Enhanced dehydrogenation kinetics for ascorbic acid electrooxidation with ultra-low cell voltage and large current density

doi:10.1016/S1872-2067(23)64446-8

Abstract

Abstract:

Dehydroascorbic acid (DHA) production from ascorbic acid electrochemical oxidation (AAOR) can be used to upgrade biomass derivatives and hydrogen production with low energy consumption. Carbon materials are a promising class of nonmetal AAOR electrocatalysts; however, their performance does not meet the requirements for practical applications. In this study, an oxygen-containing group (OCG)-modified carbon electrocatalyst was prepared via oxygen plasma treatment. It could drive a current density of 100 mA cm^-2 at only 0.65 V_RHE and realize a Faradaic efficiency of over 90% for DHA production with long-term stability of 20 h. A proton exchange membrane-type electrolyzer integrating the anodic AAOR and the cathodic hydrogen evolution reaction (HER) was assessed. It only requires a cell voltage input of 0.98 V to deliver a current density of 1000 mA cm^-2, which is superior to most reported organic upgrading reactions. Moreover, it only needs 1.54 kWh to produce normal cubic H₂, which is one-third of that of traditional water electrolysis. Importantly, the contribution of each type of OCG was investigated by combining electrochemical measurements and theoretical calculations. It was revealed that the OCGs, especially the carboxyl groups (-COOH) of carbon materials, could enhance the dehydrogenation kinetics of the AAOR, thereby boosting the electrocatalytic activity. This study presents a low-energy and eco-friendly strategy for electrochemical biomass upgrading and hydrogen production, provides an in-depth understanding of the role of oxygen-containing functional groups in the AAOR, and guides the design of carbon-based electrocatalysts for AAOR.

Key words: Electrocatalysis, L-ascorbic acid electro-oxidation, Oxygen plasma, Hydrogen production, Metal-free electrocatalyst, Dehydrogenation kinetics

Bo Zhou, Jianqiao Shi, Yimin Jiang, Lei Xiao, Yuxuan Lu, Fan Dong, Chen Chen, Tehua Wang, Shuangyin Wang, Yuqin Zou. Enhanced dehydrogenation kinetics for ascorbic acid electrooxidation with ultra-low cell voltage and large current density[J]. Chinese Journal of Catalysis, 2023, 50: 372-380.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64446-8

https://www.cjcatal.com/EN/Y2023/V50/I7/372

Figures/Tables 3

Fig. 1. Physical and chemical characterization of electrocatalysts and electrocatalytic activity towards AAOR in 0.5 mol L?1 H2SO4 and 0.1 mol L?1 AA electrolyte. High-resolution XPS spectra of C 1s (a) and O 1s (b) for CP, Po-CP, and Po-CP-H2. (c) Content of various oxygenated groups at CP, Po-CP, and Po-CP-H2 surface. The content of different structures equals the content of total oxygen from wide XPS spectra times the ratio of the typical structure obtained from high-resolution XPS of O 1s spectra; (d) LSV curves for PO-CP with and without 0.1 mol L?1 AA in 0.5 mol L?1 H2SO4. (e) LSV curves for CP, Po-CP, and Po-CP-H2. (f) Tafel slopes of AAOR at CP, Po-CP, and Po-CP-H2 electrodes. (g) Conversion of AA and Faraday efficiencies of DHA at different potentials. (h) Long-term stability of electrocatalytic AA oxidation at 50 mA cm-2 in 0.5 mol L?1 H2SO4 with 0.1 mol L?1 AA; the inset is the SEM images of PO-CP before and after AAOR for 20 h. (i) Content of various oxygenated groups at the Po-CP surface before and after the 20-h electrolysis test. The content of different OCGs equals the content of total oxygen from wide XPS spectra times the ratio of typical OCGs obtained from the high-resolution XPS of O 1s spectra.

Fig. 2. Oxygen-enhanced dehydrogenation kinetics. (a) High-resolution XPS of C 1s of XC 72, PO-XC 72, PO-XC 72-H2. (b,c) LSV curves of AAOR at XC 72 with different treatments. (d) Most stable configurations of the intermediates on the carbon surface. (e) Corresponding free-energy diagram for the AAOR on different OCG-decorated surfaces.

Fig. 3. Evaluation of hydrogen production capacity. (a) Comparison of the cell voltage to obtain a specific current density of prior works about H2 production based on organic oxidation; inset presents the catalysts couple. (b) Polarization curves for AAOR/HER in the electrolyzer. (c) Measured H2 production compared with theoretically calculated H2 quantity at 0.6 to 1.0 V. (d) Comparative analysis of the calculated electricity consumption for hydrogen production via our system and conventional water electrolysis. (e) Durability measurement of PO-CP || Pt/C couple for DHA and hydrogen production at 30 °C.

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