Facile Synthesis of Cu-Exchanged Zeolite Catalysts with Only Cu2+-2Z Species: Enhancing Hydrothermal Stability and Sulfur Resistance for NH3–SCR

IF 11.3 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL 环境科学与技术 Pub Date : 2024-12-19 DOI:10.1021/acs.est.4c09820
Jinhan Lin, Xueyang Hu, Xuechao Tan, Yan Zhang, Chunxi Lin, Wenpo Shan, Hong He
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Abstract

For Cu-exchanged zeolite catalysts, Cu2+ ions existing as Cu2+-2Z and [Cu(OH)]+-Z (where Z represents a framework negative charge) are considered the active sites for the selective catalytic reduction of NOx with NH3 (NH3–SCR). Cu2+-2Z is more hydrothermally stable and sulfur poisoning-resistant than [Cu(OH)]+-Z. In this work, Cu-CHA and Cu-LTA catalysts containing only Cu2+-2Z species were successfully synthesized by a novel impregnation (NIM) method, exhibiting remarkably enhanced hydrothermal stability and sulfur resistance compared with any reported Cu-exchanged zeolite catalysts. It was also found that the [Cu(OH)]+-Z sites can convert to Cu2+-2Z by treating at high temperature (850 °C) due to the self-reduction of Cu2+ to highly mobile Cu+. The use of the NIM method not only significantly simplifies the preparation of the catalysts but also can precisely control the Cu loading, which is very important for the control of Cu species. Many other zeolite catalysts can be prepared by this method.

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仅含有 Cu2+-2Z 物种的铜变化沸石催化剂的简易合成:增强 NH3-SCR 的水热稳定性和抗硫性
对于铜交换沸石催化剂,Cu2+ 离子以 Cu2+-2Z 和 [Cu(OH)]+-Z(其中 Z 代表框架负电荷)的形式存在,被认为是氮氧化物与 NH3 选择性催化还原(NH3-SCR)的活性位点。与[Cu(OH)]+-Z 相比,Cu2+-2Z 具有更高的热稳定性和抗硫中毒性。本研究采用新型浸渍 (NIM) 方法成功合成了仅含 Cu2+-2Z 物种的 Cu-CHA 和 Cu-LTA 催化剂,与已报道的铜交换沸石催化剂相比,其水热稳定性和抗硫性显著增强。研究还发现,[Cu(OH)]+-Z 位点在高温(850 °C)处理下可转化为 Cu2+-2Z,这是由于 Cu2+ 自还原为高流动性的 Cu+。使用 NIM 方法不仅大大简化了催化剂的制备,而且可以精确控制 Cu 的负载量,这对于控制 Cu 种类非常重要。用这种方法还可以制备许多其他沸石催化剂。
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来源期刊
环境科学与技术
环境科学与技术 环境科学-工程:环境
CiteScore
17.50
自引率
9.60%
发文量
12359
审稿时长
2.8 months
期刊介绍: Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences. Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.
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