Bidentate-coordinated Mn/C catalyst for high-efficiency aerobic oxidation of cyclohexanone to adipic acid

Adipic acid (AA), a crucial industrial dicarboxylic acid, faces sustainability challenges due to its conventional nitric acid-based production process that emits significant amounts of N 2 O greenhouse gas. This study introduces a novel carbon-supported catalyst for oxidative cleavage of cyclohexanone under O 2 atmosphere, achieving 92.4 % AA selectivity. The catalyst, synthesized via a solution-based precursor followed by high-temperature carbonization, immobilizes manganese in a bidentate coordination on the carbon support. It exhibits remarkable stability over 10 cycles without metal leaching or performance decay. The effects of different carbon sources and transition metals on the catalyst were systematically investigated within this methodology, and comprehensive characterization using FT-IR, Py-IR, Raman spectra, ICP, XRD, XPS, SEM, TEM and BET was conducted. Analysis of the reaction process enabled proposal of a plausible mechanism. This work establishes a green AA synthesis route while advancing carbon-supported catalyst design through simplified, cost-effective strategies with enhanced stability. • The catalyst anchors active sites via bidentate chelation. • This method surpasses the MOF carbonization method in simplicity and economy. • The oxidation of cyclohexanone with O₂ achieved 92.4 % AA selectivity. • The catalyst retains over 95 % of its activity after 10 cycles. • A radical chain autoxidation mechanism is proposed.

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Publication Details

Journal
Applied Catalysis O Open
Published
2025-06-17
DOI
https://doi.org/10.1016/j.apcato.2025.207060
Primary Topic
Catalytic Processes in Materials Science
Type
article
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article

Bidentate-coordinated Mn/C catalyst for high-efficiency aerobic oxidation of cyclohexanone to adipic acid

Tun Wu, Liqiu Mao, Haoyu Peng, Wenzhou Zhong et al.
Applied Catalysis O Open
Catalytic Processes in Materials Science
article

Bidentate-coordinated Mn/C catalyst for high-efficiency aerobic oxidation of cyclohexanone to adipic acid

Tun Wu, Liqiu Mao, Haoyu Peng, Wenzhou Zhong, Yani Liu, X. Tu
article en

Abstract

Adipic acid (AA), a crucial industrial dicarboxylic acid, faces sustainability challenges due to its conventional nitric acid-based production process that emits significant amounts of N 2 O greenhouse gas. This study introduces a novel carbon-supported catalyst for oxidative cleavage of cyclohexanone under O 2 atmosphere, achieving 92.4 % AA selectivity. The catalyst, synthesized via a solution-based precursor followed by high-temperature carbonization, immobilizes manganese in a bidentate coordination on the carbon support. It exhibits remarkable stability over 10 cycles without metal leaching or performance decay. The effects of different carbon sources and transition metals on the catalyst were systematically investigated within this methodology, and comprehensive characterization using FT-IR, Py-IR, Raman spectra, ICP, XRD, XPS, SEM, TEM and BET was conducted. Analysis of the reaction process enabled proposal of a plausible mechanism. This work establishes a green AA synthesis route while advancing carbon-supported catalyst design through simplified, cost-effective strategies with enhanced stability. • The catalyst anchors active sites via bidentate chelation. • This method surpasses the MOF carbonization method in simplicity and economy. • The oxidation of cyclohexanone with O₂ achieved 92.4 % AA selectivity. • The catalyst retains over 95 % of its activity after 10 cycles. • A radical chain autoxidation mechanism is proposed.

Applied Catalysis O OpenVol. 206
Hunan Normal University (CN)
Openalex Percentile: Top 90%
Catalytic Processes in Materials Science
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