纳米氧化锡在锌-硝基苯电池反应中的电催化
收稿日期: 2016-11-05
修回日期: 2017-03-16
网络出版日期: 2017-03-30
基金资助
江苏省自然科学基金项目(BK20141261)、江苏省产学研前瞻性项目(BY2015057-35)、盐城市科技项目(YKA201219)资助
Electrocatalysis of NanoTin Dioxide in the Battery Reaction of Zinc-Nitrobenzene
Received date: 2016-11-05
Revised date: 2017-03-16
Online published: 2017-03-30
以氯化锡为原料,四丙基溴化铵为表面活性剂水热法制备纳米二氧化锡(SnO2)催化剂,并以钛网为基材,制备催化电极. 应用SEM,XRD等手段对催化剂进行表征. 考察了反应物浓度、反应温度和反应时间对催化剂形貌的影响. 研究了纳米SnO2催化剂对锌还原硝基苯原电池反应的电催化性能. 结果表明,当 NaOH浓度为0. 5 mol•L-1、水热反应温度160 ℃、水热反应时间15 h时,得到的SnO2催化剂是由纳米片构成的刺球状颗粒,粒径最小,约17 nm. 与平板铂电极相比,制备的催化电极对硝基苯电还原具有更高的催化活性,硝基苯转化率为74%,最大放电功率为21.9 mW•cm-2,远大于平板铂电极. 硝基苯的主要还原产物为苯胺、对乙氧基苯胺和对氯苯胺.
涂序国 , 马翔宇 , 何瑞楠 , 王晓娟 , 凌晨 , 孙云霞 , 陈松 . 纳米氧化锡在锌-硝基苯电池反应中的电催化[J]. 电化学, 2017 , 23(3) : 356 -363 . DOI: 10.13208/j.electrochem.161049
The tin dioxide (SnO2) nanoparticles were synthesized by using a simple hydrothermal route in the presence of tetrapropyl ammonium bromide (TPAB) as a surfactant. Accordingly, the titanium mesh based SnO2 catalyst electrode was prepared. The morphologies and structures of SnO2 nanostructures were characterized by scanning electron microscopy and X-ray diffraction spectrometry. The influences of reactant concentration, reaction temperature and time on the morphology of the products were investigated in detail. The electrocatalytic performance of SnO2 for the reduction of nitrobenzene with zinc was studied. Possible formation process and growth mechanism for such hierarchical SnO2 nanostructures have been proposed based on the experimental results. The results showed that when the concentration of NaOH was 0.5 mol•L-1, the hydrothermal reaction temperature was 160 ℃, hydrothermal reaction time was 9 h, the as-prepared SnO2 catalyst appeared thorny spheric particles consisting of nanosheets with the particle size as small as 17 nm. Compared with Pt electrode, the catalyst electrode exhibited higher catalytic activity toward the electrochemical reduction of nitrobenzene. The conversion rate of nitrobenzene was up to 74% and the maximum discharge power density was 21.9 mW•cm-2, which are much better than those with platinum electrode. The main reduction products of nitrobenzene were aniline, p-phenetidine and p-chloroaniline.
Key words: Tin dioxide; Nanometer; Electrocatalysis; Nitrobenzene; Reduction
[1] Ge J P, Wang J, Zhang H X, et al. High ethanol sensitive SnO2 microspheres[J].Sensor Actual B, 2006,113(2):937-943.
[2] Wang H Z, Liang J B, Fan H, et al. Synthesis and gas sensitivities of SnO2 nanorods and hollow microspheres[J]. J Solid State Chem, 2008,181 (1):122-129.
[3] Leite E R, Weber I T, Longo E, et al. A new method to control particle size and particle size distribution of SnO2 nanoparticles for gas sensor applications[J].Adv Mater, 2000,12(13):965-968.
[4] Wang L W, Wang S R, Wang Y S, et al. Synthesis of hierarchical SnO2 nanostructures assembled with nanosheets and their improved gas sensing properties[J].Sensor and Actuators B:Chemical,2013,188:85-93.
[5] Wang W W, Zhu Y J, Yang L X, Nanosheets:hydrothermal preparation,formation mechanism,
and photocatalytic properties[J]. Adv Funct Mater, 2007,17(1):59-64.
[6] Lou X W, Wang Y, Yuan C L, et al. Template-free synthesis of SnO2 hollow nanostructure with high lithium storage capacity[J]. Adv Mater. 2006,18(17):2325-2329.
[7] Li X F, Meng X B, Liu J, et,al, Y Zhang, Tin oxide with controlled morphology and crystallinity by atomic layer deposition onto grapheme nanosheets for enhanced lithium storage[J].
Advanced Functional Materials, 2012,22(8) :1647-1654.
[8] Wang H, Liang Q Q , Wang W J, et al. Preparation of flower-like SnO2 nanostructures and their applications in gas-sensing and lithium storage[J].American Chemical Society,2011,11,
2942-2947.
[9] Li Y M, Lv X , Lu J, et al. Preparation of SnO2-nanocrystal/grapheme-nanosheets composition
and their lithium storage ability[J]. Phys Chem C, 2010,114(49):21770-21774.
[10] Wang C, Zhou Y, Ge M Y, et al. Large-scale synthesis of SnO2 nanosheets with high lithium storage capacity[J]. J Am Chem Soc, 2010,132(1):46-47.
[11] Lee K T, Lytle J C, Ergang N S, et al. Synthesis and rate performance of monolithic macropor
-ous carbon electrodes for lithium-ion secondary batteries[J]. Adv Funct Mater, 2005,15(4):547-
556.
[12] Liu J, Huang J M, Hao L L, et al. SnO2 nano-spheres/grapheme hybrid for high performance lithium ion battery anodes[J].Ceram Int,2013,39(8):8623-8627.
[13] Wang M S, Lei M, Wang Z Q, et al. Scalable preparation of porous micron SnO2/C
composites as high performance anode material for lithium ion battery[J]. J Power Sources,2016,309,238-244.
[14] Kwon C W, Campet G, Portier J, et al. A new single molecular precursor route to fluorine-
doped nanocrystalline tin oxide anodes for lithium batteries[J]. J Inorg Mater,2001,3(3):211-214.
[15] Ha H W, Kim K, Borniol M D, et al. Fluorine-doped nanocrystalline SnO2 powders prepared
via a single molecular precursor method as anode materials for Li-ion batteries[J]. J Solid State Chem,2006,179(3):702-707.
[16] Hui C C, Chen S Y. Hydrothermal synthesis of SnO2 nanoparticles and their gas-sensing of alcohol[J]. J Phys Chem C, 2007,111(20):7256-7259.
[17] Mali S S, Shim C S, Kim H, et al. Hierarchical SnO2 microspheres prepared by hydrothermal process for efficient improvement of dye-sensitized solar cell properties[J]. Journal of Nanopartic-
Le Research,2015,17(12):1-13.
[18] Sudhaparimala S, Vaishnavi M. Biological synthesis of nano composite SnO2-ZnO-Screening
for efficient photocatalytic degradation and antimicrobial activity[J]. MaterialsToday:Proceedings,
2016,3(6);2373-2380.
[19] Moghadam L N, Karimabad A E B, Niasari M S, et al. Synthesis and characterization of SnO2 nanoparticles prepared by a facile precipitation method[J]. Journal of Nanostructures,2015,7(5):47
-53.
[20] Liu B, Guo Z P, Du G D, et al. In situ synthesis of ultra-fine, porous, tin oxide-carbon nano-
composites via a molten salt method for lithium-ion batteries[J]. Journal of Power Sources,2010,
195(16):5382-5386.
[21] Wang Y, Lee J Y, Chen B H. Microemulsion syntheses of Sn and SnO2-graphite nanocomposi
-te anodes for Li-ion batteries[J]. Journal of Vegetation Science,2004,151(4):744-760.
[22] Gu L G N(古丽戈娜), Nu R M G L(努热曼古丽), Zhang W H(张文河),et al. The study on using sea-urchin like SnO2 nano -spheres catalyst and its effect of CO2 on the performance of electrochemical reduction[J].Acta Sciencetiae Circumstantiae(环境科学学报), 2016,34(3):
102-106.
[23] Yang R, Gu Y, Li Y, et al. Self-assembled 3-D flower-shaped SnO2 nanostructures with
improved electrochemical performance for lithium storage[J]. Acta Materialia, 2010, 58(3):866-
874.
[24] Gao G, Tao Y, Jiang J Y. Environmentally benign and selective reduction of nitroarenes with Fe in pressurized CO2-H2O medium [J]. Green Chemistry, 2008, 10: 439-441.
[25] Jiang H F, Dong Y S, et al. Water as a direct hydrogen donor in supercritical carbon dioxide: A novel and efficient Zn-H2O-CO2 system for chemoselective reduction of Nitrobenzenes to Anilines [J]. Chinese Journal of Chemistry, 2008, 26: 1407-1410.
[26] You H, Wu D H, Yao J, et al. Photo-degradation of the nitrobenzene in water[J]. Journal of Safety and Environment[J], 2008, 8(2): 16-19.
[27] Ma C A, Tong S P, Gao X P, et al. Electrosynthesis of 3,5-Dichloroaniline[J]. You Ji Hua Xue, 1998, 18: 334-336.
[28] Li Y T, Yang Y, Sun Y X, et al. A novel reaction system for cogeneration of chemicals and electric energy by electrochemical reduction of Nitrobenzene with Iron [J].Int. J. Electrochem. Sci,
2016,11:3502-3511.
/
〈 |
|
〉 |