Polyarylimide-Based COF/MOF Nanoparticle Hybrids for CO₂ Conversion, Hydrogen Generation, and Organic Pollutant Degradation

Abstract

The continuous rise in atmospheric CO 2 concentration, overconsumption of energy resources, and release of extraordinary organic pollutants are challenging issues of the modern era. Catalytic technology offers a promising solution to tackle these energy and environmental challenges in parallel by facilitating highly effective and sustainable processes. Herein, we report the fabrication of a series of different nature polyarylimide (PAI)-based covalent−organic frameworks (COFs) via the polycondensation reaction by altering linkers, organic solvents, and other experimental conditions. To optimize their catalytic performance, the resultant PAI-COFs were further decorated with metal−organic frameworks (ZIF-67). The decoration of COF4 with ZIF-67 led to adjusted bandgaps, created an active site, enhanced charge separation and migration of photoexcited electron−hole (e−h) pairs, extended the light absorption to the visible region, and also facilitated the transferring of electrons between the COFs and MOFs via the photoelectron modulation approach. Based on our findings, it is confirmed that COF4 and ZIF-67 (MOFs) are the optimal catalysts compared to the other COFs (COF1, COF2, and COF3) and MOFs (ZIF-8). Interestingly, compared to the pristine COF4, the 5ZIF-67/COF4 nanohybrid revealed ∼8-fold and ∼5.3-fold for CO 2 conversion, direct CO 2 capturing, and photoelectrochemical CO 2 conversion with a faradaic efficiency of 50%. Likewise, the as-fabricated catalyst also exhibits exceptional activities for photocatalytic hydrogen production and pollutant oxidation. Ultimately, this work will provide a roadmap for the design and fabrication of COF-based nanohybrids for energy and environmental applications.

Biomass-Derived Carbon Materials for Advanced Metal-Ion Hybrid Supercapacitors: A Step Towards More Sustainable Energy

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Metal/Covalent Organic Framework Encapsulated Lead-Free Halide Perovskite Hybrid Nanocatalysts: Multifunctional Applications, Design, Recent Trends, Challenges, and Prospects

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Ultrathin and Self-Supporting MOF/COF-Based Composite Membranes for Hydrogen Separation and Purification from Coke Oven Gas

“…However, they are still up against several problems, such as complex preparation processes, insufficient separation efficiency, and film stability, so it is difficult to solve these deficiencies solely by relying on a single MOF or COF. Benefiting from the diversity of the constituent units and easy postsynthetic modification of MOFs or COFs, MOF/COF-based composite materials have emerged as a new choice. − Generally, the unit cell size of MOFs falls in a range of several nanometers (such as the cubic cell dimension of ZIF-8 and ZIF-67 is a = b = c = ∼1.7 nm), which is close to the inner pore width of COFs. , …”