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Essential features of weak current for excellent enhancement of NOx reduction over monoatomic V-based catalyst

Daying ZhengGanjiang Innovation Academy, Chinese Academy of Sciences, No.1, Science Academy Road, Ganzhou, 341000, ChinaKaijie LiuGanjiang Innovation Academy, Chinese Academy of Sciences, No.1, Science Academy Road, Ganzhou, 341000, China. [email protected]Zeshu ZhangGanjiang Innovation Academy, Chinese Academy of Sciences, No.1, Science Academy Road, Ganzhou, 341000, ChinaQi FuGanjiang Innovation Academy, Chinese Academy of Sciences, No.1, Science Academy Road, Ganzhou, 341000, ChinaMengyao BianGanjiang Innovation Academy, Chinese Academy of Sciences, No.1, Science Academy Road, Ganzhou, 341000, ChinaXinyu HanGanjiang Innovation Academy, Chinese Academy of Sciences, No.1, Science Academy Road, Ganzhou, 341000, ChinaXin ShenGanjiang Innovation Academy, Chinese Academy of Sciences, No.1, Science Academy Road, Ganzhou, 341000, ChinaXiaohui ChenGanjiang Innovation Academy, Chinese Academy of Sciences, No.1, Science Academy Road, Ganzhou, 341000, ChinaHaijiao XieXiao WangState Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, ChinaXiangguang YangGanjiang Innovation Academy, Chinese Academy of Sciences, No.1, Science Academy Road, Ganzhou, 341000, ChinaYibo ZhangGanjiang Innovation Academy, Chinese Academy of Sciences, No.1, Science Academy Road, Ganzhou, 341000, China. [email protected]Shuyan SongState Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, China. [email protected]
2024en
ABI

Annotatsiya

Human society is facing increasingly serious problems of environmental pollution and energy shortage, and up to now, achieving high NH3-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 NOx into N2 at ultra-low temperature with V content of 1.36%, which shows the preeminent turnover frequencies (TOF145 °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. Achieving high NH3 selective catalytic reduction activity at ultra-low temperatures (below 150 °C) remains a challenge for V-based catalysts. Here the authors explore the electron scissors effect of current-assisted catalysis, which enables a monoatomic V-based catalyst to exhibit exceptional denitration performance at ultra-low temperatures.

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