Monsalve Karen, Roger Magali, Gutierrez-Sanchez Cristina, Ilbert Marianne, Nitsche Serge, Byrne-Kodjabachian Deborah, Marchi Valérie, Lojou Elisabeth
Bioénergétique et Ingénierie des Protéines, UMR 7281, CNRS-AMU, 31 Chemin Aiguier, 13009 Marseille, France.
CINaM, Campus de Luminy, Case 913, 13288 Marseille Cedex 9, France.
Bioelectrochemistry. 2015 Dec;106(Pt A):47-55. doi: 10.1016/j.bioelechem.2015.04.010. Epub 2015 Apr 24.
For the first time, gold nanoparticle-based electrodes have been used as platforms for efficient immobilization of the [NiFe] hydrogenase from the hyperthermophilic bacterium Aquifex aeolicus. AuNPs were characterized by electronic microscopy, dynamic light scattering and UV-Vis spectroscopy. Two sizes around 20.0±5.3 nm and 37.2±4.3 nm nm were synthesized. After thiol-based functionalization, the AuNPs were proved to allow direct H2 oxidation over a large range of temperatures. A high current density up to 1.85±0.15 mA·cm(-2) was reached at the smallest AuNPs, which is 170 times higher than the one recorded at the bare gold electrode. The catalytic current was especially studied as a function of the AuNP size and amount, and procedure for deposition. A synergetic effect between the AuNP porous deposit and the increase surface area was shown. Compared to previously used nanomaterials such as carbon nanofibers, the covalent grafting of the enzyme on the thiol-modified gold nanoparticles was shown to enhance the stability of the hydrogenase. This bioanode was finally coupled to a biocathode where BOD from Myrothecium verrucaria was immobilized on AuNP-based film. The performance of the so-mounted H2/O2 biofuel cell was evaluated, and a power density of 0.25 mW·cm(-2) was recorded.
首次将基于金纳米颗粒的电极用作高效固定来自嗜热栖热菌的[NiFe]氢化酶的平台。通过电子显微镜、动态光散射和紫外可见光谱对金纳米颗粒进行了表征。合成了两种尺寸分别约为20.0±5.3纳米和37.2±4.3纳米的金纳米颗粒。经过基于硫醇的功能化后,证明金纳米颗粒在很宽的温度范围内都能实现直接的氢气氧化。在最小尺寸的金纳米颗粒上达到了高达1.85±0.15毫安·厘米⁻²的高电流密度,这比在裸金电极上记录的电流密度高170倍。特别研究了催化电流与金纳米颗粒尺寸、数量以及沉积过程的关系。结果表明金纳米颗粒多孔沉积物与增加的表面积之间存在协同效应。与先前使用的纳米材料如碳纳米纤维相比,酶在硫醇修饰的金纳米颗粒上的共价接枝显示出增强了氢化酶的稳定性。该生物阳极最终与一个生物阴极耦合,在该生物阴极上,疣孢漆斑菌的生化需氧量被固定在基于金纳米颗粒的薄膜上。对如此组装的氢氧生物燃料电池的性能进行了评估,记录到功率密度为0.25毫瓦·厘米⁻²。