The high-performance anodic electrocatalysts is pivotal for realizing the commercial application of the direct formic acid fuel cells.In this work,a simple polyethyleneimine-assisted galvanic replacement reaction is a...The high-performance anodic electrocatalysts is pivotal for realizing the commercial application of the direct formic acid fuel cells.In this work,a simple polyethyleneimine-assisted galvanic replacement reaction is applied to synthesize the high-quality PtTe alloy nanowires(PtTe NW)by using Te NW as an efficient sacrificial template.The existence of Te atoms separates the continuous Pt atoms,triggering a direct reaction pathway of formic acid electrooxidation reaction(FAEOR)at PtTe NW.The one-dimensional architecture and highly active sites have enabled PtTe NW to reveal outstanding electrocatalytic activity towards FAEOR with the mass/specific activities of 1091.25 mA mg^(-1)/45.34 A m^(-2)at 0.643 V potential,which are 44.72/23.16 and 20.26/11.75 times bigger than those of the commercial Pt and Pd nanoparticles,respectively.Density functional theory calculations reveal that Te atoms optimize the electronic structure of Pt atoms,which decreases the adsorption capacity of CO intermediate and simultaneously improves the durability of PtTe NW towards FAEOR.This work provides the valuable insights into the synthesis and design of efficient Pt-based alloy FAEOR electrocatalysts.展开更多
Engineering the composition and/or morphology of noble metal nanocrystals is a highly effective strategy for enhancing their electrocatalytic performance.Recently,metallenes with specific chemical and physical propert...Engineering the composition and/or morphology of noble metal nanocrystals is a highly effective strategy for enhancing their electrocatalytic performance.Recently,metallenes with specific chemical and physical properties have increasingly attracted attention in the field of electrocatalysis.In this work,two-dimensional ultrathin platinum-tellurium alloy metallene(PtTe A-ML)is synthesized using a conventional liquid-phase chemical reduction method.The high atomic utilization as well as alloy effect endow PtTe A-ML with preeminent electrocatalytic activity for the formic acid oxidation reaction(FAOR).Specifically,the direct oxidation pathway of FAOR can be completely achieved using PtTe A-ML,which suppresses the production of toxic carbon monoxide(CO)intermediates and improves the reaction kinetics of FAOR.Accordingly,the FAOR activity of PtTe AML in acidic media is 43 and 5.6 times higher than that of commercial Pt and Pd nanocrystals,respectively.Meanwhile,PtTe A-ML also exhibits excellent electrocatalytic activity for the CO oxidation reaction because of the introduction of oxygenophilic Te atoms and electron transfer between Pt and Te,which elevates the durability of PtTe A-ML for FAOR.This study provides a simple synthesis strategy for PtTe A-ML and demonstrates that PtTe A-ML has a promising practical prospect for direct formic acid fuel cells.展开更多
基金supported by the National Natural Science Foundation of China(22272103 and 52171145)the Science and Technology Innovation Team of Shaanxi Province(2023-CX-TD27)+1 种基金the Fundamental Research Funds for the Central Universities(GK202202001)the 111 Project(B14041 and D20015)。
文摘The high-performance anodic electrocatalysts is pivotal for realizing the commercial application of the direct formic acid fuel cells.In this work,a simple polyethyleneimine-assisted galvanic replacement reaction is applied to synthesize the high-quality PtTe alloy nanowires(PtTe NW)by using Te NW as an efficient sacrificial template.The existence of Te atoms separates the continuous Pt atoms,triggering a direct reaction pathway of formic acid electrooxidation reaction(FAEOR)at PtTe NW.The one-dimensional architecture and highly active sites have enabled PtTe NW to reveal outstanding electrocatalytic activity towards FAEOR with the mass/specific activities of 1091.25 mA mg^(-1)/45.34 A m^(-2)at 0.643 V potential,which are 44.72/23.16 and 20.26/11.75 times bigger than those of the commercial Pt and Pd nanoparticles,respectively.Density functional theory calculations reveal that Te atoms optimize the electronic structure of Pt atoms,which decreases the adsorption capacity of CO intermediate and simultaneously improves the durability of PtTe NW towards FAEOR.This work provides the valuable insights into the synthesis and design of efficient Pt-based alloy FAEOR electrocatalysts.
基金the National Natural Science Foundation of China(Grant No.22272103)Science and Technology Innovation Team of Shaanxi Province(Grant No.2023-CX-TD-27)+1 种基金the Young Scientist Innovation Project of the School of Materials Science and Engineering at Shaanxi Normal University(Grant No.2022YSIP-MSE-SNNU005)the Fundamental Research Funds for the Central Universities(Grant No.GK202202001).
文摘Engineering the composition and/or morphology of noble metal nanocrystals is a highly effective strategy for enhancing their electrocatalytic performance.Recently,metallenes with specific chemical and physical properties have increasingly attracted attention in the field of electrocatalysis.In this work,two-dimensional ultrathin platinum-tellurium alloy metallene(PtTe A-ML)is synthesized using a conventional liquid-phase chemical reduction method.The high atomic utilization as well as alloy effect endow PtTe A-ML with preeminent electrocatalytic activity for the formic acid oxidation reaction(FAOR).Specifically,the direct oxidation pathway of FAOR can be completely achieved using PtTe A-ML,which suppresses the production of toxic carbon monoxide(CO)intermediates and improves the reaction kinetics of FAOR.Accordingly,the FAOR activity of PtTe AML in acidic media is 43 and 5.6 times higher than that of commercial Pt and Pd nanocrystals,respectively.Meanwhile,PtTe A-ML also exhibits excellent electrocatalytic activity for the CO oxidation reaction because of the introduction of oxygenophilic Te atoms and electron transfer between Pt and Te,which elevates the durability of PtTe A-ML for FAOR.This study provides a simple synthesis strategy for PtTe A-ML and demonstrates that PtTe A-ML has a promising practical prospect for direct formic acid fuel cells.
