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Decoding the entropy-stabilized matrix of high-entropy layered double hydroxides: Harnessing strain dynamics for peroxymonosulfate activation and tetracycline degradation
Citation
Ma, R., Song, J., Ding, H., Han, Q., Tang, X., Lv, F., Wen, S., Yin, J., & Ang, E. H. (2024). Decoding the entropy-stabilized matrix of high-entropy layered double hydroxides: Harnessing strain dynamics for peroxymonosulfate activation and tetracycline degradation. Journal of Colloid and Interface Science, 680(Part B), 676-688. https://doi.org/10.1016/j.jcis.2024.11.123
Author
MA, Rongyao
•
Song, Jianhua
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Ding, Huiwei
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Han, Qiaofeng
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Tang, Xin
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Lv, Fujian
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Wen, Shizheng
•
Yin, Jingzhou
•
Abstract
The current understanding of the mechanism of high-entropy layered double hydroxide (LDH) on enhancing the efficiency of activating peroxymonosulfate (PMS) remains limited. This work reveals that a strong strain effect, driven by high entropy, modulates the structure of FeCoNiCuZn-LDH (HE-LDH) as evidenced by geometric phase analysis (GPA) and density functional theory (DFT) calculations. Compared to FeCoNiZn-LDH and FeCoNi-LDH with weaker strain effects, the high entropy-driven strain effect in HE-LDH shortens metal–oxygen-hydrogen (Msingle bondOsingle bondH) bond lengths, allows system to be in a constant steady state during catalysis, reduces the leaching of active M−OH sites, and enhances the adsorption capacity of these sites and the excess strain strength of the interfacial stretches the IO-O of the PMS, facilitates reactive oxygen species (·OH, SO4·−, 1O2 and O2·-) generation, and thereby improving the efficiency of PMS in degrading tetracycline (TC). Consequently, HE-LDH demonstrated a 90% TC degradation within 3 min, maintained over 92% TC removal across a wide pH range (3–11), and achieved over 90% degradation performance after 6 cycles. This study reports the first use of high-entropy LDH material as a non-homogeneous catalyst and provides insights into the extremely different catalytic behaviors of high entropy mechanisms for the activation of PMS.
Publisher
Elsevier
Journal
Journal of Colloid and Interface Science
Project
RP 1/22 EAH
Grant ID
51772155
HAQ202301
2023J1036
Funding Agency
National Natural Science Foundation of China
Key R&D Projects of Huai’an City
Scientific Research Fund Project of the Yunnan Provincial Department of Education
Ministry of Education, Singapore