Citation: Ruifang Wei, Dongfeng Li, Heng Yin, Xiuli Wang, Can Li. Operando Electrochemical UV-Vis Absorption Spectroscopy with Microsecond Time Resolution[J]. Acta Physico-Chimica Sinica, ;2023, 39(2): 220703. doi: 10.3866/PKU.WHXB202207035 shu

Operando Electrochemical UV-Vis Absorption Spectroscopy with Microsecond Time Resolution

Ruifang Wei ^{1, 2} ,
Dongfeng Li ^{2, 3} ,
Heng Yin ² ,
Xiuli Wang ^2,, ,
Can Li ^{1, 2, 3,,}

1.
Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China
2.
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning Province, China
3.
University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: Xiuli Wang, xiuliwang@dicp.ac.cn Can Li, canli@dicp.ac.cn
Received Date: 15 July 2022
Revised Date: 22 August 2022
Accepted Date: 5 September 2022
Available Online: 8 September 2022
Fund Project: the National Key R & D Program of China 2021YFA1500600the DICP Foundation of Innovative Research DICP I202122

Operando spectroscopic characterization is effective for examining electrocatalytic reaction mechanisms. However, most operando characterization techniques currently used are based on (quasi-)steady-state spectroscopy, which often cannot directly measure transient changes occurring on the micro-millisecond time scale. Herein, an operando electrochemical UV-Vis absorption spectroscopy with 3 μs time resolution was realized by introducing bias pulses and synchronizing the bias pulse and spectral signals. Comparing the time-dependence curves of the bias pulse, collected spectral curve, and controlling voltage, a good time consistence for the three signals was observed, demonstrating the time-resolved ability of the novel apparatus. More importantly, two oxidation reactions, water oxidation reaction and hole sacrifice reagent oxidation reaction, showed distinct dynamics, verifying the reliability of the time-resolved kinetics. The water oxidation kinetics on a ferrihydrite (Fh) electrocatalyst were studied by this novel operando spectroscopic system. Different water oxidation steps were decoupled by analyzing the accumulation and decay dynamics of the operando time-resolved UV-Vis absorption data with various pulse widths and magnitudes of applied bias. A long bias pulse with width above 1s enabled the continuous accumulation of reaction intermediates in Fh electrocatalyst to reach a quasi-equilibrium state with electron extraction into the external circuit. In addition, a fast decay for water oxidation was observed after the applied bias was turned off. Importantly, when a short bias pulse with tens of ms width was applied, an abnormal intermediate accumulation process was observed after the applied bias was shut off, revealing a spontaneous species transformation process. These results confirm the validity of this novel method for examining species transformation kinetics at a fast timescale. The formation, transformation, and reaction kinetics of water oxidation reaction intermediates were directly studied on a µs to s time scale. Therefore, operando electrochemical UV-Vis absorption spectroscopy with µs time resolution can promote the understanding of various electrocatalytic reaction mechanisms and be used to guide the design and synthesis of novel high-efficiency electrocatalysts.
- Electrocatalysis,
- Operando electrochemistry,
- UV-Vis absorption spectroscopy,
- Bias pulse,
- Time-resolved
1. [1]
  Chu, S.; Majumdar, A. Nature 2012, 488, 294. doi: 10.1038/nature11475 doi: 10.1038/nature11475
2. [2]
  Dusastre, V.; Martiradonna, L. Nat. Mater. 2016, 16, 15. doi: 10.1038/nmat4838 doi: 10.1038/nmat4838
3. [3]
  Yang, H.; Han, X.; Douka, A. I.; Huang, L.; Gong, L.; Xia, C.; Park, H. S.; Xia, B. Y. Adv. Funct. Mater. 2020, 31, 2007602. doi: 10.1002/adfm.202007602 doi: 10.1002/adfm.202007602
4. [4]
  Seh, Z. W.; Kibsgaard, J.; Dickens, C. F.; Chorkendorff, I.; Norskov, J. K.; Jaramillo, T. F. Science 2017, 355, eaad4998. doi: 10.1126/science.aad4998 doi: 10.1126/science.aad4998
5. [5]
  Suen, N. T.; Hung, S. F.; Quan, Q.; Zhang, N.; Xu, Y. J.; Chen, H. M. Chem. Soc. Rev. 2017, 46, 337. doi: 10.1039/c6cs00328a doi: 10.1039/c6cs00328a
6. [6]
  Moysiadou, A.; Lee, S.; Hsu, C. S.; Chen, H. M.; Hu, X. J. Am. Chem. Soc. 2020, 142, 11901. doi: 10.1021/jacs.0c04867 doi: 10.1021/jacs.0c04867
7. [7]
  An, H.; Chen, Z.; Yang, J.; Feng, Z.; Wang, X.; Fan, F.; Li, C. J. Catal. 2018, 367, 53. doi: 10.1016/j.jcat.2018.08.007 doi: 10.1016/j.jcat.2018.08.007
8. [8]
  Cho, K. H.; Park, S.; Seo, H.; Choi, S.; Lee, M. Y.; Ko, C.; Nam, K. T. Angew. Chem. Int. Ed. 2021, 60, 4673. doi: 10.1002/anie.202014551 doi: 10.1002/anie.202014551
9. [9]
  Liu, H.; Frei, H. ACS Catal. 2020, 10, 2138. doi: 10.1021/acscatal.9b03281 doi: 10.1021/acscatal.9b03281
10. [10]
  Zhang, B.; Daniel, Q.; Fan, L.; Liu, T.; Meng, Q.; Sun, L. iScience 2018, 4, 144. doi: 10.1016/j.isci.2018.05.018 doi: 10.1016/j.isci.2018.05.018
11. [11]
  Mo, C.; Dicko, C.; Shao, Z.; Chen, X. Acta Chim. Sin. 2009, 67, 2641. doi: 10.3321/j.issn:0567-7351.2009.22.019
12. [12]
  Chang, H. W.; Lu, Y. R.; Chen, J. L.; Chen, C. L.; Lee, J. F.; Chen, J. M.; Tsai, Y. C.; Yeh, P. H.; Chou, W. C.; Dong, C. L. Phys. Chem. Chem. Phys. 2016, 18, 18705. doi: 10.1039/c6cp01192f doi: 10.1039/c6cp01192f
13. [13]
  Lee, S.; Moysiadou, A.; Chu, Y. -C.; Chen, H. M.; Hu, X. Energy Environ. Sci. 2022, 15, 206. doi: 10.1039/d1ee02999a doi: 10.1039/d1ee02999a
14. [14]
  Zahran, Z. N.; Mohamed, E. A.; Naruta, Y. ACS Catal. 2016, 6, 4470. doi: 10.1021/acscatal.6b00413 doi: 10.1021/acscatal.6b00413
15. [15]
  Jin, K.; Chu, A.; Park, J.; Jeong, D.; Jerng, S. E.; Sim, U.; Jeong, H. Y.; Lee, C. W.; Park, Y. S.; Yang, K. D.; et al. Sci. Rep. 2015, 5, 10279. doi: 10.1038/srep10279 doi: 10.1038/srep10279
16. [16]
  Tan, T.; Yang, J.; Zhu, C.; Wang, G.; Chen, J.; Su, J. Acta Phys. -Chim. Sin. 2016, 32, 1929. doi: 10.3866/PKU.WHXB201605092
17. [17]
  Zhang, S.; Yao, Y.; Jiao, X.; Ma, M.; Huang, H.; Zhou, X.; Wang, L.; Bai, J.; Yu, Y. Adv. Mater. 2021, 33, e2103846. doi: 10.1002/adma.202103846 doi: 10.1002/adma.202103846
18. [18]
  Feng, L.; Wang, R.; Zhang, Y.; Ji, S.; Chuan, Y.; Zhang, W.; Liu, B.; Yuan, C.; Du, C. J. Mater. Sci. 2018, 54, 1520. doi: 10.1007/s10853-018-2885-0 doi: 10.1007/s10853-018-2885-0
19. [19]
  Sheng, C.; Yu, F.; Li, C.; Zhang, H.; Huang, J.; Wu, Y.; Armand, M.; Chen, Y. J. Phys. Chem. Lett. 2021, 12, 2064. doi: 10.1021/acs.jpclett.1c00118 doi: 10.1021/acs.jpclett.1c00118
20. [20]
  Morales-Guio, C. G.; Liardet, L.; Hu, X. J. Am. Chem. Soc. 2016, 138, 8946. doi: 10.1021/jacs.6b05196 doi: 10.1021/jacs.6b05196
21. [21]
  Rao, R. R.; Corby, S.; Bucci, A.; Garcia-Tecedor, M.; Mesa, C. A.; Rossmeisl, J.; Gimenez, S.; Lloret-Fillol, J.; Stephens, I. E. L.; Durrant, J. R. J. Am. Chem. Soc. 2022, 144, 7622. doi: 10.1021/jacs.1c08152 doi: 10.1021/jacs.1c08152
22. [22]
  Gorlin, M.; Ferreira de Araujo, J.; Schmies, H.; Bernsmeier, D.; Dresp, S.; Gliech, M.; Jusys, Z.; Chernev, P.; Kraehnert, R.; Dau, H.; et al. J. Am. Chem. Soc. 2017, 139, 2070. doi: 10.1021/jacs.6b12250 doi: 10.1021/jacs.6b12250
23. [23]
  Zaharieva, I.; González-Flores, D.; Asfari, B.; Pasquini, C.; Mohammadi, M. R.; Klingan, K.; Zizak, I.; Loos, S.; Chernev, P.; Dau, H. Energy Environ. Sci. 2016, 9, 2433. doi: 10.1039/c6ee01222a doi: 10.1039/c6ee01222a
24. [24]
  Takashima, T.; Hashimoto, K.; Nakamura, R. J. Am. Chem. Soc. 2012, 134, 1519. doi: 10.1021/ja206511w doi: 10.1021/ja206511w
25. [25]
  Francas, L.; Selim, S.; Corby, S.; Lee, D.; Mesa, C. A.; Pastor, E.; Choi, K. S.; Durrant, J. R. Chem. Sci. 2021, 12, 7442. doi: 10.1039/d0sc06429g doi: 10.1039/d0sc06429g
26. [26]
  Wu, L. L.; Huang, H. G.; Li, J. X.; Luo, J.; Lin, Z. H. Electrochim. Acta 2000, 45, 2877. doi: 10.1016/S0013-4686(00)00362-5 doi: 10.1016/S0013-4686(00)00362-5
27. [27]
  Wang, P.; Li, D.; Chi, H.; Zhao, Y.; Wang, J.; Li, D.; Pang, S.; Fu, P.; Shi, J.; Li, C. Angew. Chem. Int. Ed. 2021, 60, 6691. doi: 10.1002/anie.202014871 doi: 10.1002/anie.202014871
28. [28]
  Risch, M.; Ringleb, F.; Kohlhoff, M.; Bogdanoff, P.; Chernev, P.; Zaharieva, I.; Dau, H. Energy Environ. Sci. 2015, 8, 661. doi: 10.1039/c4ee03004d doi: 10.1039/c4ee03004d
29. [29]
  Francas, L.; Corby, S.; Selim, S.; Lee, D.; Mesa, C. A.; Godin, R.; Pastor, E.; Stephens, I. E. L.; Choi, K. S.; Durrant, J. R. Nat. Commun. 2019, 10, 5208. doi: 10.1038/s41467-019-13061-0 doi: 10.1038/s41467-019-13061-0
30. [30]
  Yin, H.; Li, D.; Wang, X.; Li, C. J. Phys. Chem. C 2021, 125, 8369. doi: 10.1021/acs.jpcc.1c02369 doi: 10.1021/acs.jpcc.1c02369
31. [31]
  Yin, H.; Shao, C.; Wang, H.; Zhang, H.; Li, D.; Zong, X.; Wang, X.; Li, C. J. Phys. Chem. Lett. 2021, 12, 3698. doi: 10.1021/acs.jpclett.1c00767 doi: 10.1021/acs.jpclett.1c00767
32. [32]
  Kok, B.; Forbush, B.; McGloin, M. Photochem. Photobiol. 1970, 11, 457. doi: 10.1111/j.1751-1097.1970.tb06017.x doi: 10.1111/j.1751-1097.1970.tb06017.x
33. [33]
  Zhang, Y.; Zhang, H.; Liu, A.; Chen, C.; Song, W.; Zhao, J. J. Am. Chem. Soc. 2018, 140, 3264. doi: 10.1021/jacs.7b10979 doi: 10.1021/jacs.7b10979
34. [34]
  Zhang, H.; Li, D.; Byun, W. J.; Wang, X.; Shin, T. J.; Jeong, H. Y.; Han, H.; Li, C.; Lee, J. S. Nat. Commun. 2020, 11, 4622. doi: 10.1038/s41467-020-18484-8 doi: 10.1038/s41467-020-18484-8
35. [35]
  Ma, Y.; Kafizas, A.; Pendlebury, S. R.; Le Formal, F.; Durrant, J. R. Adv. Funct. Mater. 2016, 26, 4951. doi: 10.1002/adfm.201600711 doi: 10.1002/adfm.201600711
36. [36]
  Zahran, Z. N.; Mohamed, E. A.; Ohta, T.; Naruta, Y. ChemCatChem 2016, 8, 532. doi: 10.1002/cctc.201501073 doi: 10.1002/cctc.201501073
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