氨的催化氧化:在 Ag-CuOx/Al2O3 催化剂上以低银负载增大银纳米颗粒并提高活性和选择性的预占位策略

IF 20.2 1区 化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2023-12-22 DOI:10.1016/j.apcatb.2023.123655
Zhao Li , Fei Wang , Fudong Liu , Shaohua Xie , Changbin Zhang , Ping Ning , Kai Li , Hong He , Xiao Cheng Zeng
{"title":"氨的催化氧化:在 Ag-CuOx/Al2O3 催化剂上以低银负载增大银纳米颗粒并提高活性和选择性的预占位策略","authors":"Zhao Li ,&nbsp;Fei Wang ,&nbsp;Fudong Liu ,&nbsp;Shaohua Xie ,&nbsp;Changbin Zhang ,&nbsp;Ping Ning ,&nbsp;Kai Li ,&nbsp;Hong He ,&nbsp;Xiao Cheng Zeng","doi":"10.1016/j.apcatb.2023.123655","DOIUrl":null,"url":null,"abstract":"<div><p><span>The Ag nanoparticles (Ag</span><sub>NPs</sub>) in Ag/Al<sub>2</sub>O<sub>3</sub><span> catalysts play a crucial role in the selective catalytic oxidation of NH</span><sub>3</sub> (NH<sub>3</sub>-SCO). To enhance NH<sub>3</sub>-SCO activity, Cu, which has stronger anchoring ability than Ag, is introduced onto Al<sub>2</sub>O<sub>3</sub>, reducing available anchoring sites for Ag. As Ag cannot displace anchored Cu species, Ag species agglomerate into larger Ag<sub>NPs</sub> even with low Ag loading. Consequently, these enlarged Ag<sub>NPs</sub> become more active centers for NH<sub>3</sub>-SCO. The optimal Ag:Cu molar ratio is confirmed as 2:3. This 'pre-occupied-anchoring-site’ strategy decreases Ag loading to 1/5 of the original, reducing catalyst costs while maintaining activity. <em>In situ</em> diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) studies reveal that NH<sub>3</sub>-SCO on 2Ag1.8Cu/Al (weight ratio) catalyst follows the hydrazine mechanism below 200 °C, coexisting with the imide mechanism from 200–250 °C, and solely the imide mechanism beyond 250 °C. This strategy is applicable to various transition metals, including Mn, Co, Ni, and Fe, promoting cost-effective Ag<sub>NPs</sub> formation.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"344 ","pages":"Article 123655"},"PeriodicalIF":20.2000,"publicationDate":"2023-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Catalytic oxidation of ammonia: A pre-occupied-anchoring-site strategy for enlarging Ag nanoparticles at low Ag loading and achieving enhanced activity and selectivity on Ag-CuOx/Al2O3 catalyst\",\"authors\":\"Zhao Li ,&nbsp;Fei Wang ,&nbsp;Fudong Liu ,&nbsp;Shaohua Xie ,&nbsp;Changbin Zhang ,&nbsp;Ping Ning ,&nbsp;Kai Li ,&nbsp;Hong He ,&nbsp;Xiao Cheng Zeng\",\"doi\":\"10.1016/j.apcatb.2023.123655\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p><span>The Ag nanoparticles (Ag</span><sub>NPs</sub>) in Ag/Al<sub>2</sub>O<sub>3</sub><span> catalysts play a crucial role in the selective catalytic oxidation of NH</span><sub>3</sub> (NH<sub>3</sub>-SCO). To enhance NH<sub>3</sub>-SCO activity, Cu, which has stronger anchoring ability than Ag, is introduced onto Al<sub>2</sub>O<sub>3</sub>, reducing available anchoring sites for Ag. As Ag cannot displace anchored Cu species, Ag species agglomerate into larger Ag<sub>NPs</sub> even with low Ag loading. Consequently, these enlarged Ag<sub>NPs</sub> become more active centers for NH<sub>3</sub>-SCO. The optimal Ag:Cu molar ratio is confirmed as 2:3. This 'pre-occupied-anchoring-site’ strategy decreases Ag loading to 1/5 of the original, reducing catalyst costs while maintaining activity. <em>In situ</em> diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) studies reveal that NH<sub>3</sub>-SCO on 2Ag1.8Cu/Al (weight ratio) catalyst follows the hydrazine mechanism below 200 °C, coexisting with the imide mechanism from 200–250 °C, and solely the imide mechanism beyond 250 °C. This strategy is applicable to various transition metals, including Mn, Co, Ni, and Fe, promoting cost-effective Ag<sub>NPs</sub> formation.</p></div>\",\"PeriodicalId\":244,\"journal\":{\"name\":\"Applied Catalysis B: Environmental\",\"volume\":\"344 \",\"pages\":\"Article 123655\"},\"PeriodicalIF\":20.2000,\"publicationDate\":\"2023-12-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis B: Environmental\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926337323012985\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis B: Environmental","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926337323012985","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

摘要

Ag/Al2O3 催化剂中的 Ag 纳米粒子(AgNPs)在选择性催化氧化 NH3(NH3-SCO)中发挥着至关重要的作用。为了提高 NH3-SCO 的活性,在 Al2O3 上引入了锚定能力比 Ag 更强的 Cu,从而减少了 Ag 的可用锚定位点。由于 Ag 无法取代锚定的 Cu 物种,因此即使 Ag 负载较低,Ag 物种也会聚集成较大的 AgNPs。因此,这些增大的 AgNPs 成为 NH3-SCO 更为活跃的中心。最佳的银铜摩尔比为 2:3。这种 "预占锚定位 "策略可将银负载量减少到原来的 1/5,从而在保持活性的同时降低催化剂成本。原位漫反射红外傅立叶变换光谱(DRIFTS)研究表明,2Ag1.8Cu/Al(重量比)催化剂上的 NH3-SCO 在 200 °C 以下遵循肼机理,200-250 °C 期间与酰亚胺机理共存,250 °C 以上则完全遵循酰亚胺机理。这种策略适用于各种过渡金属,包括锰、钴、镍和铁,从而促进了具有成本效益的 AgNPs 的形成。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

摘要图片

查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
Catalytic oxidation of ammonia: A pre-occupied-anchoring-site strategy for enlarging Ag nanoparticles at low Ag loading and achieving enhanced activity and selectivity on Ag-CuOx/Al2O3 catalyst

The Ag nanoparticles (AgNPs) in Ag/Al2O3 catalysts play a crucial role in the selective catalytic oxidation of NH3 (NH3-SCO). To enhance NH3-SCO activity, Cu, which has stronger anchoring ability than Ag, is introduced onto Al2O3, reducing available anchoring sites for Ag. As Ag cannot displace anchored Cu species, Ag species agglomerate into larger AgNPs even with low Ag loading. Consequently, these enlarged AgNPs become more active centers for NH3-SCO. The optimal Ag:Cu molar ratio is confirmed as 2:3. This 'pre-occupied-anchoring-site’ strategy decreases Ag loading to 1/5 of the original, reducing catalyst costs while maintaining activity. In situ diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) studies reveal that NH3-SCO on 2Ag1.8Cu/Al (weight ratio) catalyst follows the hydrazine mechanism below 200 °C, coexisting with the imide mechanism from 200–250 °C, and solely the imide mechanism beyond 250 °C. This strategy is applicable to various transition metals, including Mn, Co, Ni, and Fe, promoting cost-effective AgNPs formation.

求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Applied Catalysis B: Environmental
Applied Catalysis B: Environmental 环境科学-工程:化工
CiteScore
38.60
自引率
6.30%
发文量
1117
审稿时长
24 days
期刊介绍: Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.
期刊最新文献
Conversion of CO2 to higher alcohols on K-CuZnAl/Zr-CuFe composite Effects of the chemical states of N sites and mesoporosity of N-doped carbon supports on single-atom Ru catalysts during CO2-to-formate conversion Visible-light responsive TiO2 for the complete photocatalytic decomposition of volatile organic compounds (VOCs) and its efficient acceleration by thermal energy Controlled doping of ultralow amounts Ru on Ni cathode for PEMWE: Experimental and theoretical elucidation of enhanced performance Mesoporous zeolite ZSM-5 confined Cu nanoclusters for efficient selective catalytic reduction of NOx by NH3
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1