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Advanced materials: high efficiency synthesis of ammonia at room temperature with mixed valence copper controlled TiO2 nano electrocatalyst

wallpapers News 2020-12-23

ammonia is widely used in daily life such as fertilizer food transportation. At present the industrial preparation of ammonia is mainly completed by Haber method which requires high temperature high pressure the harsh reaction conditions of noble metal ruthenium catalyst. This process will consume more than 3% of the total energy every year release a large amount of carbon dioxide gas. At the same time hydrogen is also required as the proton source. Therefore a green way to replace the industrialization of Habermas is expected. The process of electrocatalytic synthesis of ammonia (NRR) in aqueous solution at normal temperature pressure has zero carbon emission energy saving meets the needs of environmental protection. At present the main challenge of this method is how to obtain a high activity low cost electrocatalyst. So far TiO2 nanomaterials have been widely used in the electro catalytic synthesis of ammonia in which the presence of Ti3 greatly improves its NRR performance. We know that Ti3 is distributed in different positions in TiO2 there are different coordination numbers. However the structure-activity relationship between Ti3 structure NRR properties is still unclear.

recently Professor Zhang Yanning sun Xuping's team from the basic Frontier Research Institute of University of Electronic Science technology of China fully confirmed that the introduction of mixed valence copper can effectively improve the NRR performance of TiO2 nano electrocatalyst through experiments DFT calculations. In this paper we synthesized different concentrations of Cu doped TiO2 nanoparticles by hydrothermal method found different concentrations of Ti3 in the system by EPR technology. Synchrotron radiation confirmed that Cu ions were distributed in the TiO2 materials in valence states of 1 2 . NRR electrochemical test results showed that in 0.5 m LiClO4 solution the catalyst could obtain 21.31 μ g h – 1 mg – 1 cat. NH3 yield 21.99% Faraday efficiency at - 0.55 V (relative to reversible hydrogen electrode) which were better than many reported Ti based catalysts for electrochemical synthesis of ammonia. The density functional theory (DFT) reveals that the mixed valence state Cu doping can produce multiple oxygen vacancies different kinds of Ti3 defect electronic states on the surface of TiO2. When the Ti3 defect electronic state presents t 2G eg orbital splitting the activation adsorption of N2 molecules are effectively activated. The hydrogenation process of tinr3 tinr3 Ti4 was promoted. "Identifying the origin of Ti3 activity toward enhanced electrochemical N2 reduction over TiO2 nanoparticle modulated by mixed value copper" has been published in advanced materials


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