Silver salts of 12-tungstophosphoric acid supported on SBA-15: effect of enhanced specific surface area on ethanol dehydration

IF 2.8 3区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Research on Chemical Intermediates Pub Date : 2025-01-06 DOI:10.1007/s11164-024-05481-5

Mayara A. Resende, Maria Clara Hortencio Clemente, Gesley Alex Veloso Martins, Luís Carlos Cides da Silva, Marcia C. A. Fantini, Sílvia C. L. Dias, José A. Dias

{"title":"Silver salts of 12-tungstophosphoric acid supported on SBA-15: effect of enhanced specific surface area on ethanol dehydration","authors":"Mayara A. Resende, Maria Clara Hortencio Clemente, Gesley Alex Veloso Martins, Luís Carlos Cides da Silva, Marcia C. A. Fantini, Sílvia C. L. Dias, José A. Dias","doi":"10.1007/s11164-024-05481-5","DOIUrl":null,"url":null,"abstract":"<div><p>This work reports the preparation, characterization, and application of silver salt derivatives of HPW (Ag<sub>x</sub>HPW) in ethanol dehydration. The materials were fully characterized by elemental EDXRF analysis, XRD, SAXS, SEM, FT-IR, <sup>31</sup>P MAS NMR, thermal analysis (TG/DTG), N<sub>2</sub> sorption at low temperature (− 196 °C), and pyridine adsorption acidity. The results of the characterization demonstrated that the Keggin structure was preserved in all the synthesized materials. Using the ethanol dehydration model reaction, it was possible to select the most active catalyst in the series: Ag<sub>2</sub>HPW. Activation of this salt at 200 and 300 °C revealed that the degree of hydration is an important parameter for catalytic activity. In addition, a dependence on the BET specific surface area was detected for both conversion and selectivity towards ethylene in the salt series. The conversion of ethanol was significantly enhanced after loading 20 wt.% of Ag<sub>2</sub>HPW onto ordered mesoporous silica type SBA-15. The reaction conditions were optimized, and the best catalyst (20%Ag<sub>2</sub>HPW/SBA-15, calcined at 300 °C) achieved complete ethanol conversion with about 100% selectivity towards ethylene at a temperature of 400 °C.</p><h3>Graphical abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"51 2","pages":"633 - 655"},"PeriodicalIF":2.8000,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Research on Chemical Intermediates","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s11164-024-05481-5","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

Abstract

This work reports the preparation, characterization, and application of silver salt derivatives of HPW (Ag_xHPW) in ethanol dehydration. The materials were fully characterized by elemental EDXRF analysis, XRD, SAXS, SEM, FT-IR, ³¹P MAS NMR, thermal analysis (TG/DTG), N₂ sorption at low temperature (− 196 °C), and pyridine adsorption acidity. The results of the characterization demonstrated that the Keggin structure was preserved in all the synthesized materials. Using the ethanol dehydration model reaction, it was possible to select the most active catalyst in the series: Ag₂HPW. Activation of this salt at 200 and 300 °C revealed that the degree of hydration is an important parameter for catalytic activity. In addition, a dependence on the BET specific surface area was detected for both conversion and selectivity towards ethylene in the salt series. The conversion of ethanol was significantly enhanced after loading 20 wt.% of Ag₂HPW onto ordered mesoporous silica type SBA-15. The reaction conditions were optimized, and the best catalyst (20%Ag₂HPW/SBA-15, calcined at 300 °C) achieved complete ethanol conversion with about 100% selectivity towards ethylene at a temperature of 400 °C.

Graphical abstract

Abstract Image

查看原文本刊更多论文

SBA-15负载的12-钨磷酸银盐：提高比表面积对乙醇脱水的影响

本文报道了HPW银盐衍生物（AgxHPW）的制备、表征及其在乙醇脱水中的应用。通过元素分析EDXRF、XRD、SAXS、SEM、FT-IR、31P MAS NMR、热分析（TG/DTG）、低温N2吸附（- 196℃）、吡啶吸附酸度等手段对材料进行了表征。表征结果表明，所有合成材料都保持了Keggin结构。采用乙醇脱水模型反应，可以选择该系列中活性最高的催化剂：Ag2HPW。该盐在200和300℃下的活化表明，水化程度是催化活性的重要参数。此外，在盐系中，对乙烯的转化率和选择性都与BET比表面积有关。在有序介孔硅型SBA-15上负载20 wt.%的Ag2HPW后，乙醇的转化率显著提高。对反应条件进行了优化，最佳催化剂（20%Ag2HPW/SBA-15, 300℃煅烧）在400℃下对乙烯的选择性约为100%，实现了乙醇的完全转化。图形抽象

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Research on Chemical Intermediates 化学-化学综合

CiteScore

5.70

自引率

18.20%

发文量

229

审稿时长

2.6 months

期刊介绍： Research on Chemical Intermediates publishes current research articles and concise dynamic reviews on the properties, structures and reactivities of intermediate species in all the various domains of chemistry. The journal also contains articles in related disciplines such as spectroscopy, molecular biology and biochemistry, atmospheric and environmental sciences, catalysis, photochemistry and photophysics. In addition, special issues dedicated to specific topics in the field are regularly published.