{"title":"Designing water resistant high entropy oxide materials","authors":"Mengyuan Zhang, Ying Gao, Chengmin Xie, Xiaolan Duan, Xiaoyan Lu, Kongliang Luo, Jian Ye, Xiaopeng Wang, Xinhua Gao, Qiang Niu, Pengfei Zhang, Sheng Dai","doi":"10.1038/s41467-024-52531-y","DOIUrl":null,"url":null,"abstract":"<p>The ubiquitous presence of moisture usually shows adverse effects on industrial catalysis. Herein, a concept of engineering entropy to design water-resistant oxide catalysts is proposed. The C<sub>3</sub>H<sub>6</sub> oxidation by spinel ACr<sub>2</sub>O<sub>4</sub> (A=Ni, Mg, Cu, Zn, Co) catalysts is selected as a model. Through DFT calculation, the adsorption energy of C<sub>3</sub>H<sub>6</sub>, the dissociation energy of molecular H<sub>2</sub>O on the oxide surface, and the formation energy of oxygen vacancy all suggest better performance induced by higher configurational entropy. Indeed, (Ni<sub>0.2</sub>Mg<sub>0.2</sub>Cu<sub>0.2</sub>Zn<sub>0.2</sub>Co<sub>0.2</sub>)Cr<sub>2</sub>O<sub>4</sub> experimentally show excellent water resistance (>100 h) in C<sub>3</sub>H<sub>6</sub> oxidation, while in sharp contrast binary oxides (e.g., NiCr<sub>2</sub>O<sub>4</sub>, CoCr<sub>2</sub>O<sub>4</sub>) are deactivated in 20 h. H<sub>2</sub>O-TPD, in-situ Raman, and in-situ FTIR all confirm the low H<sub>2</sub>O adsorption energy and strong hydrothermal stability of high entropy oxide, which is attributed to their lower Gibbs free energy. This work may inspire the rational design of water-resistant catalysts.</p>","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":null,"pages":null},"PeriodicalIF":14.7000,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-024-52531-y","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
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Abstract
The ubiquitous presence of moisture usually shows adverse effects on industrial catalysis. Herein, a concept of engineering entropy to design water-resistant oxide catalysts is proposed. The C3H6 oxidation by spinel ACr2O4 (A=Ni, Mg, Cu, Zn, Co) catalysts is selected as a model. Through DFT calculation, the adsorption energy of C3H6, the dissociation energy of molecular H2O on the oxide surface, and the formation energy of oxygen vacancy all suggest better performance induced by higher configurational entropy. Indeed, (Ni0.2Mg0.2Cu0.2Zn0.2Co0.2)Cr2O4 experimentally show excellent water resistance (>100 h) in C3H6 oxidation, while in sharp contrast binary oxides (e.g., NiCr2O4, CoCr2O4) are deactivated in 20 h. H2O-TPD, in-situ Raman, and in-situ FTIR all confirm the low H2O adsorption energy and strong hydrothermal stability of high entropy oxide, which is attributed to their lower Gibbs free energy. This work may inspire the rational design of water-resistant catalysts.
期刊介绍：
Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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