Intensifying Electron Utilization by Surface-Anchored Rh Complex for Enhanced Nicotinamide Cofactor Regeneration and Photoenzymatic CO2 Reduction
| العنوان: | Intensifying Electron Utilization by Surface-Anchored Rh Complex for Enhanced Nicotinamide Cofactor Regeneration and Photoenzymatic CO2 Reduction |
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| المؤلفون: | Yiying Sun, Yuqing Cheng, Yizhou Wu, Jiafu Shi, Zhongyi Jiang, Xueying Wang, Yu Chen, Ziyi Cai |
| المصدر: | Research Research, Vol 2021 (2021) |
| بيانات النشر: | AAAS, 2021. |
| سنة النشر: | 2021 |
| مصطلحات موضوعية: | Flavin adenine dinucleotide, Multidisciplinary, biology, Nicotinamide, 010405 organic chemistry, Science, NADH regeneration, macromolecular substances, 010402 general chemistry, Photochemistry, Formate dehydrogenase, 01 natural sciences, Cofactor, 0104 chemical sciences, Enzyme catalysis, chemistry.chemical_compound, Electron transfer, chemistry, biology.protein, Formate, Research Article |
| الوصف: | Solar-driven photocatalytic regeneration of cofactors, including reduced nicotinamide adenine dinucleotide (NADH), reduced nicotinamide adenine dinucleotide phosphate (NADPH), and reduced flavin adenine dinucleotide (FADH 2 ), 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 ∗ Rh(bpy)H 2 O] 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 (CO 2 ). Our study may provide a generic and effective strategy to elevate the catalytic efficiency of a photocatalyst through intensifying the electron utilization. |
| اللغة: | English |
| تدمد: | 2639-5274 |
| الوصول الحر: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::4a4d240c9c08af00aa8c32591bd2234dTest http://europepmc.org/articles/PMC7910525Test |
| حقوق: | OPEN |
| رقم الانضمام: | edsair.doi.dedup.....4a4d240c9c08af00aa8c32591bd2234d |
| قاعدة البيانات: | OpenAIRE |
| تدمد: | 26395274 |
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