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65. Spatial Distribution of Brønsted Acid Sites Determines the Mobility of Reactive Cu Ions in the Cu-SSZ-13 Catalyst during the Selective Catalytic Reduction of NOxwith NH3

Author

Fu, Yu, Ding, Wenqing, Lei, Huarong, Sun, Yu, Du, Jinpeng, Yu, Yunbo, Simon, Ulrich, Chen, Peirong, Shan, Yulong, He, Guangzhi, and He, Hong

Abstract

The formation of dimer-Cu species, which serve as the active sites of the low-temperature selective catalytic reduction of NOxwith NH3(NH3-SCR), relies on the mobility of CuIspecies in the channels of the Cu-SSZ-13 catalysts. Herein, the key role of framework Brønsted acid sites in the mobility of reactive Cu ions was elucidated via a combination of density functional theory calculations, in situimpedance spectroscopy, and in situdiffuse reflectance ultraviolet–visible spectroscopy. When the number of framework Al sites decreases, the Brønsted acid sites decrease, leading to a systematic increase in the diffusion barrier for [Cu(NH3)2]+and less formation of highly reactive dimer-Cu species, which inhibits the low-temperature NH3-SCR reactivity and vice versa. When the spatial distribution of Al sites is uneven, the [Cu(NH3)2]+complexes tend to migrate from an Al-poor cage to an Al-rich cage (e.g., cage with paired Al sites), which effectively accelerates the formation of dimer-Cu species and hence promotes the SCR reaction. These findings unveil the mechanism by which framework Brønsted acid sites influence the intercage diffusion and reactivity of [Cu(NH3)2]+complexes in Cu-SSZ-13 catalysts and provide new insights for the development of zeolite-based catalysts with excellent SCR activity by regulating the microscopic spatial distribution of framework Brønsted acid sites.

Published
2024
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70. Facile and Scalable Mechanochemical Synthesis of Defective MoS 2 with Ru Single Atoms Toward High‐Current‐Density Hydrogen Evolution

Author

Lang, Chengguang, primary, Jiang, Wenbin, additional, Yang, Cheng‐Jie, additional, Zhong, Hao, additional, Chen, Peirong, additional, Wu, Qilong, additional, Yan, Xuecheng, additional, Dong, Chung‐Li, additional, Lin, Yue, additional, Ouyang, Liuzhang, additional, Jia, Yi, additional, and Yao, Xiangdong, additional

Published
2023
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71. Supplementary Table from The Fibronectin–ILT3 Interaction Functions as a Stromal Checkpoint that Suppresses Myeloid Cells

Author

Paavola, Kevin J., primary, Roda, Julie M., primary, Lin, Vicky Y., primary, Chen, Peirong, primary, O'Hollaren, Kyle P., primary, Ventura, Richard, primary, Crawley, Suzanne C., primary, Li, Betty, primary, Chen, Hung-I H., primary, Malmersjö, Seth, primary, Sharkov, Nikolai A., primary, Horner, Geoffrey, primary, Guo, Wei, primary, Kutach, Alan K., primary, Mondal, Kalyani, primary, Zhang, Zhen, primary, Lichtman, Joshua S., primary, Song, Christina, primary, Rivera, Lee B., primary, Liu, Wenhui, primary, Luo, Jian, primary, Wang, Yan, primary, Solloway, Mark J., primary, Allan, Bernard B., primary, Kekatpure, Avantika, primary, Starck, Shelley R., primary, Haldankar, Raj, primary, Fan, Bin, primary, Chu, Chun, primary, Tang, Jie, primary, Molgora, Martina, primary, Colonna, Marco, primary, Kaplan, Daniel D., primary, and Hsu, Jer-Yuan, primary

Published
2023
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72. Supplementary Figure from The Fibronectin–ILT3 Interaction Functions as a Stromal Checkpoint that Suppresses Myeloid Cells

Author

Paavola, Kevin J., primary, Roda, Julie M., primary, Lin, Vicky Y., primary, Chen, Peirong, primary, O'Hollaren, Kyle P., primary, Ventura, Richard, primary, Crawley, Suzanne C., primary, Li, Betty, primary, Chen, Hung-I H., primary, Malmersjö, Seth, primary, Sharkov, Nikolai A., primary, Horner, Geoffrey, primary, Guo, Wei, primary, Kutach, Alan K., primary, Mondal, Kalyani, primary, Zhang, Zhen, primary, Lichtman, Joshua S., primary, Song, Christina, primary, Rivera, Lee B., primary, Liu, Wenhui, primary, Luo, Jian, primary, Wang, Yan, primary, Solloway, Mark J., primary, Allan, Bernard B., primary, Kekatpure, Avantika, primary, Starck, Shelley R., primary, Haldankar, Raj, primary, Fan, Bin, primary, Chu, Chun, primary, Tang, Jie, primary, Molgora, Martina, primary, Colonna, Marco, primary, Kaplan, Daniel D., primary, and Hsu, Jer-Yuan, primary

Published
2023
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73. Data from The Fibronectin–ILT3 Interaction Functions as a Stromal Checkpoint that Suppresses Myeloid Cells

Author

Paavola, Kevin J., primary, Roda, Julie M., primary, Lin, Vicky Y., primary, Chen, Peirong, primary, O'Hollaren, Kyle P., primary, Ventura, Richard, primary, Crawley, Suzanne C., primary, Li, Betty, primary, Chen, Hung-I H., primary, Malmersjö, Seth, primary, Sharkov, Nikolai A., primary, Horner, Geoffrey, primary, Guo, Wei, primary, Kutach, Alan K., primary, Mondal, Kalyani, primary, Zhang, Zhen, primary, Lichtman, Joshua S., primary, Song, Christina, primary, Rivera, Lee B., primary, Liu, Wenhui, primary, Luo, Jian, primary, Wang, Yan, primary, Solloway, Mark J., primary, Allan, Bernard B., primary, Kekatpure, Avantika, primary, Starck, Shelley R., primary, Haldankar, Raj, primary, Fan, Bin, primary, Chu, Chun, primary, Tang, Jie, primary, Molgora, Martina, primary, Colonna, Marco, primary, Kaplan, Daniel D., primary, and Hsu, Jer-Yuan, primary

Published
2023
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99. Copper Site Motion Promotes Catalytic NOxReduction under Zeolite Confinement

Author

Chen, Dongdong, Khetan, Abhishek, Lei, Huarong, Rizzotto, Valentina, Yang, Jia-Yue, Jiang, Jiuxing, Sun, Qiming, Peng, Baoxiang, Chen, Peirong, Palkovits, Regina, Ye, Daiqi, and Simon, Ulrich

Abstract

Ammonia-mediated selective catalytic reduction (NH3-SCR) is currently the key approach to abate nitrogen oxides (NOx) emitted from heavy-duty lean-burn vehicles. The state-of-art NH3-SCR catalysts, namely, copper ion-exchanged chabazite (Cu-CHA) zeolites, perform rather poorly at low temperatures (below 200 °C) and are thus incapable of eliminating effectively NOxemissions under cold-start conditions. Here, we demonstrate a significant promotion of low-temperature NOxreduction by reinforcing the dynamic motion of zeolite-confined Cu sites during NH3-SCR. Combining complex impedance-based in situspectroscopy (IS) and extended density-functional tight-binding molecular dynamics simulation, we revealed an environment- and temperature-dependent nature of the dynamic Cu motion within the zeolite lattice. Further coupling in situIS with infrared spectroscopy allows us to unravel the critical role of monovalent Cu in the overall Cu mobility at a molecular level. Based on these mechanistic understandings, we elicit a boost of NOxreduction below 200 °C by reinforcing the dynamic Cu motion in various Cu-zeolites (Cu-CHA, Cu-ZSM-5, Cu-Beta, etc.) via facile postsynthesis treatments, either in a reductive mixture at low temperatures (below 250 °C) or in a nonoxidative atmosphere at high temperatures (above 450 °C).

Published
2023
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