Synergistic effects of core-shell poly(ionic liquids)@ZIF-8 nanocomposites for enhancing additive-free CO2 conversion.

The present study, for the first time, reports the fabrication of core-shell poly(ionic liquids)@ZIF-8 nanocomposites through a facile in-situ polymerization strategy. These composites exhibited exceptional structural characteristics including high specific surface areas and the integration of high-density Lewis acid/base and nucleophilic active sites. The structure-activity relationship, reusability, and versatility of the poly(ionic liquids)@ZIF-8 composites were investigated for the cycloaddition reaction between CO2 and epoxide. By optimizing the composites structures and their catalytic performance, PIL-Br@ZIF-8(2:1) was identified as an exciting catalyst that exhibits high activity and selectivity in the synthesis of various cyclic carbonates under mild or even atmospheric pressure or simulated flue gas conditions. Moreover, the catalyst demonstrated excellent structural stability while maintaining its catalytic activity throughout multiple usage cycles. By combining DFT calculations, we investigated the transition states and intermediate geometries of the cycloaddition reaction in different coordination microenvironments, thereby proposing a synergistic catalytic mechanism involving multiple active sites.

Engineering the activity and stability of ZIF-8(Zn/Co)@g-C3N4 nanocomposites and their synergistic action in converting atmospheric CO2 into cyclic carbonates.

The development of novel catalytic materials that integrate multifunctional sites has significant implications for expanding the utilization of CO2 resources. However, simultaneously achieving high activity and stability remains a formidable challenge. In this study, a series of ZIF-8(Zn/Co)@g-C3N4 nanocomposites were prepared by employing a thermo-physical compounding strategy that involved the combination of nitrogen-rich graphitic carbon nitride (g-C3N4) nanosheets with ZIF-8(ZnCo). The influences of different compositions of g-C3N4 and ZIF-8(Zn/Co) on the catalyst structure were systematically investigated. Subsequently, the catalytic activities of these nanocomposites towards the cycloaddition reaction between CO2 and epoxide were examined under different conditions. The presence of abundant Lewis base sites in g-C3N4 facilitates CO2 activation, while multiple Lewis acid sites in ZIF-8(Zn/Co) enable efficient epoxide activation. By working synergistically with a co-catalyst, tetrabutylammonium bromide (TBAB), CO2 and epoxides can be efficiently reacted to synthesize the corresponding cyclic carbonates under mild or even atmospheric pressure conditions. The catalytic reaction conditions were optimized, and both the catalyst's recycling performance and the scope of epoxides with various substituents were investigated. The integration of g-C3N4 and ZIF-8(Zn/Co) endows the catalytic material with exceptional structural stability and remarkable catalytic activity, thereby providing a new platform for highly efficient CO2 conversion.

High-Quality Draft Genome Sequence of Pseudomonas songnenensis L103, a Denitrifier Isolated from a 100-Meter-Deep Aquifer in a Heavily Nitrogen-Fertilized Agricultural Area.

Pseudomonas songnenensis strain L103 was isolated from a 100-m-deep aquifer in the North China Plain, a heavily nitrogen-fertilized agricultural area. The genome is 4.8 Mb and contains 4,409 protein-coding genes, including a full set of genes (nar, nir, nor, and nos) for complete denitrification.

Periodic Mesoporous Organosilica with a Basic Urea-Derived Framework for Enhanced Carbon Dioxide Capture and Conversion Under Mild Conditions.

A periodic mesoporous organosilica with a basic urea-derived framework (PMO-UDF) was prepared and characterized thoroughly. The PMO-UDF showed an enhanced CO2 capture capacity at low pressure (≤1 atm) and an exceptional catalytic activity in CO2 coupling reactions with various epoxides to yield the corresponding cyclic carbonates under mild conditions because of the presence of a high surface area, basic pyridine units, and multiple hydrogen-bond donors. The highly stable catalyst could be reused at least six successive times without a significant decrease of the catalytic efficiency or structural deterioration, thus the PMO-UDF composite is considered as a promising material for CO2 capture and conversion.

Ag2CrO4 nanoparticles loaded on two-dimensional large surface area graphite-like carbon nitride sheets: simple synthesis and excellent photocatalytic performance.

Graphite-like carbon nitride (g-C3N4) with a large surface area was prepared through thermal condensation of guanidine hydrochloride at 650 °C. Various amounts of silver chromate (Ag2CrO4) nanoparticles with small size were highly loaded on the g-C3N4 by a simple co-precipitation method at room temperature. The chemical constituents, surface structure and optical properties of the resultant Ag2CrO4/g-C3N4 composites were thoroughly characterized. And the photocatalytic performances were evaluated by degradation of Rhodamine B (RhB) and phenol, the experimental results indicated that the as-prepared Ag2CrO4/g-C3N4 composites presented excellent photocatalytic activity under visible-light irradiation. With the mass ratio of Ag2CrO4 to g-C3N4 at 1 : 2, the Ag2CrO4/g-C3N4 composites exhibited optimal photocatalytic activity for degrading RhB, approximately 6.1 and 10.4 times higher than those on pure g-C3N4 and bare Ag2CrO4 particles. The improved photocatalytic activity was mainly attributed to the combined effect including the larger surface area, highly dispersed smaller Ag2CrO4 nanoparticles, stronger visible absorption and higher charge separation efficiency of the Ag2CrO4/g-C3N4 composites. Moreover, the possible mechanism for the photocatalytic activity was tentatively proposed.

Insights into hydrogen bond donor promoted fixation of carbon dioxide with epoxides catalyzed by ionic liquids.

Catalytic coupling of carbon dioxide with epoxides to obtain cyclic carbonates is an important reaction that has been receiving renewed interest. In this contribution, the cycloaddition reaction in the presence of various hydrogen bond donors (HBDs) catalyzed by hydroxyl/carboxyl task-specific ionic liquids (ILs) is studied in detail. It was found that the activity of ILs could be significantly enhanced in the presence of ethylene glycol (EG), and EG/HEBimBr were the most efficient catalysts for the CO2 cycloaddition to propylene oxide. Moreover, the binary catalysts were also efficiently versatile for the CO2 cycloaddition to less active epoxides such as styrene oxide and cyclohexene oxide. Besides, the minimum energy paths for this hydrogen bond-promoted catalytic reaction were calculated using the density functional theory (DFT) method. The DFT results suggested that the ring-closing reaction was the rate-determining step in the HEBimBr-catalyzed cycloaddition reaction but the EG addition could remarkably reduce its energy barrier as the formation of a hydrogen bond between EG and the oxygen atom of epoxides led this process along the standard SN2 mechanism. As a result, the ring-opening reaction became the rate-determining step in the EG/HEBimBr-catalyzed cycloaddition reaction. The work reported herein helped the understanding and design of catalysts for efficient fixation of CO2 to epoxides via hydrogen bond activation.

A Facile and One-Step Synthesis of Visible-Light-Responsive Silver and Mesoporous Carbon Comodified Carbon-Zinc Oxide Composites.

Silver and mesoporous carbon (mC) comodified CZnO composites (Ag/mC/CZnO) were fabricated by a facile, one-step process directly from C, Ag, and Zn precursors in CO2 -expanded ethanol, which provided a unique medium and did not require additional precipitant and mesoscaled organic templates. When the composite photocatalyst was applied to the degradation of rhodamine B and phenol, Ag/mC/CZnO exhibited excellent photocatalytic activity in visible light. The remarkably improved catalytic activity of the composites was attributed to the following synergistic effects. The modification of mC enriched the adsorption of pollutants on the photocatalyst. Additionally, the mesopores of carbon provided a spacious path for the separation of photogenerated electrons and holes. In addition to mC, carbon was also doped into ZnO, which narrowed the ZnO band gap. The modification of silver strengthened the absorbance of the visible region and improved the electron-trapping ability.

CO2-assisted synthesis of mesoporous carbon/C-doped ZnO composites for enhanced photocatalytic performance under visible light.

Visible-light-responsive mesoporous carbon/C-doped ZnO (mC/C-ZnO) composites were fabricated using a facile, fast, one-step process in CO2-expanded ethanol solution. It is a green and sustainable process that does not need tedious pretreatment, surfactants or precipitants. CO2 played triple roles in the synthesis of mC/C-ZnO composites; the first was to provide a simple physical expansion to evenly dope the carbon in the ZnO; the second was to offer some chemical groups such as CO3(2-) and HCO3(-), facilitating the uniform and complete deposition through the coordination of a metallic cation with these anions; and the third was to offer CO3(2-) acting as a template for the formation of mesoporosity in the carbon. When used as a photocatalyst for the photodegradation of RhB and the organic pollutant phenol, the mC/C-ZnO composites with glucose content at 22 wt% (mC/C-ZnO-CE-2) synthesized in CO2-expanded ethanol exhibited better recycling stability and photodegradation rate than the corresponding sample synthesized in pure ethanol. Such improved photocatalytic performance was attributed to the well-mixing of the mesoporous carbon and the small sized C-doped ZnO particles in the mC/C-ZnO-CE-2 composites. The facile and fast synthesis method could be extended to other mesoporous carbon/C-doped metal oxide composites, which are expected to be good photocatalyst candidates, or in other application fields.