Intensifying electron utilization by surface-anchored rh complex for enhanced nicotinamide cofactor regeneration and photoenzymatic CO2 reduction
文献类型：期刊论文
| 作者 | Cheng, Yuqing3,4; Shi, Jiafu1,2,4; Wu, Yizhou3,4; Wang, Xueying1; Sun, Yiying3,4; Cai, Ziyi3,4; Chen, Yu1,4; Jiang, Zhongyi3 |
| 刊名 | Research
 |
| 出版日期 | 2021-02-18 |
| 卷号 | 2021 |
| 关键词 | Electrons - Image enhancement - Nucleotides - Carbon dioxide - Rhodium compounds - Adhesives - Light - Amides - Photocatalytic activity |
| ISSN号 | 20965168 |
| DOI | 10.34133/2021/8175709 |
| 英文摘要 | Solar-driven photocatalytic regeneration of cofactors, including reduced nicotinamide adenine dinucleotide (NADH), reduced nicotinamide adenine dinucleotide phosphate (NADPH), and reduced flavin adenine dinucleotide (FADH2), could ensure the sustainable energy supply of enzymatic reactions catalyzed by oxidoreductases for the efficient synthesis of chemicals. However, the elevation of cofactor regeneration efficiency is severely hindered by the inefficient utilization of electrons transferred on the surface of photocatalysts. Inspired by the phenomenon of ferredoxin-NADP+ reductase (FNR) anchoring on thylakoid membrane, herein, a homogeneous catalyst of rhodium (Rh) complex, [Cp鈭桼h(bpy)H2O]2+, was anchored on polymeric carbon nitride (PCN) mediated by a tannic acid/polyethyleneimine (TA/PEI) adhesive layer, acquiring PCN@TA/PEI-Rh core@shell photocatalyst. Illuminated by visible light, electrons were excited from the PCN core, then transferred through the TA/PEI shell, and finally captured by the surface-anchored Rh for instant utilization during the regeneration of NADH. The TA/PEI-Rh shell could facilitate the electron transfer from the PCN core and, more importantly, achieved ~1.3-fold elevation of electron utilization efficiency compared with PCN. Accordingly, the PCN@TA/PEI-Rh afforded the NADH regeneration efficiency of 37.8% after 20 min reaction under LED light (405 nm) illumination, over 1.5 times higher than PCN with free Rh. Coupling of the NADH regeneration system with formate dehydrogenase achieved continuous production of formate from carbon dioxide (CO2). Our study may provide a generic and effective strategy to elevate the catalytic efficiency of a photocatalyst through intensifying the electron utilization. Copyright 漏 2021 Yuqing Cheng et al. Exclusive Licensee Science and Technology Review Publishing House. Distributed under a Creative Commons Attribution License (CC BY 4.0). |
| 学科主题 | Carbon Nitride |
| 项目编号 | This work was supported by the National Natural Science Funds of China (21776213 and 21621004), the Natural Science Fund of Tianjin (19JCYBJC19700), the Open Funding Project of the State Key Laboratory of Biochemical Engineering (2020KF-06), the Open Funding Project of the State Key Laboratory of Chemical Engineering (SKL-ChE-19B01), the Tianjin Synthetic Biotechnology Innovation Capacity Improvement Project (TSBICIP-KJGG-003), and the Royal Society International Collaboration Award (ICA\R1\180317) for the financial support. The National Supercomputing Center in Shenzhen is acknowledged for the computational support. |
| 出版者 | American Association for the Advancement of Science |
| 源URL | [http://ir.ipe.ac.cn/handle/122111/60342]  |
| 作者单位 | 1.School of Environmental Science and Engineering, Tianjin University, 92 Weijin Road, Nankai District, Tianjin; 300072, China 2.State Key Laboratory of Biochemical Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing; 10090, China 3.Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, 92 Weijin Road, Nankai District, Tianjin; 300072, China 4.Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), 92 Weijin Road, Nankai District, Tianjin; 300072, China |
| 推荐引用方式 GB/T 7714 | Cheng, Yuqing,Shi, Jiafu,Wu, Yizhou,et al. Intensifying electron utilization by surface-anchored rh complex for enhanced nicotinamide cofactor regeneration and photoenzymatic CO2 reduction[J]. Research,2021,2021. |
| APA | Cheng, Yuqing.,Shi, Jiafu.,Wu, Yizhou.,Wang, Xueying.,Sun, Yiying.,...&Jiang, Zhongyi.(2021).Intensifying electron utilization by surface-anchored rh complex for enhanced nicotinamide cofactor regeneration and photoenzymatic CO2 reduction.Research,2021. |
| MLA | Cheng, Yuqing,et al."Intensifying electron utilization by surface-anchored rh complex for enhanced nicotinamide cofactor regeneration and photoenzymatic CO2 reduction".Research 2021(2021). |
入库方式： OAI收割
来源：过程工程研究所
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