Metal-organic frameworks loaded on phosphorus-doped tubular carbon nitride for enhanced photocatalytic hydrogen production and amine oxidation

Jianan Liu; Qi Li; Xudong Xiao; Fuxiang Li; Chen Zhao; Qi Sun; Panzhe Qiao; Jing Zhou; Jie Wu; Baiyan Li; Hongliang Bao; Baojiang Jiang

doi:10.1016/j.jcis.2021.01.031

Metal-organic frameworks loaded on phosphorus-doped tubular carbon nitride for enhanced photocatalytic hydrogen production and amine oxidation

J Colloid Interface Sci. 2021 May 15:590:1-11. doi: 10.1016/j.jcis.2021.01.031. Epub 2021 Jan 16.

Authors

Jianan Liu¹, Qi Li¹, Xudong Xiao¹, Fuxiang Li¹, Chen Zhao², Qi Sun², Panzhe Qiao³, Jing Zhou⁴, Jie Wu¹, Baiyan Li⁵, Hongliang Bao⁴, Baojiang Jiang⁶

Affiliations

¹ Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, School of Chemistry and Materials Science, Heilongjiang University, Harbin 150080, PR China.
² Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, PR China.
³ Shanghai Synchrotron Radiation Facility, Zhangjiang National Lab, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201204, PR China.
⁴ Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800, PR China.
⁵ School of Materials Science and Engineering, National Institute for Advanced Materials, TKL of Metal and Molecule-Based Material Chemistry, Nankai University, Tianjin 300350, PR China. Electronic address: libaiyan@nankai.edu.cn.
⁶ Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, School of Chemistry and Materials Science, Heilongjiang University, Harbin 150080, PR China. Electronic address: jbj@hlju.edu.cn.

PMID: 33517246
DOI: 10.1016/j.jcis.2021.01.031

Abstract

It is still a challenge to evolve visible light photocatalysts that possess both efficient oxidation and reduction capabilities. In this paper, phosphorus-doped tubular carbon nitride@UiO-66-NH₂ (p-TCN@U6-X) composites were prepared by in-situ load of UiO-66-NH₂ on the surface of p-TCN based on solvothermal method, which exhibit excellent photocatalytic oxidation and reduction ability. As a result, under visible light irradiation (λ > 420 nm), the photocatalytic H₂ production performance of p-TCN@U6-3 reached 2628 μmol g^-1h^-l, which was 8.19 and 5.36 times higher than that of p-TCN and UiO-66-NH₂, respectively. Meanwhile, p-TCN@U6-3 also exhibited well selectivity rate (99%) and conversion rate (98%) for oxidative coupling of amine compounds. The high photocatalytic activities can be assigned to the improved visible light adsorption resulted from the tubular structure of p-TCN and enhanced electrical conductivity because of the phosphorus doping in p-TCN. Furthermore, UiO-66-NH₂ plays the role of co-catalyst and active centers in the photocatalytic system to synergistically catalyze the reactions. Transient photocurrent spectra, steady-state photoluminescence (PL) and time-resolved photoluminescence (TRPL) further prove the more effective charge separation and transfer happened in the p-TCN@U6-X system compared with sole p-TCN and UiO-66-NH₂, respectively. This work provides an effective method for creating novel carbon nitride-based photocatalytic systems with efficient capability for photocatalytic oxidation and reduction.

Keywords: Benzylamine oxidative; Carbon nitride; Charge transfer; Hydrogen evolution reaction; MOF.