Commercial indium-tin oxide glass: A catalyst electrode for efficient N2 reduction at ambient conditions

doi:10.1016/S1872-2067(20)63704-4

Abstract

Abstract:

The typical Haber technical process for industrial NH₃ production involves plenty of energy-consumption and large quantities of greenhouse gas emission. In contrast, electrochemical N₂ reduction proffers environment-friendly and energy-efficient avenues to synthesize NH₃ at mild conditions but demands efficient electrocatalysts for the N₂ reduction reaction (NRR). Herein we report for the first time that commercial indium-tin oxide glass (ITO/G) can be used as a catalyst electrode toward artificial N₂ fixation, as it demonstrates excellent selectivity at mild conditions. Such ITO/G delivers excellent NRR performance with a NH₃ yield of 1.06 × 10^-10 mol s^-1 cm^-2 and a faradaic efficiency of 6.17% at -0.40 V versus the reversible hydrogen electrode (RHE) in 0.5 M LiClO₄. Furthermore, the ITO/G also possesses good electrochemical stability and durability. Finally, the possible reaction mechanism for the NRR on the ITO catalysts was explored using first-principles calculations.

Key words: N₂ reduction reaction, NH₃, Indium-tin oxide, Electrocatalyst, Ambient conditions, Density functional theory

Ting Wang, Shaoxiong Li, Bingling He, Xiaojuan Zhu, Yonglan Luo, Qian Liu, Tingshuai Li, Siyu Lu, Chen Ye, Abdullah M. Asiri, Xuping Sun. Commercial indium-tin oxide glass: A catalyst electrode for efficient N₂ reduction at ambient conditions[J]. Chinese Journal of Catalysis, 2021, 42(6): 1024-1029.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63704-4

https://www.cjcatal.com/EN/Y2021/V42/I6/1024

Figures/Tables 6

Fig. 1. (a) XRD pattern of ITO/G; (b,c) SEM images of ITO/G; (d) SEM and corresponding EDX elemental mapping images of In, Sn, and O elements for ITO/G.

Fig. 2. (a) XPS survey spectrum for ITO/G; XPS spectra of ITO/G in the In 3d (b), Sn 3d (c), and O 1s (d) regions.

Fig. 3. (a) LSV curves of ITO/G in Ar- and N2-saturated 0.5 M LiClO4 with a scan rate of 2 mV s-1; (b) Chronoamperometry curves of ITO/G at various potentials for 2 h; (c) UV-Vis absorption spectra of the electrolytes colored with indophenol indicator; (d) Corresponding NH3 yields and FEs for ITO/G at all potentials.

Fig. 4. (a) UV-Vis absorption spectra of the electrolytes stained with indophenol indicator at -0.40 V under different electrochemical conditions using ITO/G; (b) NH3 yields and FEs of ITO/G at -0.40 V with alternating at the interval of 2 h cycles between Ar-saturated and N2-saturated electrolytes; (c) Cycling stability over ITO/G at -0.40 V; (d) NH3 yields and FEs at -0.40 V for 2 h over initial ITO/G and ITO/G subjected to 24 h operation.

Fig. 5. (a) XRD pattern and (b) SEM images of ITO/G after stability test.

Fig. 6. Free energy (in eV) diagrams and the local atomic structures of the reaction intermediates for the NRR on the ITO (400) surface through the alternating pathway. The blue, green, pink, red, and grey spheres represent the N, H, In, O, and Sn atoms, respectively.

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Commercial indium-tin oxide glass: A catalyst electrode for efficient N₂ reduction at ambient conditions

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