Rucheng Duan, Yu Fu, Zhuocan Li, Xin Wang, Meng Gao, Yunbo Yu, Guangzhi He, Hong He
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引用次数: 0
摘要
在低温下运行的催化剂对于各种非电力行业的烟气脱硝至关重要。目前的催化剂通常在 100 °C 以上的温度条件下表现出显著的氮氧化物与 NH3 选择性催化还原(NH3-SCR)活性。在此,我们首次在碳基催化剂表面观察到显著的室温 NH3-SCR 活性。室温下,表面 C-O-C 基团将 NO 氧化成 NO2,这是引发快速 SCR 反应的关键第一步。作为活性位点的 C-OH 基团通过 H 迁移过程直接参与了 SCR 的基本反应途径,从而将决定速率步骤的能障显著降低到 1 eV 以下,从而使快速 SCR 在室温下发生。本研究中报道的室温 SCR 及其新颖的反应机理势必会拓展氮氧化物减排的研究领域。
Unexpected Room-Temperature Selective Catalytic Reduction of NOx with NH3 over Metal-Free Carbon-Based Catalysts
Catalysts operating at low temperatures are imperative for the denitrification of flue gases from various non-electric industries. Current catalysts typically exhibit significant activity for the selective catalytic reduction of NOx with NH3 (NH3–SCR) at temperatures above 100 °C. Here, we observed for the first time remarkable room-temperature NH3–SCR activity on the surface of carbon-based catalysts. The oxidation of NO to NO2 by surface C–O–C groups at room temperature serves as a key initial step, triggering a fast SCR reaction. The C–OH groups, as active sites, directly participate in the elementary reaction pathways of the SCR through an H migration process, significantly reducing the energy barrier of the rate-determining step to below 1 eV, thereby enabling fast SCR to occur at room temperature. The room-temperature SCR and its novel reaction mechanism reported in this study would inevitably expand the research boundaries of NOx abatement.
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.