4.8 Article

Nano-Polycrystalline Cu Layer Interlaced with Ti3+-Self-Doped TiO2 Nanotube Arrays as an Electrocatalyst for Reduction of Nitrate to Ammonia

期刊

ACS APPLIED MATERIALS & INTERFACES
卷 15, 期 13, 页码 16680-16691

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c22399

关键词

nano-polycrystalline Cu; TiO2 nanotube arrays; Ti3+-self-doping; built-in electric field; electrochemical reduction of nitrate

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The integration of copper oxides-derived nano-polycrystalline Cu (NPC Cu) with Ti3+-self-doped TiO2 nanotube arrays (NTA) was used to fabricate NPC Cu/H-TiO2 NTA, which showed potential in degrading nitrate-containing wastewater and synthesizing recyclable ammonia at atmospheric pressure and room temperature. The unique nanostructure of interlaced Cu nano-polycrystals and TiO2 nanotubes accelerated electron transfer and improved adsorption characteristics. Under specific reaction conditions, the NPC Cu/H-TiO2 NTA achieved high NO3- conversion, Faradic efficiency, and ammonia production yield. This well-designed electrocatalyst possesses promising potential in ammonia production.
The electrochemical nitrate reduction reaction (NO3RR) is considered as a promising strategy to degrade nitrate-containing wastewater and synthesize recyclable ammonia at atmospheric pressure and room temperature. In this work, the copper oxides-derived nano-polycrystalline Cu (NPC Cu) was integrated with Ti3+-self-doped TiO2 nanotube arrays (NTA) to fabricate the NPC Cu/H-TiO2 NTA. Ti3+-self-doped TiO2 NTAs and the NPC Cu facilitate electron transfer and mass transportation and create abundant active sites. The unique nanostructure in which Cu nano-polycrystals interlace with the TiO2 nanotube accelerates the electron transfer from the substrate to surface NPC Cu. The density functional theory calculations confirm that the built-in electric field between Cu and TiO2 improves the adsorption characteristic of the NPC Cu/H-TiO2 NTA, thereby converting the endothermic NO3- adsorption step into an exothermic process. Therefore, the high NO3- conversion of 98.97%, the Faradic efficiency of 95.59%, and the ammonia production yield of 0.81 mg cm-2 h-1 are achieved at -0.45 V vs reversible hydrogen electrode in 10 mM NaNO3 (140 mg L-1)-0.1 M Na2SO4. This well-designed NPC Cu/H-TiO2 NTA as an effective electrocatalyst for the 8e- NO3RR possesses promising potential in the applications of ammonia production.

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