The anaerobic fermentation gas (AFG) with CO2 removed is a sustainable energy resource, and converting CO2 in AFG to value‐added chemicals can kill two birds with one stone. Herein, an ionic porous organic polymer (IPOP‐3) catalyst, with triply synergistic effect of its hydroxide anions, nitrogen activation sites and porous structure, is synthesized. IPOP‐3 exhibits an excellent ability to enrich and convert 50 vol.% CO2 by the reactions with various amines into corresponding formamides. The catalyst is also successfully applied to the N‐formylation of CO2 in AFG, and can be easily recovered and reused. The plausible mechanism for the catalytic N‐formylation is proposed. The hydroxide anion in IPOP‐3 activates the Si−H bond of phenyl silane which reacts with the captured CO2 to form formate anion to facilitate the subsequent conversion into formamide. Our work provides a new idea for the purification of AFG and the resource utilization of CO2.

Effective N‐formylation of Amines with CO2 in Anaerobic Fermentation Gas Catalyzed by Triply Synergistic Effect of Ionic Porous Organic Polymer

The direct utilization of diluted CO2 skips the additional enrichment and purification operations required for high-purity CO2, making it shine in the green catalytic process. However, achieving diluted CO2 cycloaddition coupling transesterification with epoxide and methanol over poly(ionic liquids) catalyst and understanding the relevant mechanism at the molecular level are still challenging. Here, a novel porous sulfonyl binuclear carbonate poly(ionic liquid)s (SC-PILs) were successfully prepared by the integration of acidic monomers pre-polymerization with basic anions post-etching, regulating the chemical property of free anions and increasing the specific surface area of copolymerized materials. Relying on the synergy of the built abundant pores and the exposed basic anions, SC-PILs could one-pot efficiently catalyze the cycloaddition coupling transesterification reaction of the simulated flue gas (15% CO2 + 85% N2) without any co-catalyst, and dimethyl carbonate (DMC) with the yield of 80% was obtained. Theoretical studies deeply understood the activation difference of binuclear CO32− anion on CO2 compared with mononuclear CH3COO− anion and the ring-opening mechanism of [CO32−+CO2] adduct on epoxides, providing a better choice for high-value utilization of diluted CO2 from flue gas. 

Porous sulfonyl binuclear carbonate poly(ionic liquid)s for one-pot fixation of diluted CO2 into dimethyl carbonate

Transformations of Carbon Dioxide under Homogeneous Catalysis Conditions (A Review)

Constructing green and efficient porous material platforms for carbon dioxide (CO2) adsorption and chemical conversion can effectively solve a series of environmental problems caused by the greenhouse effect. Herein, four melamine-based polymer networks PANs (PAN-P, PAN-PY, PAN-PZ, and PAN-IM) with abundant N sites and hydrogen bond donor (HBD) groups were synthesized by simple polymerization. The chemical structure of PANs was determined by various characterizations, and then the CO2 uptake of PANs and their catalytic activity for the cycloaddition of CO2 with epoxides were investigated. Among them, PAN-P has the largest CO2 adsorption capacity, reaching values of 73.5 cm3/g at 273 K. Meanwhile, PAN-IM exhibits the best catalytic activity with 93 % yield and 99 % selectivity under metal-, halogen-, solvent-, and cocatalyst-free conditions (120 ◦C, 1.0 MPa CO2, 8 h), which mainly attribute to the multi-site synergistic activation of the imidazole heterocycle. In addition, PAN-IM also has satisfactory activity to various epoxides and exhibited good recyclability. Density functional theory (DFT) and FT-IR analysis were used to further reveal the interaction of PANs towards CO2 and epoxides. Finally, a possible mechanism was suggested, including activation of CO2 and epoxide, ring-opening of epoxide, insertion of CO2 and ring-closing to form cyclic carbonate. The research in this paper will provide a reference for the development of a green and efficient CO2 adsorption conversion platform. 

Melamine-based nitrogen-heterocyclic polymer networks as efficient platforms for CO2 adsorption and conversion

Herein, a highly efficient magnetically separable hybrid GO/SrFe12O19 nanocomposite was synthesized via dispersing M-type strontium hexaferrite (SrFe12O19) on graphene oxide (GO) sheets. First, SrFe12O19 nanoparticles (NPs) and GO sheets were prepared via chemical coprecipitation and chemical oxidation of graphite powder, respectively. Chemically reduced GO (rGO) and rGO/SrFe12O19 were also prepared for comparison purposes. Thereafter, the prepared nanostructured materials were explored by XRD, FTIR, FESEM-EDX, BET, and Zetasizer analyses. All the characterizations confirm the nanoscale and the high stability structures of the prepared materials. The prepared hybrid magnetic nanocomposite GO/SrFe12O19 exhibited a high surface area value resulting in a high catalytic activity and selectivity for the epoxide ring-opening with amines in neat water. The use of hybrid GO/SrFe12O19 compared with pure SrFe12O19 and GO sheets is of great interest for using environmentally benign heterogeneous nanocatalysts, for the synthesis of β-amino alcohols, with excellent recyclability under eco-friendly conditions. Moreover, a mechanistic study was performed through density functional theory (DFT) calculations and Parr functions to explain the observed reactivity and selectivity of SrFe-GO catalyst in the epoxide ring-opening reactions.

/pdf/synergistic-effect-of-go-srfe12o19-as-magnetic-hybrid-c5vzmec7.pdf

Synergistic effect of GO/SrFe12O19 as magnetic hybrid nanocatalyst for regioselective ring-opening of epoxides with amines under eco-friendly conditions

Insight into the reversible behavior of Lewis–Brønsted basic poly(ionic liquid)s in one-pot two-step chemical fixation of CO2 to linear carbonates

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Insight into the reversible behavior of Lewis–Brønsted basic poly(ionic liquid)s in one-pot two-step chemical fixation of CO2 to linear carbonates