Citation: Yang Hu, Bin Liu, Luyao Xu, Ziqiang Dong, Yating Wu, Jie Liu, Cheng Zhong, Wenbin Hu. High-Throughput Synthesis and Screening of Pt-Based Ternary Electrocatalysts Using a Microfluidic-Based Platform[J]. Acta Physico-Chimica Sinica, ;2023, 39(3): 220900. doi: 10.3866/PKU.WHXB202209004 shu

High-Throughput Synthesis and Screening of Pt-Based Ternary Electrocatalysts Using a Microfluidic-Based Platform

Yang Hu ¹ ,
Bin Liu ² ,
Luyao Xu ³ ,
Ziqiang Dong ⁴ ,
Yating Wu ¹ ,
Jie Liu ^2,, ,
Cheng Zhong ^{2, 5, 6,,} ,
Wenbin Hu ^{2, 5, 6,,}

1.
State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
2.
Key Laboratory of Advanced Ceramics and Machining Technology (Ministry of Education), School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China
3.
Shenzhen Zhongwu Technology Co., Ltd, Shenzhen 518052, Guangdong Province, China
4.
Materials Genome Institute, Shanghai University, Shanghai 200444, China
5.
Tianjin Key Laboratory of Composite and Functional Materials, School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China
6.
Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Fuzhou 350207, China

Corresponding author: Jie Liu, jieliu0109@tju.edu.cn Cheng Zhong, cheng.zhong@tju.edu.cn Wenbin Hu, wbhu@tju.edu.cn
Received Date: 5 September 2022
Revised Date: 3 October 2022
Accepted Date: 4 October 2022
Available Online: 11 October 2022
Fund Project: the National Key Research and Development Program 2016YFB0700205the Tianjin Natural Science Foundation for Distinguished Young Scholar 18JCJQJC46500the National Youth Talent Support Program, and the National Science Foundation for Excellent Young Scholar 51722403

Pt-based electrocatalysts have received extensive attention owing to their wide applications in various fields, including fuel cells, hydrogen production, degradation of organic pollutants, electrochemical sensors, and oxidation of small molecules. Therefore, the efficient synthesis and screening of high-performance Pt-based electrocatalysts is necessary for accelerating their further development and application in these fields. The conventional method for developing the advanced materials and optimizing their synthesis parameters is time-consuming, inefficient, and costly. Microfluidic high-throughput techniques have the great potential for optimizing the synthesis parameters of Pt-based electrocatalysts. However, microfluidic high-throughput synthesis without performance evaluation cannot maximize its advantages. Therefore, it is highly desirable to develop a platform that combines the high-throughput synthesis of materials and the evaluation of their properties in a high-throughput fashion to improve the overall screening efficiency of the novel materials. In this study, a versatile microfluidic high-throughput platform, combining the high-throughput synthesis and screening of materials, was constructed. The microfluidic chip generated 20-level concentration gradients of the three different precursors. Microreactor arrays with 100 microchannels were used for the material synthesis and electrochemical characterization. A wide range of concentration combinations of the three different precursor solutions was achieved using the microfluidic chip. Five groups of Pt-based ternary electrocatalysts (100 different components in total) were synthesized and electrochemically characterized using the designed platform. The obtained Pt-based electrocatalysts exhibited a loose particle morphology, and were composed of small nanoparticles. The efficient preparation of Pt-based electrocatalysts with controllable compositions was also achieved through the high-throughput synthesis platform. The catalytic performance of the Pt-based catalysts towards oxygen evolution reaction (OER) was characterized by chronoamperometry. The optimal composition of Pt-based ternary electrocatalysts for OER was directly determined using the designed platform. For NiPtCu, the samples with a relatively high atomic percentage (approximately 50%) of Pt (i.e., Ni_0.30Pt_0.56Cu_0.14, Ni_0.17Pt_0.52Cu_0.31 and Ni_0.12Pt_0.48Cu_0.40) exhibited higher electrocatalytic activity and stability, whereas the samples with a relatively high atomic percentage (> 50%) of Cu possessed lower activity and stability. For AuPtNi and AuPtCu, the samples wherein Au and Pt accounted for a large proportion of the sample (i.e., Ni or Cu < 10%) and the atomic ratios of Au : Pt were (3–4) : 1, e.g., Au_0.71Pt_0.25Ni_0.04 and Au_0.77Pt_0.18Cu_0.05, displayed high electrocatalytic activity and stability. As the atomic fraction of Au decreased, the atomic ratio of Pt and Ni in AuPtNi approached 3 : 1 or that of Pt and Cu in AuPtCu reached to 1 : 1, the samples (Au_0.54Pt_0.35Ni_0.11, Au_0.35Pt_0.42Cu_0.23, Au_0.27Pt_0.41Cu_0.32 and Au_0.12Pt_0.32Cu_0.56) all demonstrated high electrocatalytic activity and stability. The samples (Pt_0.06Cu_0.94) wherein the atomic percentages of Au and Pt were all less than 10%, exhibited poor electrocatalytic activity and stability. For RhPtNi and RhPtCu, when the atomic percentage of Rh in RhPtNi and RhPtCu was high (50%–90%) and almost no Ni or Cu was present, the samples (Rh_0.91Pt_0.09 and Rh_0.82Pt_0.18 for RhPtNi, as well as Rh_0.88Pt_0.12 and Rh_0.75Pt_0.21Cu_0.04 for RhPtCu) all had high electrocatalytic activity and stability. As the atomic percentage of Rh decreased and that of Pt increased, the atomic percentages of Rh and Pt were relatively close, Rh_0.54Pt_0.32Ni_0.14 and Rh_0.51Pt_0.36Cu_0.14 showing high electrocatalytic activity and stability. When the atomic percentages of Ni and Cu were high (> 50%), the RhPtNi and RhPtCu samples all showed the relatively poor electrocatalytic activity and stability. These results demonstrate the high efficiency and flexibility of the constructed microfluidic high-throughput platform, which significantly shortens the cycle for the development cycle of new materials and the optimization of their properties.
- High-throughput method,
- Electrocatalyst,
- Microfluidic technique,
- Electrochemical evaluation,
- Oxygen evolution reaction
1. [1]
  Li, M.; Xia, Z.; Huang, Y. H.; Tao, L.; Chao, Y.; Yin, K.; Yang, W.; Yang, W.; Yu, Y.; Guo, S. Acta Phys. -Chim. Sin. 2020, 36, 1912049. doi: 10.3866/PKU.WHXB201912049
2. [2]
  Liang, J.; Liu, X.; Li, Q. Acta Phys. -Chim. Sin. 2021, 37, 2010072. doi: 10.3866/PKU.WHXB202010072
3. [3]
  Xiao, Y.; Pei, Y.; Hu, Y.; Ma, R.; Wang, D.; Wang, J. Acta Phys. -Chim. Sin. 2021, 37, 2009051. doi: 10.3866/PKU.WHXB202009051
4. [4]
  Rao, P.; Luo, J.; Li, J.; Huang, W.; Sun, W.; Chen, Q.; Jia, C.; Liu, Z.; Deng, P.; Shen, Y.; et al. Carbon Energy 2022, 1. doi: 10.1002/cey2.192 doi: 10.1002/cey2.192
5. [5]
  Lin, L.; Zhou, W.; Gao, R.; Yao, S.; Zhang, X.; Xu, W.; Zheng, S.; Jiang, Z.; Yu, Q.; Li, Y. -W.; et al. Nature 2017, 544, 80. doi: 10.1038/nature21672 doi: 10.1038/nature21672
6. [6]
  Luo, M.; Yao, W.; Huang, C.; Wu, Q.; Xu, Q. J. Mater. Chem. A 2015, 3, 13884. doi: 10.1039/C5TA00218D doi: 10.1039/C5TA00218D
7. [7]
  Xu, J.; Amorim, I.; Li, Y.; Li, J.; Yu, Z.; Zhang, B.; Araujo, A.; Zhang, N.; Liu, L. Carbon Energy 2020, 2, 646. doi: 10.1002/cey2.56 doi: 10.1002/cey2.56
8. [8]
  Song, W.; Li, M.; Wang, C.; Lu, X. Carbon Energy 2021, 3, 101. doi: 10.1002/cey2.85 doi: 10.1002/cey2.85
9. [9]
  Cao, B.; Li, G.; Li, H. Appl. Catal. B-Environ. 2016, 194, 42. doi: 10.1016/j.apcatb.2016.04.033 doi: 10.1016/j.apcatb.2016.04.033
10. [10]
  Xu, T.; Zhao, H.; Zheng, H.; Zhang, P. Chem. Eng. J. 2020, 385, 123832. doi: 10.1016/j.cej.2019.123832 doi: 10.1016/j.cej.2019.123832
11. [11]
  Zhai, D.; Liu, B.; Shi, Y.; Pan, L.; Wang, Y.; Li, W.; Zhang, R.; Yu, G. ACS Nano 2013, 7, 3540. doi: 10.1021/nn400482d doi: 10.1021/nn400482d
12. [12]
  Kumar, M. K.; Ramaprabhu, S. J. Phys. Chem. B 2006, 110, 11291. doi: 10.1021/jp0611525 doi: 10.1021/jp0611525
13. [13]
  Liu, J.; Chen, B.; Kou, Y.; Liu, Z.; Chen, X.; Li, Y.; Deng, Y.; Han, X.; Hu, W.; Zhong, C. J. Mater. Chem. A 2016, 4, 11060. doi: 10.1039/C6TA02284G doi: 10.1039/C6TA02284G
14. [14]
  Liu, J.; Liu, Z.; Wang, H.; Liu, B.; Zhao, N.; Zhong, C.; Hu, W. Adv. Funct. Mater. 2022, 32, 2110702. doi: 10.1002/adfm.202110702 doi: 10.1002/adfm.202110702
15. [15]
  Li, G.; Wen, P.; Gao, C.; Zhang, T.; Hu, J.; Zhang, Y.; Guan, S.; Li, Q.; Li, B. Int. J. Min. Met. Mater. 2021, 28, 1224. doi: 10.1007/s12613-020-2076-2 doi: 10.1007/s12613-020-2076-2
16. [16]
  Wang, X.; Zhang, J.; Cao, X.; Jiang, Y.; Zhu, H. Int. J. Min. Met. Mater. 2011, 18, 594. doi: 10.1007/s12613-011-0483-0 doi: 10.1007/s12613-011-0483-0
17. [17]
  Zhong, C.; Liu, J.; Ni, Z.; Deng, Y.; Chen, B.; Hu, W. Sci. China Mater. 2014, 57, 13. doi: 10.1007/s40843-014-0010-5 doi: 10.1007/s40843-014-0010-5
18. [18]
  Scheidtmann, J.; Weiß, P. A.; Maier, W. F. Appl. Catal. A-Gen. 2001, 222, 79. doi: 10.1016/S0926-860X(01)00831-6 doi: 10.1016/S0926-860X(01)00831-6
19. [19]
  Nursam, N. M.; Wang, X.; Caruso, R. A. ACS Comb. Sci. 2015, 17, 548. doi: 10.1021/acscombsci.5b00049 doi: 10.1021/acscombsci.5b00049
20. [20]
  Liu, D.; Cito, S.; Zhang, Y.; Wang, C. -F.; Sikanen, T. M.; Santos, H. A. Adv. Mater. 2015, 27, 2298. doi: 10.1002/adma.201405408 doi: 10.1002/adma.201405408
21. [21]
  Liu, X.; Liu, B.; Ding, J.; Deng, Y.; Han, X.; Zhong, C.; Hu, W. Adv. Funct. Mater. 2022, 32, 2107862. doi: 10.1002/adfm.202107862 doi: 10.1002/adfm.202107862
22. [22]
  Hu, Y.; Liu, B.; Wu, Y.; Li, M.; Liu, X.; Ding, J.; Han, X.; Deng, Y.; Hu, W.; Zhong, C. Front. Chem. 2020, 8, 579828. doi: 10.3389/fchem.2020.579828 doi: 10.3389/fchem.2020.579828
23. [23]
  Manz, A.; Harrison, D. J.; Verpoort, E. M. J.; Fettinger, J. C.; Paulus, A.; Lüdi, H.; Widmer, H. M. J. Chromatogr. A 1992, 593, 253. doi: 10.1016/0021-9673(92)80293-4 doi: 10.1016/0021-9673(92)80293-4
24. [24]
  Agresti, J. J.; Antipov, E.; Abate, A. R.; Ahn, K.; Rowat, A. C.; Baret, J. -C.; Marquez, M.; Klibanov, A. M.; Griffiths, A. D.; Weitz, D. A. Proc. Natl. Acad. Sci. 2010, 107, 4004. doi: 10.1073/pnas.0910781107 doi: 10.1073/pnas.0910781107
25. [25]
  Huang, M. C.; Cheong, W. C.; Lim, L. S.; Li, M. -H. Electrophoresis 2012, 33, 788. doi: 10.1002/elps.201100460 doi: 10.1002/elps.201100460
26. [26]
  Whitesides, G. M. Nature 2006, 442, 368. doi: 10.1038/nature05058 doi: 10.1038/nature05058
27. [27]
  Atencia, J.; Beebe, D. J. Nature 2005, 437, 648. doi: 10.1038/nature04163 doi: 10.1038/nature04163
28. [28]
  Du, G.; Fang, Q.; den Toonder, J. M. J. Anal. Chim. Acta 2016, 903, 36. doi: 10.1016/j.aca.2015.11.023 doi: 10.1016/j.aca.2015.11.023
29. [29]
  Lu, Q.; Huan, J.; Han, C.; Sun, L.; Yang, X. Electrochim. Acta 2018, 266, 305. doi: 10.1016/j.electacta.2018.02.021 doi: 10.1016/j.electacta.2018.02.021
30. [30]
  Huang, X.; Zhu, E.; Chen, Y.; Li, Y.; Chiu, C. -Y.; Xu, Y.; Lin, Z.; Duan, X.; Huang, Y. Adv. Mater. 2013, 25, 2974. doi: 10.1002/adma.201205315 doi: 10.1002/adma.201205315
31. [31]
  Jiang, Y.; Jia, Y.; Zhang, J.; Zhang, L.; Huang, H.; Xie, Z.; Zheng, L. Chem. -Eur. J. 2013, 19, 3119. doi: 10.1002/chem.201203729 doi: 10.1002/chem.201203729
32. [32]
  Mott, D.; Luo, J.; Njoki, P. N.; Lin, Y.; Wang, L.; Zhong, C. -J. Catal. Today 2007, 122, 378. doi: 10.1016/j.cattod.2007.01.007 doi: 10.1016/j.cattod.2007.01.007
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