Bioinspired Approach to Multienzyme Cascade System Construction for Efficient Carbon Dioxide Reduction
Wang, Xiaoli1,2,3; Li, Zheng1,3; Shi, Jiafu1,3; Wu, Hong1,3; Jiang, Zhongyi1,2,3; Zhang, Wenyan1,3; Song, Xiaokai1,3; Ai, Qinghong1,3
刊名ACS CATALYSIS
2014-03-01
卷号4期号:3页码:962-972
关键词CO2 conversion multienzyme cascade system mussel-inspired chemistry biomimetic mineralization hybrid microcapsules
ISSN号2155-5435
其他题名ACS Catal.
中文摘要An efficient multienzyme cascade system based on ultrathin, hybrid microcapsules was constructed for converting CO2 to methanol by combining the unique functions of catechol and gelatin. Gelatin was modified with catechol groups (GelC) via well-defined EDC/NHS chemistry, thus endowed with the ability to covalently attach enzyme molecules. Next, the first enzyme (FateDH)-containing CaCO3 templates were synthesized via coprecipitation and coated with a GelC layer. Afterward, GelC was covalently attached with the second enzyme (FaldDH) via Michael addition and Schiff base reactions. Then, GelC induced the hydrolysis and condensation of silicate, and the third enzyme (YADH) was entrapped accompanying the formation of silica particles. After removal of CaCO3 templates, the GelCSi-based multienzyme system was obtained, in which the three enzymes were appropriately positioned in different places of the GelCSi microcapsules, and the amount of individual enzyme was regulated according to enzyme activity. The system exhibited high activity and stability for converting CO2 into methanol. In detail, the system displayed much higher methanol yield and selectivity (71.6%, 86.7%) than that of multienzyme in free form (35.5%, 47.3%). The methanol yield remained 52.6% after nine times of recycling. This study will provide some guidance on constructing diverse scaffolds for applications in catalysis, drug and gene delivery, and biosensors.
英文摘要An efficient multienzyme cascade system based on ultrathin, hybrid microcapsules was constructed for converting CO2 to methanol by combining the unique functions of catechol and gelatin. Gelatin was modified with catechol groups (GelC) via well-defined EDC/NHS chemistry, thus endowed with the ability to covalently attach enzyme molecules. Next, the first enzyme (FateDH)-containing CaCO3 templates were synthesized via coprecipitation and coated with a GelC layer. Afterward, GelC was covalently attached with the second enzyme (FaldDH) via Michael addition and Schiff base reactions. Then, GelC induced the hydrolysis and condensation of silicate, and the third enzyme (YADH) was entrapped accompanying the formation of silica particles. After removal of CaCO3 templates, the GelCSi-based multienzyme system was obtained, in which the three enzymes were appropriately positioned in different places of the GelCSi microcapsules, and the amount of individual enzyme was regulated according to enzyme activity. The system exhibited high activity and stability for converting CO2 into methanol. In detail, the system displayed much higher methanol yield and selectivity (71.6%, 86.7%) than that of multienzyme in free form (35.5%, 47.3%). The methanol yield remained 52.6% after nine times of recycling. This study will provide some guidance on constructing diverse scaffolds for applications in catalysis, drug and gene delivery, and biosensors.
WOS标题词Science & Technology ; Physical Sciences
类目[WOS]Chemistry, Physical
研究领域[WOS]Chemistry
关键词[WOS]RAY PHOTOELECTRON-SPECTROSCOPY ; GELATIN NANOPARTICLES ; ENZYME IMMOBILIZATION ; AMINO-ACIDS ; COATINGS ; CONVERSION ; HYDROGELS ; METHANOL ; CHEMISTRY ; MICROCAPSULES
收录类别SCI
原文出处://WOS:000332756700028
语种英语
WOS记录号WOS:000332756700028
公开日期2014-05-06
内容类型期刊论文
版本出版稿
源URL[http://ir.ipe.ac.cn/handle/122111/8041]  
专题过程工程研究所_研究所(批量导入)
作者单位1.Tianjin Univ, Sch Chem Engn & Technol, Minist Educ, Key Lab Green Chem Technol, Tianjin 300072, Peoples R China
2.Chinese Acad Sci, Inst Proc Engn, Natl Key Lab Biochem Engn, Beijing 100190, Peoples R China
3.Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China
推荐引用方式
GB/T 7714
Wang, Xiaoli,Li, Zheng,Shi, Jiafu,et al. Bioinspired Approach to Multienzyme Cascade System Construction for Efficient Carbon Dioxide Reduction[J]. ACS CATALYSIS,2014,4(3):962-972.
APA Wang, Xiaoli.,Li, Zheng.,Shi, Jiafu.,Wu, Hong.,Jiang, Zhongyi.,...&Ai, Qinghong.(2014).Bioinspired Approach to Multienzyme Cascade System Construction for Efficient Carbon Dioxide Reduction.ACS CATALYSIS,4(3),962-972.
MLA Wang, Xiaoli,et al."Bioinspired Approach to Multienzyme Cascade System Construction for Efficient Carbon Dioxide Reduction".ACS CATALYSIS 4.3(2014):962-972.
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