Electrocatalytic Performance of Pd-Sn/C Catalyst Prepared with Different Complexants for Ethanol Oxidation in Alkaline Solution†

doi:10.7503/cjcu20130795

Abstract

Abstract:

Three complexants, sodium citrate, trans-1,2-diaminocyclohexane-N,N,N',N' -tetraacetic acid hydrate(C₁₄H₂₂N₂O₈·H₂O, CyDTA) and ammonia, were used to prepare Pd-Sn/C catalysts. It is found that the electrocatalytic performances of these three catalysts for ethanol oxidation in alkaline solution are better than commercialized Pd/C catalyst. The average particle diameter, morphology and composition of the Pd-Sn/C catalysts prepared were characterized by energy dispersive X-ray spectroscopy(EDS), X-ray diffraction(XRD) and transmission electron microscopy(TEM). X-ray photoclectron spectroscopy(XPS) measurement reveales that tin oxide and tin exist on the surface of the catalysts. The results of the electrochemical measurements indicate that the Pd-Sn/C-CyDTA catalyst has the best electrocatalytic performance for ethanol oxidation in alkaline solution.

Key words: Ethanol oxidation, Palladium-tin catalyst, Complexant, Electrocatalytic performance

CLC Number:

O646

TrendMD:

LI Qiaoxia, MAO Hongmin, ZHU Pingping, CAO Xiaolu, LU Tianhong, XU Qunjie. Electrocatalytic Performance of Pd-Sn/C Catalyst Prepared with Different Complexants for Ethanol Oxidation in Alkaline Solution^†[J]. Chem. J. Chinese Universities, 2014, 35(3): 602.

Figures/Tables 9

Fig.1 TEM images(A—C) and histogram of particle size distribution(D—F) of Pd-Sn/C-ammonia(A, D), Pd-Sn/C-CyDTA(B, E) and Pd-Sn/C-trisodium citrate(C, F) catalysts

Fig.2 EDS spectra of Pd-Sn/C-ammonia(A), Pd-Sn/C-CyDTA(B), Pd-Sn/C-trisodium citrate(C) catalysts

Fig.3 XRD patterns of the Pd-Sn/C-ammonia(a), Pd-Sn/C-CyDTA(b), Pd-Sn/C-trisodium citrate(c) and Pd/C catalysts(d)

Fig.4 XPS spectra of Pd-Sn/C-CyDTA

Fig.5 Cyclic voltammograms of Pd-Sn/C-ammonia(a), Pd-Sn/C-CyDTA(b), Pd-Sn/C-trisodium citrate(c), Pd/C(d), Pd-Sn/C(e), Sn/C catalysts(f) in 1.0 mol/L KOH(A) or 1.0 mol/L KOH+1.0 mol/L C2H5OH(B) at a scan rate of 50 mV/s

Table 1 Physical and electrochemical patameters of Pd-Sn/C-ammonia, Pd-Sn/C-CyDTA, Pd-Sn/C-trisodium citrate and Pd/C, Pd-Sn/C*

Catalyst	Crystallite size/nm		EASA/(m²·g^-1)	E_op/V	E_p/V	i_p/(mA·cm^-2)
Catalyst	XRD		EASA/(m²·g^-1)	E_op/V	E_p/V	TEM
Pd-Sn/C-CyDTA	4.5	5.09	297.62	-0.632	-0.046	122.06
Pd-Sn/C-trisodium citrate	6.0	4.76	212.24	-0.702	-0.089	111.51
Pd-Sn/C-ammonia	5.4	5.18	178.59	-0.655	-0.125	97.83
Pd-Sn/C			131.09	-0.587	-0.081	60.16
Pd/C	10.1		88.53	-0.615	-0.177	49.16

Fig.6 Cycle stabilities of Pd-Sn/C-ammonia(a), Pd-Sn/C-CyDTA(b), Pd-Sn/C-trisodium citrate(c), Pd/C(d), Pd-Sn/C(e) catalysts in 1.0 mol/L KOH+1.0 mol/L C2H5OH at a scan rate of 50 mV/s

Fig.7 Chronoamperpmetric curves of Pd-Sn/C-ammonia(a), Pd-Sn/C-CyDTA(b), Pd-Sn/C-triso-dium citrate(c), Pd/C(d), Pd-Sn/C(e), Sn/C catalysts(f) in 1.0 mol/L KOH+1.0 mol/L C2H5OH solution for 3600 s at -0.25 V

Fig.8 Polarization curves for the Pd-Sn/C-CyDTA electrocalyst in 1.0 mol/L KOH and different concentrations of ethanolc(C2H5OH)/(mol·L-1): a. 1.0; b. 2.0; c. 3.0; d. 4.0; e. 5.0.

References 23

[1]	Guo J., Zhao T., Prabhuram J., Chen R., Wong C., Electrochimica Acta,2005, 51(4), 754—763
[2]	Salgado J., Paganin V., Gonzalez E., Montemor M., Tacchini I., Ansón A., Salvador M., Ferreira P., Figueiredo F., Ferreira M., Inter. J. Hydrogen Energy,2013, 38, 901—909
[3]	Xu Q. J., Zhou X. J., Li Q. X., Li J. G., Acta Physico-Chimica Sinica,2010, 26(08), 2135—2138
	(徐群杰, 周小金, 李巧霞, 李金光. 物理化学学报, 2010, 26(08), 2135—2138)
[4]	Maiyalagan T., Scott K., J. Power Sources,2010, 195(16), 5246—5251
[5]	Li Q., Xu Q., Zhou X., Li J., J. Biobased Materials and Bioenergy,2013, 7(4), 525—528
[6]	Ma J., Sun H. J., Zhao H., Tang Y. W., Lu T. H., Zheng J. W., Chem. J. Chinese Universities,2011, 32(12), 2856—2860
	(马娟, 孙瀚君, 赵宏, 唐亚文, 陆天虹, 郑军伟. 高等学校化学学报, 2011, 32(12), 2856—2860)
[7]	Zhu M., Sun G., Xin Q., Electrochimica Acta,2009, 54(5), 1511—1518
[8]	Ruiz Camacho B., Morais C., Valenzuela M., Alonso-Vante N., Catalysis Today,2012, 202, 36—43
[9]	Liu C. P., Yang H., Xing W., Lu T. H., Chem. J. Chinese Universities,2002, 23(7), 1367—1370
	(刘长鹏, 杨辉, 邢巍, 陆天虹, 高等学校化学学报, 2002, 23(7), 1367—1370)
[10]	Pang H., Lu J., Chen J., Huang C., Liu B., Zhang X., Electrochimica Acta,2009, 54(9), 2610—2615
[11]	Camara G., Iwasita T., J. Electroanal. Chem., 2005, 578(2), 315—321
[12]	Wang H., Jusys Z., Behm R., J. Phys. Chem. B,2004, 108(50), 19413—19424
[13]	Yang Y. Y., Ren J., Zhang H. X., Zhou Z. Y., Sun S. G., Cai W. B., Langmuir,2013, 29(5), 1709—1716
[14]	Xu C., Liu Y., J. Power Sources,2007, 164(2), 527—531
[15]	Wang Y., Shi F. F., Yang Y. Y., Cai W. B., J. Power Sources,2013, 243, 369—373
[16]	Mahendiran C., Maiyalagan T., Scott K., Gedanken A., Mater. Chem. Phys., 2011, 128(3), 341—347
[17]	Modibedi R. M., Masombuka T., Mathe M. K., Inter. J. Hydrogen Energy,2011, 36(8), 4664—4672
[18]	Zhou W., Lee J. Y., J. Phys. Chem. C,2008, 112(10), 3789—3793
[19]	Lewera A., Barczuk P. J., Skorupska K., Miecznikowski K., Salamonczyk M., Kulesza P. J., J. Electroanal. Chem., 2011, 662(1), 93—99
[20]	Singh R., Singh A., Carbon,2009, 47(1), 271—278
[21]	Wen Z., Yang S., Liang Y., He W., Tong H., Hao L., Zhang X., Song Q., Electrochimica Acta,2010, 56(1), 139—144
[22]	Zhu F., Ma G., Bai Z., Hang R., Tang B., Zhang Z., Wang X., J. Power Sources,2013, 242, 610—620
[23]	Wu B., Wang B., Deng C., Gao Y., Appl. Catal. B: Environmental,2011, 103(1), 163—168