AI Article Synopsis
- - A new concentrated solar-driven system enhances CO reduction efficiency by combining a dual-metal single-atom catalyst (DSAC) with nickel and iron sites, even under low sunlight conditions.
- - The (Ni, Fe)-N-C DSAC outperforms existing catalysts, achieving significant improvements in gas-solid CO reduction rates, producing CO, methane (CH₄), and methanol (CH₃OH) at rates 1.7 to 1.23 times higher than predecessor catalysts.
- - The research highlights the importance of electronic interactions between nickel and iron atoms, which optimize the energy barriers in the reaction, creating efficient pathways for solar-driven photothermal CO conversion.
Article Abstract
Solar-to-chemical energy conversion under weak solar irradiation is generally difficult to meet the heat demand of CO reduction. Herein, a new concentrated solar-driven photothermal system coupling a dual-metal single-atom catalyst (DSAC) with adjacent Ni-N and Fe-N pair sites is designed for boosting gas-solid CO reduction with H O under simulated solar irradiation, even under ambient sunlight. As expected, the (Ni, Fe)-N-C DSAC exhibits a superior photothermal catalytic performance for CO reduction to CO (86.16 μmol g h ), CH (135.35 μmol g h ) and CH OH (59.81 μmol g h ), which are equivalent to 1.70-fold, 1.27-fold and 1.23-fold higher than those of the Fe-N-C catalyst, respectively. Based on theoretical simulations, the Fermi level and d-band center of Fe atom is efficiently regulated in non-interacting Ni and Fe dual-atom pair sites with electronic interaction through electron orbital hybridization on (Ni, Fe)-N-C DSAC. Crucially, the distance between adjacent Ni and Fe atoms of the Ni-N-N-Fe configuration means that the additional Ni atom as a new active site contributes to the main *COOH and *HCO dissociation to optimize the corresponding energy barriers in the reaction process, leading to specific dual reaction pathways (COOH and HCO pathways) for solar-driven photothermal CO reduction to initial CO production.
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| http://dx.doi.org/10.1002/anie.202313868 | DOI Listing |
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