Abstract
The low efficiency of photocatalytic nitrogen fixation to ammonia is determined by the low quantum efficiency photocatalyst and the configuration of the reactor.Therefore, a new method was adopted to introduce a gas-liquid-solid optofluidic microreactor with gas-liquid two-chambers into the photocatalytic nitrogen fixation reaction, and a novel and efficient TiO2−x-Ag@HKUST-1/ carbon paper composite membrane was successfully synthesized. The porous structure of HKUST-1/carbon paper can well adsorb N2, and the uniformly dispersed Ag and Ti3+ in the TiO2−x are bridged by O vacancies to form the Ti3+-Ov-Ag active center. These together improve the activity of photocatalytic nitrogen fixation to ammonia. The experimental results show that the TiO2−x-Ag@HKUST-1/carbon paper composite membrane can continuously reduce N2 to ammonia under visible light, and the yield can reach 10.62 mg.h-1.gcat-1and the corresponding apparent quantum yield (AQY) under 450 nm illumination reaches 2.08%, which is much higher than that of commercial TiO2(P25), HKUST-1, and also higher than most of the reported TiO2-based photocatalysts. This shows the superiority of the gas-liquid two-chambers gas-liquid-solid optofluidic microreactor in photocatalytic nitrogen fixation.This work can also be seen as a step towards the development of high-efficiency continuous photocatalytic nitrogen fixation to ammonia technology.
Published Version
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