Journal of the American Chemical Society·· 1 天前精选AI 评分58
叔丁醇微环境抑制木质素β-O-4键电催化断裂中的醛过度氧化
The Dual Role of tert-Butanol toward Highly Selective Electrocatalytic Oxidative Cleavage of Lignin β-O-4 Cα-Cβ Bond to Aromatic Aldehydes
AI 导读
研究者在pH 9水相电解液中加入45 vol.%叔丁醇，将木质素β-O-4键电催化氧化断裂的芳香醛选择性提升至最高96%，并适用于商用与合成电极材料。作者将高选择性归因于叔丁醇的两重作用：在电极界面形成疏水边界层抑制醛水合，以及淬灭会进一步氧化醛的活性氧。该策略还扩展到18种β-O-4、β-1和α-O-4木质素模型二聚体以及真实硫酸盐木质素。
推荐理由
原文用叔丁醇共溶剂在电极界面构建疏水边界层并淬灭活性氧，为抑制木质素解聚中醛的过度氧化提供了一条可迁移的微环境调控思路。
创新点
不同于依赖催化剂本身调控选择性的做法，该工作通过叔丁醇共溶剂在电极界面构建疏水边界层并淬灭活性氧，从微环境层面同时抑制醛水合与过度氧化，且对多种电极材料和木质素连接类型通用。
图表、补充材料与最终表述以原文为准。阅读原文
来源：Journal of the American Chemical Society · doi.org
%20Microsoft%20Corporation.%20Permission%20is%20hereby%20granted,%20free%20of%20charge,%20to%20any%20person%20obtaining%20a%20copy%20of%20this%20software%20and%20associated%20documentation%20files%20(the%20'Software'),%20to%20deal%20in%20the%20Software%20without%20restriction,%20including%20without%20limitation%20the%20rights%20to%20use,%20copy,%20modify,%20merge,%20publish,%20distribute,%20sublicense,%20and/or%20sell%20copies%20of%20the%20Software,%20and%20to%20permit%20persons%20to%20whom%20the%20Software%20is%20furnished%20to%20do%20so,%20subject%20to%20the%20following%20conditions:%20The%20above%20copyright%20notice%20and%20this%20permission%20notice%20shall%20be%20included%20in%20all%20copies%20or%20substantial%20portions%20of%20the%20Software.%20THE%20SOFTWARE%20IS%20PROVIDED%20'AS%20IS',%20WITHOUT%20WARRANTY%20OF%20ANY%20KIND,%20EXPRESS%20OR%20IMPLIED,%20INCLUDING%20BUT%20NOT%20LIMITED%20TO%20THE%20WARRANTIES%20OF%20MERCHANTABILITY,%20FITNESS%20FOR%20A%20PARTICULAR%20PURPOSE%20AND%20NONINFRINGEMENT.%20IN%20NO%20EVENT%20SHALL%20THE%20AUTHORS%20OR%20COPYRIGHT%20HOLDERS%20BE%20LIABLE%20FOR%20ANY%20CLAIM,%20DAMAGES%20OR%20OTHER%20LIABILITY,%20WHETHER%20IN%20AN%20ACTION%20OF%20CONTRACT,%20TORT%20OR%20OTHERWISE,%20ARISING%20FROM,%20OUT%20OF%20OR%20IN%20CONNECTION%20WITH%20THE%20SOFTWARE%20OR%20THE%20USE%20OR%20OTHER%20DEALINGS%20IN%20THE%20SOFTWARE%20--%3e%3csvg%20width='32'%20height='32'%20viewBox='0%200%2032%2032'%20fill='none'%20xmlns='http://www.w3.org/2000/svg'%3e%3cpath%20d='M20.3432%202.29289C20.1556%202.10536%2019.9013%202%2019.6361%202H7C5.89543%202%205%202.89543%205%204V28C5%2029.1046%205.89543%2030%207%2030H25C26.1046%2030%2027%2029.1046%2027%2028V9.36394C27%209.09872%2026.8946%208.84437%2026.7071%208.65683L20.3432%202.29289Z'%20fill='%23B4ACBC'/%3e%3cpath%20d='M19.6821%203.00001L7%203C6.44772%203%206%203.44772%206%204V28C6%2028.5523%206.44772%2029%207%2029L25%2029C25.5523%2029%2026%2028.5523%2026%2028V9.45333L19.6821%203.00001Z'%20fill='%23F3EEF8'/%3e%3cpath%20d='M9.5%2012H22.5C22.7761%2012%2023%2012.2239%2023%2012.5C23%2012.7761%2022.7761%2013%2022.5%2013H9.5C9.22386%2013%209%2012.7761%209%2012.5C9%2012.2239%209.22386%2012%209.5%2012ZM9.5%2015C9.22386%2015%209%2015.2239%209%2015.5C9%2015.7761%209.22386%2016%209.5%2016H22.5C22.7761%2016%2023%2015.7761%2023%2015.5C23%2015.2239%2022.7761%2015%2022.5%2015H9.5ZM9%2018.5C9%2018.2239%209.22386%2018%209.5%2018H22.5C22.7761%2018%2023%2018.2239%2023%2018.5C23%2018.7761%2022.7761%2019%2022.5%2019H9.5C9.22386%2019%209%2018.7761%209%2018.5ZM9.5%2021C9.22386%2021%209%2021.2239%209%2021.5C9%2021.7761%209.22386%2022%209.5%2022H17.5C17.7761%2022%2018%2021.7761%2018%2021.5C18%2021.2239%2017.7761%2021%2017.5%2021H9.5Z'%20fill='%23998EA4'/%3e%3cpath%20d='M26%209.45325H21.3892C20.4464%209.45325%2019.6821%208.68896%2019.6821%207.74614V3L26%209.45325Z'%20fill='%23CDC4D6'/%3e%3c/svg%3e){kind=small}
%20Microsoft%20Corporation.%20Permission%20is%20hereby%20granted,%20free%20of%20charge,%20to%20any%20person%20obtaining%20a%20copy%20of%20this%20software%20and%20associated%20documentation%20files%20(the%20'Software'),%20to%20deal%20in%20the%20Software%20without%20restriction,%20including%20without%20limitation%20the%20rights%20to%20use,%20copy,%20modify,%20merge,%20publish,%20distribute,%20sublicense,%20and/or%20sell%20copies%20of%20the%20Software,%20and%20to%20permit%20persons%20to%20whom%20the%20Software%20is%20furnished%20to%20do%20so,%20subject%20to%20the%20following%20conditions:%20The%20above%20copyright%20notice%20and%20this%20permission%20notice%20shall%20be%20included%20in%20all%20copies%20or%20substantial%20portions%20of%20the%20Software.%20THE%20SOFTWARE%20IS%20PROVIDED%20'AS%20IS',%20WITHOUT%20WARRANTY%20OF%20ANY%20KIND,%20EXPRESS%20OR%20IMPLIED,%20INCLUDING%20BUT%20NOT%20LIMITED%20TO%20THE%20WARRANTIES%20OF%20MERCHANTABILITY,%20FITNESS%20FOR%20A%20PARTICULAR%20PURPOSE%20AND%20NONINFRINGEMENT.%20IN%20NO%20EVENT%20SHALL%20THE%20AUTHORS%20OR%20COPYRIGHT%20HOLDERS%20BE%20LIABLE%20FOR%20ANY%20CLAIM,%20DAMAGES%20OR%20OTHER%20LIABILITY,%20WHETHER%20IN%20AN%20ACTION%20OF%20CONTRACT,%20TORT%20OR%20OTHERWISE,%20ARISING%20FROM,%20OUT%20OF%20OR%20IN%20CONNECTION%20WITH%20THE%20SOFTWARE%20OR%20THE%20USE%20OR%20OTHER%20DEALINGS%20IN%20THE%20SOFTWARE%20--%3e%3csvg%20width='32'%20height='32'%20viewBox='0%200%2032%2032'%20fill='none'%20xmlns='http://www.w3.org/2000/svg'%3e%3cpath%20d='M22.39%206.45001C20.1%206.45001%2018.07%207.53001%2016.76%209.20001V9.15001V8.73001H16.75C16.53%204.98001%2013.42%202%209.61%202H2C2%205.95%205.20001%209.15001%209.15001%209.15001H14.34V21.61H16.76V13.61H22.85C26.8%2013.61%2030%2010.41%2030%206.46001H22.39V6.45001Z'%20fill='%2386D72F'/%3e%3cpath%20d='M15.5501%2021C10.5854%2021%206.56024%2025.0252%206.56024%2029.9899H24.5499C24.5499%2025.0252%2020.5248%2021%2015.5501%2021Z'%20fill='%236D4534'/%3e%3c/svg%3e){kind=small}
%20Microsoft%20Corporation.%20Permission%20is%20hereby%20granted,%20free%20of%20charge,%20to%20any%20person%20obtaining%20a%20copy%20of%20this%20software%20and%20associated%20documentation%20files%20(the%20'Software'),%20to%20deal%20in%20the%20Software%20without%20restriction,%20including%20without%20limitation%20the%20rights%20to%20use,%20copy,%20modify,%20merge,%20publish,%20distribute,%20sublicense,%20and/or%20sell%20copies%20of%20the%20Software,%20and%20to%20permit%20persons%20to%20whom%20the%20Software%20is%20furnished%20to%20do%20so,%20subject%20to%20the%20following%20conditions:%20The%20above%20copyright%20notice%20and%20this%20permission%20notice%20shall%20be%20included%20in%20all%20copies%20or%20substantial%20portions%20of%20the%20Software.%20THE%20SOFTWARE%20IS%20PROVIDED%20'AS%20IS',%20WITHOUT%20WARRANTY%20OF%20ANY%20KIND,%20EXPRESS%20OR%20IMPLIED,%20INCLUDING%20BUT%20NOT%20LIMITED%20TO%20THE%20WARRANTIES%20OF%20MERCHANTABILITY,%20FITNESS%20FOR%20A%20PARTICULAR%20PURPOSE%20AND%20NONINFRINGEMENT.%20IN%20NO%20EVENT%20SHALL%20THE%20AUTHORS%20OR%20COPYRIGHT%20HOLDERS%20BE%20LIABLE%20FOR%20ANY%20CLAIM,%20DAMAGES%20OR%20OTHER%20LIABILITY,%20WHETHER%20IN%20AN%20ACTION%20OF%20CONTRACT,%20TORT%20OR%20OTHERWISE,%20ARISING%20FROM,%20OUT%20OF%20OR%20IN%20CONNECTION%20WITH%20THE%20SOFTWARE%20OR%20THE%20USE%20OR%20OTHER%20DEALINGS%20IN%20THE%20SOFTWARE%20--%3e%3csvg%20width='32'%20height='32'%20viewBox='0%200%2032%2032'%20fill='none'%20xmlns='http://www.w3.org/2000/svg'%3e%3cpath%20d='M4.71839%2018.0233C5.11525%2017.458%205.8952%2017.3215%206.46045%2017.7184L18.5318%2026.1936L17.0946%2028.2406L5.02328%2019.7653C4.45803%2019.3685%204.32152%2018.5885%204.71839%2018.0233Z'%20fill='%235092FF'/%3e%3cpath%20d='M18.5013%202.80347C18.8302%202.3598%2019.4615%202.25982%2019.9114%202.58017L21.5841%203.77124C22.034%204.09158%2022.1321%204.71094%2021.8032%205.15461L13.1102%2016.8809C12.4436%2017.7801%2011.1641%2017.9827%2010.2523%2017.3335C9.34053%2016.6842%209.14176%2015.429%209.80835%2014.5298L18.5013%202.80347Z'%20fill='%23636363'/%3e%3cpath%20d='M18.0472%203.66594C16.8384%203.31432%2015.3804%203.86071%2014.5971%204.91739L11.7749%208.7243L11.9999%2010.0001L10.6024%2010.306L10.3989%2010.5805C9.07399%2012.3677%209.47824%2014.8692%2011.3018%2016.1677C13.1254%2017.4662%2015.6778%2017.07%2017.0027%2015.2828L17.1623%2015.0675L16.9999%2013.5001H18.3242L18.4883%2013.2787C21.992%2013.9302%2023.8684%2016.851%2023.963%2019.8545C24.0149%2021.5041%2023.5209%2023.1307%2022.4806%2024.3899C21.4537%2025.6329%2019.8112%2026.6185%2017.3793%2026.8486C16.5451%2026.9276%2015.9304%2027.6956%2016.0062%2028.564C16.082%2029.4325%2016.8197%2030.0725%2017.6539%2029.9935C20.7829%2029.6974%2023.1847%2028.3804%2024.7802%2026.4491C26.3624%2024.5339%2027.069%2022.1145%2026.9946%2019.751C26.8719%2015.8564%2024.6058%2011.9837%2020.5048%2010.5586L21.2008%209.61967C21.9842%208.56299%2022.0639%207.03517%2021.3491%206.01708L18.0472%203.66594Z'%20fill='%23BEBEBE'/%3e%3cpath%20d='M2%2029.2C2%2027.4327%203.43269%2026%205.2%2026H26.8C28.5673%2026%2030%2027.4327%2030%2029.2C30%2029.6418%2029.6418%2030%2029.2%2030H2.8C2.35817%2030%202%2029.6418%202%2029.2Z'%20fill='%239B9B9B'/%3e%3cpath%20d='M11.7757%208.70947L18.3343%2013.4746L17.1588%2015.0927L10.6001%2010.3275L11.7757%208.70947Z'%20fill='%23D3D3D3'/%3e%3c/svg%3e){kind=small}