金属体系中NO非均相还原的氧催化机制OA
Oxygen-catalyzed mechanism of heterogeneous NO reduction in metal-based systems
一氧化氮(NO)是主要的大气污染物之一,其高效脱除对环境保护与人类健康具有重要意义.尽管金属修饰被广泛应用于改进生物吸附剂对NO的还原性能,但氧元素在其中的协同催化作用仍缺乏深入的理论解释.本文基于密度泛函理论系统研究了金属Be、Mg、Ca、Sr及其氧协同体系对NO初始吸附与非均相还原的影响.结果表明金属修饰能够促进NO的协同吸附,而氧原子的催化作用表现在两方面:进一步促进NO的协同吸附与降低IM1至TS1的反应活化能.静电势等分析揭示氧原子具有"电子通道"效应,能够引导电子从碳质向金属或NO分子迁移,从而实现能量调控.此外,金属/氧体系对NO2的吸附具有与NO类似的表现.本文全面揭示了金属体系中NO非均相还原的氧催化机制,为高性能NOx吸附剂的设计提供了更加完善的理论依据.
Nitric oxide(NO)is a major air pollutant,and its efficient removal is essential for environmental pro-tection and human health.While metal modification has been widely used to improve the NO reduction perform-ance of bio-based adsorbents,the synergistic role of oxygen atoms remains unclear.In this study,density func-tional theory(DFT)was used to investigate the effects of Be,Mg,Ca,and Sr metals and their oxygen-coordi-nated systems on NO adsorption and heterogeneous reduction.The results show that metal loading enhances coop-erative NO adsorption,and oxygen atoms further improve this effect by promoting adsorption and lowering the ac-tivation energy from IM1 to TS1.Electrostatic potential analysis reveals that oxygen atoms act as"electron chan-nels,"facilitating electron transfer from the carbon surface to metal or NO molecules.Similar behavior was ob-served for NO2 adsorption.This work clarifies the catalytic role of oxygen in metal-modified systems and provides theoretical guidance for designing efficient NO2 adsorbents.
薛文彬;陈斌;陈珂鑫;范茂佳;曾玉洁;李金颖;徐诚信
上海理工大学,上海 200093上海理工大学,上海 200093上海理工大学,上海 200093上海理工大学,上海 200093上海理工大学,上海 200093上海理工大学,上海 200093上海理工大学,上海 200093
化学化工
非均相还原NO密度泛函理论
Heterogeneous reductionNODensity functional theory
《原子与分子物理学报》 2026 (6)
9-17,9
国家自然科学基金(52176016)上海市科技带头人(21XD1433400)
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