Citation: ZHANG Yuan-Yuan, YI Qing-Feng, LI Guang, ZHOU Xiu-Lin. Carbon Nanotube-Supported Ternary Pd-Ag-Sn Catalysts for Formic Acid Electro-Oxidation[J]. Chinese Journal of Inorganic Chemistry, ;2018, 34(7): 1209-1220. doi: 10.11862/CJIC.2018.167 shu

Carbon Nanotube-Supported Ternary Pd-Ag-Sn Catalysts for Formic Acid Electro-Oxidation

1.
School of Chemistry and Chemical Engineering, Hunan University of Science and Technology, Xiangtan, Hunan 411201, China
2.
Key Laboratory of Theoretical Organic Chemistry and Functional Molecule, Ministry of Education, Xiangtan, Hunan 411201, China

Corresponding author: YI Qing-Feng, yqfyy2001@hnust.edu.cn
Received Date: 4 March 2018
Revised Date: 8 May 2018

Figures(10)

Carbon nanotube-supported Pd-based binary and ternary nanocatalysts (Pd/CNT, Pd₇Ag₃/CNT, Pd₇Sn₂/CNT, Pd₇Ag₁Sn₂/CNT, Pd₇Ag₂Sn₂/CNT and Pd₇Ag₃Sn₂/CNT) have been fabricated by the NaBH₄ reduction method. They have been characterized by using XRD, TEM and XPS techniques. The ternary Pd-Ag-Sn nanoparticles exhibit a smaller average particle size of ca. 2.3 nm compared to Pd/CNT and binary Pd-Ag (or Pd-Sn) nanoparticles. The electrocatalytic activity of these catalysts towards formic acid oxidation in both H₂SO₄ and NaOH solutions has been investigated using cyclic voltammetry (CV) and chronoamperometry (CA). In both acidic and alkaline media, the ternary Pd-Ag-Sn/CNT catalysts present higher anodic current density for formic acid oxidation than Pd/CNT and binary PdAg/CNT or PdSn/CNT catalysts. Among the prepared catalysts, the Pd₇Ag₂Sn₂/CNT catalyst displays the highest HCOOH oxidation current density of 108.8 mA·cm^-2 in 0.5 mol·L^-1 H₂SO₄ solution or 211.3 mA·cm^-2 in 1 mol·L^-1 NaOH solution, corresponding to the Pd mass current density of 1 364 or 2 640 mA·mg^-1, respectively. These currents are extremely larger than those obtained from the commercial Pd/C. Results exhibit the excellent electrocatalytic activity of the ternary Pd₇Ag₂Sn₂/CNT catalyst towards formic acid oxidation.
- Pd catalyst,
- formic acid oxidation,
- fuel cell,
- electrocatalyst
1. [1]
  Lu X Y, Zheng L, Zhang M S, et al. Electrochim. Acta, 2017, 238:194-201 doi: 10.1016/j.electacta.2017.03.115
2. [2]
  Xu H, Yan B, Zhang K, et al. Appl. Surf. Sci., 2017, 416:191-199 doi: 10.1016/j.apsusc.2017.04.160
3. [3]
  Budischak C, Sewell D, Thomson H, et al. J. Power Sources, 2013, 225(3):60-74
4. [4]
  Miao K H, LuoY, Zou J S, et al. Electrochim. Acta, 2017, 251:588-594 doi: 10.1016/j.electacta.2017.08.167
5. [5]
  El-Nagar G A, Dawood K M, El-Deab M S, et al. Appl. Catal., B, 2017, 213:118-126 doi: 10.1016/j.apcatb.2017.05.006
6. [6]
  Yi Q F, Zou T, Zhang Y Y, et al. J. Power Sources, 2016, 321:219-225 doi: 10.1016/j.jpowsour.2016.04.134
7. [7]
  Yu X W, Pickup P G. J. Power Sources, 2008, 182(1):124-132 doi: 10.1016/j.jpowsour.2008.03.075
8. [8]
  Rhee Y W, Ha S Y, Masel R I. J. Power Sources, 2003, 117(1/2):35-38
9. [9]
  ZOU Tao, YI Qing-Feng, ZHANG Yuan-Yuan, et al. Chem. J. Chinese Universities, 2017, 38(1):101-107 doi: 10.7503/cjcu20160457
10. [10]
  Winjobi O, Zhang Z Y, Liang C H, et al. Electrochim. Acta, 2010, 55(13):4217-4221 doi: 10.1016/j.electacta.2010.02.062
11. [11]
  Yi Q F, Zhang J J, Chen A C, et al. J. Appl. Electrochem., 2008, 38(5):695-701 doi: 10.1007/s10800-008-9490-x
12. [12]
  Zhu C X, Liu D, Chen Z, et al. J. Colloid Interface Sci., 2018, 511:77-83 doi: 10.1016/j.jcis.2017.09.109
13. [13]
  Cabello G, Davoglio R A, Hartl F W, et al. Electrochim. Acta, 2017, 224:56-63 doi: 10.1016/j.electacta.2016.12.022
14. [14]
  Han Y, Ouyang Y J, Xie Z H, et al. J. Mater. Sci. Technol., 2016, 32(7):639-645 doi: 10.1016/j.jmst.2016.04.014
15. [15]
  Awaludin Z, Okajima T, Ohsaka T. Electrochem. Commun., 2013, 31:100-103 doi: 10.1016/j.elecom.2013.03.020
16. [16]
  Yang H Z, Dai L, Xu D, et al. Electrochim. Acta, 2010, 55(27):8000-8004 doi: 10.1016/j.electacta.2010.03.026
17. [17]
  Yi Q F, Chen A C, Huang W, et al. Electrochem. Commun., 2007, 9(7):1513-1518 doi: 10.1016/j.elecom.2007.02.014
18. [18]
  Choi J H, Jeong K J, Dong Y J, et al. J. Power Sources, 2006, 163(1):71-75 doi: 10.1016/j.jpowsour.2006.02.072
19. [19]
  Yi Q F, Li L, Yu W Q, et al. J. Alloys Compd., 2008, 466(1/2):52-58
20. [20]
  ZHANG Li-Juan, XIA Ding-Guo. Chinese J. Inorg. Chem., 2006, 22(6):1085-1089
21. [21]
  Li R X, Ma Z Z, Zhang F, et al. Electrochim. Acta, 2016, 220:193-204 doi: 10.1016/j.electacta.2016.10.105
22. [22]
  Xu H, Zhang K, Yan B, et al. J. Power Sources, 2017, 356:27-35 doi: 10.1016/j.jpowsour.2017.04.070
23. [23]
  Xin Z L, Wang S H, Wang J, et al. Electrochem. Commun., 2016, 67:26-30 doi: 10.1016/j.elecom.2016.03.008
24. [24]
  Wang Y R, He Q L, Wei H G, et al. Electrochim. Acta, 2015, 184:452-465 doi: 10.1016/j.electacta.2015.10.046
25. [25]
  Krishna R, Fernandes D M, Marinoiu A, et al. Int. J. Hydrogen Energy, 2017, 42(37):23639-23646 doi: 10.1016/j.ijhydene.2017.04.263
26. [26]
  CHEN Ying, TANG Ya-Wen, GAO Ying, et al. Chinese J. Inorg. Chem., 2008, 24(4):560-564
27. [27]
  SHEN Juan-Zhang, TANG Ya-Wen, LU Tian-Hong. Chinese J. Inorg. Chem., 2012, 28(2):326-330
28. [28]
  Li J D, Tian Q F, Jiang S Y, et al. Electrochim. Acta, 2016, 213:21-30 doi: 10.1016/j.electacta.2016.06.041
29. [29]
  Hu S Z, Munoz F, Noborikawa J, et al. Appl. Catal., B, 2016, 180:758-765 doi: 10.1016/j.apcatb.2015.07.023
30. [30]
  Jiang K, Zhang H X, Zou S Z, et al. Phys. Chem. Chem. Phys., 2014, 16(38):20360-20376 doi: 10.1039/C4CP03151B
31. [31]
  Haan J L, Stafford K M, Masel R I. J. Phys. Chem. C, 2010, 114(26):11665-11672 doi: 10.1021/jp102990t
32. [32]
  Yi Q F, Huang W, Liu X P, et al. J. Electroanal. Chem., 2008, 619(1):197-205
33. [33]
  Liu D, Xie M L, Wang C M, et al. Nano Res., 2016, 9(6):1590-1599 doi: 10.1007/s12274-016-1053-6
34. [34]
  Tu D D, Wu B, Wang B X, et al. Appl. Catal., B, 2011, 103(1/2):163-168
35. [35]
  Yi Q F, Chen Q H, Yang Z. J. Power Sources, 2015, 298:171-176 doi: 10.1016/j.jpowsour.2015.08.050
36. [36]
  Zhang Y Y, Yi Q F, Zou T, et al. Ionics, 2017, 23:3169-3176 doi: 10.1007/s11581-017-2113-y
37. [37]
  Suo Y G, Hsing I M. Electrochim. Acta, 2011, 56:2174-2183 doi: 10.1016/j.electacta.2010.12.037
38. [38]
  Yurderi M, Bulut A, Zahmakirana M, et al. Appl. Catal., B, 2014, 160(7):514-524
39. [39]
  Zhang J M, Wang R X, Nong R J, et al. Int. J. Hydrogen Energy, 2017, 42(10):7226-7234 doi: 10.1016/j.ijhydene.2016.05.198
40. [40]
  Lu Y Z, Chen W. J. Phys. Chem. C, 2010, 114(49):21190-21200 doi: 10.1021/jp107768n
41. [41]
  Liu Z L, Zhang X H. Electrochem. Commun., 2009, 11(8):1667-1670 doi: 10.1016/j.elecom.2009.06.023
42. [42]
  Zhu F C, Ma G S, Bai Z C, et al. J. Power Sources, 2013, 242(22):610-620
43. [43]
  Shen Y Y, Sun Y, Zhou L N, et al. J. Mater. Chem. A, 2014, 2(9):2977-2984 doi: 10.1039/c3ta14502f
44. [44]
  Marinšek M, Šala M, Jančar B. J. Power Sources, 2013, 235(8):111-116
45. [45]
  Yi Q F, Chu H, Tang M X, et al. J. Electroanal. Chem., 2015, 739:178-186 doi: 10.1016/j.jelechem.2014.12.029
46. [46]
  Cazares-Ávila E, Ruiz-Ruiz E J, Hernández-Ramírez A, et al. Int. J. Hydrogen Energy, 2017, 42(51):30349-30358 doi: 10.1016/j.ijhydene.2017.08.156
47. [47]
  Carmo M, Paganin V A, Rosolen J M, et al. J. Power Sources, 2005, 142(1):169-176
48. [48]
  Zhang Y Y, Yi Q F, Deng Z L, et al. Catal. Lett., 2018, 148:1190-1201 doi: 10.1007/s10562-018-2335-2
49. [49]
  Xiong B, Zhou Y K, Zhao Y Y, et al. Carbon, 2013, 52(2):181-192
50. [50]
  Yang Z Z, Wang X L, Kang X, et al. Electrochim. Acta, 2017, 236:72-81 doi: 10.1016/j.electacta.2017.03.165
51. [51]
  Lewera A, Barczuk P J, Skorupska K, et al. J. Electroanal. Chem., 2011, 662(1):93-99 doi: 10.1016/j.jelechem.2011.03.038
52. [52]
  Kakaei K, Dorraji M. Electrochim. Acta, 2014, 143:207-215 doi: 10.1016/j.electacta.2014.07.134
53. [53]
  Li S S, Wang A J, Hu Y Y, et al. J. Mater. Chem. A, 2014, 2(43):18177-18183 doi: 10.1039/C4TA04164J
54. [54]
  Ha S, Larsen R, Masel R I. J. Power Sources, 2005, 144(1):28-34 doi: 10.1016/j.jpowsour.2004.12.031
55. [55]
  Wang Y Y, Qi Y Y, Zhang D J. Comput. Theor. Chem., 2014, 1049:51-54 doi: 10.1016/j.comptc.2014.09.020
56. [56]
  Zhang S X, Qing M, Zhang H, et al. Electrochem. Commun., 2009, 11(11):2249-2252 doi: 10.1016/j.elecom.2009.10.001
57. [57]
  Vafaei M, Rezaei M, Tabaian S H, et al. J. Solid State Electrochem., 2015, 19(1):289-298 doi: 10.1007/s10008-014-2561-5
1. [1]
  Kun Wang , Tianxue Gong , Yaohuang Huang , Boyang Han , Hanxiao Yang , Pavlo O. Dral , Weiwei Fang . Bornylimidazo[1,5–a]pyridin-3-ylidene allylic Pd catalyst with optimal electronic and steric properties for synthesis of 3,3′-disubstituted oxindoles. Chinese Chemical Letters, 2025, 36(7): 110539-. doi: 10.1016/j.cclet.2024.110539
2. [2]
  Yanxin Jiang , Kwai Wun Cheng , Zhiping Yang , Jun (Joelle) Wang . Pd-catalyzed enantioselective and regioselective asymmetric hydrophosphorylation and hydrophosphinylation of enynes. Chinese Chemical Letters, 2025, 36(5): 110231-. doi: 10.1016/j.cclet.2024.110231
3. [3]
  Tian TIAN , Meng ZHOU , Jiale WEI , Yize LIU , Yifan MO , Yuhan YE , Wenzhi JIA , Bin HE . Ru-doped Co₃O₄/reduced graphene oxide: Preparation and electrocatalytic oxygen evolution property. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 385-394. doi: 10.11862/CJIC.20240298
4. [4]
  Xiaoxiao Huang , Zhi-Long He , Yangpeng Chen , Lei Li , Zhenyu Yang , Chunyang Zhai , Mingshan Zhu . Novel P-doping-tuned Pd nanoflowers/S,N-GQDs photo-electrocatalyst for high-efficient ethylene glycol oxidation. Chinese Chemical Letters, 2024, 35(6): 109271-. doi: 10.1016/j.cclet.2023.109271
5. [5]
  Xichen YAO , Shuxian WANG , Yun WANG , Cheng WANG , Chuang ZHANG . Oxygen reduction performance of self?supported Fe/N/C three-dimensional aerogel catalyst layers. Chinese Journal of Inorganic Chemistry, 2025, 41(7): 1387-1396. doi: 10.11862/CJIC.20240384
6. [6]
  Yi Zhang , Biao Wang , Chao Hu , Muhammad Humayun , Yaping Huang , Yulin Cao , Mosaad Negem , Yigang Ding , Chundong Wang . Fe–Ni–F electrocatalyst for enhancing reaction kinetics of water oxidation. Chinese Journal of Structural Chemistry, 2024, 43(2): 100243-100243. doi: 10.1016/j.cjsc.2024.100243
7. [7]
  Min Song , Qian Zhang , Tao Shen , Guanyu Luo , Deli Wang . Surface reconstruction enabled o-PdTe@Pd core-shell electrocatalyst for efficient oxygen reduction reaction. Chinese Chemical Letters, 2024, 35(8): 109083-. doi: 10.1016/j.cclet.2023.109083
8. [8]
  Haodong JIN , Qingqing LIU , Chaoyang SHI , Danyang WEI , Jie YU , Xuhui XU , Mingli XU . NiCu/ZnO heterostructure photothermal electrocatalyst for efficient hydrogen evolution reaction. Chinese Journal of Inorganic Chemistry, 2025, 41(6): 1068-1082. doi: 10.11862/CJIC.20250048
9. [9]
  Huafeng SHI . Construction of MnCoNi layered double hydroxide@Co-Ni-S amorphous hollow polyhedron composite with excellent electrocatalytic oxygen evolution performance. Chinese Journal of Inorganic Chemistry, 2025, 41(7): 1380-1386. doi: 10.11862/CJIC.20240378
10. [10]
  Ruige ZHANG , Zhe ZHANG , He ZHENG , Zhan SHI . Recent advances of metal-organic frameworks for alkaline electrocatalytic oxygen evolution reaction. Chinese Journal of Inorganic Chemistry, 2025, 41(10): 2011-2028. doi: 10.11862/CJIC.20250185
11. [11]
  Jing Cao , Dezheng Zhang , Bianqing Ren , Ping Song , Weilin Xu . Mn incorporated RuO₂ nanocrystals as an efficient and stable bifunctional electrocatalyst for oxygen evolution reaction and hydrogen evolution reaction in acid and alkaline. Chinese Chemical Letters, 2024, 35(10): 109863-. doi: 10.1016/j.cclet.2024.109863
12. [12]
  Jun Luo , Yanya Liu , Jianghuaxiong Zhu , Chengxiong Wang , Yunkun Zhao , Dong Yan , Jian Li , Lichao Jia . A proton-conducting solid oxide fuel cell for co-production of ethylene and power via ethane conversion. Chinese Chemical Letters, 2025, 36(7): 110171-. doi: 10.1016/j.cclet.2024.110171
13. [13]
  Huipeng Zhao , Xiaoqiang Du . Polyoxometalates as the redox anolyte for efficient conversion of biomass to formic acid. Chinese Journal of Structural Chemistry, 2024, 43(2): 100246-100246. doi: 10.1016/j.cjsc.2024.100246
14. [14]
  Yang Liu , Jing Liang , Mengzhu Zheng , Haoze Song , Lixia Chen , Hua Li . PD-L1/SHP2 dual PROTACs inhibit melanoma by enhancing T-cell killing activity. Chinese Chemical Letters, 2025, 36(6): 110317-. doi: 10.1016/j.cclet.2024.110317
15. [15]
  Linhui Liu , Wuwan Xiong , Mingli Fu , Junliang Wu , Zhenguo Li , Daiqi Ye , Peirong Chen . Efficient NO_x abatement by passive adsorption over a Pd-SAPO-34 catalyst prepared by solid-state ion exchange. Chinese Chemical Letters, 2024, 35(4): 108870-. doi: 10.1016/j.cclet.2023.108870
16. [16]
  Juhong Zhou , Hui Zhao , Ping Han , Ziyue Wang , Yan Zhang , Xiaoxia Mao , Konglin Wu , Shengjue Deng , Wenxiang He , Binbin Jiang . Strategic modulation of CoFe sites for advanced bifunctional oxygen electrocatalyst. Chinese Journal of Structural Chemistry, 2025, 44(1): 100470-100470. doi: 10.1016/j.cjsc.2024.100470
17. [17]
  Hanqing Zhang , Xiaoxia Wang , Chen Chen , Xianfeng Yang , Chungli Dong , Yucheng Huang , Xiaoliang Zhao , Dongjiang Yang . Selective CO2-to-formic acid electrochemical conversion by modulating electronic environment of copper phthalocyanine with defective graphene. Chinese Journal of Structural Chemistry, 2023, 42(10): 100089-100089. doi: 10.1016/j.cjsc.2023.100089
18. [18]
  Di Wang , Qing-Song Chen , Yi-Ran Lin , Yun-Xin Hou , Wei Han , Juan Yang , Xin Li , Zhen-Hai Wen . Tuning strategies and electrolyzer design for Bi-based nanomaterials towards efficient CO2 reduction to formic acid. Chinese Journal of Structural Chemistry, 2024, 43(8): 100346-100346. doi: 10.1016/j.cjsc.2024.100346
19. [19]
  Gang Hu , Chun Wang , Qinqin Wang , Mingyuan Zhu , Lihua Kang . The controlled oxidation states of the H₄PMo₁₁VO₄₀ catalyst induced by plasma for the selective oxidation of methacrolein. Chinese Chemical Letters, 2025, 36(2): 110298-. doi: 10.1016/j.cclet.2024.110298
20. [20]
  Yiyue Ding , Qiuxiang Zhang , Lei Zhang , Qilu Yao , Gang Feng , Zhang-Hui Lu . Exceptional activity of amino-modified rGO-immobilized PdAu nanoclusters for visible light-promoted dehydrogenation of formic acid. Chinese Chemical Letters, 2024, 35(7): 109593-. doi: 10.1016/j.cclet.2024.109593

Get Citation

PDF

XML

Metrics

PDF Downloads(18)
Abstract views(1670)
HTML views(341)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142