Catalytic Synthesis of Formamides by Integrating CO2 Capture and Morpholine Formylation on Supported Iridium Catalyst

Danyang Cheng; Meng Wang; Lipeng Tang; Zirui Gao; Xuetao Qin; Yongjun Gao; Dequan Xiao; Wu Zhou; Ding Ma

doi:10.1002/anie.202202654

Catalytic Synthesis of Formamides by Integrating CO₂ Capture and Morpholine Formylation on Supported Iridium Catalyst

Angew Chem Int Ed Engl. 2022 Jun 27;61(26):e202202654. doi: 10.1002/anie.202202654. Epub 2022 May 3.

Authors

Danyang Cheng¹, Meng Wang¹, Lipeng Tang¹, Zirui Gao¹, Xuetao Qin¹, Yongjun Gao², Dequan Xiao³, Wu Zhou⁴, Ding Ma¹

Affiliations

¹ Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.
² Key Laboratory of Analytical Science and Technology of Hebei Province, College of Chemistry and Environmental Science, Hebei University, Baoding, 071002, P. R. China.
³ Center for Integrative Materials Discovery, Department of Chemistry and Chemical and Biomedical Engineering, University of New Haven, West Haven, CT 06516, USA.
⁴ School of Physical Sciences and CAS Key Laboratory of Vacuum Sciences, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.

PMID: 35394704
DOI: 10.1002/anie.202202654

Abstract

Herein we report an efficient and recyclable catalytic system for tandem CO₂ capture and N-formylation to value-added chemicals. CO₂ is apt to be captured by morpholine solution, while a highly efficient heterogeneous catalyst, isolated iridium atoms supported over nanadiamond/graphene, is discovered to be highly reactive for the formylation of morpholine, leading to the formation of N-formylmorpholine with excellent productivity (with a turnover number of 5 120 000 in a single batch reaction) and selectivity (>99 %). In addition, the CO₂ captured by morpholine under atmospheric conditions can be converted to N-formylmorpholine with decent conversion (51 %), which realizes the integration of CO₂ capture and conversion to value-added chemicals.

Keywords: CO Poison Effect; CO2 Capture; CO2 Utilization; Isolated Ir/ND@G; Morpholine Formylation.

Abstract

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