†Graduate School of Science and Technology, Kumamoto University, Kumamoto 860-8555, Japan.
‡Kumamoto Institute for Photo-Electro Organics, Kumamoto 862-0901, Japan.
Anal Chem. 2015;87(10):5417-21. doi: 10.1021/acs.analchem.5b00858. Epub 2015 May 7.
Achieving oxygen reduction at high positive potentials with fast heterogeneous electron transfer is desirable for the biocathode of fuel cells based on enzymes. Here, we present an effective interface for obtaining direct electron transfer from a laccase (Lac)-based cathode for O2 reduction, starting from a potential very close to the redox equilibrium potential of the oxygen/water couple. The interface between Lac and single-walled carbon nanotubes was improved by modification with the steroid biosurfactant sodium cholate. The heterogeneous electron-transfer rate between the type-1 Cu site of Lac and the modified electrode was determined to be 3000 s(-1). The electron-transfer rate was sensitive to the side chain of the steroid biosurfactant, and the rate decreased more than 10-fold when sodium deoxycholate was used as the side chain.
对于基于酶的燃料电池的生物阴极而言,在高正电势下实现氧还原并伴有快速的非均相电子转移是非常理想的。在这里,我们提出了一种有效的界面,可从非常接近氧/水偶联的氧化还原平衡电势的电势开始,从基于漆酶(Lac)的阴极获得氧还原的直接电子转移。通过用甾体生物表面活性剂胆酸钠修饰,改善了 Lac 与单壁碳纳米管之间的界面。确定 Lac 的 I 型 Cu 位与修饰电极之间的非均相电子转移速率为 3000 s(-1)。电子转移速率对甾体生物表面活性剂的侧链敏感,当使用脱氧胆酸钠作为侧链时,速率降低了 10 多倍。