氮氧化物
催化作用
反键分子轨道
材料科学
选择性催化还原
单原子气体
电流(流体)
化学物理
化学
化学工程
电子
纳米技术
原子轨道
物理
物理化学
热力学
有机化学
燃烧
工程类
量子力学
作者
Daying Zheng,Kaijie Liu,Zeshu Zhang,Qi Fu,Mengyao Bian,Xinyu Han,Xin Shen,Xiaohui Chen,Haijiao Xie,Xiao Wang,Xiangguang Yang,Yibo Zhang,Shuyan Song
标识
DOI:10.1038/s41467-024-51034-0
摘要
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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