欢迎登录材料期刊网

材料期刊网

高级检索

采用多元醇法制备了不同原子比例和载量的PtSnRu/C催化剂,利用透射电镜和X射线光电子能谱表征了所制备催化剂的物化性能,采用直接乙醇燃料电池(DEFC)单池性能测试了其电化学性能,并利用电化学原位光谱、气相色谱和中和滴定分析了乙醇电氧化过程和产物. DEFC单电池测试表明Pt2.6Sn1Ru0.4/C催化剂具有较高的电池性能,其中,以60 wt% Pt2.6Sn1Ru0.4/C催化剂为阳极的DEFC性能最高,90oC下最高功率密度为121 mW/cm2.电化学原位红外光谱和阳极产物分析表明乙酸、乙醛、乙酸乙酯和CO2是乙醇电化学氧化产物, Pt2.6Sn1Ru0.4/C催化剂上乙醇的氧化效率较高.阳极乙醇氧化活化能和催化剂表面组成分析结果表明,表面组成的相互作用使Pt2.6Sn1Ru0.4/C催化剂具有较低的乙醇氧化活化能和较高的乙醇氧化活性.

PtSnRu/C catalysts with different atomic ratios and metal loadings were prepared using a polyol process to improve the performance of direct ethanol fuel cells (DEFCs). The catalysts were charac-terized using transmission electron microscopy and X-ray photoelectron spectroscopy. The DEFC performance was evaluated using a single-cell test. The ethanol electro-oxidation process and anode products were analyzed using in situ Fourier-transform infrared spectroscopy (FTIRS), gas chro-matography, and neutralization titration. The performance of the Pt2.6Sn1Ru0.4/C catalyst was better than those of the Pt3Sn1/C and Pt2Sn1Ru1/C catalysts. The carbon-supported Pt2.6Sn1Ru0.4 catalyst with a 60 wt%metal loading gave a maximum power density of 121 mW/cm2 at 90 °C. In situ FTIRS and anode product analysis indicated that ethanol was electro-oxidized to acetaldehyde, acetic acid, ethyl acetate, and CO2. The ethanol oxidation efficiency on the Pt2.6Sn1Ru0.4/C catalyst was higher than that on the Pt3Sn1/C catalyst. The activation energy of ethanol electro-oxidation at the anode and surface composition analysis indicated that interactions among the surface elements resulted in a lower apparent activation energy and greater ethanol electro-oxidation efficiency on the Pt2.6Sn1Ru0.4/C catalyst.

参考文献

[1] Arico A S;Creti P;Antonucci P L;Antonucci V .[J].Electrochem Sol-id-State Lett,1998,1:66.
[2] Lamy C;Lima A;LeRhun V;Delime F Coutanceau C Lèger J M .[J].Journal of Power Sources,2002,105:283.
[3] Xu Z F;Wang Y X .[J].J Phys Chem C,2011,115:20565.
[4] 宋树芹,王毅,沈培康.直接乙醇燃料电池中乙醇电氧化过程的热力学和动力学考虑[J].催化学报,2007(09):752-754.
[5] 张洁,唐水花,廖龙渝,郁卫飞.低温燃料电池非铂催化剂研究进展[J].催化学报,2013(06):1051-1065.
[6] Karim-Nezhad G;Pashazadeh S;Pashazadeh A .[J].催化学报,2012,33:1809.
[7] Purgato F L S;Pronier S;Olivi P;de Andrade A R Léger J M Tre-miliosi-Filho G Kokoh K B .[J].Journal of Power Sources,2012,198:95.
[8] Alzate V;Fatih K;Wang H .[J].Journal of Power Sources,2011,196:10625.
[9] Beyhan S;Leger J M;Kad?rgan F .[J].Applied Catalysis B:Environmental,2013,130-131:305.
[10] Beyhan S;Coutanceau C;Leger J M;Napporn T W Kad?rgan F .[J].International Journal of Hydrogen Energy,2013,38:6830.
[11] Tayal J;Rawat B;Basu S .[J].International Journal of Hydrogen Energy,2011,36:14884.
[12] Wang Q;Sun G Q;Cao L;Jiang L H Wang G X Wang S L Yang S H Xin Q .[J].Journal of Power Sources,2008,177:142.
[13] Antolini E;Colmati F;Gonzalez ER .Effect of Ru addition on the structural characteristics and the electrochemical activity for ethanol oxidation of carbon supported Pt-Sn alloy catalysts[J].Electrochemistry communications,2007(3):398-404.
[14] Rousseau S;Coutanceau C;Lamy C;Léger J M .[J].Journal of Power Sources,2006,158:18.
[15] Jiang L H;Sun G Q;Zhou Z Z;Sun S G Wang Q Yan S Y Li H Q Tian J Guo J S Zhou B Xin Q .[J].Journal of Physical Chemistry B,2005,109:8774.
[16] Song S;Wang G;Zhou W;Zhao X Sun G Xin Q Kontou S Tsiakaras P .[J].Journal of Power Sources,2005,140:103.
[17] Zhou W J;Li W Z;Song S Q;Zhou Z H Jiang L H Sun G Q Xin Q Poulianitis K Kontou S Tsiakaras P .[J].Journal of Power Sources,2004,131:217.
[18] Ayoub J M S;De Souza R F B;Silva J C M;Piasentin R M Spinace E V Santos M C Neto A O .[J].International Journal of Electrochemical Science,2012,7:11351.
[19] Tayal J;Rawat B;Basu S .[J].International Journal of Hydrogen Energy,2012,37:4597.
[20] García-Rodriguez S;Rojas S;Pena M A;Fierro J L G Baranton S Leger J M .[J].Applied Catalysis B:Environmental,2011,106:520.
[21] De Souza R F B;Parreira L S;Silva J C M;Simoes F C Calegaro M L Giz M J Camara G A Neto A O Santos M C .[J].International Journal of Hydrogen Energy,2011,36:11519.
[22] Iwasita T;Pastor E .[J].Electrochimica Acta,1994,39:531.
[23] Tsiakaras P E .[J].Journal of Power Sources,2007,171:107.
[24] 张海艳,曹春晖,赵健,林瑞,马建新.燃料电池Pt基核壳结构电催化剂的最新研究进展[J].催化学报,2012(02):222-229.
[25] Nepel T C M;Lopes P P;Paganin V A;Ticianelli E A .[J].Electrochimica Acta,2013,88:217.
[26] 唐水花,林文锋,PaulA.CHRISTENSEN,GeirMartinHAARBERG.甲醇浓度对Pt/C催化剂氧还原活性的影响[J].催化学报,2013(06):1105-1111.
[27] Jiang L H;Colmenares L;Jusys Z;Sun G Q Behm R J .[J].Electrochimica Acta,2007,53:377.
[28] Nakagawa N;Kaneda Y;Wagatsuma M;Tsujiguchi T .[J].Journal of Power Sources,2012,199:103.
[29] Wang Q;Sun G Q;Jiang L H;Xin Q Sun S G Jiang Y X Chen S P Jusys Z Behm R J .[J].Physical Chemistry Chemical Physics,2007,9:2686.
[30] Thepkaew J;Therdthianwong S;Therdthianwong A;Kucernak A Wongyao N .[J].International Journal of Hydrogen Energy,2013,38:9454.
[31] Song S Q;Zhou W J;Zhou Z H;Jiang L H Sun G Q Xin Q Leontidis V Kontou S Tsiakaras P .[J].International Journal of Hydrogen Energy,2005,30:995.
[32] Cunha E M;Ribeiro J;Kokoh K B;de Andrade A R .[J].International Journal of Hydrogen Energy,2011,36:11034.
[33] Wang G X;Takeguchi T;Muhamad E N;Yamanaka T Ueda W .[J].International Journal of Hydrogen Energy,2011,36:3322.
[34] 姜鲁华,臧海霞,孙公权,辛勤.制备方法对直接乙醇燃料电池阳极PtSn/C催化剂性能的影响[J].催化学报,2006(01):15-19.
[35] Zhou Z H;Wang S L;Zhou W J;Wang G X Jiang L H Li W Z Song S Q Liu J G,Sun G Q,Xin Q .[J].Chemistry Communications,2003,3:394.
[36] Wang G X;Sun G Q;Wang Q;Wang S L Sun H Xin Q .[J].International Journal of Hydrogen Energy,2010,35:11245.
[37] Wang G X;Takeguchi T;Yamanaka T;Muhamad E N Mastuda M Ueda W .[J].Applied Catalysis B:Environmental,2010,98:86.
[38] Zhu J;Cheng FY;Tao ZL;Chen J .Electrocatalytic methanol oxidation of Pt0.5Ru0.5-xSnx/C (x=0-0.5)[J].The journal of physical chemistry, C. Nanomaterials and interfaces,2008(16):6337-6345.
[39] Kim H J;Choi S M;Green S;Tompsett G A Lee S H Huber G W Kim W B .[J].Applied Catalysis B:Environmental,2011,101:366.
[40] 王琪,孙公权,闫世友,汪国雄,辛勤,陈青松,李君涛,姜艳霞,孙世刚.PtRu/C电催化剂上甲醇吸附氧化过程的电化学原位红外光谱[J].高等学校化学学报,2006(11):2123-2127.
[41] Kim J H;Choi S M;Nam S H;Seo M H Choi S H Kim W B .[J].Applied Catalysis B:Environmental,2008,82:89.
[42] Mann J;Yao N;Bocarsly A B .[J].LANGMUIR,2006,22:10432.
[43] Beden B;Morin M C;Hahn F;Lamy C .[J].Journal of Electroanalytical Chemistry and Interfacial Electrochemistry,1987,229:353.
[44] Jusys Z.;Behm RJ.;Kaiser J. .Electrooxidation of COH2/CO and mixtures on a carbon-supported Pt catalyst - a kinetic and mechanistic study by differential electrochemical mass spectrometry[J].Physical chemistry chemical physics: PCCP,2001(21):4650-4660.
[45] Colmenares L;Wang H;Jusys Z;Jiang L Yan S Sun G Q Behm R J .[J].Electrochimica Acta,2006,52:221.
[46] Lu GQ.;Cai LR.;Chen SP.;Tian ZW.;Shiu KK.;Sun SG. .In situ FTIR spectroscopic studies of adsorption of CO, SCN-, and poly(o-phenylenediamine) on electrodes of nanometer thin films of Pt, Pd, and Rh: Abnormal infrared effects (AIREs)[J].Langmuir: The ACS Journal of Surfaces and Colloids,2000(2):778-786.
上一张 下一张
上一张 下一张
计量
  • 下载量()
  • 访问量()
文章评分
  • 您的评分:
  • 1
    0%
  • 2
    0%
  • 3
    0%
  • 4
    0%
  • 5
    0%