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Investigating the use of conducting oligomers and redox molecules in CdS–MoFeP biohybrids
Nanoscale Advances ( IF 4.7 ) Pub Date : 2020-12-28 , DOI: 10.1039/d0na00678e
Alexander W Harris 1 , Shambojit Roy 1 , Saheli Ganguly 1 , Ashray V Parameswar 2 , Francisco W S Lucas 1 , Adam Holewinski 1, 3 , Andrew P Goodwin 1, 2 , Jennifer N Cha 1, 2
Affiliation  

In this work we report the effect of incorporating conducting oligophenylenes and a cobaltocene-based redox mediator on photodriven electron transfer between thioglycolic acid (TGA) capped CdS nanorods (NR) and the native nitrogenase MoFe protein (MoFeP) by following the reduction of H+ to H2. First, we demonstrate that the addition of benzidine-a conductive diphenylene- to TGA-CdS and MoFeP increased catalytic activity by up to 3-fold as compared to CdS–MoFeP alone. In addition, in comparing the use of oligophenylenes composed of one (p-phenylenediamine), two (benzidine) or three (4,4′′-diamino-p-terphenyl)phenylene groups, the largest gain in H2 was observed with the addition of benzidine and the lowest with phenylenediamine. As a comparison to the conductive oligophenylenes, a cobaltocene-based redox mediator was also tested with the TGA-CdS NRs and MoFeP. However, adding either cobaltocene diacid or diamine caused negligible gains in H2 production and at higher concentrations, caused a significant decrease. Agarose gel electrophoresis revealed little to no detectable interaction between benzidine and TGA-CdS but strong binding between cobaltocene and TGA-CdS. These results suggest that the tight binding of the cobaltocene mediator to CdS may hinder electron transfer between CdS and MoFe and cause the mediator to undergo continuous reduction/oxidation events at the surface of CdS.

中文翻译:

研究导电低聚物和氧化还原分子在 CdS-MoFeP 生物杂化物中的应用

在这项工作中,我们报告了结合导电低聚苯和基于钴茂的氧化还原介质对巯基乙酸 (TGA) 封端的 CdS 纳米棒 (NR) 和天然固氮酶 MoFe 蛋白 (MoFeP) 之间的光驱动电子转移的影响,方法是减少 H +到 H 2。首先,我们证明与单独的 CdS-MoFeP 相比,向 TGA-CdS 和 MoFeP 添加联苯胺 - 一种导电二亚苯基 - 可将催化活性提高 3 倍。此外,在比较使用由一个(对苯二胺)、两个(联苯胺)或三个(4,4''-二氨基-对-三联苯)亚苯基组成的低聚亚苯基时,H 2的最大增益在加入联苯胺时观察到,而在苯二胺时最低。作为与导电低聚苯的比较,还使用 ​​TGA-CdS NRs 和 MoFeP 测试了基于钴茂的氧化还原介质。然而,添加茂钴二酸或二胺对 H 2产量的影响可以忽略不计,而在较高浓度下,则会导致显着下降。琼脂糖凝胶电泳显示联苯胺和 TGA-CdS 之间几乎没有可检测到的相互作用,但钴茂和 TGA-CdS 之间的结合力很强。这些结果表明,茂钴介体与 CdS 的紧密结合可能会阻碍 CdS 和 MoFe 之间的电子转移,并导致介体在 CdS 表面发生连续的还原/氧化事件。
更新日期:2021-01-21
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