铂合金纳米立方块催化剂的氧还原反应活性比较（英文）  

Comparison of Oxygen Reduction Reaction Activity of Pt-Alloy Nanocubes

作　　者：汤永安[1,3] 代琳[1] 邹受忠 Yongan Tang Lin Dai Shouzhong Zou(Department of Chemistry and Biochemistry, Miami University, Oxford, OH 45056,USA Department of Chemistry, American University, Washington DC 20016, USA Department of Chemistry, Oakland University, Rochester, M148039, USA)

机构地区：[1]美国迈阿密大学化学与生物化学系,牛津俄亥俄45056 [2]美国美利坚大学化学系,华盛顿特区20016 [3]美国奥克兰大学化学系,罗切斯特密歇根48039

出　　处：《电化学》2017年第2期199-206,共8页Journal of Electrochemistry

基　　金：supported by the US National Science Foundation(CHE 1156425,CHE 1559670)

摘　　要：氧还原反应是质子交换膜燃料电池和金属-空气电池的重要反应.贵金属铂(Pt)与元素周期表中第一排的非贵过渡金属(M)形成铂合金催化剂(PtM)可以提高氧还原反应活性.但是,有关活性的提高有多大程度上是来自合金元素的贡献却仍然存在争议.为研究合金元素对PtM催化活性的影响,本工作合成了颗粒形状与合金元素含量相似的铂锰(PtMn)、铂铁(PtFe)、铂钴(PtCo)和铂镍(PtNi)纳米立方块催化剂,并考察了不同铂合金催化剂在酸性介质中的氧还原反应活性.选择制备立方块形状纳米颗粒催化剂进行比较,可以将颗粒表面结构对催化活性的影响降到最小.结果表明,氧还原反应活性与铂d-能带中心值曲线呈现火山形关系,其中PtCo纳米立方块催化剂的活性最高.本文所得到的实验结果与基于d-能带理论框架已知表面的密度泛函理论计算结果一致.Alloying Pt with the first row non-noble transition metals has been demonstrated to increase the catalytic activity toward oxygen reduction reaction （ORR）, which is the cathode reaction of the proton exchange membrane fuel cells （PEMFCs） and metal-air batteries. However, how much the ORR activity improvement comes from the alloying elements remains controversial. In this paper, the nanocubes of PtMn, PtFe, PtCo, and PtNi with the similar size and composition were prepared and their ORR activities were explored, in order to investigate the effects of alloying elements on the catalytic activity. The use of cubic shape particles minimizes the contribution to the activity from particle surface structural difference. The results showed that the ORR activity vs. Pt d-band center plot had a volcano shape and PtCo nanocube is the most active. These observations are in harmony with density functional theory calculations on well-defined surfaces in the framework of the d-band theory.

关 键 词：铂合金纳米立方块 氧还原反应 质子交换膜燃料电池 d-能带理论 

分 类 号：O643.36[理学—物理化学] TB383.1[理学—化学]