Qiao Wei, Yang Xudong, Li Meng, Feng Ligang
School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, 225002, China.
Nanoscale. 2021 Apr 14;13(14):6884-6889. doi: 10.1039/d1nr01005k. Epub 2021 Mar 30.
Methanol electrooxidation is significant in realizing effective C1 liquid fuel applications. Herein, hollow Pd/Te nanorods were fabricated and evaluated for methanol oxidation, and they were found to exhibit high catalytic efficiency for methanol oxidation in alkaline electrolyte compared to Pd or Pd/C catalysts. The hybrid structure of hexagonal crystal Te and face-centered cubic Pd was formed by microwave assisted Pd nanoparticle deposition over the surface of Te nanorods. Strong electronic effects and facile oxophilic properties were indicated in the Pd/Te system by spectroscopic analysis, which mainly accounts for the high catalytic performance for methanol oxidation. Specifically, they showed a peak current density of 90.1 mA cm for methanol oxidation, around 3.5 times higher than that of commercial Pd/C (26.3 mA cm). High catalytic stability was also observed for Pd/Te, with a current retention of 64.3% after 3600 s of chronoamperometric testing, much higher than for Pd catalysts (20.1%). High anti-CO poisoning ability of the Pd/Te catalyst was demonstrated in the CO-stripping voltammetry results, and faster catalytic kinetics were also observed for this catalyst system. The electron-rich state of Pd and high active site exposure are responsible for the high performance of the Pd/Te catalyst in methanol oxidation.
甲醇电氧化对于实现有效的C1液体燃料应用具有重要意义。在此,制备了中空的Pd/Te纳米棒并对其甲醇氧化性能进行了评估,结果发现与Pd或Pd/C催化剂相比,它们在碱性电解质中对甲醇氧化表现出高催化效率。通过微波辅助将Pd纳米颗粒沉积在Te纳米棒表面,形成了六方晶体Te和面心立方Pd的混合结构。光谱分析表明,Pd/Te体系具有强电子效应和易亲氧性质,这主要是其对甲醇氧化具有高催化性能的原因。具体而言,它们对甲醇氧化的峰值电流密度为90.1 mA cm,约为商业Pd/C(26.3 mA cm)的3.5倍。还观察到Pd/Te具有高催化稳定性,在计时电流测试3600 s后电流保留率为64.3%,远高于Pd催化剂(20.1%)。CO溶出伏安法结果表明Pd/Te催化剂具有高抗CO中毒能力,并且该催化剂体系还观察到更快的催化动力学。Pd的富电子状态和高活性位点暴露是Pd/Te催化剂在甲醇氧化中具有高性能的原因。