Lee Chang Hyun, Lee So Young, Lee Young Moo, McGrath James E
School of Chemical Engineering, Hanyang University, Seoul 133-791, Korea.
Langmuir. 2009 Jul 21;25(14):8217-25. doi: 10.1021/la900406d.
An anode for direct methanol fuel cells was chemically tuned by tailoring an aqueous hydrocarbon catalyst (SPI-BT) binder instead of using a conventional perfluorinated sulfonic acid ionomer (PFSI). SPI-BT designed in triethylamine salt form showed lower proton conductivity than PFSI, but it was stable in the catalyst ink forming the aqueous colloids. The aqueous colloidal particle size of SPI-BT was much smaller than that of PFSI. The small SPI-BT colloidal particles contributed to forming small catalyst agglomerates and simultaneously reducing their pore volume. Consequently, the high filling level of binders in the pores, where Pt-Ru catalysts are mainly located on the wall and physically interconnected, resulted in increased electrochemical active surface area of the anode, leading to high catalyst utilization. In addition, the chemical affinity between the SPI-BT binder and the membrane material derived from their similar chemical structure induced a stable interface on the membrane-electrode assembly (MEA) and showed low electric resistance. Upon adding SPI-BT, the synergistic effect of high catalyst utilization, improved mass transfer behavior to Pt-Ru catalyst, and low interfacial resistance of MEA became greater than the influence of reduced proton conductivity in the electrochemical performance of single cells. The electrochemical performance of MEAs with SPI-BT anode was enhanced to almost the same degree or somewhat higher than that with PFSI at 90 degrees C.
通过定制水性烃类催化剂(SPI-BT)粘合剂而非使用传统的全氟磺酸离聚物(PFSI),对直接甲醇燃料电池的阳极进行了化学调整。以三乙胺盐形式设计的SPI-BT的质子传导率低于PFSI,但它在形成水性胶体的催化剂油墨中很稳定。SPI-BT的水性胶体粒径远小于PFSI。小的SPI-BT胶体颗粒有助于形成小的催化剂团聚体,同时减小其孔体积。因此,在Pt-Ru催化剂主要位于孔壁并物理互连的孔中,粘合剂的高填充水平导致阳极的电化学活性表面积增加,从而提高了催化剂利用率。此外,SPI-BT粘合剂与膜材料之间的化学亲和力源于它们相似的化学结构,在膜电极组件(MEA)上形成了稳定的界面,且电阻较低。添加SPI-BT后,在单电池的电化学性能方面,高催化剂利用率、改善的向Pt-Ru催化剂的传质行为以及MEA的低界面电阻的协同效应大于质子传导率降低的影响。在90℃时,具有SPI-BT阳极的MEA的电化学性能提高到与具有PFSI的MEA几乎相同的程度或略高。