التفاصيل البيبلوغرافية
| العنوان: |
Supported Au single atoms and nanoparticles on MoS2 for highly selective CO2-to-CH3COOH photoreduction. |
| المؤلفون: |
Chen, Cai, Ye, Chunyin, Zhao, Xinglei, Zhang, Yizhen, Li, Ruilong, Zhang, Qun, Zhang, Hui, Wu, Yuen |
| المصدر: |
Nature Communications; 9/7/2024, Vol. 15 Issue 1, p1-11, 11p |
| مصطلحات موضوعية: |
ELECTRON relaxation time, GOLD nanoparticles, ENERGY levels (Quantum mechanics), NEAR infrared radiation, MOLECULAR orbitals |
| مستخلص: |
Effectively controlling the selective conversion of CO2 photoreduction to C2 products presents a significant challenge. Here, we develop a heterojunction photocatalyst by controllably implanting Au nanoparticles and single atoms into unsaturated Mo atoms of edge-rich MoS2, denoted as Aun/Au1-CMS. Photoreduction of CO2 results in the production of CH3COOH with a selectivity of 86.4%, which represents a 6.4-fold increase compared to samples lacking single atoms, and the overall selectivity for C2 products is 95.1%. Furthermore, the yield of CH3COOH is 22.4 times higher compared to samples containing single atoms and without nanoparticles. Optical experiments demonstrate that the single atoms domains can effectively capture photoexcited electrons by the Au nanoparticles, or the local electric field generated by the nanoparticles promotes the transfer of photogenerated electrons in MoS2 to Au single atoms, prolonging the relaxation time of photogenerated electrons. Mechanistic investigations reveal that the orbital coupling of Au5d and Mo4d strengthens the oxygen affinity of Mo and carbon affinity of Au. The hybridized orbitals reduce energy splitting levels of CO molecular orbitals, aiding C–C coupling. Moreover, the Mo−Au dual-site stabilize the crucial oxygen-associated intermediate *CH2CO, thereby enhancing the selectivity towards CH3COOH. The cross-scale heterojunctions provide an effective strategy to simultaneously address the kinetical and thermodynamical limitations of CO2-to-CH3COOH conversion. Reducing CO2 to CH3COOH using visible and near-infrared light is challenging. Here, Wu and Zhang et al. incorporate Au nanoparticles and single atoms into Mo-edge-rich MoS2 to provide a pathway to overcome limitations and boost productivity. [ABSTRACT FROM AUTHOR] |
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| قاعدة البيانات: |
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