In order to enhance the Pd based anodic catalysts for direct formic acid fuel cells (DFAFCs), the research work includes increasing catalyst activity and preventing CO poison. In this study, various zirconium oxides-m...In order to enhance the Pd based anodic catalysts for direct formic acid fuel cells (DFAFCs), the research work includes increasing catalyst activity and preventing CO poison. In this study, various zirconium oxides-modified multi-walled carbon nanotubes (MWCNTs) were prepared as the supports of Pd catalysts for DFAFCs by adjusting the preparation parameters: metal adding, sintering temperature and atmospheres. The prepared pure zirconia has both monoclinic and tetragonal phases. The addition of MWCNTs depresses the growth of monoclinic phase. A small amount of Pd adding allows both monoclinic and tetragonal zirconia structures to appear again. Pd nanoparticles of 20 wt% synthesized on MWCNTs and tetragonal ZrO2/MWCNTs have similar particle size, while Pd/[Pd:ZrO2/AO-MWCNTs-300Air-900Ar] have more nanoparticles aggregation. The electrochemical surface area can be improved by adding zirconia which implies those zirconia modified Pd catalysts better electrocatalytic performance. By analyzing the maximum current density and the corresponding potential, Pd/AO-MWCNTs are inferred to undergo the formic acid direct oxidation initially. The Pd catalysts modified by tetragonal ZrO2 have higher current density. Those having both tetragonal and monoclinic ZrO2 modified Pd catalysts have lower potential of formic acid oxidation. All the Pd based catalysts with zirconia modification possess better CO resist ability and electrocatalytic activity. Pd/[ZrO2/AO-MWCNTs-300Air-900Ar] and Pd/[Pd:ZrO2/AO-MWCNTs-300Air-900Ar] which catalyze formic acid in direct oxidation path are the two best catalysts.展开更多
The electrochemical oxidation of formic acid has been attracting significant attention in the past few years due to the great potential prospect of direct formic acid fuel cell (DFAFC) in applications, including high ...The electrochemical oxidation of formic acid has been attracting significant attention in the past few years due to the great potential prospect of direct formic acid fuel cell (DFAFC) in applications, including high theoretical open circuit potential (1.48 V), low fuel crossover, high practical power densities at low temperature, facilitating of proton transport in catalyst layers and low toxicity [1-5].展开更多
Developing efficient and stable bimetallic Pdbased anode electrocatalysts toward formic acid oxidation(FAO)is of great significance for commercial applications of direct formic acid fuel cells(DFAFCs).Herein,we report...Developing efficient and stable bimetallic Pdbased anode electrocatalysts toward formic acid oxidation(FAO)is of great significance for commercial applications of direct formic acid fuel cells(DFAFCs).Herein,we report a facile synthesis approach to fabricate PdCu nanoclusters(NCs)catalysts with granular-film structure.The introduction of Cu can adjust the electronic structure and d-band center of Pd,which can improve the catalytic performance of the catalysts.Compared with Pd NCs catalyst,the catalytic durability and activity of PdCu NCs catalysts for FAO are greatly improved.The order for catalytic activity of NC metals is Pd_(85)Cu_(15)NCs>Pd_(70)Cu_(30)NCs>Pd NCs.The maximum mass activity can be acquired with the Pd_(85)Cu_(15)NCs catalyst,which is about1.7 times that of the Pd NCs catalyst.And Pd_(85)Cu_(15)NCs catalyst still maintains the highest catalytic current density after 50 cycles,indicating that Pd_(85)Cu_(15)NCs catalyst has the best durability and electrocatalytic activity for FAO.Our work provides a new prospect for the design of highly efficient anode catalysts materials for DFAFCs.展开更多
文摘In order to enhance the Pd based anodic catalysts for direct formic acid fuel cells (DFAFCs), the research work includes increasing catalyst activity and preventing CO poison. In this study, various zirconium oxides-modified multi-walled carbon nanotubes (MWCNTs) were prepared as the supports of Pd catalysts for DFAFCs by adjusting the preparation parameters: metal adding, sintering temperature and atmospheres. The prepared pure zirconia has both monoclinic and tetragonal phases. The addition of MWCNTs depresses the growth of monoclinic phase. A small amount of Pd adding allows both monoclinic and tetragonal zirconia structures to appear again. Pd nanoparticles of 20 wt% synthesized on MWCNTs and tetragonal ZrO2/MWCNTs have similar particle size, while Pd/[Pd:ZrO2/AO-MWCNTs-300Air-900Ar] have more nanoparticles aggregation. The electrochemical surface area can be improved by adding zirconia which implies those zirconia modified Pd catalysts better electrocatalytic performance. By analyzing the maximum current density and the corresponding potential, Pd/AO-MWCNTs are inferred to undergo the formic acid direct oxidation initially. The Pd catalysts modified by tetragonal ZrO2 have higher current density. Those having both tetragonal and monoclinic ZrO2 modified Pd catalysts have lower potential of formic acid oxidation. All the Pd based catalysts with zirconia modification possess better CO resist ability and electrocatalytic activity. Pd/[ZrO2/AO-MWCNTs-300Air-900Ar] and Pd/[Pd:ZrO2/AO-MWCNTs-300Air-900Ar] which catalyze formic acid in direct oxidation path are the two best catalysts.
基金supported by the National Natural Science Foundation of China (21433003, 21733004, U1601211, 21811530078)Jilin Province Science and Technology Development Program (20180101030JC, 20160622037JC, 20170203003SF)+1 种基金the Hundred Talents Program of Chinese Academy of Sciences and the Recruitment Program of Foreign Experts (WQ2012220007)RFBR (18-5353025)
文摘The electrochemical oxidation of formic acid has been attracting significant attention in the past few years due to the great potential prospect of direct formic acid fuel cell (DFAFC) in applications, including high theoretical open circuit potential (1.48 V), low fuel crossover, high practical power densities at low temperature, facilitating of proton transport in catalyst layers and low toxicity [1-5].
基金financially supported by the National Natural Science Foundation of China (No.51901197, 51971184 and 51771157)the Open Fund of Fujian Provincial Key Laboratory of Eco-Industrial Green Technology in Wuyi University (No.WYKF-EIGT2021-6)
文摘Developing efficient and stable bimetallic Pdbased anode electrocatalysts toward formic acid oxidation(FAO)is of great significance for commercial applications of direct formic acid fuel cells(DFAFCs).Herein,we report a facile synthesis approach to fabricate PdCu nanoclusters(NCs)catalysts with granular-film structure.The introduction of Cu can adjust the electronic structure and d-band center of Pd,which can improve the catalytic performance of the catalysts.Compared with Pd NCs catalyst,the catalytic durability and activity of PdCu NCs catalysts for FAO are greatly improved.The order for catalytic activity of NC metals is Pd_(85)Cu_(15)NCs>Pd_(70)Cu_(30)NCs>Pd NCs.The maximum mass activity can be acquired with the Pd_(85)Cu_(15)NCs catalyst,which is about1.7 times that of the Pd NCs catalyst.And Pd_(85)Cu_(15)NCs catalyst still maintains the highest catalytic current density after 50 cycles,indicating that Pd_(85)Cu_(15)NCs catalyst has the best durability and electrocatalytic activity for FAO.Our work provides a new prospect for the design of highly efficient anode catalysts materials for DFAFCs.
