Designing water resistant high entropy oxide materials

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.

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Publication Details

Journal
Nature Communications
Published
2024-09-27
DOI
https://doi.org/10.1038/s41467-024-52531-y
Citations
36
Primary Topic
High Entropy Alloys Studies
Type
article
Field-Weighted Citation Impact
7.65

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article

Designing water resistant high entropy oxide materials

Sheng Dai, Ying Gao, Xinhua Gao, Qiang Niu et al.
36 citations
Nature Communications
High Entropy Alloys Studies
7.65
article

Designing water resistant high entropy oxide materials

Sheng Dai, Ying Gao, Xinhua Gao, Qiang Niu, Jian Ye, Pengfei Zhang, Xiaopeng Wang, Mengyuan Zhang, Chengmin Xie, Xiaoyan Lu, Kongliang Luo, Xiaolan Duan
article en
36 citations

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 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.

Nature CommunicationsVol. 15(1)
Oak Ridge National Laboratory (US), Shanghai Jiao Tong University (CN), Ningxia University (CN), Inner Mongolia Electric Power (China) (CN)
National Natural Science Foundation of China
Openalex Percentile: Top 1%
High Entropy Alloys Studies
7.65
DOIOpen Access PDFOpenAlex
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