Deep insights into the promotion role of Sm doping in the sulfur resistance of Fe2O3 catalyst for NH3-SCR: A combined experimental and DFT study

催化作用 硫酸化 化学 X射线光电子能谱 吸附 选择性催化还原 氮氧化物 硫黄 无机化学 化学工程 物理化学 有机化学 生物化学 燃烧 工程类
作者
Pengfei Sun,Shuangling Jin,Jitong Wang,Jiahui Wu,Lilin Cai,Yang Zhou,Xiaorui Wang,Rui Zhang,Licheng Ling,Minglin Jin
出处
期刊:Journal of Physics and Chemistry of Solids [Elsevier BV]
卷期号:184: 111666-111666 被引量:3
标识
DOI:10.1016/j.jpcs.2023.111666
摘要

To investigate the inherent role of Sm doping in metal sulfation over the surface of Fe2O3 catalyst and reveal the reason for the SO2 tolerance enhancement of Sm/Fe2O3 catalyst at low temperatures (<320 °C), sulfated Fe2O3 and Sm/Fe2O3 catalysts were prepared by pretreating fresh catalysts in SO2+O2 atmosphere. Selective catalytic reduction (SCR) of NOx by NH3 activities and physicochemical characteristics of fresh and sulfated catalysts were studied, and the reaction mechanisms on sulfated catalysts analyzed. The minor shift of Fe signal to high value and larger shift of S signal to low value of sulfated Sm/Fe2O3 compared with sulfated Fe2O3 was observed with X-ray photoelectron spectroscopy (XPS), indicating that Sm modification could weaken the sulfation of active Fe sites. Consistent with the XPS results, density functional theory calculations showed that SO2 is more easily adsorbed on the Sm/Fe2O3 catalyst with the adsorption sites located at Sm atom and its neighboring Fe atoms. In-situ DRIFTS results showed that the SCR reaction over the sulfated Fe2O3 catalyst followed both L-H (the adsorbed NH3 species react with adsorbed nitrate species) and E-R (the adsorbed NH3 species react with gaseous NO) mechanisms at 250 °C, with the L-H route much faster, whereas only the L-H pathway occurred over sulfated Sm/Fe2O3 catalyst because of too strong affinity of NH3 on the sulfated sites to inhibit NH3 activation – this was also the reason for its enhanced Lewis and Brønsted acidity. More reactive nitrate species were formed on the sulfated Sm/Fe2O3 catalyst due to the existence of more un-sulfated Fe sites, making the Sm/Fe2O3 catalyst resistant to SO2 poisoning at relatively low temperatures.
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
量子星尘发布了新的文献求助10
2秒前
风信子完成签到,获得积分10
2秒前
小熊完成签到 ,获得积分10
4秒前
8秒前
shu完成签到,获得积分10
8秒前
8秒前
勤奋的毛豆完成签到,获得积分10
11秒前
行者无疆完成签到,获得积分10
11秒前
12秒前
Jackylee完成签到,获得积分10
12秒前
careyzhou发布了新的文献求助10
13秒前
舒心之云完成签到,获得积分10
15秒前
Desire发布了新的文献求助10
15秒前
独自受罪完成签到 ,获得积分10
16秒前
甘蓝型油菜完成签到,获得积分10
17秒前
Distance发布了新的文献求助10
18秒前
大橙子发布了新的文献求助10
19秒前
毛哥看文献完成签到 ,获得积分10
19秒前
Desire完成签到,获得积分10
21秒前
AiQi完成签到 ,获得积分10
22秒前
月月鸟完成签到 ,获得积分10
23秒前
陈永伟完成签到,获得积分10
25秒前
传奇3应助qq采纳,获得10
25秒前
feihua1完成签到 ,获得积分10
26秒前
大轩完成签到 ,获得积分10
27秒前
miemie66完成签到,获得积分10
28秒前
29秒前
Sun1c7完成签到,获得积分10
29秒前
大仁哥完成签到,获得积分10
29秒前
qqy完成签到,获得积分10
30秒前
失眠的香菇完成签到 ,获得积分10
32秒前
机灵的笼包完成签到,获得积分10
32秒前
兔子发布了新的文献求助10
33秒前
ohwhale完成签到 ,获得积分10
34秒前
chaotianjiao完成签到 ,获得积分10
35秒前
阳光的耳机完成签到,获得积分10
36秒前
K珑完成签到,获得积分10
36秒前
Solar energy完成签到,获得积分10
38秒前
鲤鱼青雪发布了新的文献求助10
39秒前
云淡风轻一宝完成签到,获得积分10
40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
Handbook of Industrial Diamonds.Vol2 1100
Global Eyelash Assessment scale (GEA) 1000
Picture Books with Same-sex Parented Families: Unintentional Censorship 550
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 4038201
求助须知:如何正确求助?哪些是违规求助? 3575940
关于积分的说明 11373987
捐赠科研通 3305747
什么是DOI,文献DOI怎么找? 1819274
邀请新用户注册赠送积分活动 892662
科研通“疑难数据库(出版商)”最低求助积分说明 815022