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Conjugated Microporous Polymer Catalysts with Well-Defined Molecular Metal Sites and Tunable Coordination Environments for Electrocatalytic Synthesis of C-N Coupling Compounds

Project description

New catalysts with precise structures for efficient CO2–nitrate conversion

Reducing CO2 emissions while converting it into valuable chemicals is a key step towards achieving carbon neutrality. With the support of the Marie Skłodowska-Curie Actions programme, the COMPACT-CN project will explore a new approach combining CO2 with nitrate to produce valuable nitrogen-containing compounds like amides and amines. Existing catalysts often possess poorly defined structures, which limits their efficiency and selectivity. To this end, COMPACT-CN will design metalated conjugated microporous polymers with well-defined architectures. These materials are engineered with precision to improve reaction efficiency and selectivity. By studying how these catalysts work at a molecular level, COMPACT-CN will open new doors for sustainable CO2 conversion processes.

Objective

The electrochemical CO2 reduction reaction (CO2RR) effectively converts and fixes CO2 but currently produces a limited range of short-chain carbon-hydrogen-oxygen compounds in aqueous electrolytes. By using small molecules like nitrate as co-reactants, CO2RR can yield valuable C-N coupling products (e.g. amide, amine), expanding its applications. Although typical metal-based, single-atom, or dual-atomic-site catalysts have been reported to catalyze electrochemical C-N coupling, their inherent structural heterogeneity, arising from defect states, high-temperature pyrolysis, non-uniform support materials, and unclear active site structures/environment, limits their selectivity, energy efficiency, and utility in mechanistic studies. To progress, a well-defined system with definite coordination environments to form structurally defined active sites is crucial for advancing electrochemical C-N coupling reactions. The COMPACT-CN project aims to develop metalated conjugated microporous polymer (M-CMP) electrocatalysts with uniform molecular metal sites to explore catalytic selectivity and kinetics for C-N coupling reactions. The key objectives are: 1) to synthesize and characterize structurally engineered M-CMPs with high performance and selectivity for C-N coupling; 2) to investigate reaction mechanisms using advanced electrochemical and in situ surface-sensitive techniques; and 3) to establish the relationship between structural properties (metal site-spacing, proton relay distance, and electron push-pull effects) and C-N coupling performance. COMPACT-CN's achievements will deepen molecular-level insights into electrochemical C-N bond coupling mechanisms and structure-function relationships in catalysts, advancing CO2/NOx conversion techniques. These approaches are essential for achieving carbon neutrality by reducing CO2/NOx emissions while converting them into valuable chemicals, which are highly attractive for both academic research and industrial applications.

Fields of science (EuroSciVoc)

Keywords

Programme(s)

Topic(s)

Funding Scheme

HORIZON-TMA-MSCA-PF-EF - HORIZON TMA MSCA Postdoctoral Fellowships - European Fellowships

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Call for proposal

(opens in new window) HORIZON-MSCA-2024-PF-01

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Coordinator

UNIVERSITEIT LEIDEN
Net EU contribution
€ 232 916,16
Address
RAPENBURG 70
2311 EZ Leiden
Netherlands
Activity type
Higher or Secondary Education Establishments
Links
Total cost
No data