Charge Transfer Analysis on the Direct Decomposition of Nitrous Oxide over Fe-BEA Zeolite: An Experimental and Density Functional Study
Charge Transfer Analysis on the Direct Decomposition of Nitrous Oxide over Fe-BEA Zeolite: An Experimental and Density Functional Study
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Fe-BEA 沸石上一氧化二氮直接分解的电荷转移分析：实验和密度泛函研究
DOI：
10.1021/jp200389r
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发表时间：
2011-06
影响因子：
3.7
通讯作者：
Lei Zhigang
中科院分区：
文献类型：
--
作者：
Liu Ning;Chen Biaohua;Li Yaping;Zhang Runduo;Liang Xin;Li Yingda;Lei Zhigang
采用密度泛函理论（DFT）计算的Mulliken布居分析方法，研究了N_2O在Fe ~（2+）沸石上直接分解的电荷转移过程，提出了一个包含O_2生成的三部分九步反应机理.沸石骨架作为电荷库在N2 O分子的分解过程中起着重要的作用，特别是在吸附和活化过程中（第一部分）。然而，在第二个N_2O分子的分解过程中（第二部分），活性中心Fe和α-O的作用变得至关重要。CT分析也证实了α-O的高反应活性。在这两部分中，N_2O作为电荷供体，其O端同时吸附在Fe-12O_3分子筛上，末端N和原子O作为主要电荷供体。在这两个部分的分解过程中，N2 O的中间N作为主要的电荷接受体接受了大量的电荷给体的电荷，从而导致了N2 O的分解。
Mulliken population analysis calculated by density functional theory (DFT) has been introduced to investigate the charge transfer (CT) during N2O direct decomposition over Fe-BEA zeolite, associated with a mechanism, involving an O2 formation, being divided into three parts and nine steps. The zeolite framework acting as a charge reservoir played an important role in the decomposition of the first N2O molecule, especially in the adsorption and activation processes (Part 1). However, during the decomposition of the second N2O molecule (Part 2), the roles of active center Fe and α-O became crucial. The high reactivity of α-O was also verified through CT analysis. In both of these two parts, N2O acted as a charge donor with its O end adsorbed on the Fe-BEA zeolite simultaneously with the terminal N and atomic O as the main charge donors. During the decomposition steps of these two parts, the middle N of N2O acting as the main charge acceptor accepted a large amount of charges from the charge donors, which co...
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影响因子：
3.7
作者：
H. Guesmi;D. Berthomieu;L. Kiwi-Minsker
通讯作者：
H. Guesmi;D. Berthomieu;L. Kiwi-Minsker
影响因子：
7.3
作者：
Keqiang Sun;Haian Xia;Ejm Emiel Hensen;V. Santen;Can Li
通讯作者：
Keqiang Sun;Haian Xia;Ejm Emiel Hensen;V. Santen;Can Li
影响因子：
5.5
作者：
G. Panov;A. S. Kharitonov;V. Sobolev
通讯作者：
G. Panov;A. S. Kharitonov;V. Sobolev
影响因子：
3.3
作者：
Martínez, A;Goursot, A;Delahay, G
通讯作者：
Delahay, G
DOI：
10.1016/s0144-2449(88)80219-7
发表时间：
1988-11-01
期刊：
ZEOLITES
影响因子：
--
作者：
HIGGINS, JB;LAPIERRE, RB;ROHRBAUGH, WJ
通讯作者：
ROHRBAUGH, WJ