Tianjin Key Laboratory of Aquatic Science and Technology, School of Environmental and Municipal Engineering, Tianjin Chengjian University, Tianjin, 300384, China; National Technology Innovation Center of Synthetic Biology, Tianjin Institute of Industrial Biotechnology, Chinese Academy of Sciences, Tianjin, 300308, China.
Tianjin Key Laboratory of Aquatic Science and Technology, School of Environmental and Municipal Engineering, Tianjin Chengjian University, Tianjin, 300384, China; National Technology Innovation Center of Synthetic Biology, Tianjin Institute of Industrial Biotechnology, Chinese Academy of Sciences, Tianjin, 300308, China.
Environ Res. 2022 Mar;204(Pt B):112086. doi: 10.1016/j.envres.2021.112086. Epub 2021 Sep 22.
The green biogenic PdAu nanoparticles (bio-PdAu NPs) exhibits remarkable catalytic performance in hydrogenation, which is highly desired. However, the catalytic principles and effectiveness of bio-PdAu NPs in response to various catalytic systems (electrocatalysis and suspension-catalysis) are unclear. Herein, a facile synthetic strategy for bio-PdAu NPs synthesis with controlled size and the catalytic principles for hydrogen evolution reaction (HER) and azo dye degradation is reported. In the biosynthetic process, the size and composition of the bio-PdAu NPs could be precisely controlled by predesigning the precursor mass ratio of Pd/Au, and the Au proportion showed a linear relationship with the size of NPs (R = 0.92). The obtained bio-PdAu NPs exhibit variable activity in electrocatalysis (HER) and suspension-catalysis (azo dye degradation). For electrocatalysis, the formation of conductive networks that facilitates the extracellular electron transfer is crucial. It was revealed that the bio-PdAu exhibited superior electrocatalytic performance in HER/toward hydrogen evolution, with a maximum current density of 1.65 mA cm, which was 1.54 times higher than that commercial Pd/C (1.07 mA cm). The high electrocatalytic activity was attributed to its appropriate size (81.38 ± 6.14 nm) and uniform distribution on the cell surface, which promoted the extracellular electron transfer by constructing a conductive network between catalyst and electrode. However, for suspension-catalysis, the size effect and synergistic effect of bimetallic NPs have a more prominent effect on the degradation of azo dyes. As the increase of Au proportion the particle size decreases, and the catalytic activity of bio-PdAu improved significantly. The response principles of bio-PdAu proposed in this study provide a reliable reference for the rational design of bio-based bimetallic catalysts with enhanced catalytic performance.
绿色生物合成的 PdAu 纳米颗粒(bio-PdAu NPs)在加氢反应中表现出显著的催化性能,这是非常理想的。然而,bio-PdAu NPs 在各种催化体系(电催化和悬浮催化)中的催化原理和效果尚不清楚。本文报道了一种简便的生物合成策略,可控制尺寸并研究了其在析氢反应(HER)和偶氮染料降解中的催化原理。在生物合成过程中,可以通过预设计 Pd/Au 前驱体的质量比来精确控制 bio-PdAu NPs 的尺寸和组成,并且 Au 比例与 NPs 的尺寸呈线性关系(R = 0.92)。所获得的 bio-PdAu NPs 在电催化(HER)和悬浮催化(偶氮染料降解)中表现出不同的活性。对于电催化,形成有利于细胞外电子转移的导电网络至关重要。结果表明,bio-PdAu 在 HER/析氢反应中表现出优异的电催化性能,最大电流密度为 1.65 mA cm,比商业 Pd/C(1.07 mA cm)高 1.54 倍。高电催化活性归因于其适当的尺寸(81.38 ± 6.14 nm)和在细胞表面的均匀分布,通过在催化剂和电极之间构建导电网络促进了细胞外电子转移。然而,对于悬浮催化,双金属 NPs 的尺寸效应和协同效应对偶氮染料的降解具有更显著的影响。随着 Au 比例的增加,粒径减小,bio-PdAu 的催化活性显著提高。本研究提出的 bio-PdAu 响应原理为设计具有增强催化性能的基于生物的双金属催化剂提供了可靠的参考。