Duchesne Paul N, Li Z Y, Deming Christopher P, Fung Victor, Zhao Xiaojing, Yuan Jun, Regier Tom, Aldalbahi Ali, Almarhoon Zainab, Chen Shaowei, Jiang De-En, Zheng Nanfeng, Zhang Peng
Department of Chemistry, Dalhousie University, Halifax, NS, Canada.
Nanoscale Physics Research Laboratory, School of Physics & Astronomy, University of Birmingham, Birmingham, UK.
Nat Mater. 2018 Nov;17(11):1033-1039. doi: 10.1038/s41563-018-0167-5. Epub 2018 Sep 24.
Bimetallic nanoparticles with tailored structures constitute a desirable model system for catalysts, as crucial factors such as geometric and electronic effects can be readily controlled by tailoring the structure and alloy bonding of the catalytic site. Here we report a facile colloidal method to prepare a series of platinum-gold (PtAu) nanoparticles with tailored surface structures and particle diameters on the order of 7 nm. Samples with low Pt content, particularly PtAu, exhibited unprecedented electrocatalytic activity for the oxidation of formic acid. A high forward current density of 3.77 A mg was observed for PtAu, a value two orders of magnitude greater than those observed for core-shell structured PtAu and a commercial Pt nanocatalyst. Extensive structural characterization and theoretical density functional theory simulations of the best-performing catalysts revealed densely packed single-atom Pt surface sites surrounded by Au atoms, which suggests that their superior catalytic activity and selectivity could be attributed to the unique structural and alloy-bonding properties of these single-atomic-site catalysts.
具有定制结构的双金属纳米颗粒构成了一种理想的催化剂模型体系，因为诸如几何效应和电子效应等关键因素可以通过定制催化位点的结构和合金键合来轻松控制。在此，我们报告了一种简便的胶体方法，用于制备一系列具有定制表面结构且粒径约为7纳米的铂 - 金（PtAu）纳米颗粒。低铂含量的样品，特别是PtAu，对甲酸氧化表现出前所未有的电催化活性。对于PtAu，观察到3.77 A mg的高正向电流密度，该值比核壳结构的PtAu和商业铂纳米催化剂所观察到的值大两个数量级。对性能最佳的催化剂进行的广泛结构表征和理论密度泛函理论模拟表明，密集排列的单原子铂表面位点被金原子包围，这表明它们优异的催化活性和选择性可归因于这些单原子位点催化剂独特的结构和合金键合性质。
