Switching on photocatalytic NO oxidation and proton reduction of NH2-MIL-125(Ti) by convenient linker defect engineering

Abstract

Photocatalysis technology has been widely adopted to abate typical air pollutants. Nevertheless, developing photocatalysts aimed at improving photocatalytic efficiency is a challenge. Herein, the linker-defect NH2-MIL-125(Ti) photocatalyst was synthesized through a convenient one-step heating-stirring method (just adjusting multiple temperatures) to firstly realize efficient photocatalytic performances of NO removal and hydrogen evolution. The optimal sample (named 65-NMIL) with a linker-defect content of 32.08% exhibited a NO removal ratio of 65.49%, which was 37.57% higher than that of pristine NH2-MIL-125(Ti), and displayed better H2-production activity. Through ESR, it was confirmed that 65-NMIL can generate more •O2- and •OH under visible light, and the radical trapping experiment further proved that •O2- played a more important role in photocatalytic activity. Moreover, the photocatalytic NO oxidation process was also monitored by in situ DRIFTS, it was found that the defective samples could promote the oxidation of NO and intermediates to the final product (NO3-). On the basis of the above-mentioned photocatalytic experimental results and characterization, a possible mechanism or pathway was proposed and illustrated. This work can provide a new strategy for the subsequent defect engineering for photocatalytic MOFs materials to further solve environmental and energy crises.