":"<p>The use of light as abundant, renewable, and clean energy source to boost lytic polysaccharide monooxygenase (LPMO) reactions represents an exciting and yet under-explored opportunity. Herein we demonstrated that photosensitizers, commonly used in photodynamic therapy, which act through the photocatalytic Type I mechanism can drive the oxidation of PASC by LPMOs, whereas Type II photosensitizers are not capable of promoting the LPMO activity. We analyzed Type I and Type II photosensitizers (methylene blue and tetraiodide salt of <i>meso</i>-tetrakis-(4-<i>N</i>-methylpyridyl) porphyrin, respectively) and demonstrated that, even without an addition of external reductant, Type I was capable of boosting <i>Thermothelomyces thermophila Mt</i>LPMO9A activity in the presence of light. We also evaluated the photobiosystem in the presence and/or absence of molecular oxygen (O<sub>2</sub>) and hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>), and investigated the role of superoxide radical in the methylene blue fueled reactions. Furthermore, we demonstrated that sodium bisulfite (NaHSO<sub>3</sub>), a chemical scavenger of H<sub>2</sub>O<sub>2</sub>, acts by safeguarding the enzyme from oxidative damage caused by accumulation of H<sub>2</sub>O<sub>2</sub> early in photosensitizer-driven LPMO reactions. Finally, the results of the present work demonstrated that light-driven LPMO reactions mediated photodynamic therapy (PDT) Type I photosensitizers, which also includes molecules such as curcumin and riboflavin, is a general phenomenon.</p>","PeriodicalId":140,"journal":{"name":"ChemBioChem","volume":"25 23","pages":""},"PeriodicalIF":2.6000,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ChemBioChem","FirstCategoryId":"99","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/cbic.202400486","RegionNum":4,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"BIOCHEMISTRY & MOLECULAR BIOLOGY","Score":null,"Total":0}
引用次数: 0

Abstract

The use of light as abundant, renewable, and clean energy source to boost lytic polysaccharide monooxygenase (LPMO) reactions represents an exciting and yet under-explored opportunity. Herein we demonstrated that photosensitizers, commonly used in photodynamic therapy, which act through the photocatalytic Type I mechanism can drive the oxidation of PASC by LPMOs, whereas Type II photosensitizers are not capable of promoting the LPMO activity. We analyzed Type I and Type II photosensitizers (methylene blue and tetraiodide salt of meso-tetrakis-(4-N-methylpyridyl) porphyrin, respectively) and demonstrated that, even without an addition of external reductant, Type I was capable of boosting Thermothelomyces thermophila MtLPMO9A activity in the presence of light. We also evaluated the photobiosystem in the presence and/or absence of molecular oxygen (O2) and hydrogen peroxide (H2O2), and investigated the role of superoxide radical in the methylene blue fueled reactions. Furthermore, we demonstrated that sodium bisulfite (NaHSO3), a chemical scavenger of H2O2, acts by safeguarding the enzyme from oxidative damage caused by accumulation of H2O2 early in photosensitizer-driven LPMO reactions. Finally, the results of the present work demonstrated that light-driven LPMO reactions mediated photodynamic therapy (PDT) Type I photosensitizers, which also includes molecules such as curcumin and riboflavin, is a general phenomenon.

Abstract Image

由 I 型光敏剂介导的光驱动溶解多糖单氧化酶催化。
利用光这种丰富、可再生的清洁能源来促进溶菌多糖单加氧酶(LPMO)反应是一个令人兴奋但尚未得到充分探索的机会。在这里,我们证明了光动力疗法中常用的光敏剂(通过光催化 I 型机制起作用)可以推动 LPMOs 氧化 PASC,而 II 型光敏剂则不能促进 LPMO 的活性。我们分析了 I 型和 II 型光敏剂(分别是亚甲基蓝和介-四-(4-N-甲基吡啶基)卟啉的四碘盐),结果表明,即使不添加外部还原剂,I 型光敏剂也能在光照条件下提高嗜热热酵母菌 MtLPMO9A 的活性。我们还评估了存在和/或不存在分子氧(O2)和过氧化氢(H2O2)时的光生物系统,并研究了超氧自由基在亚甲基蓝助燃反应中的作用。此外,我们还证明了亚硫酸氢钠(NaHSO3)是一种 H2O2 的化学清除剂,它能保护酶免受光敏剂驱动的 LPMO 反应早期 H2O2 积累造成的氧化损伤。最后,本研究结果表明,光动力疗法(PDT)I型光敏剂(也包括姜黄素和核黄素等分子)介导的光驱动LPMO反应是一种普遍现象。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 求助全文
来源期刊
ChemBioChem
ChemBioChem 生物-生化与分子生物学
CiteScore
6.10
自引率
3.10%
发文量
407
审稿时长
1 months
期刊介绍: ChemBioChem (Impact Factor 2018: 2.641) publishes important breakthroughs across all areas at the interface of chemistry and biology, including the fields of chemical biology, bioorganic chemistry, bioinorganic chemistry, synthetic biology, biocatalysis, bionanotechnology, and biomaterials. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and supported by the Asian Chemical Editorial Society (ACES).
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信