Rare earth-incorporated high entropy oxides for energy and environmental catalysis

doi:10.1016/S1872-2067(24)60012-4

Chinese Journal of Catalysis ›› 2024, Vol. 61: 54-70.DOI: 10.1016/S1872-2067(24)60012-4

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Rare earth-incorporated high entropy oxides for energy and environmental catalysis

Yuou Li^a^,^b, Ke Wang^a^,^b, Xiaomei Wang^a^,^b, Zijian Wang^a^,^b, Jing Xu^a^,^b, Meng Zhao^a^,^b, Xiao Wang^a^,^b^,^*(), Shuyan Song^a^,^b^,^*(), Hongjie Zhang^a^,^b^,^c^,^*()

^aState Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, Jilin, China
^bSchool of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, Anhui, China
^cDepartment of Chemistry, Tsinghua University, Beijing 100084, China

Received:2024-02-12 Accepted:2024-03-13 Online:2024-06-18 Published:2024-06-20
Contact: * E-mail: wangxiao@ciac.ac.cn (X. Wang),songsy@ciac.ac.cn (S. Song),hongjie@ciac.ac.cn (H. Zhang).
About author:Xiao Wang received his BSc degree in Chemistry in 2008 from Jilin University. Then, he joined the group of Prof. Hongjie Zhang at Changchun Institute of Applied Chemistry, Chinese Academy of Sciences (CAS), and received his PhD degree in Inorganic Chemistry in 2013. His research focus is primarily on the fabrication of functional inorganic materials for heterogeneous catalytic reactions and energy-related applications.
Shuyan Song received his BSc degree in Chemistry in 2003 and MSc in inorganic chemistry in 2006 both from Northeast Normal University. He joined the group of Prof. Hongjie Zhang at Changchun Institute of Applied Chemistry, Chinese Academy of Sciences (CAS), where he received his PhD in inorganic chemistry in 2009. He is working as a professor under the direction of Prof. Zhang at Changchun Institute of Applied Chemistry, CAS. His research focus is primarily on the development of porous functional materials for heterogeneous catalysis, proton conduction, chemical sensing and detection.
Hongjie Zhang received his BSc degree from Peking University in 1978. He then worked as a research assistant in Changchun Institute of Applied Chemistry, where he received his MSc degree in Inorganic Chemistry in 1985. Then, he worked as an assistant professor at the same institute from 1985-1989. He then studied at Universite de Bordeaux I, Laboratoire de Chimie du Solide du CNRS (France), where he received his PhD degree in Solid State Chemistry and Materials Sciences in 1993. He joined Changchun Institute of Applied Chemistry, CAS, as a professor in 1994. His current research interests include lanthanide organic-inorganic hybrid materials, electroluminescent devices, functional nanomaterials, and the structure and properties of rare earth magnesium alloys.
Supported by:
National Science and Technology Major Project of China(2021YFB3500700);National Natural Science Foundation of China(22020102003);National Natural Science Foundation of China(22025506);National Natural Science Foundation of China(22271274);Program of Science and Technology Development Plan of Jilin Province of China(20230101035JC);Program of Science and Technology Development Plan of Jilin Province of China(20230101022JC)

Abstract

Abstract:

High entropy oxides have been regarded as one of the most promising catalysts. Their unique and diverse elemental compositions bring stable structures and abundant metal active sites to the catalysts. Notably, rare earth ions have similar radii, unique electron orbitals, and variable valence states. As a result, incorporating rare earth elements into high entropy oxides can effectively adjust the surface state of the catalyst, ultimately improving the structure and properties of the high entropy oxides. However, there is no systematic review on the development of rare earth-incorporated high entropy oxides. In this review, we target the structure, synthesis, and application of rare earth-incorporated high entropy oxides to summarize their research progress in catalysis in recent years. First, we provide an overview of three types of rare earth-incorporated high entropy oxides: fluorite-type, perovskite-type, and pyrochlore-type. Then, the main synthesis methods are discussed in detail, including solid-state reaction, nebulized spray pyrolysis, chemical co-precipitation, and solution combustion. Finally, we analyze the applications of this material in catalytic reactions and suggest possible challenges and solution strategies. It is concluded that this unique material has good prospects for development.

Key words: Rare earth, High entropy oxides, Catalysis, Single-phase structure, Synthesis

Yuou Li, Ke Wang, Xiaomei Wang, Zijian Wang, Jing Xu, Meng Zhao, Xiao Wang, Shuyan Song, Hongjie Zhang. Rare earth-incorporated high entropy oxides for energy and environmental catalysis[J]. Chinese Journal of Catalysis, 2024, 61: 54-70.

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Figures/Tables 10

Fig. 1. (a) The state of the five elements before and after mixing. Reprinted with permission from Ref. [39]. Copyright 2021, Elsevier Ltd. (b) Schematic diagram of catalytic active sites of HEO. Reprinted with permission from Ref. [25]. Copyright 2022, Elsevier B.V. (c) Categories and phase structure of HEOs. Reprinted with permission from Ref. [24]. Copyright 2022, Elsevier Inc.

Fig. 2. Three typical structures of RE-HEOs: perovskite-type HEOs, fluorite-type HEOs, pyrochlore-type HEOs.

Fig. 3. (a) The XRD image of La(FeCoNiCrMn)O3. Reprinted with permission from Ref. [36]. Copyright 2022, American Chemical Society. (b) The XRD images of La(CrMnFeCo2Ni)O3, etc. Reprinted with permission from Ref. [37]. Copyright 2021, Wiley‐VCH GmbH. (c) The XRD images of (Ce, La, Nd, Pr, Sm, Y)O2, etc. Reprinted with permission from Ref. [44]. Copyright 2021, Royal Society of Chemistry. (d) The XRD image of CeHfZrSnErOx. Reprinted with permission from Ref. [46]. Copyright 2022, Elsevier. (e) The XRD images of A2Ti2O7 (A: Gd, Dy, Ho, Er, Yb, Nd). Reprinted with permission from Ref. [48]. Copyright 2023, Elsevier Ltd. (f) The XRD images of Gd2(Ti0.25Zr0.25Hf0.25Ce0.25)2O7, etc. Reprinted with permission from Ref. [50]. Copyright 2022, Elsevier B.V.

Fig. 4. (a) Main synthesis process of (Cu, Mn, Fe, Cr)3O4 by solid-state reaction method. Reprinted with permission from Ref. [60]. Copyright 2021, American Chemical Society. (b) Preparation process of high entropy (La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Ce2O7. Reprinted with permission from Ref. [62]. Copyright 2022, Journal of Advanced Ceramics.

Fig. 5. (a) Schematic diagram for the stages of spray pyrolysis process. (b) Spray pyrolysis powder. The black spots indicate that segregation only occurs inside atomized droplets. Reprinted with permission from Ref. [70]. Copyright 2023, Journal of Materials Science: Materials in Electronics. (c) Photographs of the as-synthesized powder by spray pyrolysis and high pressure compacted pellet of RE-HEO powder. (d) SEM image of the as-synthesized RE-HEO showing spherical particles. (e) HR-TEM image of synthesized RE-HEO powder. (f) APT results show the 3D atomic distribution map of RE-HEOs. Reprinted with permission from Ref. [72]. Copyright 2019, Elsevier Ltd.

Fig. 6. (a) Schematic illustration of the preparation of the (CrMnFeCoCu)3O4 HEO. Reprinted with permission from Ref. [77]. Copyright 2023, American Chemical Society. (b) Schematic illustration of the synthesis of CeHfZrSnErOx. Reprinted with permission from Ref. [46]. Copyright 2022, Elsevier. (c) Schematic diagrams of the preparation process of high entropy pyrochlore oxide powder (I) and porous high entropy pyrochlore oxide ceramics (II). Reprinted with permission from Ref. [80]. Copyright 2023, Elsevier Ltd and Techna Group S.r.l.

Fig. 7. (a) The synthesis scheme of the UHE REO nanopowder. Reprinted with permission from Ref. [82]. Copyright 2023, The Royal Society of Chemistry. (b) Schematic of synthesis of HEO powder. Reprinted with permission from Ref. [88]. Copyright 2023, Elsevier B.V.

Fig. 8. (a) Synthesis of carbon-based loaded 10-HEO nanoparticles, TEM image of nanoparticles on a carbon matrix, LSV curves of 10-HEO/C and contrast samples, ORR stability diagram of 10-HEO/C. Reprinted with permission from Ref. [96]. Copyright 2021, Wiley-VCH GmbH. (b) OER of (LPNSE)NO thin films (LSV curves of films with different thicknesses, comparison of OER catalytic activity, Tafel slopes and electrochemical impedance spectra). Reprinted with permission from Ref. [99]. Copyright 2023, AIP Publishing. (c) Electrochemical performances of La1-xCaxB2Co (x = 0, 0.1, 0.2, 0.3, 0.4) (Polarization LSV curves, Tafel slopes, Nyquist plots at 1.627 V vs. RHE and OER durability). Reprinted with permission from Ref. [103]. Copyright 2024, Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.

Fig. 9. (a) Ce0.8(LaMnNdZr)0.2O2-y structure diagram. (b) CO conversion rate of the catalysts. (c) Performance comparison of catalysts before and after aging. Reprinted with permission from Ref. [105]. Copyright 2021, American Chemical Society. (d) Schematic diagram of entropy-driven mixing and XRD images. (e) Stability of catalysts. Reprinted with permission from Ref. [107]. Copyright 2021, Springer Nature. (f) Macroporous HEO Ce0.5Ni0.1Mg0.1Cu0.1Zn0.1Co0.1Ox formed by high temperature calcination. (g) Catalytic soot combustion performance of catalysts. (h) Water and sulfur resistance performance of Ce0.5Ni0.1Mg0.1Cu0.1Zn0.1Co0.1Ox. (Reprinted with permission from Ref. [109]. Copyright 2023, The Royal Society of Chemistry.

Fig. 10. (a) Fluorite HEO crystal structure of catalyst. (b) Time-dependent hydrogen (H2) evolution. (c) The ability of catalyst to degrade the dye MB. Reprinted with permission from Ref. [121]. Copyright 2022, Wiley-VCH GmbH. (d) EIS and the equivalent circuit of catalysts. (e) The photocatalytic performances of various photocatalysts. (f) The effect of various reaction parameters on simultaneous photocatalytic CO2 reduction and biorefinery. Reprinted with permission from Ref. [126]. Copyright 2023, The Royal Society of Chemistry. (g) XRD images of different Eu dopants. (h) Photocatalytic mechanism of Ln2-xEuxZr2O7 products. (i) RhB concentration during photodegradation. Reprinted with permission from Ref. [127]. Copyright 2022, Springer Science Business Media, LLC, part of Springer Nature.

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Rare earth-incorporated high entropy oxides for energy and environmental catalysis

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