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Synergistic Interplay of Ni Single Atoms and Neighboring Mn2 Dual Atoms Enabling Selective Photocatalytic Reduction of CO2 to Propane
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DOI：10.1002/anie.202521193.png)
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Abstract
En 中文
The photocatalytic conversion of CO2 and H2O into long carbon chain products (Cn, n >= 3) presents a sustainable strategy for synthesizing high-value fuels and chemicals. However, the synthesis of long carbon chain products under mild conditions still faces great challenges, largely due to sluggish multi-electron/proton transfer kinetics and the thermodynamically unfavorable C1-C1 and C1-C2 coupling processes. In this study, we developed tri-metal active sites composed of Ni single atoms and Mn2 dual atoms anchored on NH2-MIL-125(Ti) (Ni1/Mn2-MIL) for synergistic photocatalytic C3H8 production. The synthesized Ni1/Mn2-MIL catalyst achieved efficient CO2 photoreduction (CO2PR) in pure water, yielding 32.2 mu mol g-1 h-1 of C3H8 with 81.3% electron-based selectivity, significantly outperforming Ni1-MIL and Mn2-MIL. Remarkably, the catalyst exhibited exceptional stability over 50 cycles without degradation. Integrated experimental and theoretical investigations revealed that the Ni1 site activates CO2 to form CO, while the adjacent Mn2 site promotes the formation of *COCHO intermediates. Strong electronic interactions between Ni1 and Mn2 create charge-polarized active sites, which mitigate electrostatic repulsion between C1 and C2 intermediates, thereby promoting C-C coupling and subsequent formation of the *CH2OCOCO intermediates. Consequently, both the selectivity and catalytic efficiency toward C3H8 production are significantly enhanced.
Keywords:
CO2 reduction
Multisite cooperation
Photocatalysis
Propane
Single-atom catalysts
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16.9
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5.6W
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53.0W
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