Synthesis of Pyrazinesfrom Biomass-Derived VicinalDiols Using Ammonia over Heterogeneous Pt/CeO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> Catalysts

One-pot amination coupling of vicinal diols toward the synthesis of pyrazines provides an efficient and economically viable route to access N-heterocycles from biomass, yet the current methodology relies on a fragile homogeneous catalyst system, which limits the sustainability of the chemistry. In this work, we developed a highly efficient heterogeneous catalyst 0.8Pt/13CeO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> which afforded diverse substituted pyrazines from readily available vicinal diols and ammonia with a yield up to 94% under mild reaction conditions and could be reused at least 6 times without obvious activity decay. Compared to the Pt/Al<sub>2</sub>O<sub>3</sub> catalyst, the 0.8Pt/13CeO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> catalyst exhibited a 30-fold faster conversion rate of diols and an increased pyrazine selectivity from 48% to 79%. Characterizations revealed that doped CeO<sub>2</sub> improved the dispersion of Pt, increased the electron density on the Pt sites, optimized the acid/basic property of the catalyst, and enhanced the adsorption strength and dehydrogenation ability of diols. All these features contributed to the increased activity and selectivity.

Publication Details

Journal
Figshare
Published
2025-03-21
DOI
https://doi.org/10.1021/acscatal.5c00372.s001
Primary Topic
Catalysis for Biomass Conversion
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article
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Synthesis of Pyrazinesfrom Biomass-Derived VicinalDiols Using Ammonia over Heterogeneous Pt/CeO2/Al2O3 Catalysts

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Catalysis for Biomass Conversion
article

Synthesis of Pyrazinesfrom Biomass-Derived VicinalDiols Using Ammonia over Heterogeneous Pt/CeO2/Al2O3 Catalysts

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Abstract

One-pot amination coupling of vicinal diols toward the synthesis of pyrazines provides an efficient and economically viable route to access N-heterocycles from biomass, yet the current methodology relies on a fragile homogeneous catalyst system, which limits the sustainability of the chemistry. In this work, we developed a highly efficient heterogeneous catalyst 0.8Pt/13CeO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> which afforded diverse substituted pyrazines from readily available vicinal diols and ammonia with a yield up to 94% under mild reaction conditions and could be reused at least 6 times without obvious activity decay. Compared to the Pt/Al<sub>2</sub>O<sub>3</sub> catalyst, the 0.8Pt/13CeO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> catalyst exhibited a 30-fold faster conversion rate of diols and an increased pyrazine selectivity from 48% to 79%. Characterizations revealed that doped CeO<sub>2</sub> improved the dispersion of Pt, increased the electron density on the Pt sites, optimized the acid/basic property of the catalyst, and enhanced the adsorption strength and dehydrogenation ability of diols. All these features contributed to the increased activity and selectivity.

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Synthesis of Pyrazinesfrom Biomass-Derived VicinalDiols Using Ammonia over Heterogeneous Pt/CeO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> Catalysts · Figshare (2025) | TGRS Research Map | TGRS