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Mixing 3d-cations strategy to construct stable high-entropy Bi-pyrochlore oxides with superior near-infrared optical absorption and (photo)electrochemical activity.

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Title: Mixing 3d-cations strategy to construct stable high-entropy Bi-pyrochlore oxides with superior near-infrared optical absorption and (photo)electrochemical activity.
Authors: Sun, Shujie1,2 (AUTHOR) sjsun@xynu.edu.cn, Shen, Junya1 (AUTHOR), Han, Wenle1 (AUTHOR), Liu, Chaowei1 (AUTHOR), Hou, Haoran2 (AUTHOR), Ti, Ruixia3 (AUTHOR), Chen, Wenjin1,2 (AUTHOR), Yin, Xiaofeng1,2 (AUTHOR) yxfeng@xynu.edu.cn
Source: Ceramics International. Jun2026:Part C, Vol. 52 Issue 14, p27156-27168. 13p.
Subjects: Pyrochlore, Infrared absorption, Photoelectrochemistry, Transition metal ions, Oxygen evolution reactions, Oxides, Sol-gel processes
Abstract: Cubic Bi-pyrochlores possess excellently structural stability and compositional flexibility, therefore, utilizing configurational entropy to engineer such single-phase oxides has driven the significant research activity. Herein, single-phase and high-entropy cubic Bi-pyrochlore oxides were constructed by magnetic 3d -cations entropy engineering in a Bi 1.68 MNb 1.32 O 6 O' (M = equimolar 3d -ions) system and successfully synthesized using a modified sol-gel combustion technology. The pyrochlore-type structure and designed stoichiometric ratio were carefully confirmed by utilizing X-ray diffraction and electron microtechniques, and effects of high-entropy engineering on microstructure, optical adsorption and catalytic activity were studied in detail. Significantly, as increasing the entropy-level, evolutions of pyrochlore-phase structure and morphology were clearly observed from big cube-grains with large lattice volume towards relatively smaller polyhedral-crystals with decreased lattice volume. What is more, high-entropy by adopting multi-type 3d -cations not only remain stable up to 1000 °C, but also induce an obvious enhancement of optical absorption from visible-light to near-infrared-light, ascribed to d -orbital energy splitting and localized d-d transitions, thereby achieving a superior near-infrared photoresponse in neutral electrolytes under laser irradiation. For electrocatalysis, such high-entropy pyrochlore-catalysts can also exhibit excellent oxygen evolution reaction activities, with a low overpotential <330 mV and a small Tafel slope <50 mV/dec, even their activities are comparable to the 3d -metal-based catalysts. [ABSTRACT FROM AUTHOR]
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Database: Engineering Source
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Abstract:Cubic Bi-pyrochlores possess excellently structural stability and compositional flexibility, therefore, utilizing configurational entropy to engineer such single-phase oxides has driven the significant research activity. Herein, single-phase and high-entropy cubic Bi-pyrochlore oxides were constructed by magnetic 3d -cations entropy engineering in a Bi 1.68 MNb 1.32 O 6 O' (M = equimolar 3d -ions) system and successfully synthesized using a modified sol-gel combustion technology. The pyrochlore-type structure and designed stoichiometric ratio were carefully confirmed by utilizing X-ray diffraction and electron microtechniques, and effects of high-entropy engineering on microstructure, optical adsorption and catalytic activity were studied in detail. Significantly, as increasing the entropy-level, evolutions of pyrochlore-phase structure and morphology were clearly observed from big cube-grains with large lattice volume towards relatively smaller polyhedral-crystals with decreased lattice volume. What is more, high-entropy by adopting multi-type 3d -cations not only remain stable up to 1000 °C, but also induce an obvious enhancement of optical absorption from visible-light to near-infrared-light, ascribed to d -orbital energy splitting and localized d-d transitions, thereby achieving a superior near-infrared photoresponse in neutral electrolytes under laser irradiation. For electrocatalysis, such high-entropy pyrochlore-catalysts can also exhibit excellent oxygen evolution reaction activities, with a low overpotential <330 mV and a small Tafel slope <50 mV/dec, even their activities are comparable to the 3d -metal-based catalysts. [ABSTRACT FROM AUTHOR]
ISSN:02728842
DOI:10.1016/j.ceramint.2026.04.264