Uniform octahedral ZrO2@C from carbonized UiO-66 for electrocatalytic nitrogen reduction. (December 2021)

• Record Type: Journal Article
• Authors: Dong, Changchang; Wei, Feng; Li, Jiadong; Lu, Qiao; Han, Xiaojun
• Is Part Of: Materials today energy. Volume 22(2021)
• Publication Date: 2021-12
• Subjects: Two-step annealing method -- Uniform octahedral structure -- Electrocatalytic ammonia synthesis -- MOF-derived materials; Energy development -- Periodicals; Energy industries -- Periodicals; Power resources -- Periodicals; Energy policy -- Periodicals; Energy development; Energy industries; Energy policy; Power resources; Electronic journals; Periodicals; 621.042
• DOI: 10.1016/j.mtener.2021.100884
• Languages: English
• ISSNs: 2468-6069

Abstract

Abstract: The electrochemical ammonia synthesis under ambient conditions is a promising process instead of the energy-intensity Haber-Bosch process with the release of huge greenhouse gases. But it still faces sluggish catalytic kinetics owing to difficulty of N2 adsorption and N≡N bond cleavage. Herein, the uniform ZrO2 @C with octahedral structure is synthesized via two-step annealing treatment of UiO-66. The formation of ZrO2 originates from Zr and O elements in UiO-66, and the grain size is confined by the produced carbon matrix from the carbonization of the organic ligand, resulting in more exposure of the active sites. ZrO2 @C obtained at 650 °C presents excellent electrocatalytic nitrogen reduction performance with a NH3 yield rate of 6.72 μg h −1 mgcat. −1 and a Faradaic efficiency of 2.68% at −0.6 V versus reversible hydrogen electrode (RHE). This work provides a strategy to design metal oxide@C from metal-organic frameworks for nitrogen fixation. Graphical abstract: Image 1 Highlights: A uniform ZrO2 @C with octahedral structure was synthesized via two-step annealing treatment of UiO-66. The effect of annealing temperature on electrocatalytic nitrogen reduction performance of ZrO2 @C was investigated. The ZrO2 @C-650 prepared in 650 °C exhibits the excellent electrocatalytic ammonia synthesis performance.