具有保留氧化还原特性的高熵氧载体的化学环燃烧性能

IF 4.1 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science Pub Date : 2025-04-25 DOI:10.1016/j.ces.2025.121674

Tianxu Shen, Tao Song, Zihan Geng, Laihong Shen, Muchuan Yang

{"title":"具有保留氧化还原特性的高熵氧载体的化学环燃烧性能","authors":"Tianxu Shen, Tao Song, Zihan Geng, Laihong Shen, Muchuan Yang","doi":"10.1016/j.ces.2025.121674","DOIUrl":null,"url":null,"abstract":"Adopting the multi-principal element trend, four high entropy oxide (HEO) OCs were developed to fulfill diverse performance demands. These HEO OCs exhibited a distinctive redox pattern characterized by rapid reduction but slower oxidation. The reduction rate of HEO OCs is 1.9 and 2.6 times higher than that of perovskite and hematite OCs, but oxidation rates are only 25% of these reference OCs. Sluggish diffusion effect contributed to exceptional redox stability, exhibiting consistent reactivity, minimal agglomeration, and no phase decomposition across 30 deep redox cycles. Elemental synergies enabled exceptional CH4 conversion, with HEO OCs achieving methane conversion efficiency and CO2 selectivity both exceeding 90%. HEO OCs predominantly formed partially inverted spinel structures. Aluminum incorporation extended benefits beyond anti-sintering, also enhancing solid solution effects and oxygen vacancy formation. Sodium addition was discouraged due to limited solubility and high-temperature instability, with over 60% precepting as secondary phases and undergoing volatilization loss.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"8 1","pages":""},"PeriodicalIF":4.1000,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Chemical looping combustion performance of High-Entropy dominated oxygen carriers with reserved redox characteristics\",\"authors\":\"Tianxu Shen, Tao Song, Zihan Geng, Laihong Shen, Muchuan Yang\",\"doi\":\"10.1016/j.ces.2025.121674\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Adopting the multi-principal element trend, four high entropy oxide (HEO) OCs were developed to fulfill diverse performance demands. These HEO OCs exhibited a distinctive redox pattern characterized by rapid reduction but slower oxidation. The reduction rate of HEO OCs is 1.9 and 2.6 times higher than that of perovskite and hematite OCs, but oxidation rates are only 25% of these reference OCs. Sluggish diffusion effect contributed to exceptional redox stability, exhibiting consistent reactivity, minimal agglomeration, and no phase decomposition across 30 deep redox cycles. Elemental synergies enabled exceptional CH4 conversion, with HEO OCs achieving methane conversion efficiency and CO2 selectivity both exceeding 90%. HEO OCs predominantly formed partially inverted spinel structures. Aluminum incorporation extended benefits beyond anti-sintering, also enhancing solid solution effects and oxygen vacancy formation. Sodium addition was discouraged due to limited solubility and high-temperature instability, with over 60% precepting as secondary phases and undergoing volatilization loss.\",\"PeriodicalId\":271,\"journal\":{\"name\":\"Chemical Engineering Science\",\"volume\":\"8 1\",\"pages\":\"\"},\"PeriodicalIF\":4.1000,\"publicationDate\":\"2025-04-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Engineering Science\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.ces.2025.121674\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Science","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.ces.2025.121674","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}

引用次数: 0

摘要

采用多主元趋势，开发了四种高熵氧化物（HEO） OCs，以满足不同的性能要求。这些HEO oc表现出独特的氧化还原模式，其特征是快速还原但缓慢氧化。HEO oc的还原率分别是钙钛矿oc和赤铁矿oc的1.9倍和2.6倍，但氧化率仅为参考oc的25%。缓慢的扩散效应有助于优异的氧化还原稳定性，在30个深度氧化还原循环中表现出一致的反应性、最小的团聚和无相分解。元素的协同作用使得甲烷转化效果显著，HEO oc的甲烷转化效率和二氧化碳选择性均超过90%。HEO oc主要形成部分倒置尖晶石结构。铝的加入不仅有抗烧结的好处，还能提高固溶效果和氧空位的形成。由于钠的溶解度有限和高温不稳定性，超过60%的钠析出为次级相，并发生挥发损失，因此不建议添加钠。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Chemical looping combustion performance of High-Entropy dominated oxygen carriers with reserved redox characteristics

查看原文本刊更多论文

Chemical looping combustion performance of High-Entropy dominated oxygen carriers with reserved redox characteristics

Adopting the multi-principal element trend, four high entropy oxide (HEO) OCs were developed to fulfill diverse performance demands. These HEO OCs exhibited a distinctive redox pattern characterized by rapid reduction but slower oxidation. The reduction rate of HEO OCs is 1.9 and 2.6 times higher than that of perovskite and hematite OCs, but oxidation rates are only 25% of these reference OCs. Sluggish diffusion effect contributed to exceptional redox stability, exhibiting consistent reactivity, minimal agglomeration, and no phase decomposition across 30 deep redox cycles. Elemental synergies enabled exceptional CH₄ conversion, with HEO OCs achieving methane conversion efficiency and CO₂ selectivity both exceeding 90%. HEO OCs predominantly formed partially inverted spinel structures. Aluminum incorporation extended benefits beyond anti-sintering, also enhancing solid solution effects and oxygen vacancy formation. Sodium addition was discouraged due to limited solubility and high-temperature instability, with over 60% precepting as secondary phases and undergoing volatilization loss.

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

Chemical Engineering Science 工程技术-工程：化工

CiteScore

7.50

自引率

8.50%

发文量

1025

审稿时长

50 days

期刊介绍： Chemical engineering enables the transformation of natural resources and energy into useful products for society. It draws on and applies natural sciences, mathematics and economics, and has developed fundamental engineering science that underpins the discipline. Chemical Engineering Science (CES) has been publishing papers on the fundamentals of chemical engineering since 1951. CES is the platform where the most significant advances in the discipline have ever since been published. Chemical Engineering Science has accompanied and sustained chemical engineering through its development into the vibrant and broad scientific discipline it is today.