Unspecific peroxygenases immobilized on Pd-loaded three-dimensional ordered macroporous (3DOM) titania photocatalyst for photo-enzyme integrated catalysis

被引:47
作者
Deng, Xuewu [1 ]
Zheng, Xiaobing [1 ]
Jia, Feifei [1 ]
Cao, Cuiyao [1 ]
Song, Haolei [2 ]
Jiang, Yanjun [1 ]
Liu, Yunting [1 ]
Liu, Guanhua [1 ]
Li, Shijie [3 ]
Wang, Lihui [1 ,4 ]
机构
[1] Hebei Univ Technol, Sch Chem Engn & Technol, Tianjin 300401, Peoples R China
[2] Hebei Yanuo Biosci Co Ltd Shares, 19 Alishan St,Econ & Technol Dev Zone, Shijiazhuang 052165, Hebei, Peoples R China
[3] Zhejiang Ocean Univ, Natl Engn Res Ctr Marine Aquaculture, Zhoushan 316022, Zhejiang, Peoples R China
[4] Tianjin Modern Vocat Technol Coll, Dept Biochem Engn, 3 Yaguan Rd, Tianjin 300350, Peoples R China
来源
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2023年 / 330卷
基金
中国国家自然科学基金;
关键词
Photo-enzyme integrated catalyst; 3DOM; Enzyme immobilization; Chiral synthesis; TiO2; HYDROGEN-PEROXIDE; DEGRADATION; IRRADIATION; REDUCTION; MECHANISM; SILICA; TIO2;
D O I
10.1016/j.apcatb.2023.122622
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The selective oxyfunctionalization of C-H and C--C bonds is highly important and catalyzed by unspecific peroxygenases (UPOs) which suffer from inactivation by hydrogen peroxide (H2O2). Herein, photo-enzyme in-tegrated catalysts were constructed by immobilizing AaeUPO as cross-linked enzyme aggregates (CLEAs) in Pd-loaded three-dimensional ordered macroporous titania (3DOM TiO2) with in situ photocatalytic H2O2 produc-tion. The prepared AaeUPO@3DOM TiO2-Pd obtained higher catalytic efficiency compared with CLEAs-AaeUPO. The conversion of ethylbenzene to (R)-1-phenethyl alcohol was significantly improved, reaching 99 % compared with free enzyme (38 %) and CLEAs-AaeUPO (49 %), with ee value of > 99 %. AaeUPO@3DOM TiO2-Pd exhibited good stability and reusability attributed to the protection of macropores and in situ H2O2 production. By using the designed 3DOM platform for photocatalysis and enzyme immobilization, the in situ photocatalytic generation of H2O2 was highly efficient, and the monodisperse CLEAs-AaeUPO in the macropores facilitated the contact of substrate and enzyme, thus obtaining excellent photo-enzyme coupled catalysis.
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页数:12
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