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Improving CO₂ photoconversion with ionic liquid and Co single atoms.

ABSTRACT: Photocatalytic CO₂ conversion promises an ideal route to store solar energy into chemical bonds. However, sluggish electron kinetics and unfavorable product selectivity remain unresolved challenges. Here, an ionic liquid, 1-ethyl-3-methylimidazolium tetrafluoroborate, and borate-anchored Co single atoms were separately loaded on ultrathin g-C₃N₄ nanosheets. The optimized nanocomposite photocatalyst produces CO and CH₄ from CO₂ and water under UV-vis light irradiation, exhibiting a 42-fold photoactivity enhancement compared with g-C₃N₄ and nearly 100% selectivity towards CO₂ reduction. Experimental and theoretical results reveal that the ionic liquid extracts electrons and facilitates CO₂ reduction, whereas Co single atoms trap holes and catalyze water oxidation. More importantly, the maximum electron transfer efficiency for CO₂ photoreduction, as measured with in-situ μs-transient absorption spectroscopy, is found to be 35.3%, owing to the combined effect of the ionic liquid and Co single atoms. This work offers a feasible strategy for efficiently converting CO₂ to valuable chemicals.

SUBMITTER: Liu Y

PROVIDER: S-EPMC10020152 | biostudies-literature | 2023 Mar

REPOSITORIES: biostudies-literature

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Improving CO2 photoconversion with ionic liquid and Co single atoms.

Liu Yang Y Sun Jianhui J Huang Houhou H Bai Linlu L Zhao Xiaomeng X Qu Binhong B Xiong Lunqiao L Bai Fuquan F Tang Junwang J Jing Liqiang L

Nature communications 20230316 1

Photocatalytic CO2 conversion promises an ideal route to store solar energy into chemical bonds. However, sluggish electron kinetics and unfavorable product selectivity remain unresolved challenges. Here, an ionic liquid, 1-ethyl-3-methylimidazolium tetrafluoroborate, and borate-anchored Co single atoms were separately loaded on ultrathin g-C3N4 nanosheets. The optimized nanocomposite photocatalyst produces CO and CH4 from CO2 and water unde ...[more]

PMID: 36928357

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Project description:Global warming is arguably the biggest scientific challenge of the twenty-first century and its environmental consequences are already noticeable. To mitigate the emissions of greenhouse gases, particularly of CO2, there is an urgent need to design materials with improved adsorbent properties. Five different magnetic ionic liquids were impregnated into the metal-organic framework ZIF-8. The composites were produced by a direct-contact method, and their performance as sorbents for gas separation applications was studied. The impact of the ionic liquid anion on the sorption capacity and ideal CO2/CH4 and CO2/N2 selectivities were studied, focusing on understanding the influence of metal atom and ligand on the adsorbent properties. Reproducible methodology, along with rigorous characterization, were established to assess the impact of the ionic liquid on the performance of the composite materials. Results show that the ionic liquid was well-impregnated, and the ZIF-8 structure was maintained after ionic liquid impregnation. The produced composites were of microporous nature and were thermally stable. CO2, CH4, and N2 adsorption-desorption isotherms were obtained at 303 K and between 0 and 16 bar. The adsorption-desorption data of the composites were compared with that obtained for original ZIF-8. The general trend in composites is that the increased gas uptake per available pore volume compensates the pore volume loss. Adsorption data per unit mass showed that composites have reversible sorption, but inferior gas uptake at all pressure ranges. This is due to the observed total pore volume loss by the ionic liquid pore occupation/blockage. In most cases, composites showed superior selectivity performance at all pressure range. In particular, the composite [C4MIM]2[MnCl4]@ZIF-8 shows a different low-pressure selectivity trend from the original MOF, with a 33% increase in the CO2/N2 selectivity at 1 bar and 19% increase in the CO2/CH4 selectivity at 10 bar. This material shows potential for use in a post-combustion CO2 capture application that can contribute to greenhouse gas mitigation.

Project description:The demand for new ionic liquid (IL)-based systems to selectively sequester carbon dioxide from gas mixtures has prompted the development of individual components involving the tailored design of IL themselves or solid-supported materials that provide excellent gas permeability of the overall material as well as the ability to incorporate large amounts of ionic liquid. In this work, novel IL-encapsulated microparticles comprising a cross-linked copolymer shell of β-myrcene and styrene and a hydrophilic core of the ionic liquid 1-ethyl-3-methylimidazolium dicyanamide ([EMIM][DCA]) are proposed as viable materials for CO2 capture. Water-in-oil (w/o) emulsion polymerization of different mass ratios of β-myrcene to styrene (i.e. 100/0, 70/30, 50/50, 0/100) yielded IL-encapsulated microparticles, where the encapsulation efficiency of [EMIM][DCA] was dependent on the copolymer shell composition. Thermal analysis using thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC) revealed that both thermal stability and glass transition temperatures depend on the mass ratio of β-myrcene to styrene. Images from scanning electron microscopy (SEM) and transmission electron microscopy (TEM) were used to observe the microparticle shell morphology as well as measure the particle size perimeter. Particle sizes were found to be between 5 and 44 μm. CO2 sorption experiments were conducted gravimetrically using TGA instrumentation. Interestingly, a trade-off between CO2 absorption capacity and ionic liquid encapsulation was observed. While increasing the β-myrcene content within the microparticle shell increases the amount of encapsulated [EMIM][DCA], the observed CO2 absorption capacity did not increase as expected due to reduced porosity compared to microparticles with higher styrene content in the microparticle shell. [EMIM][DCA] microcapsules with a 50/50 weight ratio of β-myrcene/styrene showed the best synergistic effect between spherical particle diameter (32.2 μm), pore size (0.75 μm), and high CO2 sorption capacity of ∼0.5 mmol CO2/g sample within a short absorption period of 20 min. Therefore, core-shell microcapsules composed of β-myrcene and styrene are envisioned as a promising material for CO2 sequestration applications.

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Improving CO₂ photoconversion with ionic liquid and Co single atoms.

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Improving CO<sub>2</sub> photoconversion with ionic liquid and Co single atoms.

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