首页> 中文期刊> 《物理化学学报》 >Pt纳米晶上CO电吸附及电氧化的表面增强红外吸收光谱研究

Pt纳米晶上CO电吸附及电氧化的表面增强红外吸收光谱研究

         

摘要

Electrochemical attenuated total reflection-surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) has been used to investigate the facet-dependent adsorption and oxidation of CO on the{100}-preferred Pt nanocrystals (NCs). The cyclic voltammogram for the synthesized and then cleaned Pt NCs in a sulfuric acid solution displayed four pairs of redox peaks. The peaks located at 0.26 and 0.36 V were attributed to interfacial hydrogen electro-adsorption/desorption processes on the short-and long-range Pt{100}domains, respectively. Furthermore, the Pt{100}and Pt{111}domains were estimated to account for 34%and 14%of the active sites on the surfaces of the Pt NCs, respectively, based on Bi and Ge irreversible adsorption methods. Potential-dependent spectral features can be used to differentiate the adsorption and oxidation processes of linearly adsorbed CO (COL) species on the three basic planes of the Pt NCs. COL species on the Pt{110}facets were oxidized preferential y, fol owed sequential y by those on the Pt{111}and Pt{100}facets. COL on Pt{100}required the highest overpotential for their oxidation.%为理解Pt纳米晶(NCs)表面上吸附与反应的结构效应,本文利用电化学衰减全反射-表面增强红外吸收光谱(ATR-SEIRAS)初步研究了{100}优先取向的Pt纳米晶表面CO电吸附和电氧化.合成并清洗过的Pt纳米晶在硫酸溶液中的循环伏安图出现了四对氧化还原峰,其中位于0.26和0.36 V的峰分别对应于短程有序和长程有序Pt{100}上的氢吸脱附.利用Bi、Ge不可逆吸附法估算出Pt{100}和Pt{111}纳米晶筹分别占34%和17%.在原位红外光谱研究中,首次分辨出线性吸附的CO (COL)物种在Pt纳米晶的三个基础小晶面上的振动谱峰.动电位光谱分析结果表明Pt{110}上吸附的COL优先电氧化,其次{111}上的COL发生氧化,而Pt{100}上COL氧化过电位最高.

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