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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.

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Topic(s)

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Funding Scheme

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

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Call for proposal

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

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Coordinator

UNIVERSITEIT LEIDEN
Net EU contribution

Net EU financial contribution. The sum of money that the participant receives, deducted by the EU contribution to its linked third party. It considers the distribution of the EU financial contribution between direct beneficiaries of the project and other types of participants, like third-party participants.

€ 232 916,16
Address
RAPENBURG 70
2311 EZ Leiden
Netherlands

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Activity type
Higher or Secondary Education Establishments
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Total cost

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