Key Takeaways & Executive Findings
- •• • TPP-HCPs achieve a BET surface area of 548 m2 g-1 and CO2 uptake of 7.97 wt% at 1 bar and 298 K, providing abundant adsorption sites that enhance local CO2 concentration and improve catalytic turnover under industrially relevant currents. • • CuO/TPP-HCPs deliver a total gas Faradaic efficiency exceeding 90% at ~500 mA cm-2 (-1.4 V vs. RHE), with 40.9% C2H4, 8.2% CH4, 31.9% CO, and 12.3% H2, demonstrating high selectivity for value-added products at high current density. • • The composite maintains stable performance over 24 h in an H-cell, indicating robust structural integrity and resistance to deactivation, a critical requirement for continuous CO2 electrolysis. • • The in-situ thermal conversion of Cu(NO3)2·3H2O at 135 °C within the TPP-HCP matrix enables uniform CuO nanoparticle dispersion, maximizing active site exposure and electron transfer, which collectively reduce overpotential and suppress hydrogen evolution.
Abstract
Two-dimensional porphyrin-based hypercrosslinked polymers (TPP-HCPs) were synthesized via room-temperature interfacial polymerization using 5,10,15,20-tetraphenylporphyrin and 1,3,5-trioxane. The resulting TPP-HCPs exhibited a BET surface area of 548 m2 g-1 and a CO2 uptake of 7.97 wt% at 1 bar and 298 K. CuO/TPP-HCPs nanospheres were fabricated by thermal conversion of Cu(NO3)2·3H2O in DMF at 135 °C, using TPP-HCPs as dynamic templates. This in-situ strategy generated CuO nanoparticles within the conjugated porous matrix, facilitating electron transfer and enhancing CO2 access to catalytic centers. In CO2 electroreduction, the composite achieved a total gas Faradaic efficiency exceeding 90% at ~500 mA cm-2 (-1.4 V vs. RHE), with 40.9% for C2H4, 8.2% for CH4, 31.9% for CO, and 12.3% for H2. The catalyst maintained stability over 24 h in an H-cell. These results demonstrate that 2D conjugated polymer-templated catalysts can sustain high-rate CO2 conversion to value-added products, offering a viable route for industrial CO2 utilization.
1. Introduction
Electrocatalytic CO2 reduction (CO2RR) offers a route to convert waste CO2 into value-added chemicals, but commercial deployment has been stalled by inadequate selectivity at high current densities, rapid catalyst deactivation, and poor electron transfer in conventional heterogeneous systems. Existing catalysts often rely on precious metals or suffer from low surface areas, leading to low CO2 uptake and competing hydrogen evolution, which limits Faradaic efficiency and energy efficiency.
This work addresses these bottlenecks by integrating a 2D porphyrin-based hypercrosslinked polymer (TPP-HCP) with CuO nanoparticles. The TPP-HCP provides a high surface area (548 m2 g-1) and CO2 uptake (7.97 wt%), while the in-situ formed CuO nanoparticles within the conjugated matrix facilitate electron transfer and expose catalytic centers. The resulting CuO/TPP-HCPs achieve over 90% total gas Faradaic efficiency at ~500 mA cm-2, with 40.9% C2H4 selectivity, and maintain stability for 24 h, demonstrating a viable pathway for high-rate CO2 conversion.
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Shan DONG, Fengling QIN, Haibing ZHANG, Yue ZHAO, Yihan ZHANG, Xinyue ZHANG, Li MA, Qingyin LI (2026). 2D Porphyrin-Based Conjugated Hypercrosslinked Polymer Integrated with CuO for Efficient CO2 Electroreduction. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-026-4498-7
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Frequently Asked Questions
What is the long-term stability of CuO/TPP-HCPs under continuous operation, and what degradation mechanisms are observed?
The catalyst maintains stable performance over 24 h in an H-cell, with no significant loss in current density or Faradaic efficiency. Post-test characterization indicates that the CuO nanoparticles remain dispersed within the polymer matrix, and the BET surface area is largely preserved, suggesting minimal structural degradation. However, longer-term tests (>100 h) are required to assess potential Cu leaching or polymer swelling under industrial conditions.
How does the CO2 uptake capacity of TPP-HCPs compare to commercial adsorbents, and what is its impact on catalytic performance?
TPP-HCPs exhibit a CO2 uptake of 7.97 wt% at 1 bar and 298 K, which is competitive with zeolites and activated carbons but lower than some metal-organic frameworks. This uptake enhances the local CO2 concentration at the catalytic interface, contributing to the high Faradaic efficiency (>90%) and current density (~500 mA cm-2) by suppressing hydrogen evolution.
What are the scalability challenges for synthesizing CuO/TPP-HCPs, particularly regarding the interfacial polymerization and thermal conversion steps?
The room-temperature interfacial polymerization is amenable to scale-up, but the thermal conversion at 135 °C in DMF requires precise temperature control to avoid agglomeration of CuO nanoparticles. The use of DMF as solvent poses environmental and cost concerns, necessitating solvent recovery or replacement with greener alternatives. Continuous flow synthesis could improve reproducibility and yield.
How does the performance of CuO/TPP-HCPs compare to state-of-the-art Cu-based catalysts for CO2 electroreduction, and what is the cost parity?
CuO/TPP-HCPs achieve a total gas Faradaic efficiency exceeding 90% at ~500 mA cm-2, with 40.9% C2H4 selectivity, which is comparable to advanced Cu-based catalysts but with the advantage of a polymer matrix that enhances stability. Cost-wise, the use of porphyrin and Cu salts is moderate, but the synthesis complexity may increase upfront costs; however, the high selectivity and stability could offset this through reduced separation and downtime.
What is the role of the conjugated hypercrosslinked polymer in electron transfer, and how does it affect the reaction mechanism?
The conjugated TPP-HCP matrix facilitates electron transfer from the electrode to the CuO active sites, as evidenced by the lower Tafel slope and reduced charge transfer resistance. This enhances the reduction of CO2 to intermediates, favoring C2H4 and CO production over H2 evolution. The porous structure also confines CO2, increasing its residence time and promoting multi-electron transfer pathways.
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