Exploring Step-by-Step Assembly of Nanoparticle:Cytochrome Biohybrid Photoanodes.
Exploring Step-by-Step Assembly of Nanoparticle:Cytochrome Biohybrid Photoanodes.
复制标题
探索纳米颗粒的逐步组装：细胞色素生物杂化光射流。
DOI：
10.1002/celc.201700030
复制
发表时间：
2017-08
期刊：
影响因子：
4
通讯作者：
Jeuken LJC
中科院分区：
文献类型：
--
作者：
Hwang ET;Orchard KL;Hojo D;Beton J;Lockwood CWJ;Adschiri T;Butt JN;Reisner E;Jeuken LJC
将捕光半导体纳米颗粒（NPs）与氧化还原酶结合，已被证明可以创造人工光合系统，有望用于合成太阳能燃料。高量子产率需要从纳米颗粒到氧化还原蛋白质的有效电子转移，这是一种难以控制的特性。在这里，我们比较了染料敏化的TiO2纳米晶体或CdS量子点与光阳极上的两种十血红素细胞色素之间的结合和电子转移。通过制备用胺或羧酸官能团封端的NP来评估NP表面化学的影响。对于二氧化钛纳米晶体，结合到细胞色素是最佳的，当用羧酸配体封端时，而对于CdS量子点，观察到胺封端的配体壳层具有更好的粘附性。当使用用膦酸化联吡啶Ru（II）染料敏化的TiO 2纳米晶体时，观察到光电流取决于十血红素的氧化还原状态，证实电子通过十血红素导管从TiO 2纳米晶体转移到表面。相反，当使用CdS纳米颗粒时，光电流不依赖于十血红素的氧化还原状态，这与电子从CdS转移到光阳极绕过十血红素蛋白的模型一致。这些结果说明，尽管NPs纳米颗粒的有机壳严重影响与蛋白质材料的偶联，但偶联可能难以预测或工程化。
Coupling light‐harvesting semiconducting nanoparticles (NPs) with redox enzymes has been shown to create artificial photosynthetic systems that hold promise for the synthesis of solar fuels. High quantum yields require efficient electron transfer from the nanoparticle to the redox protein, a property that can be difficult to control. Here, we have compared binding and electron transfer between dye‐sensitized TiO2 nanocrystals or CdS quantum dots and two decaheme cytochromes on photoanodes. The effect of NP surface chemistry was assessed by preparing NPs capped with amine or carboxylic acid functionalities. For the TiO2 nanocrystals, binding to the cytochromes was optimal when capped with a carboxylic acid ligand, whereas for the CdS QDs, better adhesion was observed for amine capped ligand shells. When using TiO2 nanocrystals, dye‐sensitized with a phosphonated bipyridine Ru(II) dye, photocurrents are observed that are dependent on the redox state of the decaheme, confirming that electrons are transferred from the TiO2 nanocrystals to the surface via the decaheme conduit. In contrast, when CdS NPs are used, photocurrents are not dependent on the redox state of the decaheme, consistent with a model in which electron transfer from CdS to the photoanode bypasses the decaheme protein. These results illustrate that although the organic shell of NPs nanoparticles crucially affects coupling with proteinaceous material, the coupling can be difficult to predict or engineer.
登录
查看更多内容
影响因子：
8.4
作者：
Caputo CA;Wang L;Beranek R;Reisner E
通讯作者：
Reisner E
影响因子：
32.5
作者：
Badura, Adrian;Kothe, Tim;Roegner, Matthias
通讯作者：
Roegner, Matthias
DOI：
10.1073/pnas.1316156111
发表时间：
2014-01-14
影响因子：
11.1
作者：
Breuer, Marian;Rosso, Kevin M.;Blumberger, Jochen
通讯作者：
Blumberger, Jochen
影响因子：
4.9
作者：
Katz, E;Zayats, M;Lisdat, F
通讯作者：
Lisdat, F
影响因子：
19
作者：
Hwang, Ee Taek;Sheikh, Khizar;Orchard, Katherine L.;Hojo, Daisuke;Radu, Valentin;Lee, Chong-Yong;Ainsworth, Emma;Lockwood, Colin;Gross, Manuela A.;Adschiri, Tadafumi;Reisner, Erwin;Butt, Julea N.;Jeuken, Lars J. C.
通讯作者：
Jeuken, Lars J. C.