Oxygen Reduction Reaction Performance Tuning on Pt Nanoparticle/MWCNT Catalysts by Gd Species
Oxygen Reduction Reaction Performance Tuning on Pt Nanoparticle/MWCNT Catalysts by Gd Species
复制标题
DOI：
10.1021/acs.jpcc.0c09308
复制
发表时间：
2020-12
影响因子：
3.7
通讯作者：
Kentaro Ichihashi;Satoshi Muratsugu;H. Matsui;K. Higashi;O. Sekizawa;T. Uruga;Mizuki Tada
中科院分区：
文献类型：
--
作者：
Kentaro Ichihashi;Satoshi Muratsugu;H. Matsui;K. Higashi;O. Sekizawa;T. Uruga;Mizuki Tada
在含有聚吡咯基质的多壁碳纳米管(MWCNTs)表面制备了Gd3+氢氧化物/氧化物功能化的铂纳米粒子，发现其在氧还原反应(ORR)中表现出显著的电催化性能。通过透射电子显微镜、电子能量损失谱扫描电子显微镜、X射线吸收精细结构和X射线光电子能谱的表征表明，Gd3+氢氧化物/氧化物物种与Pt0纳米粒子紧密相连。循环伏安法和潜在应用条件下的铂LIII边X射线吸收近边结构分析表明，所制备的铂纳米粒子-Gd氢氧化物/氧化物复合材料的ORR活性高于以类似方法制备的不含Gd的铂纳米粒子，Gd物种的修饰抑制了铂的氧化，加速了铂的氧化还原。还考察了Gd负载量对ORR性能的影响，发现存在一个最佳的Gd负载量，超过这个最佳负载量，Gd的进一步掺入会导致Gd3+结构域的聚集，并降低了铂纳米粒子的结晶度。
Fine Pt nanoparticles functionalized with Gd3+hydroxide/oxide species were prepared on multiwalled carbon nanotubes (MWCNTs) containing polypyrrole matrix overlayers and found to exhibit remarkable electrocatalytic performance in the oxygen reduction reaction (ORR). Characterization via transmission electron microscopy, scanning transmission electron microscopy with electron energy loss spectroscopy, X-ray absorption fine structure, and X-ray photoelectron spectroscopy revealed that the Gd3+hydroxide/oxide species were located in close proximity to the Pt0nanoparticles on the MWCNTs. The prepared Pt nanoparticle–Gd hydroxide/oxide composites exhibited superior ORR activity to Gd-free Pt nanoparticles prepared in a similar manner, and the decoration with the Gd species suppressed Pt oxidation and accelerated Pt oxide reduction, as demonstrated by cyclic voltammetry andin situPt LIII-edge X-ray absorption near-edge structure analysis under potential application. The effect of the Gd loading on the ORR performance was also examined, revealing the existence of an optimal Gd loading beyond which further Gd incorporation resulted in aggregation of the Gd3+domains and decreased crystallinity of the Pt nanoparticles.