Negatively Charged Single-Atom Pt Catalyst Shows Superior SO2 Tolerance in NOx Reduction by CO

Yongjun Ji; Shaomian Liu; Shaojia Song; Wenqing Xu; Liang Li; Yu Zhang; Wenxing Chen; Huifang Li; Jingang Jiang; Tingyu Zhu; Zhenxing Li; Ziyi Zhong; Dingsheng Wang; Guangwen Xu; Fabing Su

doi:10.1021/acscatal.2c04918

Negatively Charged Single-Atom Pt Catalyst Shows Superior SO₂ Tolerance in NO_x Reduction by CO

Yongjun Ji^*, Shaomian Liu, Shaojia Song, Wenqing Xu^*, Liang Li, Yu Zhang, Wenxing Chen, Huifang Li, Jingang Jiang^*, Tingyu Zhu, Zhenxing Li^*, Ziyi Zhong, Dingsheng Wang, Guangwen Xu, Fabing Su^*

^*Corresponding author for this work

Chemical Engineering

Research output: Contribution to journal › Article › peer-review

22 Scopus citations

Abstract

Pt-based catalysts are promising for the selective catalytic reduction of NOx by CO (CO-SCR), but some technical issues hinder their practical application, including the high Pt loading needed, high reduction temperature, and the low tolerance toward SO2. Here, we report a novel Pt catalyst for CO-SCR, which has negatively charged single-atom Pt embedded on CuO squares, and the latter is supported on CoAlO nanosheets. This Pt–CuO/CoAlO catalyst with an ultra-low Pt loading (0.02 wt %) exhibited 91% NO conversion and 80% N2 selectivity in 3% O2 at 200 °C. More importantly, it showed almost no activity loss in 200 ppm SO2 over a 15 h test. The theoretical calculations reveal that the negatively charged Pt has a stronger NO adsorption ability than the positively charged Pt, and Cu serves as the CO adsorption site. The much-weakened SO2 adsorption on Pt–CuO/CoAlO relative to the NO and CO adsorption effectively avoids the catalyst poisoning by SO2.

Original language	English
Pages (from-to)	224-236
Journal	ACS Catalysis
DOIs	https://doi.org/10.1021/acscatal.2c04918
State	Published - 14 Dec 2022

Keywords

Pt-based catalysts
hydrotalcite-like oxide
negatively charged Pt atoms
NOx reduction by CO
SO2 tolerance

Access to Document

10.1021/acscatal.2c04918

Cite this

@article{cd33330459d74fa8a0a5c9c0dbae6388,

title = "Negatively Charged Single-Atom Pt Catalyst Shows Superior SO2 Tolerance in NOx Reduction by CO",

abstract = "Pt-based catalysts are promising for the selective catalytic reduction of NOx by CO (CO-SCR), but some technical issues hinder their practical application, including the high Pt loading needed, high reduction temperature, and the low tolerance toward SO2. Here, we report a novel Pt catalyst for CO-SCR, which has negatively charged single-atom Pt embedded on CuO squares, and the latter is supported on CoAlO nanosheets. This Pt–CuO/CoAlO catalyst with an ultra-low Pt loading (0.02 wt %) exhibited 91% NO conversion and 80% N2 selectivity in 3% O2 at 200 °C. More importantly, it showed almost no activity loss in 200 ppm SO2 over a 15 h test. The theoretical calculations reveal that the negatively charged Pt has a stronger NO adsorption ability than the positively charged Pt, and Cu serves as the CO adsorption site. The much-weakened SO2 adsorption on Pt–CuO/CoAlO relative to the NO and CO adsorption effectively avoids the catalyst poisoning by SO2.",

keywords = "Pt-based catalysts, hydrotalcite-like oxide, negatively charged Pt atoms, NOx reduction by CO, SO2 tolerance",

author = "Yongjun Ji and Shaomian Liu and Shaojia Song and Wenqing Xu and Liang Li and Yu Zhang and Wenxing Chen and Huifang Li and Jingang Jiang and Tingyu Zhu and Zhenxing Li and Ziyi Zhong and Dingsheng Wang and Guangwen Xu and Fabing Su",

year = "2022",

month = dec,

day = "14",

doi = "10.1021/acscatal.2c04918",

language = "英语",

pages = "224--236",

journal = "ACS Catalysis",

issn = "2155-5435",

publisher = "American Chemical Society",

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TY - JOUR

T1 - Negatively Charged Single-Atom Pt Catalyst Shows Superior SO2 Tolerance in NOx Reduction by CO

AU - Ji, Yongjun

AU - Liu, Shaomian

AU - Song, Shaojia

AU - Xu, Wenqing

AU - Li, Liang

AU - Zhang, Yu

AU - Chen, Wenxing

AU - Li, Huifang

AU - Jiang, Jingang

AU - Zhu, Tingyu

AU - Li, Zhenxing

AU - Zhong, Ziyi

AU - Wang, Dingsheng

AU - Xu, Guangwen

AU - Su, Fabing

PY - 2022/12/14

Y1 - 2022/12/14

N2 - Pt-based catalysts are promising for the selective catalytic reduction of NOx by CO (CO-SCR), but some technical issues hinder their practical application, including the high Pt loading needed, high reduction temperature, and the low tolerance toward SO2. Here, we report a novel Pt catalyst for CO-SCR, which has negatively charged single-atom Pt embedded on CuO squares, and the latter is supported on CoAlO nanosheets. This Pt–CuO/CoAlO catalyst with an ultra-low Pt loading (0.02 wt %) exhibited 91% NO conversion and 80% N2 selectivity in 3% O2 at 200 °C. More importantly, it showed almost no activity loss in 200 ppm SO2 over a 15 h test. The theoretical calculations reveal that the negatively charged Pt has a stronger NO adsorption ability than the positively charged Pt, and Cu serves as the CO adsorption site. The much-weakened SO2 adsorption on Pt–CuO/CoAlO relative to the NO and CO adsorption effectively avoids the catalyst poisoning by SO2.

AB - Pt-based catalysts are promising for the selective catalytic reduction of NOx by CO (CO-SCR), but some technical issues hinder their practical application, including the high Pt loading needed, high reduction temperature, and the low tolerance toward SO2. Here, we report a novel Pt catalyst for CO-SCR, which has negatively charged single-atom Pt embedded on CuO squares, and the latter is supported on CoAlO nanosheets. This Pt–CuO/CoAlO catalyst with an ultra-low Pt loading (0.02 wt %) exhibited 91% NO conversion and 80% N2 selectivity in 3% O2 at 200 °C. More importantly, it showed almost no activity loss in 200 ppm SO2 over a 15 h test. The theoretical calculations reveal that the negatively charged Pt has a stronger NO adsorption ability than the positively charged Pt, and Cu serves as the CO adsorption site. The much-weakened SO2 adsorption on Pt–CuO/CoAlO relative to the NO and CO adsorption effectively avoids the catalyst poisoning by SO2.

KW - Pt-based catalysts

KW - hydrotalcite-like oxide

KW - negatively charged Pt atoms

KW - NOx reduction by CO

KW - SO2 tolerance

U2 - 10.1021/acscatal.2c04918

DO - 10.1021/acscatal.2c04918

M3 - 文章

SN - 2155-5435

SP - 224

EP - 236

JO - ACS Catalysis

JF - ACS Catalysis

ER -