化学
奥斯特瓦尔德成熟
化学工程
催化作用
电解
纳米颗粒
还原剂
聚乙二醇
粒子(生态学)
电催化剂
电解质
纳米技术
无机化学
电极
电化学
有机化学
物理化学
材料科学
工程类
地质学
海洋学
作者
Menglong Liu,Ying Kong,Huifang Hu,Noémi Kovács,Changzhe Sun,Iván Zelocualtecatl Montiel,María de Jesús Gálvez‐Vázquez,Yuhui Hou,Marta Mirolo,Isaac Martens,Jakub Drnec,Soma Vesztergom,Peter Broekmann
标识
DOI:10.1016/j.jcat.2021.10.016
摘要
We apply silver nanoparticles (Ag NPs) as catalysts of CO2 reduction in a zero-gap gas-flow electrolyser. Ag NPs stabilized by different ligands —branched polyethylenimine (BPEI), polyvinylpyrrolidone (PVP), polyethylene glycol (PEG), and citrate— are used in the experiments. The as-prepared NPs have almost identical initial size distributions, yet their catalytic performance, in terms of achievable current and CO selectivity, is different. During electrolysis all Ag NPs exhibit unambiguous morphology changes; the degradation pathway they follow, however, markedly depends on the chemical nature of the capping agent stabilizing them. Scanning electron micrographs obtained before and after constant-charge electrolyses carried out at different potentials reveal that amongst the studied ligands, BPEI seems to be the most effective stabilizer of Ag NPs; in turn, however, BPEI also limits CO formation the most. In case of PVP, mostly corrosion (particle shrinkage) is observed at practically relevant electrolysing potentials, while the application of PEG leads more to particle coalescence. Ostwald ripening seems to appear only at high applied (H2 forming) potentials in case of the three afore-mentioned ligands while in case of citrate it becomes significant already at mild (CO forming) voltages. By studying the effects of capping agent removal and exchange we demonstrate that apart from ligands directly attached to the Ag NPs, also the excess of capping agents (adsorbed on the electrode surface) plays a decisive role in determining the extent and mode of catalyst degradation. The results of SEM-based particle sizing are also confirmed by synchrotron based wide-angle X-ray scattering measurements that provide further insight into the evolution of crystallite size and lattice strain in the applied Ag NPs during electrolysis.
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