Revealing the Formation and Reactivity of Cage-Confined Cu Pairs in Catalytic NOx Reduction over Cu-SSZ-13 Zeolites by In Situ UV-Vis Spectroscopy and Time-Dependent DFT Calculation

Huarong Lei; Dongdong Chen; Abhishek Khetan

首页> 外文期刊>Environmental Science & Technology: ES&T >Revealing the Formation and Reactivity of Cage-Confined Cu Pairs in Catalytic NOx Reduction over Cu-SSZ-13 Zeolites by In Situ UV-Vis Spectroscopy and Time-Dependent DFT Calculation

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Revealing the Formation and Reactivity of Cage-Confined Cu Pairs in Catalytic NOx Reduction over Cu-SSZ-13 Zeolites by In Situ UV-Vis Spectroscopy and Time-Dependent DFT Calculation

机译：Revealing the Formation and Reactivity of Cage-Confined Cu Pairs in Catalytic NOx Reduction over Cu-SSZ-13 Zeolites by In Situ UV-Vis Spectroscopy and Time-Dependent DFT Calculation

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摘要

The low-temperature mechanism of chabazite-type small-pore Cu-SSZ-13 zeolite, a state-of-the-art catalyst for ammonia-assisted selective reduction (NH3-SCR) of toxic NO1 pollutants from heavy-duty vehicles, remains a debate and needs to be clarified for further improvement of NH3-SCR performance. In this study, we established experimental protocols to follow the dynamic redox cycling (i.e., Cu11 Cu1) of Cu sites in Cu-SSZ-13 during low-temperature NH3-SCR catalysis by in situ ultraviolet-visible spectroscopy and in situ infrared spectroscopy. Further integrating the in situ spectroscopic observations with time-dependent density functional theory calculations allows us to identify two cage-confined transient states, namely, the 02-bridged Cu dimers (i.e.,-peroxodiamino dicopper) and the proximately paired, chemically nonbonded Cu'(NH3)2 sites, and to confirm the Cu'(NH3)2 pair as a precursor to the 02-bridged Cu dimer. Comparative transient experiments reveal a particularly high reactivity of the Cu'(NH3)2 pairs for NOtO-N2 reduction at low temperatures. Our study demonstrates direct experimental evidence for the transient formation and high reactivity of proximately paired Cu sites under zeolite confinement and provides new insights into the monomeric-to-dimeric Cu transformation for completing the Cu redox cycle in low-temperature NH3-SCR catalysis over Cu-SSZ-13.

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来源
《Environmental Science & Technology: ES&T》 |2023年第33期|12465-12475|共11页
作者
Huarong Lei; Dongdong Chen; Abhishek Khetan;
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作者单位

Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, National Engineering Laboratory for VOCs Pollution Control Technology and Equipment, School of Environment and Energy, South China University of Technology, 510006 Guangzhou, China;

Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, National Engineering Laboratory for VOCs Pollution Control Technology and Equipment, School of Environment and Energy, South China University of Technology, 510006 Guangzhou, China;

Fuel Science Center, RWTH Aachen University, 52074 Aachen, Germany;

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收录信息美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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正文语种英语
中图分类环境科学、安全科学;
关键词
Cu redox; in situ DRUVS; in situ DRIFTS; TD-DFT calculation; cage-confined Cu pair;

Revealing the Formation and Reactivity of Cage-Confined Cu Pairs in Catalytic NOx Reduction over Cu-SSZ-13 Zeolites by In Situ UV-Vis Spectroscopy and Time-Dependent DFT Calculation

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