Essential features of weak current for excellent enhancement of NO(x) reduction over monoatomic V-based catalyst

单原子钒基催化剂上弱电流对NO(x)还原的显著增强作用的关键特征

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Abstract

Human society is facing increasingly serious problems of environmental pollution and energy shortage, and up to now, achieving high NH(3)-SCR activity at ultra-low temperatures (<150 °C) remains challenging for the V-based catalysts with V content below 2%. In this study, the monoatomic V-based catalyst under the weak current-assisted strategy can completely convert NO(x) into N(2) at ultra-low temperature with V content of 1.36%, which shows the preeminent turnover frequencies (TOF(145 °C) = 1.97×10(-3 )s(-1)). The improvement of catalytic performance is mainly attributed to the enhancement catalysis of weak current (ECWC) rather than electric field, which significantly reduce the energy consumption of the catalytic system by more than 90%. The further mechanism research for the ECWC based on a series of weak current-assisted characterization means and DFT calculations confirms that migrated electrons mainly concentrate around the V single atoms and increase the proportion of antibonding orbitals, which make the V-O chemical bond weaker (electron scissors effect) and thus accelerate oxygen circulation. The novel current-assisted catalysis in the present work can potentially apply to other environmental and energy fields.

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