Fuel Cell Nanomaterials Center, University of Yamanashi, 4 Takeda, Kofu 400-8510, Japan.
Phys Chem Chem Phys. 2010 Apr 21;12(15):3806-14. doi: 10.1039/b923460h. Epub 2010 Feb 24.
Monodisperse Pt nanoparticles supported on a graphitized carbon black (GC; 150 m(2) g(-1)), which exhibits higher resistance to carbon corrosion than a conventional high-surface-area carbon black (CB; 800 m(2) g(-1)), were prepared by the nanocapsule method. Three kinds of 50 wt%-Pt loaded catalysts (our nanocapsule Pt/GC, a commercial Pt/GC, and a commercial Pt/CB) were subjected to the durability test by a standard potential step protocol (E = 0.9 V <--> 1.3 V vs. RHE, holding 30 s at each E, 1 min for one cycle) in N(2)-saturated 0.1 M HClO(4) solution at 25 degrees C. The oxygen reduction reaction (ORR) activities at these catalysts were evaluated from the hydrodynamic voltammograms in O(2)-saturated 0.1 M HClO(4) solution at 25 degrees C by the rotating ring-disk electrode technique. The kinetically-controlled mass activities (MA) for the ORR at these catalysts at E = 0.85 to 0.70 V vs. RHE were found to decrease in proportion to log [number of potential step cycles] from 100 to 5000 cycles. It was found that our nanpcapsule Pt/GC showed the highest durability; the time elapsed for the reduction of MA(0.8V) to 700 A g(-1) (ca. 1/2 of the initial MA(0.8V)) at our Pt/GC was 30 and 60 times longer than those for the commercial Pt/GC and Pt/CB, respectively. It was found that the most important factor leading to both high MA and high durability is highly dispersed state of Pt nanoparticles with uniform size over the whole surface of the corrosion-resistant GC support, to which our nanocapsule method has contributed greatly.
担载在石墨化炭黑(GC;比表面积为 150 m²/g)上的单分散 Pt 纳米粒子,其耐炭腐蚀能力高于常规高比表面积炭黑(CB;比表面积为 800 m²/g),采用纳米胶囊法制备。将三种 50wt%Pt 负载的催化剂(我们的纳米胶囊 Pt/GC、一种商业 Pt/GC 和一种商业 Pt/CB)在 25°C 的 N2饱和 0.1M HClO4溶液中通过标准电位阶跃法(E=0.9V<-->1.3V vs. RHE,每个 E 保持 30s,一个循环 1min)进行耐久性测试。通过旋转环盘电极技术在 25°C 的 O2饱和 0.1M HClO4溶液中从动力学控制的质量活性(MA)评估这些催化剂的氧还原反应(ORR)活性。发现这些催化剂在 E=0.85 到 0.70V vs. RHE 的 ORR 的动力学控制质量活性(MA)随着电位阶跃循环数的对数(从 100 到 5000 个循环)成比例降低。发现我们的纳米胶囊 Pt/GC 显示出最高的耐久性;在我们的 Pt/GC 上,MA(0.8V)降低到 700A g-1(约为初始 MA(0.8V)的 1/2)所需的时间比商用 Pt/GC 和 Pt/CB 分别延长了 30 倍和 60 倍。发现导致高 MA 和高耐久性的最重要因素是 Pt 纳米粒子在耐腐蚀 GC 载体整个表面上具有均匀尺寸的高度分散状态,我们的纳米胶囊方法对此做出了巨大贡献。