摘要
直接乙醇燃料电池(DEFCs)被认为是最有前途的便携式电源设备之一.目前用于DEFCs的主流催化剂是Pt基或Pd基催化剂,然而它们不能有效地断裂C–C键,只能使乙醇部分氧化为CH_(3)CHO或CH_(3)COOH.此外,大多数贵金属催化剂容易被反应中间体CO毒化,降低了催化剂的稳定性和寿命,这些因素都抑制了催化剂的实际应用.本文中,我们报道了一种用于乙醇氧化反应的具有不同Rh含量的超细三金属PtNiRh纳米线,Pt_(6)Ni_(2)Rh_(3)/C具有最优的催化活性(1.16 A mg_(Pt^(-1)))、抗CO中毒能力和稳定性.理论计算表明,在双金属PtNi中引入Rh,使得该催化剂具有良好的中间物吸附和C–C键断裂能力,有利于乙醇的完全氧化.
Direct ethanol fuel cells(DEFCs)are considered one of the most promising energy resources for portable power devices.The current mainstream catalysts used for DEFCs are Pt-or Pd-based,which facilitate the partial oxidation of ethanol to CH_(3)CHO or CH_(3)COOH,but not the C-C bond cleavage,which is the inevitable path for the complete oxidation of ethanol.In addition,most noble catalysts are easily poisoned by CO,shortening their lifespan and stability,thus inhibiting the practical application of the catalysts.Herein,we report a type of ultrathin trimetallic Pt/Ni/Rh nanowires with various Rh contents toward the ethanol oxidation reaction(EOR),and the optimized Pt_(6)Ni_(2)Rh_(3)/C demonstrates a high mass activity of 1.16 A mg_(Pt^(-1))as well as considerable stability,anti-CO poisoning ability,and complete ethanol oxidation selectivity.In addition,density functional theory calculations reveal that introducing Rh to bimetallic Pt/Ni endows the catalyst with a moderate intermediate adsorption capacity and enhanced C-C bond cleavage capacity,favorable for the complete oxidation of ethanol.
作者
王谦
朱润茜
邓培林
李静
黄玮
陈琦
苏亚琼
贾春满
刘钟馨
康振烨
沈义俊
田新龙
Qian Wang;Runxi Zhu;Peilin Deng;Jing Li;Wei Huang;Qi Chen;Ya-Qiong Su;Chunman Jia;Zhongxin Liu;Zhenye Kang;Yijun Shen;Xinlong Tian(State Key Laboratory of Marine Resource Utilization in South China Sea,Hainan Provincial Key Lab of Fine Chemistry,School of Chemical Engineering and Technology,Hainan University,Haikou 570228,China;School of Chemistry,Xi’an Key Laboratory of Sustainable Energy Materials Chemistry,MOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter,State Key Laboratory of Electrical Insulation and Power Equipment,Xi’an Jiaotong University,Xi’an 710049,China)
基金
supported by Hainan Province Science and Technology Special Fund(ZDYF2021GXJS207,ZDYF2020037,and 2020207)
the National Natural Science Foundation of China(22109034,22109035,52164028,and 62105083)
the Foundation of State Key Laboratory of Marine Resource Utilization in South China Sea(Hainan University,MRUKF2021029)
the specific research fund of the Innovation Platform for Academicians of Hainan Province
the“Young Talent Support Plan”of Xi’an Jiaotong University。
