The incorporation of Pt into an iron-nitrogen-carbon(Fe NC)catalyst for the oxygen reduction reaction(ORR)was recently shown to enhance catalyst stability without Pt directly contributing to the ORR activity.However,t...The incorporation of Pt into an iron-nitrogen-carbon(Fe NC)catalyst for the oxygen reduction reaction(ORR)was recently shown to enhance catalyst stability without Pt directly contributing to the ORR activity.However,the mechanistic origin of this stabilisation remained obscure.It is established herein with rotating ring disc experiments that the side product,H_(2)O_(2),which is known to damage FeNC catalysts,is suppressed by the presence of Pt.The formation of reactive oxygen species is additionally inhibited,independent of intrinsic H_(2)O_(2) formation,as determined by electron paramagnetic resonance.Transmission electron microscopy identifies an oxidised Fe-rich layer covering the Pt particles,thus explaining the inactivity of the latter towards the ORR.These insights develop understanding of Fe NC degradation mechanisms during ORR catalysis,and crucially establish the required properties of a precious metal free protective catalyst to improve Fe NC stability in acidic media.展开更多
As a rapid uniform and efficient heating method, microwave irradiation has been widely used in chemical reaction and preparing nanomaterials. Here Pt/carbon nanotube(CNT) catalysts with w(Pt)=18.1% and 9.4 % were rapi...As a rapid uniform and efficient heating method, microwave irradiation has been widely used in chemical reaction and preparing nanomaterials. Here Pt/carbon nanotube(CNT) catalysts with w(Pt)=18.1% and 9.4 % were rapidly synthesized by microwave irradiation heating polyol process and employing the ethylene glycol solution of H 2PtCl 6 as the precursors in the presence of CNT support. TEM imaging showed that microwave-prepared Pt nanoparticles were very uniform in size, with an average size of 3.1 nm, and uniformly dispersed on the CNT surface. Electrochemical experiments demonstrated that microwave-synthesized Pt/CNT catalysts exhibited a higher catalytic activity for electrooxidation of liquid methanol than E-TEK Pt/C. The significant improvement in catalyst performance derives from that microwave-synthesized Pt nanoparticles have a uniform small particle size and uniforml dispersion on the CNT surface.展开更多
基金a fellowship from the Alexander von Humboldt foundation。
文摘The incorporation of Pt into an iron-nitrogen-carbon(Fe NC)catalyst for the oxygen reduction reaction(ORR)was recently shown to enhance catalyst stability without Pt directly contributing to the ORR activity.However,the mechanistic origin of this stabilisation remained obscure.It is established herein with rotating ring disc experiments that the side product,H_(2)O_(2),which is known to damage FeNC catalysts,is suppressed by the presence of Pt.The formation of reactive oxygen species is additionally inhibited,independent of intrinsic H_(2)O_(2) formation,as determined by electron paramagnetic resonance.Transmission electron microscopy identifies an oxidised Fe-rich layer covering the Pt particles,thus explaining the inactivity of the latter towards the ORR.These insights develop understanding of Fe NC degradation mechanisms during ORR catalysis,and crucially establish the required properties of a precious metal free protective catalyst to improve Fe NC stability in acidic media.
文摘As a rapid uniform and efficient heating method, microwave irradiation has been widely used in chemical reaction and preparing nanomaterials. Here Pt/carbon nanotube(CNT) catalysts with w(Pt)=18.1% and 9.4 % were rapidly synthesized by microwave irradiation heating polyol process and employing the ethylene glycol solution of H 2PtCl 6 as the precursors in the presence of CNT support. TEM imaging showed that microwave-prepared Pt nanoparticles were very uniform in size, with an average size of 3.1 nm, and uniformly dispersed on the CNT surface. Electrochemical experiments demonstrated that microwave-synthesized Pt/CNT catalysts exhibited a higher catalytic activity for electrooxidation of liquid methanol than E-TEK Pt/C. The significant improvement in catalyst performance derives from that microwave-synthesized Pt nanoparticles have a uniform small particle size and uniforml dispersion on the CNT surface.
文摘利用机械混合及化学复合两种混合方式制备出用于微生物燃料电池(MFC)阴极的Mn O_2与活性炭导电材料的混合催化剂,混合质量比分别为1∶3,1∶1和3∶1。将以各催化剂制作的碳布阴极置于空气阴极MFC中运行,利用线性扫描伏安法测试碳布阴极的性能。研究表明,两种混合催化剂均在混合质量比为1∶1时具有最佳性能;化学复合催化剂MFC的最大功率密度达到336 m W/m^2,是单纯使用Mn O_2粉末时的2.51倍,优于机械混合的催化剂。
基金supported by the National Natural Science Foundation of China(21006073)the Shanghai Rising-Star Program(11QA1407200)+2 种基金the Shanghai Leading Academic Discipline Project(B303)the Open-Project Program of the State Key Laboratory of Chemical Engineering(SKL-ChE-08C07)the Program of Introducing Talents of Discipline to Universities(B08019)~~