Enhanced artificial nitrogen fixation efficiency induced by construction of ternary TiO2/MIL-88A(Fe)/g-C3N4 Z-scheme heterojunction

Qun Ding; Xuejun Zou; Jun Ke; Yuying Dong; Yubo Cui; Hongchao Ma

doi:10.1016/j.jcis.2023.06.095

Enhanced artificial nitrogen fixation efficiency induced by construction of ternary TiO₂/MIL-88A(Fe)/g-C₃N₄ Z-scheme heterojunction

J Colloid Interface Sci. 2023 Nov:649:148-158. doi: 10.1016/j.jcis.2023.06.095. Epub 2023 Jun 17.

Authors

Qun Ding¹, Xuejun Zou², Jun Ke³, Yuying Dong⁴, Yubo Cui⁴, Hongchao Ma⁵

Affiliations

¹ Department of Environmental Science and Technology, Dalian Minzu University, Dalian 116600, China; School of Light Industry & Chemical Engineering, Dalian Polytechnic University, No. 1 Qinggongyuan, Ganjingzi District, Dalian 116034, China.
² Department of Environmental Science and Technology, Dalian Minzu University, Dalian 116600, China. Electronic address: zouxuejun@dlnu.edu.cn.
³ School of Chemistry and Environmental Engineering, Wuhan Institute of Technology, Wuhan 430205, China. Electronic address: jke@wit.edu.cn.
⁴ Department of Environmental Science and Technology, Dalian Minzu University, Dalian 116600, China.
⁵ School of Light Industry & Chemical Engineering, Dalian Polytechnic University, No. 1 Qinggongyuan, Ganjingzi District, Dalian 116034, China.

PMID: 37348334
DOI: 10.1016/j.jcis.2023.06.095

Abstract

Herein, a ternary TiO₂/MIL-88A(Fe)/g-C₃N₄ heterojunction is successfully constructed through a facile hydrothermal strategy for enhancing solar energy harvesting and efficiency of catalytic nitrogen reduction induced by enlarged light absorption range, increasing interfacial charge transfer ability and desirable stability. Under the simulated sunlight irradiation, the N₂ fixation experiment shows that the yield of NH₃ reaches 1084.31 μmol/(g·h) over the TiO₂/MIL-88A(Fe)/g-C₃N₄ photocatalyst, and the yield is significantly enhanced, which is 33.68 and 13.94 times that is higher than the pure TiO₂ and g-C₃N₄, respectively. In a mean time, the excellent performance of the photocatalytic N₂ fixation over the ternary TiO₂/MIL-88A(Fe)/g-C₃N₄ is verified based on density function theory calculation and the decisive step over the composite is investigated by calculating Gibbs free energies of nitrogen reduction paths. The performance enhancement mechanism of TiO₂/MIL-88A(Fe)/g-C₃N₄ is speculated, which indicates that the hybridized three-component system presents a desirable Z-scheme band alignment, resulting in the improvement of separation and transfer efficiency of photoinduced charge carriers. The article shows a new and high-efficiency TiO₂/MIL-88A(Fe)/g-C₃N₄ photocatalysis for excellent nitrogen reduction ability.

Keywords: Density function theory; Metal organic Framework; N(2) reduction reaction; Photocatalysis; Z-scheme heterojunction.