Citation: Xiaohong Li, Limin Jin, Haihui Yu, Yuteng Zhang, Haifeng Zhang, Yanbiao Liu. Bioinspired high-entropy metal-organic frameworks towards boosted CO₂ photoconversion[J]. Chinese Chemical Letters, ;2026, 37(4): 111626. doi: 10.1016/j.cclet.2025.111626 shu

Bioinspired high-entropy metal-organic frameworks towards boosted CO₂ photoconversion

Xiaohong Li ^a ,
Limin Jin ^b ,
Haihui Yu ^a ,
Yuteng Zhang ^a ,
Haifeng Zhang ^{a, *,} ,
Yanbiao Liu ^{c, *,}

a.
School of Chemical Engineering, Northeast Electric Power University, Jilin 132012, China
b.
School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, China
c.
School of Environmental Science and Technology, Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), Dalian University of Technology, Dalian 116024, China

zhftju@163.com

yanbiaoliu@dlut.edu.cn

Received Date: 21 March 2025
Revised Date: 16 June 2025
Accepted Date: 22 July 2025
Available Online: 23 July 2025

Figures(5)

Sustainable photochemical CO₂ conversion represents a promising strategy for mitigating excess CO₂ emissions and achieving "carbon neutrality". The development of advanced catalysts with an abundance of active sites and efficient separation of photo-generated charge carriers remains a significant challenge. Here, we present a high-entropy (HE) photocatalyst by integrating five metals into Prussian blue (PB) to afford K_x(MnFeCoNiCu)[Fe(CN)₆] (HE-PBA) which exhibits a high concentration of active centers and rapid electron transfer, enabling superior CO₂-to-CO photoreduction performance. The HE-PBA composite catalyst delivered a high CO yield (up to 1220.5 µmol g^-1 h^-1), achieving near 100% product selectivity. A mechanistic analysis has revealed strong coupling and overlapping multi-atomic orbitals, which facilitates local electron redistribution and a readjustment of electron density. This effect serves to generate abundant reactive sites with CO₂ interactions that facilitate C-O bond activation. Additionally, an efficient electron transfer driven by the disparity in metal electronegativity inhibits unwanted recombination of electron-hole pairs. More significantly, the photoelectrons migrate and accumulate on the HE-PBA surface, exhibiting extended long lifetimes and robust reduction ability. The findings of this study provide important insights that can contribute to the development of high-entropy materials rich in transition metals with far-ranging potential applications.
- Photocatalytic CO₂ reaction,
- High-entropy catalyst,
- Metal-organic frameworks,
- Charge separation
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沈阳化工大学材料科学与工程学院沈阳 110142

Bioinspired high-entropy metal-organic frameworks towards boosted CO2 photoconversion

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通讯作者: 陈斌, bchen63@163.com

Bioinspired high-entropy metal-organic frameworks towards boosted CO₂ photoconversion