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首页> 外文期刊>Catalysis science & technology >A thiophene-modified doubleshell hollow g-C3N4 nanosphere boosts NADH regeneration via synergistic enhancement of charge excitation and separation
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A thiophene-modified doubleshell hollow g-C3N4 nanosphere boosts NADH regeneration via synergistic enhancement of charge excitation and separation

机译：一个thiophene-modified g-C3N4双层外壳空洞nanosphere促进NADH再生通过协同激发和增强分离

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摘要

Low efficiency in photo-regeneration of redox-active cofactors is a crucial bottleneck in restricting artificial bio-photosynthesis of fuel systems from practical applications. We herein developed novel thiophene-modified doubleshell hollow g-C3N4 nanospheres (ATCN-DSCN) via synergistically enhancing both the charge excitation and separation processes to efficiently photo-regenerate nicotinamide adenine dinucleotide (NADH), which was then utilized as the cofactor by formate dehydrogenase (FDH) to reduce CO2 to form formic acid. The ATCN-DSCN material exhibited outstanding optical and photoelectrical properties, enabling a NADH yield of approximate to 74%, which was approximate to 40 times higher than that of the bulk C3N4 (approximate to 1.76%). ATCN-DSCN enabled a turnover frequency (TOF) of 2.950 h(-1), which, to the best of our knowledge, is the highest record of TOF for the photo-regeneration of NADH. For the artificial bio-photoreduction of CO2, sustainable conversion of CO2 to formic acid was achieved with a final formic acid concentration of 290.0 M after 9 hours of light illumination. The excellent optical and photoelectrical properties of the ATCN-DSCN were enabled by the synergistic effect between the specific porous multishell hollow structure and thiophene ring incorporation, which endowed ATCN-DSCN enhanced light absorption and improved charge separation with boosted photocatalytic regeneration of NADH.
机译：photo-regeneration效率低redox-active代数余子式是一个至关重要的瓶颈限制人工bio-photosynthesis的燃料从实际应用系统。开发新型thiophene-modified双层外壳空心g-C3N4团簇(ATCN-DSCN)通过既表现为协同作用增强激发和分离过程有效photo-regenerate烟酰胺腺嘌呤二核苷酸(NADH),然后利用甲酸脱氢酶的辅助因子(外籍)减少二氧化碳形成甲酸。表现出杰出的光学和材料光电的属性,使NADH的收益率大约74%的近似比散装C3N4高出40倍(大约1.76%)。周转频率(TOF) 2.950 h (1),我们所知,是最高的photo-regeneration TOF的NADH的记录。人工bio-photoreduction的二氧化碳,可持续的二氧化碳转换成甲酸通过最后的甲酸浓度290.0 9小时后光照明。优秀的光学和光电的ATCN-DSCN被启用的属性特定的多孔之间的协同效应multishell空心结构和噻吩环结合,赋予ATCN-DSCN增强光吸收和改进的电荷分离NADH的提高光催化再生。

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