采用简单的一步浸渍法制备了还原氧化石墨烯-贵金属Pd复合改性的泡沫镍电极,采用X射线衍射和扫描电镜对复合电极的微观结构和表面形貌进行分析,通过循环伏安法、线性伏安法、计时电流法对H2O2还原反应的催化活性及稳定性进行了测试。结果表明,石墨烯包覆在泡沫镍骨架表面,在石墨烯内均匀分散着贵金属Pd纳米颗粒,直径约为100nm。该复合电极对H2O2电还原表现出较好的催化性能。在1mol/L NaOH+0.5mol/L H2O2混合溶液中,电位为-0.5V时,电流密度可达164mA/cm2,同时表现出较好的稳定性。
The foamed Ni electrode modified by reduced graphene(rGO) oxide-precious metal Pd was prepared by a simple one-step impregnation method.The microstructure and surface morphology of the composite electrode were analyzed by X-ray diffraction (XRD) and scanning electron microscopy (SEM).The catalytic activity and stability of the electrode in H2O2 reduction reaction were tested by cyclic voltammetry,linear voltammetry and chronoamperometry.The results shown that the rGO oxide was coated on the surface of the foamed Ni skeleton,and the noble metal Pd nanoparticles with the diameter of about 100nm were uniformly dispersed in the rGO oxide.The composite electrode exhibited good catalytic performance for H2O2 electroreduction.In the mixed solution of 1mol/L NaOH+0.5mol/L H2O2,the current density can reach 164 mA/cm2 when the potential was -0.5V,and it shown good stability.
[1] 李一栋,殷金玲.H2O2基燃料电池阴极催化剂的研究进展[J].化学工程师,2011,25(6):42-44.
[2] 颉苗.石墨烯负载Ni@Pd核壳结构催化剂的制备及其在联氨燃料电池中的应用[J].陇东学报,2017,28(3):43-47.
[3] 孙丽美,石乐乐,张帅帅,等.Pdn-Fe纳米合金作为Mg-H2O2半燃料电池阴极研究[J].无机材料学报,2018,33(1):81-86.
[4] Geng X Y,Zhang H M,Ye W,et al.Ni-Pt/C as anode electrocatalyst for a direct borohydride fuel cell[J].Journal of Power Sources,2008,185(2):627-632.
[5] 陈书礼,卢帮安,刘瑶,等.碱性Al-H2O2半燃料电池Au/Ni阴极性能研究[J].电化学,2010,16(2):222-226.
[6] Phan D,Chung G.Effects of Pd nanocube size of Pd nanocube-graphene hybrid on hydrogen sensing properties[J].Sensors and Actuators B:Chemical,2014,204(4):437-444.
[7] 宋聪颖,孙逊,叶克,等.还原氧化石墨烯修饰泡沫镍原位负载MnO2对H2O2电还原反应催化性能的研究[J].化学学报,2017,75(10):1003-1009.
[8] Ma J,Ji Y G,Sun H J,et al.Synthesis of carbon supported palladium nanoparticles catalyst using a facile homogeneous precipitation-reduction reaction method for formic acid electrooxidation[J].Appl Surf Sci,2011,257(24):10483-10488.
[9] 常建霞,酒红芳,焦红倩,等.三维氧化石墨烯-Ag/泡沫镍复合材料的制备及其电化学性能[J].过程工程学报,2016,16(2):341-345.
[10] 王露.改进Hummers法制备氧化石墨烯及其表征[J].包装学报,2015,7(2):28-31,37.
[11] Ogi T,Honda R,Tamaiko K,et al.Direct room-temperature synthesis of a highly dispersed Pd nanoparticle catalyst and its electrical properties in a fuel cell[J].Powder Technol,2011,205(1/3):143-148.
[12] Meng H,Xie F Y,Chen J,et al.Electrodeposited palladium nanostructure as novel anode for direct formic acid fuel cell[J].J Mater Chem,2011,21(30):11352-11356.
[13] Aravind S S J,Ramaprabhu S.Pt nanoparticle-dispersed graphene-wrapped MWNT composites as oxygen reduction reaction electrocatalyst in proton exchange membrane fuel cell[J].ACS Appl Mater Interfaces,2012,4(8):805-3810.
[14] Nesselberger M,Ashton S,Meier J,et al.The particle size effect on the oxygen reduction reaction activity of Pt catalysts:influence of electrolyte and relation to single crystal models[J].J Am Chem Soc,2011,133(43):17428-17433.
[15] 崔浩田,苏钰,胡洋阳,等.Co2O3/石墨烯复合材料的结构及电化学性能研究[J].人工晶体学报,2019,48(5):873-877,888.
[16] Xiao S Y,Michael J R,Thomas B.Three dimensional nickel graphene core shell electrodes[J].J Mater Chem,2012,22(45):23749-23754.
[17] Marinoiu A,Rzceanu M,Andrulevicius M,et al.Low-cost preparation method of well dispersed gold nanoparticles on reduced graphene oxide and electrocatalytic stability in PEM fuel cell[J].Arabian J Chem,2018,12:009.
[18] 丁春黎,朱永娟,顾薇.对浸渍法制备Pd/C催化剂表面积影响因素的讨论[J].吉林工学院学报(自然科学版),2001(1):4-6.
[19] 刘阳,肖发新,申晓妮,等.还原制备时的pH值对Pd/C催化剂性能的影响[J].贵金属,2016,37(2):19-25.