Hitaishi Vivek Pratap, Mazurenko Ievgen, Vengasseril Murali Anjali, de Poulpiquet Anne, Coustillier Gaëlle, Delaporte Philippe, Lojou Elisabeth
Aix Marseille Univ, CNRS, BIP, Bioénergétique et Ingénierie des Protéines, UMR 7281, Marseille, France.
Aix Marseille Univ, CNRS, LP3, UMR 7341, Parc Scientifique et Technologique de Luminy, Marseille, France.
Front Chem. 2020 Jun 4;8:431. doi: 10.3389/fchem.2020.00431. eCollection 2020.
Redox enzymes can be envisioned as biocatalysts in various electrocatalytic-based devices. Among factors that play roles in bioelectrochemistry limitations, the effect of enzyme-enzyme neighboring interaction on electrocatalysis has rarely been investigated, although critical . We report in this work an in-depth study of gold nanoparticles prepared by laser ablation in the ultimate goal of determining the relationship between activity and enzyme density on electrodes. Nanosecond laser interaction with nanometric gold films deposited on indium tin oxide support was used to generate gold nanoparticles (AuNPs) free from any stabilizers. A comprehensive analysis of AuNP size and coverage, as well as total geometric surface vs. electroactive surface is provided as a function of the thickness of the treated gold layer. Using microscopy and electrochemistry, the long-term stability of AuNP-based electrodes in the atmosphere and in the electrolyte is demonstrated. AuNPs formed by laser treatment are then modified by thiol chemistry and their electrochemical behavior is tested with a redox probe. Finally, enzyme adsorption and bioelectrocatalysis are evaluated in the case of two enzymes, i.e., the bilirubin oxidase and the s laccase. Behaving differently on charged surfaces, they allow demonstrating the validity of laser treated AuNPs for bioelectrocatalysis.
氧化还原酶可被视为各种基于电催化的装置中的生物催化剂。在生物电化学局限性中起作用的因素中，酶与酶相邻相互作用对电催化的影响很少被研究，尽管这很关键。我们在这项工作中报告了对通过激光烧蚀制备的金纳米颗粒的深入研究，最终目的是确定电极上活性与酶密度之间的关系。纳秒激光与沉积在氧化铟锡载体上的纳米金膜相互作用，用于生成不含任何稳定剂的金纳米颗粒（AuNPs）。作为处理过的金层厚度的函数，提供了对AuNP尺寸和覆盖率以及总几何表面积与电活性表面积的综合分析。使用显微镜和电化学方法，证明了基于AuNP的电极在大气和电解质中的长期稳定性。然后通过硫醇化学修饰激光处理形成的AuNPs，并用氧化还原探针测试其电化学行为。最后，在两种酶（即胆红素氧化酶和漆酶）的情况下评估酶吸附和生物电催化。它们在带电表面上表现不同，这证明了激光处理的AuNPs用于生物电催化的有效性。
