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• W2808205168 abstract "The active intermediate responsible for pyridine (Py)-catalyzed reduction of CO2 on a p-GaP photoelectrode is currently under debate. Exploration of the proposed intermediates’ available pathways for further reaction may yield a deeper understanding of the CO2 reduction mechanism that will be essential to designing better cocatalysts in such photoelectrochemical systems. Adsorbed 2-pyridinide (2-PyH–*) was recently proposed by Carter and co-workers to be an intermediate that facilitates hydride transfer (HT) to CO2 to produce formate. However, the lifetime of 2-PyH–*, most likely controlled by the rate of 2-PyH–* protonation to form adsorbed dihydropyridine (DHP*), is still in question. In this work, we provide evidence for the transient existence of 2-PyH–* on a p-GaP surface by comparing the activation energy for HT to CO2 to those predicted for 2-PyH–* being protonated to form either DHP* or Py* + H2 via a hydrogen evolution reaction (HER). We predict that 2-PyH–* situated next to an adjacent surface hydroxide (OH–*) will be the most effective intermediate leading to CO2 reduction on p-GaP. Predicted high barriers of HER (via either 2-PyH–* or H–*) also explain the high selectivity toward CO2 reduction observed in experiments." @default.
• W2808205168 created "2018-06-21" @default.
• W2808205168 creator A5034715756 @default.
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• W2808205168 date "2018-06-14" @default.
• W2808205168 modified "2023-10-17" @default.
• W2808205168 title "2-Pyridinide as an Active Catalytic Intermediate for CO₂ Reduction on p-GaP Photoelectrodes: Lifetime and Selectivity" @default.
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• W2808205168 doi "https://doi.org/10.1021/jacs.8b03774" @default.
• W2808205168 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/29901999" @default.
• W2808205168 hasPublicationYear "2018" @default.
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