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| Bioinspired Approach to Multienzyme Cascade System Construction for Efficient Carbon Dioxide Reduction | |
| Alternative Title | ACS Catal. |
| 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 | |
| 2014-03-01 | |
| Source Publication | ACS CATALYSIS
 |
| ISSN | 2155-5435 |
| Volume | 4Issue:3Pages:962-972 |
| Abstract | 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.; 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. |
| Keyword | Co2 Conversion Multienzyme Cascade System Mussel-inspired Chemistry Biomimetic Mineralization Hybrid Microcapsules |
| Subtype | Article |
| WOS Headings | Science & Technology ; Physical Sciences |
| DOI | 10.1021/cs401096c |
| URL | 查看原文 |
| Indexed By | SCI |
| Language | 英语 |
| WOS Keyword | RAY PHOTOELECTRON-SPECTROSCOPY ; GELATIN NANOPARTICLES ; ENZYME IMMOBILIZATION ; AMINO-ACIDS ; COATINGS ; CONVERSION ; HYDROGELS ; METHANOL ; CHEMISTRY ; MICROCAPSULES |
| WOS Research Area | Chemistry |
| WOS Subject | Chemistry, Physical |
| WOS ID | WOS:000332756700028 |
| Citation statistics | |
| Document Type | 期刊论文 |
| Version | 出版稿 |
| Identifier | http://ir.ipe.ac.cn/handle/122111/8041 |
| Collection | 研究所（批量导入） |
| Affiliation | 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 |
| Recommended Citation 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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| Bioinspired Approach（3951KB） | 限制开放 | CC BY-NC-SA | Application Full Text | |||
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