Hydroxyl Radical-Mediated Efficient Photoelectrocatalytic NO Oxidation with Simultaneous Nitrate Storage Using A Flow Photoanode Reactor

Angew Chem Int Ed Engl. 2023 Jul 10;62(28):e202305538. doi: 10.1002/anie.202305538. Epub 2023 Jun 5.

Abstract

The selective conversion of dilute NO pollutant into low-toxic product and simultaneous storage of metabolic nitrogen for crop plants remains a great challenge from the perspective of waste management and sustainable chemistry. This study demonstrates that this bottleneck can be well tackled by refining the reactive oxygen species (ROS) on Ni-modified NH2 -UiO-66(Zr) (Ni@NU) using nickel foam (NF) as a three-dimensional (3D) substrate through a flow photoanode reactor via the gas-phase photoelectrocatalysis. By rationally refining the ROS to ⋅OH, Ni@NU/NF can rapidly eliminate 82 % of NO without releasing remarkable NO2 under a low bias voltage (0.3 V) and visible light irradiation. The abundant mesoporous pores on Ni@NU/NF are conducive to the diffusion and storage of the formed nitrate, which enables the progressive conversion NO into nitrate with selectivity over 99 % for long-term use. Through calculation, 90 % of NO could be recovered as the nitrate species, indicating that this state-of-the-art strategy can capture, enrich and recycle the pollutant N source from the atmosphere. This study offers a new perspective of NO pollutant treatment and sustainable nitrogen exploitation, which may possess great potential to the development of highly efficient air purification systems for industrial and indoor NOx control.

Keywords: Air Pollution Control; Hydroxyl Radical Mediated Mechanism; Nitrate Storage; Photoelectrocatalytic NO Removal; Sustainable Nitrogen Exploitation.