SnO_2纳米棒负载Pd-Sb催化甲酸电氧化
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摘要
采用溶剂热法制备了SnO_2纳米棒载体,用溶剂热还原法制备了Pd/SnO_2催化剂和不同Pd/Sb原子数比的系列PdSb/SnO_2复合催化剂。用XRD、SEM、TEM、EDS等手段对样品进行分析表征,并以循环伏安法对比评价催化剂对甲酸的电催化氧化性能。表征结果表明,制备所得SnO_2纳米棒载体为针状,大小均匀,平均直径为100 nm;负载所得催化剂中活性粒子大小约为13.5 nm,掺杂Sb后,粒径约为9.5 nm。电催化氧化性能对比结果表明,Pd/Sb原子数比为4:1的Pd_4Sb/SnO_2复合催化剂对甲酸的氧化具有较好的催化能力,当E=0.25 V(vs SCE)时,Pd_4Sb/SnO_2上甲酸氧化的峰电流密度达到25 mA/cm~2,远远高于Pd/SnO_2催化剂。
SnO_2 nanorod carrier was prepared by the solvothermal method, and the Pd/SnO_2 catalysts and a series of PdSb/SnO_2 composite catalysts with different Pd/Sb atomic ratios were prepared by the solvothermal reduction method. The samples were characterized by XRD, SEM, TEM and EDS. Cyclic voltammetry was used to investigate the catalytic activity of the Pd/SnO_2 and PdSb/SnO_2 catalysts on the formic acid oxidation. The results revealed that SnO_2 nanorod carrier was needle-shaped and its average diameter was about 100 nm; The active particle size of the supported catalyst was about 13.5 nm, while it was about 9.5 nm after the addition of Sb. The comparison results of electrocatalytic oxidation showed that Pd_4Sb/SnO_2(with n_(Pd):n_(Sb)=4:1) catalyst exhibited the best catalytic activity. And the current density of the Pd_4Sb/SnO_2 catalyst was about 25 mA/cm~2 when E= 0.25 V(vs SCE) which is far higher than that of the Pd/SnO_2.
SnO_2 nanorod carrier was prepared by the solvothermal method, and the Pd/SnO_2 catalysts and a series of PdSb/SnO_2 composite catalysts with different Pd/Sb atomic ratios were prepared by the solvothermal reduction method. The samples were characterized by XRD, SEM, TEM and EDS. Cyclic voltammetry was used to investigate the catalytic activity of the Pd/SnO_2 and PdSb/SnO_2 catalysts on the formic acid oxidation. The results revealed that SnO_2 nanorod carrier was needle-shaped and its average diameter was about 100 nm; The active particle size of the supported catalyst was about 13.5 nm, while it was about 9.5 nm after the addition of Sb. The comparison results of electrocatalytic oxidation showed that Pd_4Sb/SnO_2(with n_(Pd):n_(Sb)=4:1) catalyst exhibited the best catalytic activity. And the current density of the Pd_4Sb/SnO_2 catalyst was about 25 mA/cm~2 when E= 0.25 V(vs SCE) which is far higher than that of the Pd/SnO_2.
引文
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[3]LIAO M Y,XIONG J H,CHEN B H,et al.Phase properties of carbon-supported platinum-gold nanoparticles for formic acid eletro-oxidation[J].Journal of power sources,2015,294:201-207.
[4]LU L,LI H Z,LU T H,et al.Improvement of electrocatalytic performance of carbon supported Pd anodic catalyst in direct formic acid fuel cell by ethylene diamine-tetramethylene phosphonic acid[J].Journal of power sources,2012,210:154-157.
[5]JIA Y J,JIANG J C,SUN K,et al.Effect of Pt/Au atomic ratio in active-carbon-supported Au-Pt catalysts on its cathodic performance in direct formic acid fuel cells[J].Journal of fuel chemistry and technology,2011,39(10):792-795.
[6]贾羽洁,唐亚文,陆天虹,等.炭载Pd-Pt催化剂中Pd和Pt原子比对直接甲醇燃料电池阴极催化性能的影响[J].应用化学,2011,28(2):224-228.JIA Y J,TANG Y W,LU T H,et al.Effect of atomic ratio of Pd and Pt in carbon supported Pd-Pt catalyst on its cathodic performance in direct methanol fuel cell[J].Applied chemistry,2011,28(2):224-228.
[7]QU W L,GU D M,ZHANG J J,et al.High stability and high activity Pd/ITO-CNTs electrocatalyst for direct formic acid fuel cell[J].Electrochimica acta,2014,137:676-684.
[8]YU X W,PICKUP P G.Co deposited Pt Sb/C catalysts for direct formic acid fuel cells[J].Journal of power sources,2011,196:7951-7956.
[9]SHEN L P,LI H Z,LU T H,et al.Improvement and mechanism of electrocatalytic performance of Pd–Ni/C anodic catalyst in direct formic acid fuel cell[J].Electrochimica acta,2013,89:497-502.
[10]YAO S K,LI G Q,XING W,et al.Enhanced catalytic performance of carbon supported palladium nanoparticles by in-situ synthesis for formic acid electrooxidation[J].Journal of power sources,2015,284:355-360.
[11]WANG Q,LIAO Y X,CHEN S L,et al.One-pot synthesis of carbon-supported monodisperse palladium nanoparticles as excellent electrocatalyst for ethanol and formic acid oxidation[J].Journal of power sources,2015,292:72-77.
[12]HABIB B,MOHAMMADYARI S.Palladium nanoparticles/nanostructured carbon black composite on carbon-ceramic electrode as an electrocatalyst for formic acid fuel cells[J].Journal of the Taiwan institute of chemical engineers,2015,58:245-251.
[13]赵钦,孙丽美,周淑娟,等.氧化锡锑负载纳米Pd催化H2O2电还原反应的催化性能[J].贵金属,2013,34(1):13-14.ZHAO Q,SUN L M,ZHOU S J,et al.Electrocatalytic performance of Pd supported on Sb-doped Sn O2nanoparticles for H2O2 reduction[J].Precious metals,2013,34(1):13-14.
[14]BAIK S M,HAN J,KWON Y,et al.Effect of deactivation and reactivation of palladium anode catalyst on performance of direct formic acid fuel cell[J].International journal of hydrogen energy,2011,36:14719-14724.
[15]BARAKAT N,ABDELKAREEM M,KIM H,et al.Pd-doped Co nanofibers immobilized on achemically stable metallic bipolar plate as novel strategy for direct formic acid fuel cells[J].International journal of hydrogen energy,2013,38:7438-7447.
[16]施毅,李建苹,唐亚文,等.Ti O2纳米棒载Pd催化剂的制备及其对甲酸的电催化氧化[J].化学学报,2012,70(11):1257-1262.SHI Y,LI J P,TANG Y W,et al.Preparation of Ti O2-nanorods supported Pd catalyst and its electrocatalytic oxidation on formic acid[J].Acta chimica sinica,2012,70(11):1257-1262.
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[20]王龙龙,曹晓璐,李巧霞,等.Pd-Sb/C复合纳米催化剂对甲酸电催化氧化的性能研究[J].电化学,2015,21(4):368-374.WANG L L,CAO X L,LI Q X,et al.Preparation and characterization of carbon supported Pd-Sb composite nanocatalysts for formic acid electrooxidation[J].Electrochemistry,2015,21(4):368-374.
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