金属掺杂剂对Ni@CeMeO2甲烷干法重整嵌入催化剂(Me=Gd、Sm和Zr)

Methane Pub Date : 2022-11-28 DOI:10.3390/methane1040023
A. A. Marinho, R. Rabelo-Neto, F. Epron, F. Toniolo, F. Noronha, N. Bion
{"title":"金属掺杂剂对Ni@CeMeO2甲烷干法重整嵌入催化剂(Me=Gd、Sm和Zr)","authors":"A. A. Marinho, R. Rabelo-Neto, F. Epron, F. Toniolo, F. Noronha, N. Bion","doi":"10.3390/methane1040023","DOIUrl":null,"url":null,"abstract":"Biogas upgrading by a catalytic process has been studied in order to obtain syngas using renewable source of methane. This work evaluates the influence of metal dopant (Gd, Sm, and Zr) on the CeO2 structure for the dry reforming of methane over Ni nanoparticle embedded catalysts. The doping with Zr improved the thermal stability of the catalyst, leading to the formation of small Ni nanoparticles, while Ni metal sintering was observed for Ni@CeO2, Ni@CeGdO2, and Ni@SmO2, according to in situ XRD under reduction conditions. The ceria reducibility was affected by the dopant nature, for which the addition of Zr caused distortions in the ceria lattice, promoting the diffusion of oxygen bulk to surface. The doping with Gd and Sm created oxygen vacancies by charge compensation, and the saturation of oxygen vacancies in the fresh samples decreased the degree of Ce reduction, according to TPR results. The larger Ni particles and poor redox behavior for Ni@CeGdO2 and Ni@CeSmO2 were responsible for the high carbon formation on these catalysts during the DRM reaction. The Ni@CeZrO2 catalyst did not present coke formation because of smaller Ni crystallite size and higher ceria reducibility. Therefore, the control of Ni particle size and the high oxygen mobility in the Ni@CeZrO2 catalyst inhibits carbon deposition and enhances the mechanism of carbon removal, promoting the catalyst stability.","PeriodicalId":74177,"journal":{"name":"Methane","volume":" ","pages":""},"PeriodicalIF":0.0000,"publicationDate":"2022-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"1","resultStr":"{\"title\":\"Effect of Metal Dopant on the Performance of Ni@CeMeO2 Embedded Catalysts (Me = Gd, Sm and Zr) for Dry Reforming of Methane\",\"authors\":\"A. A. Marinho, R. Rabelo-Neto, F. Epron, F. Toniolo, F. Noronha, N. Bion\",\"doi\":\"10.3390/methane1040023\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Biogas upgrading by a catalytic process has been studied in order to obtain syngas using renewable source of methane. This work evaluates the influence of metal dopant (Gd, Sm, and Zr) on the CeO2 structure for the dry reforming of methane over Ni nanoparticle embedded catalysts. The doping with Zr improved the thermal stability of the catalyst, leading to the formation of small Ni nanoparticles, while Ni metal sintering was observed for Ni@CeO2, Ni@CeGdO2, and Ni@SmO2, according to in situ XRD under reduction conditions. The ceria reducibility was affected by the dopant nature, for which the addition of Zr caused distortions in the ceria lattice, promoting the diffusion of oxygen bulk to surface. The doping with Gd and Sm created oxygen vacancies by charge compensation, and the saturation of oxygen vacancies in the fresh samples decreased the degree of Ce reduction, according to TPR results. The larger Ni particles and poor redox behavior for Ni@CeGdO2 and Ni@CeSmO2 were responsible for the high carbon formation on these catalysts during the DRM reaction. The Ni@CeZrO2 catalyst did not present coke formation because of smaller Ni crystallite size and higher ceria reducibility. Therefore, the control of Ni particle size and the high oxygen mobility in the Ni@CeZrO2 catalyst inhibits carbon deposition and enhances the mechanism of carbon removal, promoting the catalyst stability.\",\"PeriodicalId\":74177,\"journal\":{\"name\":\"Methane\",\"volume\":\" \",\"pages\":\"\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2022-11-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"1\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Methane\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.3390/methane1040023\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Methane","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.3390/methane1040023","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 1

摘要

为了利用可再生的甲烷来源获得合成气,研究了催化过程中的沼气升级。本工作评估了金属掺杂剂(Gd、Sm和Zr)对甲烷在Ni纳米颗粒嵌入催化剂上干重整CeO2结构的影响。Zr的掺杂提高了催化剂的热稳定性,导致形成了小的Ni纳米颗粒,同时观察到Ni金属烧结Ni@CeO2,Ni@CeGdO2和Ni@SmO2,根据还原条件下的原位XRD。二氧化铈的还原性受到掺杂剂性质的影响,其中Zr的添加导致二氧化铈晶格畸变,促进了氧体向表面的扩散。根据TPR结果,Gd和Sm的掺杂通过电荷补偿产生了氧空位,并且新鲜样品中氧空位的饱和降低了Ce的还原程度。较大的Ni颗粒和较差的氧化还原行为Ni@CeGdO2和Ni@CeSmO2是DRM反应期间在这些催化剂上形成高碳的原因。这个Ni@CeZrO2由于较小的Ni晶粒尺寸和较高的二氧化铈还原性,催化剂不存在焦炭形成。因此,Ni颗粒尺寸的控制和Ni@CeZrO2催化剂抑制了积碳,增强了除碳机理,提高了催化剂的稳定性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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
Effect of Metal Dopant on the Performance of Ni@CeMeO2 Embedded Catalysts (Me = Gd, Sm and Zr) for Dry Reforming of Methane
Biogas upgrading by a catalytic process has been studied in order to obtain syngas using renewable source of methane. This work evaluates the influence of metal dopant (Gd, Sm, and Zr) on the CeO2 structure for the dry reforming of methane over Ni nanoparticle embedded catalysts. The doping with Zr improved the thermal stability of the catalyst, leading to the formation of small Ni nanoparticles, while Ni metal sintering was observed for Ni@CeO2, Ni@CeGdO2, and Ni@SmO2, according to in situ XRD under reduction conditions. The ceria reducibility was affected by the dopant nature, for which the addition of Zr caused distortions in the ceria lattice, promoting the diffusion of oxygen bulk to surface. The doping with Gd and Sm created oxygen vacancies by charge compensation, and the saturation of oxygen vacancies in the fresh samples decreased the degree of Ce reduction, according to TPR results. The larger Ni particles and poor redox behavior for Ni@CeGdO2 and Ni@CeSmO2 were responsible for the high carbon formation on these catalysts during the DRM reaction. The Ni@CeZrO2 catalyst did not present coke formation because of smaller Ni crystallite size and higher ceria reducibility. Therefore, the control of Ni particle size and the high oxygen mobility in the Ni@CeZrO2 catalyst inhibits carbon deposition and enhances the mechanism of carbon removal, promoting the catalyst stability.
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
自引率
0.00%
发文量
0
期刊最新文献
Application of Digestate from a Methane Fermentation Process for Supplying Water and Nutrients in Sweet Potato Cultivation in Sandy Soil Pathways toward Climate-Neutral Red Meat Production Recent Advances in the Use of Controlled Nanocatalysts in Methane Conversion Reactions Dry Reforming of CH4 Using a Microreactor A Study on the Heterogeneity and Anisotropy of the Porous Grout Body Created in the Stabilization of a Methane Hydrate Reservoir through Grouting
×
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