Gu Yunlong, St-Pierre Jean, Ploehn Harry J
Department of Chemical Engineering, University of South Carolina, Columbia, SC 29208, USA.
Langmuir. 2008 Nov 4;24(21):12680-9. doi: 10.1021/la802623q. Epub 2008 Oct 7.
Poly(styrene)-block-poly(2-vinylpyridine) (PS-b-P2VP) diblock copolymer was used as a micellar template to fabricate arrays of Pt nanoparticles on mica and glassy carbon (GC) supports. Polymer micellar deposition yields Pt nanoparticles with tunable particle size and surface number density on both mica and GC. After deposition of precursor-loaded micelles onto GC, oxygen plasma etching removes the polymer shell, followed by thermal treatment with H2 gas to reduce the Pt. Etching conditions were optimized to maximize removal of the polymer while minimizing damage to the GC. Arrays of Pt nanoparticles with controlled size and surface number density can be prepared on mica (for particle size characterization) and GC to make Pt/GC model catalysts. These model catalysts were characterized by tapping mode atomic force microscopy, X-ray photoelectron spectroscopy, and cyclic voltammetry to measure activity for oxidation of carbon monoxide or methanol. Cyclic voltammetry results demonstrate the existence of a correlation between Pt particle size and electrocatalytic properties including onset potential, tolerance of carbonaceous adsorbates, and intrinsic activity (based on active Pt area from CO stripping voltammetry). Results obtained with Pt/GC model catalysts duplicate prior results obtained with Pt/porous carbon catalysts therefore validating the synthesis approach and offering a new, tunable platform to study catalyst structure and other effects such as aging on proton exchange membrane fuel cell (PEMFC) reactions.
聚(苯乙烯)-嵌段-聚(2-乙烯基吡啶)(PS-b-P2VP)二嵌段共聚物被用作胶束模板,以在云母和玻碳(GC)载体上制备铂纳米颗粒阵列。聚合物胶束沉积可在云母和GC上产生粒径和表面数密度可调的铂纳米颗粒。将负载前驱体的胶束沉积到GC上后,氧等离子体蚀刻去除聚合物壳,然后用氢气进行热处理以还原铂。对蚀刻条件进行了优化,以在最大程度去除聚合物的同时,将对GC的损伤降至最低。可以在云母(用于粒径表征)和GC上制备尺寸和表面数密度可控的铂纳米颗粒阵列,以制造Pt/GC模型催化剂。通过轻敲模式原子力显微镜、X射线光电子能谱和循环伏安法对这些模型催化剂进行表征,以测量一氧化碳或甲醇氧化的活性。循环伏安法结果表明,铂颗粒尺寸与电催化性能之间存在相关性,这些电催化性能包括起始电位、对含碳吸附物的耐受性和本征活性(基于CO溶出伏安法的活性铂面积)。用Pt/GC模型催化剂获得的结果与用Pt/多孔碳催化剂获得的先前结果一致,因此验证了合成方法,并提供了一个新的、可调谐的平台来研究催化剂结构以及其他影响,如质子交换膜燃料电池(PEMFC)反应中的老化。