Liu Chuqing, Adams Ethan, Li Zhiyang, Yu Peng, Wong Hsi-Wu, Gu Zhiyong
Department of Chemical Engineering , University of Massachusetts Lowell One University Ave. , Lowell , Massachusetts 01854 , United States.
Langmuir. 2019 Oct 29;35(43):13821-13832. doi: 10.1021/acs.langmuir.9b02060. Epub 2019 Oct 16.
In this research, a high performance, ionomer-free electrocatalyst based on vertically aligned palladium (Pd) nanowire array was developed as an anode electrode toward ethanol oxidation reaction (EOR) in an alkaline environment. Using a one-step electrodeposition method, the Pd nanowires with controlled length were obtained by varying the electrodeposition current density and the synthesis time. Scanning electron microcopy (SEM), energy dispersive X-ray spectroscopy (EDS), and X-ray powder diffraction (XRD) were employed to characterize the morphology, chemical composition, and crystal structure of the Pd nanowires. The length effects of the nanowires, in the range of 0.8-4.5 μm, and various metal substrates, such as Ag, Cu, Ni, and Ti, were investigated for their electrochemical activities. The results demonstrated that Ag was the most active substrate to facilitate the ethanol oxidation reaction of the Pd nanowire array (NWA) electrocatalyst, which could be related to its good electrical conductivity. The stability test of the Pd NWA/Ag over time for EOR was also carried out, and the catalytic activity was recovered after the electrode was replaced with a new ethanol solution. Electrochemical impedance spectroscopy (EIS) measurements were performed to provide insights in the electron transfer resistance between the electrode and analyte. Gas chromatography and UV-vis spectroscopy were employed to measure the concentration of chemical species, which helped elucidate the overall reaction mechanism on the electrode surfaces.
在本研究中,开发了一种基于垂直排列钯(Pd)纳米线阵列的高性能、无离子聚合物的电催化剂,作为碱性环境中乙醇氧化反应(EOR)的阳极电极。采用一步电沉积法,通过改变电沉积电流密度和合成时间,获得了长度可控的钯纳米线。利用扫描电子显微镜(SEM)、能量色散X射线光谱(EDS)和X射线粉末衍射(XRD)对钯纳米线的形貌、化学成分和晶体结构进行了表征。研究了长度在0.8 - 4.5μm范围内的纳米线以及各种金属基底(如Ag、Cu、Ni和Ti)的电化学活性。结果表明,Ag是促进钯纳米线阵列(NWA)电催化剂乙醇氧化反应的最活泼基底,这可能与其良好的导电性有关。还对Pd NWA/Ag在EOR过程中的稳定性进行了随时间的测试,并且在用新的乙醇溶液替换电极后,催化活性得以恢复。进行了电化学阻抗谱(EIS)测量,以深入了解电极与分析物之间的电子转移电阻。采用气相色谱和紫外可见光谱测量化学物质的浓度,这有助于阐明电极表面的整体反应机理。