Rational design of biogenic PdxAuy nanoparticles with enhanced catalytic performance for electrocatalysis and azo dyes degradation.
Rational design of biogenic PdxAuy nanoparticles with enhanced catalytic performance for electrocatalysis and azo dyes degradation.
复制标题
DOI：
10.1016/j.envres.2021.112086
复制
发表时间：
2021-09
影响因子：
8.3
通讯作者：
Jinying Ma;Yaru Hou;Jianbo Guo;H. M. Sharif;Cong Huang;Jianhai Zhao;Haibo Li;Yuanyuan Song;Caicai Lu;Yi Han;Yousuo Zhang;Aijie Wang
中科院分区：
文献类型：
--
作者：
Jinying Ma;Yaru Hou;Jianbo Guo;H. M. Sharif;Cong Huang;Jianhai Zhao;Haibo Li;Yuanyuan Song;Caicai Lu;Yi Han;Yousuo Zhang;Aijie Wang
绿色的生物PdAu纳米粒子(Bio-PdAu NPs)在加氢反应中表现出显著的催化性能，这是人们非常希望看到的。然而，生物PdxAuyNPs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。本文报道了一种可控尺寸的生物合成PdxAuyNPs的简便合成策略以及对析氢反应和偶氮染料降解的催化原理。在生物合成过程中，通过预先设计Pd/Au的前驱体质量比，可以精确控制生物PdxAuyNPs的尺寸和组成，并且Au的比例与NPs的尺寸呈线性关系(R2=90.92)。得到的生物PdxAuyNPs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。对于电催化来说，促进细胞外电子转移的导电网络的形成是至关重要的。结果表明，生物型Pd2Au8具有良好的析氢电催化性能，最大电流密度为1.65mA/cm−2，是商用Pd/C(1.07mA/cm−2)的1.54倍。高的电催化活性归因于其合适的尺寸(81.38±66.14 nm)和均匀的分布在细胞表面，通过在催化剂和电极之间构建导电网络促进了胞外电子的转移。而在悬浮催化作用下，双金属纳米粒子的尺寸效应和协同效应对偶氮染料的降解效果更为显著。随着Au含量的增加，BIO-PdxAuy型催化剂的颗粒尺寸减小，催化活性显著提高。本研究提出的Bio-PdxAuy响应原理为合理设计具有更高催化性能的生物基双金属催化剂提供了可靠的参考。
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-PdxAuyNPs in response to various catalytic systems (electrocatalysis and suspension-catalysis) are unclear. Herein, a facile synthetic strategy for bio-PdxAuyNPs 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-PdxAuyNPs 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 (R2= 0.92). The obtained bio-PdxAuyNPs 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-Pd2Au8exhibited superior electrocatalytic performance in HER/toward hydrogen evolution, with a maximum current density of 1.65 mA cm−2, which was 1.54 times higher than that commercial Pd/C (1.07 mA cm−2). 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-PdxAuyimproved significantly. The response principles of bio-PdxAuyproposed in this study provide a reliable reference for the rational design of bio-based bimetallic catalysts with enhanced catalytic performance.