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弱电流对于在单原子钒基催化剂上出色增强NO还原的基本特征。

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

作者信息

Zheng Daying, Liu Kaijie, Zhang Zeshu, Fu Qi, Bian Mengyao, Han Xinyu, Shen Xin, Chen Xiaohui, Xie Haijiao, Wang Xiao, Yang Xiangguang, Zhang Yibo, Song Shuyan

机构信息

Ganjiang Innovation Academy, Chinese Academy of Sciences, No.1, Science Academy Road, Ganzhou, 341000, China.

University of Science and Technology of China, Hefei, 230026, China.

出版信息

Nat Commun. 2024 Aug 6;15(1):6688. doi: 10.1038/s41467-024-51034-0.

Abstract

Human society is facing increasingly serious problems of environmental pollution and energy shortage, and up to now, achieving high NH-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 into N at ultra-low temperature with V content of 1.36%, which shows the preeminent turnover frequencies (TOF = 1.97×10s). 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.

摘要

人类社会正面临日益严峻的环境污染和能源短缺问题,截至目前,对于钒含量低于2%的钒基催化剂而言,在超低温(<150 °C)下实现高NH-SCR活性仍然具有挑战性。在本研究中,采用弱电流辅助策略的单原子钒基催化剂在钒含量为1.36%时,能够在超低温下将NO完全转化为N,其表现出卓越的转化频率(TOF = 1.97×10s)。催化性能的提升主要归因于弱电流增强催化(ECWC)而非电场,这显著降低了催化系统超过90%的能耗。基于一系列弱电流辅助表征手段和密度泛函理论(DFT)计算对ECWC进行的进一步机理研究证实,迁移的电子主要集中在钒单原子周围,并增加了反键轨道的比例,这使得V-O化学键变弱(电子剪刀效应),从而加速了氧循环。本工作中新型的电流辅助催化有可能应用于其他环境和能源领域。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7c7f/11303551/d73a049b88f4/41467_2024_51034_Fig1_HTML.jpg

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