Valorization of lignin components into gallate by integrated biological hydroxylation, O-demethylation, and aryl side-chain oxidation.
Valorization of lignin components into gallate by integrated biological hydroxylation, O-demethylation, and aryl side-chain oxidation.
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通过集成生物羟基化、O-去甲基化和芳基侧链氧化将木质素成分转化为没食子酸酯
DOI：
10.1126/sciadv.abg4585
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发表时间：
2021-09-03
期刊：
影响因子：
13.6
通讯作者：
Jin M
中科院分区：
文献类型：
--
作者：
Cai C;Xu Z;Zhou H;Chen S;Jin M
将生物羟基化、O-脱甲基化和芳基侧链氧化整合在一个细胞中用于木质素的增值。将木质素组分转化为单一产品是一种有前途的木质素升级方法。在这里，开发了一种有效的生物催化剂，选择性地从木质素组分产生没食子酸酯，通过整合三个主要反应：羟基化，O-脱甲基化，芳基侧链氧化。首先将一个合理设计的羟化酶系统引入没食子酸生物降解途径阻断的混浊红球菌突变株中，使原儿茶酸和其上游途径的化合物积累没食子酸。然后使用天然和异源0-脱甲基化系统，导致多种木质素衍生的甲氧基芳族化合物转化为没食子酸酯。此外，芳基侧链氧化酶参与拓宽底物谱。因此，开发的生物催化剂表明，没食子酸酯产率高达0.407和0.630克没食子酸每克木质素时，碱预处理的木质素和碱解聚氨纤维爆破木质素作为底物，分别。这些结果表明，这种合理开发的生物催化剂使木质素的稳定化过程简单而有效。
Biological hydroxylation, O-demethylation, and aryl side-chain oxidation were integrated in a cell for lignin valorization. Converting lignin components into a single product is a promising way to upgrade lignin. Here, an efficient biocatalyst was developed to selectively produce gallate from lignin components by integrating three main reactions: hydroxylation, O-demethylation, and aryl side-chain oxidation. A rationally designed hydroxylase system was first introduced into a gallate biodegradation pathway–blocked Rhodococcus opacus mutant so that gallate accumulated from protocatechuate and compounds in its upper pathways. Native and heterologous O-demethylation systems were then used, leading to multiple lignin-derived methoxy aromatics being converted to gallate. Furthermore, an aryl side-chain oxidase was engaged to broaden the substrate spectrum. Consequently, the developed biocatalyst showed that gallate yields as high as 0.407 and 0.630 g of gallate per gram of lignin when alkaline-pretreated lignin and base-depolymerized ammonia fiber explosion lignin were applied as substrates, respectively. These results suggested that this rationally developed biocatalyst enabled the lignin valorization process to be simple and efficient.
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影响因子：
8
作者：
Ellis ES;Hinchen DJ;Bleem A;Bu L;Mallinson SJB;Allen MD;Streit BR;Machovina MM;Doolin QV;Michener WE;Johnson CW;Knott BC;Beckham GT;McGeehan JE;DuBois JL
通讯作者：
DuBois JL
影响因子：
16.6
作者：
Elmore JR;Dexter GN;Salvachúa D;Martinez-Baird J;Hatmaker EA;Huenemann JD;Klingeman DM;Peabody GL 5th;Peterson DJ;Singer C;Beckham GT;Guss AM
通讯作者：
Guss AM
影响因子：
4.4
作者：
Cecil, Jacob H.;Garcia, David C.;Michener, Joshua K.
通讯作者：
Michener, Joshua K.
开发用于将木质素稳定为粘康酸的混浊红球菌细胞工厂
影响因子：
8.4
作者：
Cai, Chenggu;Xu, Zhaoxian;Jin, Mingjie
通讯作者：
Jin, Mingjie
影响因子：
8.4
作者：
Henson, William R.;Campbell, Tayte;Dantas, Gautam
通讯作者：
Dantas, Gautam