Citation: Zhao Xiaoyu, Zhao Huachao, Sun Jiefang, Li Gang, Liu Rui. Blocking the defect sites on ultrathin Pt nanowires with Rh atoms to optimize the reaction path toward alcohol fuel oxidation[J]. Chinese Chemical Letters, ;2020, 31(7): 1782-1786. doi: 10.1016/j.cclet.2020.01.005 shu

Blocking the defect sites on ultrathin Pt nanowires with Rh atoms to optimize the reaction path toward alcohol fuel oxidation

Zhao Xiaoyu ^a,*, ,
Zhao Huachao ^a ,
Sun Jiefang ^c ,
Li Gang ^b ,
Liu Rui ^b

a.
Tianjin Key Laboratory of Brine Chemical Engineering and Resource Eco-utilization, College of Chemical Engineering and Materials Science, Tianjin University of Science and Technology, Tianjin 300457, China
b.
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
c.
Beijing Key Laboratory of Diagnostic and Traceability Technologies for Food Poisoning, Beijing Center for Disease Prevention and Control, Beijing 100013, China

xyz@tust.edu.cn

Received Date: 29 November 2019
Revised Date: 23 December 2019
Accepted Date: 3 January 2020
Available Online: 5 January 2020

Figures(4)

Anodic electrocatalyst plays the core role in direct alcohol fuel cells (DAFCs), while traditional Pt-catalysts suffer from limited catalytic activity, high over potential and severe CO poisoning. Herein, by selectively depositing Rh atoms on the defective-sites of Pt nanowires (NWs), we developed a new Pt@Rh NW electrocatalyst that exhibited enhanced electrocatalytic performance for both methanol oxidation (MOR) and ethanol oxidation (EOR). Both cyclic voltammetry (CV) and in-situ infrared spectroscopy revealed that the presence of Rh atoms suppressed the generation of poisonous intermediates and completely oxidized alcohols molecule into CO₂. Atomic resolusion spherical aberration corrected high-angle annular dark field scanning transmission electron microscopy (CS-HAADF-STEM) and energy-dispersive X-ray spectroscopy (EDS) mapping analysis revealed that Rh atoms were primarily deposited on the defective sites of Pt NWs. Meanwhile, the presence of Rh atoms also modified the electronic state of Pt atoms and therefore lowered the onset potential for alcohols oxidation potential. This work gives the first clear clue on the role of the defective sites of Pt nanocatalyst poisoning, and propose that selectively blocking these sites with trace amount of Rh is an effective strategy in designing advantageous electrocatalysts.
- Nanowire catalyst,
- Ethanol electrooxidation,
- In situ FTIR,
- Defect regulation,
- Fuel cells
1. [1]
  C. Jiang, J. Ma, G. Corre, S.L. Jain, J.T.S. Irvine, Chem. Soc. Rev. 46 (2017) 2889-2912. doi: 10.1039/C6CS00784H
2. [2]
  C. Pak, S.W. Lee, C. Baik, et al., Chin. Chem. Lett. 30 (2019) 1186-1189. doi: 10.1016/j.cclet.2019.02.020
3. [3]
  B. Narayanamoorthy, K.K.R. Datta, M. Eswaramoorthy, S. Balaji, ACS Catal. 4 (2014) 3621-3629. doi: 10.1021/cs500628m
4. [4]
  W. Zhang, Y. Yang, B. Huang, et al., Adv. Mater. 31 (2019) 1805833. doi: 10.1002/adma.201805833
5. [5]
  B. Liu, Z.W. Chia, C.H. Cheng, J.Y. Lee, Energy Fuels 25 (2011) 3135-3141. doi: 10.1021/ef200696v
6. [6]
  Q. Chang, S. Kattel, X. Li, et al., ACS Catal. 9 (2019) 7618-7625. doi: 10.1021/acscatal.9b02039
7. [7]
  B.F. Zheng, T. Ouyang, Z. Wang, et al., Chem. Commun. 54 (2018) 9583-9586. doi: 10.1039/C8CC04199G
8. [8]
  E.N. El Sawy, P.G. Pickup, Electrochim. Acta 302 (2019) 234-240. doi: 10.1016/j.electacta.2019.02.047
9. [9]
  L. Zhang, Y. Gong, H. Liu, W. Yuan, Z. Liu, Electrochem. Commun. 84 (2017) 1-5. doi: 10.1016/j.elecom.2017.09.008
10. [10]
  H. Su, T.H. Chen, Chin. Chem. Lett. 27 (2016) 1083-1086. doi: 10.1016/j.cclet.2016.03.010
11. [11]
  F.H.B. Lima, E.R. Gonzalez, Electrochim. Acta 53 (2008) 2963-2971. doi: 10.1016/j.electacta.2007.11.007
12. [12]
  K. Liu, W. Wang, P. Guo, et al., Adv. Funct. Mater. 29 (2019) 1806300. doi: 10.1002/adfm.201806300
13. [13]
  Y. Shen, B. Gong, K. Xiao, L. Wang, ACS Appl. Mater. Interfaces 9 (2017) 3535-3543. doi: 10.1021/acsami.6b09573
14. [14]
  L. Huang, M. Liu, H. Lin, et al., Science 365 (2019) 1159-1163. doi: 10.1126/science.aax5843
15. [15]
  H.J. Yoon, S.K. Kim, W. Huang, Y. Sohn, Chin. Chem. Lett. 29 (2018) 800-804. doi: 10.1016/j.cclet.2018.01.021
16. [16]
  N. Tian, Z.Y. Zhou, S.G. Sun, Y. Ding, Z.L. Wang, Science 316 (2007) 732-735. doi: 10.1126/science.1140484
17. [17]
  R. Wang, C. Wang, W.B. Cai, Y. Ding, Adv. Mater. 22 (2010) 1845-1848. doi: 10.1002/adma.200903548
18. [18]
  Y. Zhu, L. Bu, Q. Shao, X. Huang, ACS Catal. 9 (2019) 6607-6612. doi: 10.1021/acscatal.9b01375
19. [19]
  K. Wang, H. Du, R. Sriphathoorat, P.K. Shen, Adv. Mater. 30 (2018) 1804074. doi: 10.1002/adma.201804074
20. [20]
  H. Liu, J. Li, L. Wang, et al., Nano Res. 10 (2017) 3324-3332. doi: 10.1007/s12274-017-1545-z
21. [21]
  P. Mai, A. Haze, M. Chiku, E. Higuchi, H.J.C. Inoue, Catalysts 7 (2017) 246. doi: 10.3390/catal7090246
22. [22]
  C. Zhu, B. Lan, R.L. Wei, C.N. Wang, Y.Y. Yang, ACS Catal. 9 (2019) 4046-4053. doi: 10.1021/acscatal.9b00138
23. [23]
  R. Liu, H. Zhao, X. Zhao, et al., Environ. Sci. Technol. 52 (2018) 9992-10002. doi: 10.1021/acs.est.8b02740
24. [24]
  T. Haisch, F. Kubannek, S. Baranton, C. Coutanceau, U. Krewer, Electrochim. Acta 295 (2019) 278-285. doi: 10.1016/j.electacta.2018.10.073
25. [25]
  W. Tokarz, H. Siwek, P. Piela, A. Czerwinski, Electrochim. Acta 52 (2007) 5565-5573. doi: 10.1016/j.electacta.2006.12.016
26. [26]
  Z.Y. Zhou, Z.Z. Huang, D.J. Chen, et al., Angew. Chem. Int. Ed. 49 (2010) 411-414. doi: 10.1002/anie.200905413
27. [27]
  M.E. Paulino, L.M.S. Nunes, E.R. Gonzalez, G. Tremiliosi Filho, Electrochem. Commun. 52 (2015) 85-88. doi: 10.1016/j.elecom.2014.12.025
28. [28]
  A. Bach Delpeuch, F. Maillard, M. Chatenet, P. Soudant, C. Cremers, Appl. Catal. B:Environ. 181 (2016) 672-680. doi: 10.1016/j.apcatb.2015.08.041
29. [29]
  A.M. Hofstead Duffy, D.J. Chen, S.G. Sun, Y.J. Tong, J. Mater. Chem. 22 (2012) 5205. doi: 10.1039/c2jm15426a
30. [30]
  J.C. Dong, X.G. Zhang, V. Briega Martos, et al., Nat. Energy 4 (2019) 60-67. doi: 10.1038/s41560-018-0292-z
1. [1]
  Jin Long , Xingqun Zheng , Bin Wang , Chenzhong Wu , Qingmei Wang , Lishan Peng . Improving the electrocatalytic performances of Pt-based catalysts for oxygen reduction reaction via strong interactions with single-CoN₄-rich carbon support. Chinese Chemical Letters, 2024, 35(5): 109354-. doi: 10.1016/j.cclet.2023.109354
2. [2]
  Kunsong Hu , Yulong Zhang , Jiayi Zhu , Jinhua Mai , Gang Liu , Manoj Krishna Sugumar , Xinhua Liu , Feng Zhan , Rui Tan . Nano-engineered catalysts for high-performance oxygen reduction reaction. Chinese Chemical Letters, 2024, 35(10): 109423-. doi: 10.1016/j.cclet.2023.109423
3. [3]
  Ping Liu , Fei Yu . Covalent organic framework ionomers for medium-temperature fuel cells. Chinese Journal of Structural Chemistry, 2025, 44(4): 100465-100465. doi: 10.1016/j.cjsc.2024.100465
4. [4]
  Yaxin Sun , Huiyu Li , Shiquan Guo , Congju Li . Metal-based cathode catalysts for electrocatalytic ORR in microbial fuel cells: A review. Chinese Chemical Letters, 2024, 35(5): 109418-. doi: 10.1016/j.cclet.2023.109418
5. [5]
  Jiaqi Lin , Pupu Yang , Yimin Jiang , Shiqian Du , Dongcai Zhang , Gen Huang , Jinbo Wang , Jun Wang , Qie Liu , Miaoyu Li , Yujie Wu , Peng Long , Yangyang Zhou , Li Tao , Shuangyin Wang . Surface decoration prompting the decontamination of active sites in high-temperature proton exchange membrane fuel cells. Chinese Chemical Letters, 2024, 35(11): 109435-. doi: 10.1016/j.cclet.2023.109435
6. [6]
  Wenbiao Zhang , Bolong Yang , Zhonghua Xiang . Atomically dispersed Cu-based metal-organic framework directly for alkaline polymer electrolyte fuel cells. Chinese Chemical Letters, 2025, 36(2): 109630-. doi: 10.1016/j.cclet.2024.109630
7. [7]
  Tianhao Li , Wenguang Tu , Zhigang Zou . In situ photocatalytically enhanced thermogalvanic cells for electricity and hydrogen production. Chinese Journal of Structural Chemistry, 2024, 43(1): 100195-100195. doi: 10.1016/j.cjsc.2023.100195
8. [8]
  Yingfen Li , Zhiqi Wang , Yunhai Zhao , Dajun Luo , Xueliang Zhang , Jun Zhao , Zhenghua Su , Shuo Chen , Guangxing Liang . Potassium doping for grain boundary passivation and defect suppression enables highly-efficient kesterite solar cells. Chinese Chemical Letters, 2024, 35(11): 109468-. doi: 10.1016/j.cclet.2023.109468
9. [9]
  Bo Yang , Pu-An Lin , Tingwei Zhou , Xiaojia Zheng , Bing Cai , Wen-Hua Zhang . Facile surface regulation for highly efficient and thermally stable perovskite solar cells via chlormequat chloride. Chinese Chemical Letters, 2024, 35(10): 109425-. doi: 10.1016/j.cclet.2023.109425
10. [10]
  Rongjun Zhao , Tai Wu , Yong Hua , Yude Wang . Improving performance of perovskite solar cells enabled by defects passivation and carrier transport dynamics regulation via organic additive. Chinese Chemical Letters, 2025, 36(2): 109587-. doi: 10.1016/j.cclet.2024.109587
11. [11]
  Ming-Zhen Li , Yang Zhang , Kun Li , Ya-Nan Shang , Yi-Zhen Zhang , Yu-Jiao Kan , Zhi-Yang Jiao , Yu-Yuan Han , Xiao-Qiang Cao . In situ regeneration of catalyst for Fenton-like degradation by photogenerated electron transportation: Characterization, performance and mechanism comparison. Chinese Chemical Letters, 2025, 36(1): 109885-. doi: 10.1016/j.cclet.2024.109885
12. [12]
  Rui Liu , Yue Yu , Lu Deng , Maoxia Xu , Haorong Ren , Wenjie Luo , Xudong Cai , Zhenyu Li , Jingyu Chen , Hua Yu . The synergistic effect of A-site cation engineering and phase regulation enables efficient and stable Ruddlesden-Popper perovskite solar cells. Chinese Chemical Letters, 2024, 35(12): 109545-. doi: 10.1016/j.cclet.2024.109545
13. [13]
  Dai-Huo Liu , Ao Wang , Hong-Yan Lü , Xing-Long Wu , Dan Luo , Wen-Hao Li , Jin-Zhi Guo , Haozhen Dou , Qianyi Ma , Zhongwei Chen . In situ constructing (MnS/Mn₂SnS₄)@N,S-ACTs heterostructure with superior Na/Li-storage capabilities in half-cells and pouch full-cells. Chinese Chemical Letters, 2024, 35(11): 109285-. doi: 10.1016/j.cclet.2023.109285
14. [14]
  Shengfei Dong , Ziyu Liu , Xiaoyi Yang . Hydrothermal liquefaction of biomass for jet fuel precursors: A review. Chinese Chemical Letters, 2024, 35(8): 109142-. doi: 10.1016/j.cclet.2023.109142
15. [15]
  Tao Ban , Xi-Yang Yu , Hai-Kuo Tian , Zheng-Qing Huang , Chun-Ran Chang . One-step conversion of methane and formaldehyde to ethanol over SA-FLP dual-active-site catalysts: A DFT study. Chinese Chemical Letters, 2024, 35(4): 108549-. doi: 10.1016/j.cclet.2023.108549
16. [16]
  Xinyi Hu , Riguang Zhang , Zhao Jiang . Depositing the PtNi nanoparticles on niobium oxide to enhance the activity and CO-tolerance for alkaline methanol electrooxidation. Chinese Journal of Structural Chemistry, 2023, 42(11): 100157-100157. doi: 10.1016/j.cjsc.2023.100157
17. [17]
  Lili Wang , Ya Yan , Rulin Li , Xujie Han , Jiahui Li , Ting Ran , Jialu Li , Baichuan Xiong , Xiaorong Song , Zhaohui Yin , Hong Wang , Qingjun Zhu , Bowen Cheng , Zhen Yin . Interface engineering of 2D NiFe LDH/NiFeS heterostructure for highly efficient 5-hydroxymethylfurfural electrooxidation. Chinese Chemical Letters, 2024, 35(9): 110011-. doi: 10.1016/j.cclet.2024.110011
18. [18]
  Shengkai Li , Yuqin Zou , Chen Chen , Shuangyin Wang , Zhao-Qing Liu . Defect engineered electrocatalysts for C–N coupling reactions toward urea synthesis. Chinese Chemical Letters, 2024, 35(8): 109147-. doi: 10.1016/j.cclet.2023.109147
19. [19]
  Chengcheng Xie , Chengyi Xiao , Hongshuo Niu , Guitao Feng , Weiwei Li . Mesoporous organic solar cells. Chinese Chemical Letters, 2024, 35(11): 109849-. doi: 10.1016/j.cclet.2024.109849
20. [20]
  Ting Xie , Xun He , Lang He , Kai Dong , Yongchao Yao , Zhengwei Cai , Xuwei Liu , Xiaoya Fan , Tengyue Li , Dongdong Zheng , Shengjun Sun , Luming Li , Wei Chu , Asmaa Farouk , Mohamed S. Hamdy , Chenggang Xu , Qingquan Kong , Xuping Sun . CoSe₂ nanowire array enabled highly efficient electrocatalytic reduction of nitrate for ammonia synthesis. Chinese Chemical Letters, 2024, 35(11): 110005-. doi: 10.1016/j.cclet.2024.110005

Get Citation

PDF

XML

Metrics

PDF Downloads(6)
Abstract views(826)
HTML views(81)

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