Influence of Solvent on Selective Catalytic Reduction of Nitrogen Oxides with Ammonia over Cu-CHA Zeolite

化学 催化作用 溶剂 选择性催化还原 反应性(心理学) 沸石 催化循环 分子 无机化学 光化学 反应机理 漫反射红外傅里叶变换 质子溶剂 红外光谱学 有机化学 替代医学 病理 医学 光催化
作者
Jamal Abdul Nasir,Jingcheng Guan,Thomas W. Keal,Alec W. Desmoutier,You Lü,Andrew M. Beale,C. Richard A. Catlow,Alexey A. Sokol
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:145 (1): 247-259 被引量:26
标识
DOI:10.1021/jacs.2c09823
摘要

The copper-exchanged zeolite Cu-CHA has received considerable attention in recent years, owing to its application in the selective catalytic reduction (SCR) of NOx species. Here, we study the NH3-SCR reaction mechanism on Cu-CHA using the hybrid quantum mechanical/molecular mechanical (QM/MM) technique and investigate the effects of solvent on the reactivity of active Cu species. To this end, a comparison is made between water- and ammonia-solvated and bare Cu species. The results show the promoting effect of solvent on the oxidation component of the NH3-SCR cycle since the formation of important nitrate species is found to be energetically more favorable on the solvated Cu sites than in the absence of solvent molecules. Conversely, both solvent molecules are predicted to inhibit the reduction component of the NH3-SCR cycle. Diffuse reflectance infrared fourier-transform spectroscopy (DRIFTS) experiments exploiting (concentration) modulation excitation spectroscopy (MES) and phase-sensitive detection (PSD) identified spectroscopic signatures of Cu-nitrate and Cu-nitrosamine (H2NNO), important species which had not been previously observed experimentally. This is further supported by the QM/MM-calculated harmonic vibrational analysis. Additional insights are provided into the reactivity of solvated active sites and the formation of key intermediates including their formation energies and vibrational spectroscopic signatures, allowing the development of a detailed understanding of the reaction mechanism. We demonstrate the role of solvated active sites and their influence on the energetics of important species that must be explicitly considered for an accurate understanding of NH3-SCR kinetics.
最长约 10秒,即可获得该文献文件

科研通智能强力驱动
Strongly Powered by AbleSci AI
更新
PDF的下载单位、IP信息已删除 (2025-6-4)

科研通是完全免费的文献互助平台,具备全网最快的应助速度,最高的求助完成率。 对每一个文献求助,科研通都将尽心尽力,给求助人一个满意的交代。
实时播报
刚刚
刚刚
量子星尘发布了新的文献求助10
1秒前
demo完成签到,获得积分10
1秒前
MinQi发布了新的文献求助10
2秒前
sciq完成签到,获得积分10
2秒前
3秒前
坚定盈发布了新的文献求助10
4秒前
多走一步发布了新的文献求助10
4秒前
宋晓静完成签到,获得积分10
4秒前
pan完成签到,获得积分10
5秒前
南城不南完成签到 ,获得积分10
6秒前
笨笨友桃发布了新的文献求助10
7秒前
elivsZhou完成签到,获得积分10
8秒前
9秒前
xcx发布了新的文献求助10
9秒前
天地一体完成签到,获得积分10
10秒前
坚定盈完成签到,获得积分10
11秒前
稀里糊涂完成签到 ,获得积分10
11秒前
多走一步完成签到,获得积分10
12秒前
w_完成签到,获得积分10
13秒前
爱听歌依波完成签到 ,获得积分10
13秒前
Leon发布了新的文献求助10
13秒前
gsgg完成签到 ,获得积分20
14秒前
笨笨友桃完成签到,获得积分10
14秒前
在水一方应助Huang采纳,获得10
14秒前
15秒前
16秒前
郭郭要努力ya完成签到 ,获得积分10
17秒前
18秒前
科研通AI2S应助Saint采纳,获得10
18秒前
annafan完成签到,获得积分10
18秒前
19秒前
科目三应助雷桑采纳,获得10
19秒前
少吃顿饭并不难完成签到 ,获得积分10
20秒前
珠珠发布了新的文献求助10
20秒前
20秒前
刘三哥完成签到 ,获得积分10
21秒前
隐形曼青应助leederay采纳,获得10
22秒前
上官若男应助to_ooooo采纳,获得10
22秒前
高分求助中
【提示信息,请勿应助】关于scihub 10000
Les Mantodea de Guyane: Insecta, Polyneoptera [The Mantids of French Guiana] 3000
徐淮辽南地区新元古代叠层石及生物地层 3000
The Mother of All Tableaux: Order, Equivalence, and Geometry in the Large-scale Structure of Optimality Theory 3000
Global Eyelash Assessment scale (GEA) 1000
Picture Books with Same-sex Parented Families: Unintentional Censorship 550
Research on Disturbance Rejection Control Algorithm for Aerial Operation Robots 500
热门求助领域 (近24小时)
化学 材料科学 医学 生物 工程类 有机化学 生物化学 物理 内科学 纳米技术 计算机科学 化学工程 复合材料 遗传学 基因 物理化学 催化作用 冶金 细胞生物学 免疫学
热门帖子
关注 科研通微信公众号,转发送积分 4038619
求助须知:如何正确求助?哪些是违规求助? 3576294
关于积分的说明 11375058
捐赠科研通 3306084
什么是DOI,文献DOI怎么找? 1819374
邀请新用户注册赠送积分活动 892698
科研通“疑难数据库(出版商)”最低求助积分说明 815066