4.8 Article

Syngas Instead of Hydrogen Gas as a Reducing Agent-A Strategy To Improve the Selectivity and Efficiency of Organometallic Catalysts

Journal

ACS CATALYSIS
Volume 12, Issue 9, Pages 5145-5154

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c01000

Keywords

syngas; reduction; reductive amination; reductive alkylation; reductive esteri fi cation

Funding

  1. Russian Science Foundation [19-73-20212]
  2. Ministry of Science and Higher Education of the Russian Federation
  3. Russian Science Foundation [19-73-20212] Funding Source: Russian Science Foundation

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This study demonstrates that the usage of syngas as a reducing agent can lead to more efficient and selective catalytic reduction reactions. Based on control experiments, a plausible mechanism for the superior performance of syngas is proposed. This approach is successfully applied to three reactions, achieving high catalyst turnover numbers and improved selectivity and functional group compatibility compared to hydrogen gas.
Catalytic reduction reactions play a major role in modern chemistry and are often based on hydrogen gas as a reducing agent. However, the high reactivity of hydrogen is often accompanied by low selectivity on the simple catalysts. Herein, we showed that the usage of syngas as a reducing agent can be a more efficient and selective strategy. Based on control experiments, a plausible mechanism was proposed to explain the superior performance of syngas. The versatility of this approach was demonstrated by successful application to three reactions using tion, and the tandem CH-reductive alkylation-hydrolysis-decarboxylation. Catalyst turnover numbers up to 30,000 were achieved. Moreover, the developed strategy showed improved selectivity and functional group compatibility as compared to the use of hydrogen gas.

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