Cu-ZSM-5催化NOx直接分解反应机理的密度泛函理论研究
摘要
随着现代工业的发展,氮氧化物逐渐成为大气主要污染物之一,如何有效降解NOx受到了广泛关注。前人大量经验总结表明催化还原方法是消除贫燃发动机尾气中NOx的有效方法之一。但仅用实验方法很难深入研究其具体吸附、分解等机理。
本研究首先利用密度泛函(DFT)等理论方法对Cu+在ZSM-5分子筛内的位置进行了系统地研究,并在此基础上详细考察了NOx分子(NO,N2O,NO2)在Cu-ZSM-5中不同铜负载位上的吸附。研究采用包含完整直孔道、正弦孔道以及孔道交叉处的22T模型,确定了Cu+在ZSM-5内的三种可能位置：直孔道内(Ⅰ位)、孔道交叉处(Ⅱ位)和正弦孔道内(Ⅲ位)。结构数据表明,Cu+与2-3个骨架氧原子配位结合于ZSM-5分子筛内。在Cu-ZSM-5吸附NOx的过程中由Cu+和分子筛骨架向吸附质分子转移电子,使其带部分负电荷,从而不同程度地削弱了NO、分子中的N-N键和N-O键,使其键长增长。在所有铜位置中,NOx在铜Ⅱ位吸附对其活化作用最强,表明进一步的催化反应很有可能发生在Cu-ZSM-5的孔道交叉处。
在系统考察了NOx分子(NO,N2O,NO2)在Cu-ZSM-5中不同铜位上的吸附之后,深入的研究了NO、分子在孔道交叉处(II位)可能发生的生成及分解反应。分别详细计算了NO、N2O、N02的生成与分解等NOx分解反应的中间过程,并整理出NOx催化分解的具体步骤。首先是NO在催化活性中心Cu*上吸附并分解生成吸附态的0和一分子N20,之后N20有两种分解可能：1)进一步与S*O生成N2+O2；2)直接分解生成N2和吸附态的O。随着反应继续进行,吸附态的0与NO发生反应生成N02,之后NO2继续被催化分解,从而形成一个活性的反应循环。
Due to the development of modern industry, various nitrogen oxides have become one of the most crucial gases to our environment. Therefore how to clear up NOx has been an extremely concerned project for various countries.
In this work location of Cu+in Cu-ZSM-5 was studied using density functional theory method with a 22T model containing the straight and sinusoidal channels as well as the channel intersection of ZSM-5. It was found that Cu+is stabilized in ZSM-5 by forming two or three Cu-0 bonds with the zeolite framework oxygen atoms. Three stable sites were identified for Cu+in the ZSM-5 framework, i.e.; in the straight channel (type I site), in the sinusoidal channel (type III site) and in the intersection region of these two channels (type II site).
The adsorption of NOx molecules (NO, N2O, NO2) in different Cu+sites of Cu-ZSM-5 showed that the molecules acquired negative charges, indicating aπback donation of d electrons of Cu+toπ* antibonding orbital of the adsorbed molecules. The optimization of the adsorption complexes of NO and NO2 on type I and III Cu+ sites reached the same equilibrium geometry. Among the three Cu+sites, NOx molecules are most negatively charged in the complexes involving type II site, which indicates that the molecules are most significantly activated on this site, and therefore the catalytic reaction might occur in the intersection region of ZSM-5.
Based on this, the produce and decomposition of NOx molecules on the Cu+ center of the intersection region of Cu-ZSM-5 was investigated in details, and the catalytic reaction cycle of NOx was determined. It was found that the initial step of the reaction is that NO adsobed on the Cu+site and decomposed to adsorobed 0 (S*O) and N2O. The following decompsition of the adsorbed N2O has two possible ways:1) reacts with S*O to produce N2+O2; 2) decompses to N2 and adsorbed O, and then the adsorbed O could reaction with the new adsorbed NO to produce NO2. NO2 was then decomposed to complete the reaction cycle.
本研究首先利用密度泛函(DFT)等理论方法对Cu+在ZSM-5分子筛内的位置进行了系统地研究,并在此基础上详细考察了NOx分子(NO,N2O,NO2)在Cu-ZSM-5中不同铜负载位上的吸附。研究采用包含完整直孔道、正弦孔道以及孔道交叉处的22T模型,确定了Cu+在ZSM-5内的三种可能位置：直孔道内(Ⅰ位)、孔道交叉处(Ⅱ位)和正弦孔道内(Ⅲ位)。结构数据表明,Cu+与2-3个骨架氧原子配位结合于ZSM-5分子筛内。在Cu-ZSM-5吸附NOx的过程中由Cu+和分子筛骨架向吸附质分子转移电子,使其带部分负电荷,从而不同程度地削弱了NO、分子中的N-N键和N-O键,使其键长增长。在所有铜位置中,NOx在铜Ⅱ位吸附对其活化作用最强,表明进一步的催化反应很有可能发生在Cu-ZSM-5的孔道交叉处。
在系统考察了NOx分子(NO,N2O,NO2)在Cu-ZSM-5中不同铜位上的吸附之后,深入的研究了NO、分子在孔道交叉处(II位)可能发生的生成及分解反应。分别详细计算了NO、N2O、N02的生成与分解等NOx分解反应的中间过程,并整理出NOx催化分解的具体步骤。首先是NO在催化活性中心Cu*上吸附并分解生成吸附态的0和一分子N20,之后N20有两种分解可能：1)进一步与S*O生成N2+O2；2)直接分解生成N2和吸附态的O。随着反应继续进行,吸附态的0与NO发生反应生成N02,之后NO2继续被催化分解,从而形成一个活性的反应循环。
Due to the development of modern industry, various nitrogen oxides have become one of the most crucial gases to our environment. Therefore how to clear up NOx has been an extremely concerned project for various countries.
In this work location of Cu+in Cu-ZSM-5 was studied using density functional theory method with a 22T model containing the straight and sinusoidal channels as well as the channel intersection of ZSM-5. It was found that Cu+is stabilized in ZSM-5 by forming two or three Cu-0 bonds with the zeolite framework oxygen atoms. Three stable sites were identified for Cu+in the ZSM-5 framework, i.e.; in the straight channel (type I site), in the sinusoidal channel (type III site) and in the intersection region of these two channels (type II site).
The adsorption of NOx molecules (NO, N2O, NO2) in different Cu+sites of Cu-ZSM-5 showed that the molecules acquired negative charges, indicating aπback donation of d electrons of Cu+toπ* antibonding orbital of the adsorbed molecules. The optimization of the adsorption complexes of NO and NO2 on type I and III Cu+ sites reached the same equilibrium geometry. Among the three Cu+sites, NOx molecules are most negatively charged in the complexes involving type II site, which indicates that the molecules are most significantly activated on this site, and therefore the catalytic reaction might occur in the intersection region of ZSM-5.
Based on this, the produce and decomposition of NOx molecules on the Cu+ center of the intersection region of Cu-ZSM-5 was investigated in details, and the catalytic reaction cycle of NOx was determined. It was found that the initial step of the reaction is that NO adsobed on the Cu+site and decomposed to adsorobed 0 (S*O) and N2O. The following decompsition of the adsorbed N2O has two possible ways:1) reacts with S*O to produce N2+O2; 2) decompses to N2 and adsorbed O, and then the adsorbed O could reaction with the new adsorbed NO to produce NO2. NO2 was then decomposed to complete the reaction cycle.
引文
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