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Table · dataset · 2026

Unlocking Water as Docking Sites in Covalent Organic Frameworks for Enhanced Physisorptive Carbon Capture under Wet Conditions

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The physisorptive CO<sub>2</sub> capture process frequently faces the challenge of competing with moisture adsorption.

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Incorporating strong nucleophiles into porous materials can circumvent this issue by forming bicarbonate in the presence of moisture. However, the moisture-enhanced carbon capture (MECC) in physisorptive systems is still rarely reported.

Herein, we present a physisorptive MECC capable of operating at a wide range of relative humidity (RH), employing newly developed covalent organic frameworks (COFs) with Brønsted-acidic squaramide as linkage. Specifically, the squaramide linkage and a specific pore size jointly disrupt hydrogen bonds (HBs) in water molecules, thereby converting them into effective docking sites for CO<sub>2</sub> adsorption within the amphiphilic pores.

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Comprehensive column breakthrough experiments highlight a substantial enhancement in CO<sub>2</sub> uptake capacity in the squaramide-linked COFs in the presence of moisture (up to 75% RH) compared to dry conditions. The distinctive adsorption mechanism is further interpreted through <i>in situ</i> diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), solid-state <sup>1</sup>H magic angle spinning nuclear magnetic resonance (ss <sup>1</sup>H MAS NMR), dielectric analysis, and sorption simulation, demonstrating that the water around the squaramide linkage could play a crucial role in enhancing CO<sub>2</sub> adsorption in the presence of moisture.

This work provides new insight into converting water as an additional sorption site and a strategy for addressing the influence of moisture in physisorptive carbon capture processes.

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Magnetic resonance imaging 65% · Simulation 75%

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