通过醋酸干重整提高 H2 产量的铈强化 Ni/Al2O3 催化剂

IF 5.6 2区 工程技术 Q2 ENERGY & FUELS
{"title":"通过醋酸干重整提高 H2 产量的铈强化 Ni/Al2O3 催化剂","authors":"","doi":"10.1016/j.joei.2024.101821","DOIUrl":null,"url":null,"abstract":"<div><p>Acetic acid dry reforming (ADR) is a promising route for sustainable H<sub>2</sub> generation. However, coke inhibition during ADR is the main challenge and not resolved by using suitable promoted catalysts. In this work, Ce promotion on 10%Ni/Al<sub>2</sub>O<sub>3</sub> catalysts with 1-5 wt%Ce was evaluated for ADR at varied temperatures of 923–998 K and stoichiometric feed in a fixed-bed rig. CeO<sub>2</sub> addition of 1–3% enhanced metal dispersion, and surface area whilst basic CeO<sub>2</sub> character significantly boosted the concentration and density of basic sites on catalysts. Particularly, the CO<sub>2</sub> uptake of promoted catalysts was about 2.49–3.73 times greater than that of counterpart sample. CH<sub>3</sub>COOH and CO<sub>2</sub> conversions were enhanced with rising Ce loading and the highest reactant conversions were observed at 3 wt%Ce. The improved adsorption of acidic CH<sub>3</sub>COOH and CO<sub>2</sub> molecules due to increasing amount of basic sites as well as redox attributes of CeO<sub>2</sub> promoter could be responsible for the enhancement in ADR activity and yield of H<sub>2</sub> and CO. The mechanistic two-step pathway for coke suppression induced by CeO<sub>2</sub> promotion was elaborated in this work. Generally, carbonaceous species formation on 3%Ce–10%Ni/Al<sub>2</sub>O<sub>3</sub> was considerably reduced about 1.6–2.0 times. H<sub>2</sub>/CO ratio varied from 0.59 to 0.65 relying on ADR temperature over 3%Ce–10%Ni/Al<sub>2</sub>O<sub>3</sub>. These H<sub>2</sub>/CO values, two times higher than theoretical H<sub>2</sub>/CO ratio in ADR, are compatible for downstream gas-to-liquid processes to selectively yield high molecular weight olefins. Water formation rate increased from 8.67 × 10<sup>−6</sup> to 4.71 × 10<sup>−5</sup> <span><math><mrow><msub><mtext>mol</mtext><mrow><msub><mi>H</mi><mn>2</mn></msub><mi>O</mi></mrow></msub></mrow></math></span> g<sub>cat</sub><sup>−1</sup> s<sup>−1</sup> with rising temperature within 923–998 K on 3%Ce–10%Ni/Al<sub>2</sub>O<sub>3</sub>.</p></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":null,"pages":null},"PeriodicalIF":5.6000,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Ceria-boosted Ni/Al2O3 catalysts for enhanced H2 production via acetic acid dry reforming\",\"authors\":\"\",\"doi\":\"10.1016/j.joei.2024.101821\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Acetic acid dry reforming (ADR) is a promising route for sustainable H<sub>2</sub> generation. However, coke inhibition during ADR is the main challenge and not resolved by using suitable promoted catalysts. In this work, Ce promotion on 10%Ni/Al<sub>2</sub>O<sub>3</sub> catalysts with 1-5 wt%Ce was evaluated for ADR at varied temperatures of 923–998 K and stoichiometric feed in a fixed-bed rig. CeO<sub>2</sub> addition of 1–3% enhanced metal dispersion, and surface area whilst basic CeO<sub>2</sub> character significantly boosted the concentration and density of basic sites on catalysts. Particularly, the CO<sub>2</sub> uptake of promoted catalysts was about 2.49–3.73 times greater than that of counterpart sample. CH<sub>3</sub>COOH and CO<sub>2</sub> conversions were enhanced with rising Ce loading and the highest reactant conversions were observed at 3 wt%Ce. The improved adsorption of acidic CH<sub>3</sub>COOH and CO<sub>2</sub> molecules due to increasing amount of basic sites as well as redox attributes of CeO<sub>2</sub> promoter could be responsible for the enhancement in ADR activity and yield of H<sub>2</sub> and CO. The mechanistic two-step pathway for coke suppression induced by CeO<sub>2</sub> promotion was elaborated in this work. Generally, carbonaceous species formation on 3%Ce–10%Ni/Al<sub>2</sub>O<sub>3</sub> was considerably reduced about 1.6–2.0 times. H<sub>2</sub>/CO ratio varied from 0.59 to 0.65 relying on ADR temperature over 3%Ce–10%Ni/Al<sub>2</sub>O<sub>3</sub>. These H<sub>2</sub>/CO values, two times higher than theoretical H<sub>2</sub>/CO ratio in ADR, are compatible for downstream gas-to-liquid processes to selectively yield high molecular weight olefins. Water formation rate increased from 8.67 × 10<sup>−6</sup> to 4.71 × 10<sup>−5</sup> <span><math><mrow><msub><mtext>mol</mtext><mrow><msub><mi>H</mi><mn>2</mn></msub><mi>O</mi></mrow></msub></mrow></math></span> g<sub>cat</sub><sup>−1</sup> s<sup>−1</sup> with rising temperature within 923–998 K on 3%Ce–10%Ni/Al<sub>2</sub>O<sub>3</sub>.</p></div>\",\"PeriodicalId\":17287,\"journal\":{\"name\":\"Journal of The Energy Institute\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.6000,\"publicationDate\":\"2024-09-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of The Energy Institute\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S174396712400299X\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of The Energy Institute","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S174396712400299X","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
引用次数: 0

摘要

醋酸干法重整(ADR)是一种很有前景的可持续 H2 生成途径。然而,ADR 过程中的焦炭抑制是一个主要挑战,使用合适的促进催化剂并不能解决这一问题。在这项工作中,在固定床装置中,在 923-998 K 的不同温度下和按化学计量进料条件下,对 10%Ni/Al2O3 催化剂上 1-5 wt%Ce 的铈促进进行了 ADR 评估。添加 1-3% 的 CeO2 增强了金属分散性和表面积,而碱性 CeO2 则显著提高了催化剂上碱性位点的浓度和密度。特别是,促进催化剂对 CO2 的吸收率是对应样品的 2.49-3.73 倍。随着 Ce 含量的增加,CH3COOH 和 CO2 的转化率也得到了提高,3 wt%Ce 时的反应物转化率最高。由于碱性位点的增加以及 CeO2 促进剂的氧化还原属性,酸性 CH3COOH 和 CO2 分子的吸附性得到改善,这可能是 ADR 活性和 H2 和 CO 产率提高的原因。本研究阐述了 CeO2 促进剂诱导焦炭抑制的两步机理途径。一般来说,3%Ce-10%Ni/Al2O3 上的炭质形成大大减少了约 1.6-2.0 倍。在 3%Ce-10%Ni/Al2O3 上,根据 ADR 温度的不同,H2/CO 比率从 0.59 到 0.65 不等。这些 H2/CO 值比 ADR 中的理论 H2/CO 比值高出两倍,适合下游气变液工艺选择性地生产高分子量烯烃。在 3%Ce-10%Ni/Al2O3 上,随着温度在 923-998 K 范围内上升,水形成率从 8.67 × 10-6 增至 4.71 × 10-5 molH2O gcat-1 s-1。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Ceria-boosted Ni/Al2O3 catalysts for enhanced H2 production via acetic acid dry reforming

Ceria-boosted Ni/Al2O3 catalysts for enhanced H2 production via acetic acid dry reforming

Acetic acid dry reforming (ADR) is a promising route for sustainable H2 generation. However, coke inhibition during ADR is the main challenge and not resolved by using suitable promoted catalysts. In this work, Ce promotion on 10%Ni/Al2O3 catalysts with 1-5 wt%Ce was evaluated for ADR at varied temperatures of 923–998 K and stoichiometric feed in a fixed-bed rig. CeO2 addition of 1–3% enhanced metal dispersion, and surface area whilst basic CeO2 character significantly boosted the concentration and density of basic sites on catalysts. Particularly, the CO2 uptake of promoted catalysts was about 2.49–3.73 times greater than that of counterpart sample. CH3COOH and CO2 conversions were enhanced with rising Ce loading and the highest reactant conversions were observed at 3 wt%Ce. The improved adsorption of acidic CH3COOH and CO2 molecules due to increasing amount of basic sites as well as redox attributes of CeO2 promoter could be responsible for the enhancement in ADR activity and yield of H2 and CO. The mechanistic two-step pathway for coke suppression induced by CeO2 promotion was elaborated in this work. Generally, carbonaceous species formation on 3%Ce–10%Ni/Al2O3 was considerably reduced about 1.6–2.0 times. H2/CO ratio varied from 0.59 to 0.65 relying on ADR temperature over 3%Ce–10%Ni/Al2O3. These H2/CO values, two times higher than theoretical H2/CO ratio in ADR, are compatible for downstream gas-to-liquid processes to selectively yield high molecular weight olefins. Water formation rate increased from 8.67 × 10−6 to 4.71 × 10−5 molH2O gcat−1 s−1 with rising temperature within 923–998 K on 3%Ce–10%Ni/Al2O3.

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
Journal of The Energy Institute
Journal of The Energy Institute 工程技术-能源与燃料
CiteScore
10.60
自引率
5.30%
发文量
166
审稿时长
16 days
期刊介绍: The Journal of the Energy Institute provides peer reviewed coverage of original high quality research on energy, engineering and technology.The coverage is broad and the main areas of interest include: Combustion engineering and associated technologies; process heating; power generation; engines and propulsion; emissions and environmental pollution control; clean coal technologies; carbon abatement technologies Emissions and environmental pollution control; safety and hazards; Clean coal technologies; carbon abatement technologies, including carbon capture and storage, CCS; Petroleum engineering and fuel quality, including storage and transport Alternative energy sources; biomass utilisation and biomass conversion technologies; energy from waste, incineration and recycling Energy conversion, energy recovery and energy efficiency; space heating, fuel cells, heat pumps and cooling systems Energy storage The journal''s coverage reflects changes in energy technology that result from the transition to more efficient energy production and end use together with reduced carbon emission.
×
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
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
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 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信