镧基稀土/碳纳米管复合物的氧还原催化性能
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摘要
铂催化剂已经商用化,但存储量稀缺、高成本、稳定性差等缺点,使其无法实现广泛而大规模的应用。因此,寻找新的催化剂具有非常重要的意义。在本论文中,以稀土化合物为催化剂,添加碳纳米管提高电导率,制备稀土负载量为0%、9.1%、12.5%、16.7%、25.0%和100%的镧基稀土/碳纳米管催化剂。采用CV、RDE、RRDE和I-t研究镧基稀土/碳纳米管的氧还原(ORR)催化活性。研究发现,镧基稀土负载量为12.5%的催化剂电极的氧还原催化活性最强。虽然镧基稀土/碳纳米管的ORR活性与20%Pt./C相比较弱,但其耐甲醇毒性强于20%Pt./C。
Platinum based catalysts are has been commercialized,but its natural reserve is scarce,high cost,poor stability restricts its application.Therefore,it is very important to find new catalysts.In this paper,rare earth(RE)composites were applied as electrocatalysts,and carbon nanotubes(CNTs)were added to improve its conductivity.RE/CNTs composites with the RE mass loading of 0%,9.1%,12.5%,16.7%,25.0% and 100% were prepared.CV,RDE,RRDE,I-t are used to measure the catalytic activity of RE/CNTs towards oxygen reduction reaction(ORR).It is found out that 12.5% RE/CNTs exhibits the highest ORR activity.Although the ORR activity of RE/CNTs is weaker than that of 20% Pt./C,the methanol tolerance of RE/CNTs is better.
Platinum based catalysts are has been commercialized,but its natural reserve is scarce,high cost,poor stability restricts its application.Therefore,it is very important to find new catalysts.In this paper,rare earth(RE)composites were applied as electrocatalysts,and carbon nanotubes(CNTs)were added to improve its conductivity.RE/CNTs composites with the RE mass loading of 0%,9.1%,12.5%,16.7%,25.0% and 100% were prepared.CV,RDE,RRDE,I-t are used to measure the catalytic activity of RE/CNTs towards oxygen reduction reaction(ORR).It is found out that 12.5% RE/CNTs exhibits the highest ORR activity.Although the ORR activity of RE/CNTs is weaker than that of 20% Pt./C,the methanol tolerance of RE/CNTs is better.
引文
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[2] 赵少宁,李艾华.铝空气电池的研究现状和应用前景[J].电源技术,2014,38(10):1969-1971.
[3] 张建,辛红星,宋春军,等.钠硫电池单体的循环测试研究[J].能源工程,2011,(5):1-3.
[4] Shao M,Chang Q,Dodelet J P,et al.Recent Advances in Electrocatalysts for Oxygen Reduction Reaction[J].Chemical Reviews,2016,116(6):3594-3657.
[5] Bing Y,Liu H,Zhang L,et al.Nanostructured Pt-alloy electrocatalysts for PEM fuel cell oxygen reduction reaction[J].Chemical Society Reviews,2010,39(6):2184-2202.
[6] Shen L L,Zhang G R,Miao S,et al.Core-Shell Nanostructured Au@NimPt2Electrocatalysts with Enhanced Activity and Durability for Oxygen Reduction Reaction[J].ACS Catalysis,2016,6(3):1680-1690.
[7] Liu X T,Zang K,Lu JW,et al.Determining the Effect of Plasma Pre-Treatment on Antimony Tin Oxide to Support Pt@Pd and the Oxygen Reduction Reaction Activity[J].ChemCatChem,2015,7(10):1543-1546.
[8] Xiang L,Luo Z,Hu C,et al.Gold Nanoparticle/Multiwalled Carbon Nanotube Hybrid as a Stable Catalyst for the Oxygen Reduction Reaction[J].Chemelectrochem,2018,5(7):1073-1079.
[9] Cuixia Y,Bing H,Li X,et al.Activating Ag by even more inert Au:a peculiar effect on electrocatalysis toward oxygen reduction in alkaline media[J].Chemical Communications,2013,49(94):11023-11025.
[10]Yongprapat S,Therdthianwong S.Therdthianwong A.RuO 2promoted Au/C catalysts for alkaline direct alcohol fuel cells[J].Electrochimica Acta,2012,83(12):87-93.
[11]Deng Y,Dong Y,Wang G,et al.Well-Defined ZIFDerived Fe-N Codoped Carbon Nanoframes as Efficient Oxygen Reduction Catalysts[J]. ACS Applied Materials &Interfaces,2017,9(11):9699-9709.
[12]Aijaz A,Masa J,Christoph Rsler,et al.Co@Co3O4Encapsulated in Carbon Nanotube-Grafted Nitrogen-Doped Carbon Polyhedra as an Advanced Bifunctional Oxygen Electrode[J].Angewandte Chemie International Edition,2016,55(12):4087-4091.
[13]Sun J Q,Yin H J,Liu P R,et al.Molecular engineering of Ni-/Co-porphyrin multilayers on reduced graphene oxide sheets as bifunctional catalysts for oxygen evolution and oxygen reduction reactions[J].Chemical Science,2016,7(9):5640-5646.
[14]Xiong W,Du F,Liu Y,et al.3-D Carbon Nanotube Structures Used as High Performance Catalyst for Oxygen Reduction Reaction[J].Journal of the American Chemical Society,2010,132(45):15839-15841.
[15]Ratso,Sander,Kruusenberg,et al.Highly active nitrogendoped few-layer graphene/carbon nanotube composite electrocatalyst for oxygen reduction reaction in alkaline media[J].Carbon,2014,73(7):361-370.