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
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