Breaking the activity-selectivity trade-off in nitrogen-containing volatile organic compounds abatement via NiCu synergistic perovskite catalysts.

Efficient removal of nitrogen-containing volatile organic compounds (NVOCs) remains challenging due to the trade-off between high catalytic activity and low N2 selectivity. In this study, a series of La2CuxNi1-xO4 perovskite catalysts were developed for the catalytic oxidation of acrylonitrile (AN) and N, N-dimethylformamide (DMF). Among them, La2Cu0.5Ni0.5O4 exhibited the optimal performance, achieving superior low-temperature activity, near-complete CO2 selectivity, high N2 selectivity, and excellent stability while suppressing NOx, N2O, and NH3 formation, with a T90 of 156 °C for AN oxidation. The enhanced NVOC removal and improved N2 selectivity are attributed to the cooperative Cu-O-Ni structure. Decreased Ni3+ fraction suppresses excessive oxidation of nitrogen-containing intermediates, whereas dominant Ni2+ sites serve as mild adsorption and electronic activation centers for AN, promoting CN and/or CN bond polarization through interfacial electron transfer. Meanwhile, Cu sites facilitate O2 activation and intermediate oxidation through a dynamic Cu2+/Cu+ redox cycle, while defect-related oxygen species help maintain a moderate oxidative environment. This synergistic mechanism promotes efficient NVOCs oxidation and directs nitrogen-containing intermediates toward N2 formation rather than over-oxidation to NOx. This work provides guidance for designing Cu-Ni-based catalysts for efficient and selective NVOCs abatement.