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• Plasma partial oxidative reforming of the tar model compound was carried out. • A detailed kinetics model was established based on the calculated G-values of active species. • Performance was evaluated under pure N 2 and gasification gas atmospheres. • The highest toluene conversion was 100.0 % with an energy efficiency of 25.7 g/kWh, without catalysts usage. In this study, partial oxidation of toluene as a biomass tar surrogate was carried out in a dielectric barrier discharge (DBD) plasma reactor. In order to understand the reaction characteristics and thus potential of the approach, the effect of reaction temperature, O 2 /toluene molar ratio (OTR) and discharge power on performances was investigated by experiments and kinetic modeling. The results showed that the three factors could change the E/n and hence the G-values of species, as well as alter O 2 concentration in background gas and input energy, leading to the variation in active species production and thus, the performance. Appropriate high temperatures, as well as higher OTRs and discharge power obtained better performances by promoting toluene destruction and gas product production. Excited N 2 species play a crucial role in the process, by means of participating in reactions directly and strongly influencing on the production of secondary active species. At 300 °C, the highest toluene conversion of 100.0 % with an energy efficiency of 25.7 g/kWh was achieved without catalysts usage, a comparable performance as compared to the steam reforming by plasma catalysis, demonstrating the potential of this method for the purification of gasification gases. Furthermore, based on the rate of production (ROP) and sensitivity analyses of the model developed, as well as experimental results, the reaction mechanism was proposed. [ABSTRACT FROM AUTHOR]

• Three possible pathways for bicarbonate generation were investigated based on DFT. • Base-catalyzed CO 2 hydration is dominant in [N 1111 ][Gly]/EtOH aqueous system. • Water effect on phase change behavior is analyzed from hydrogen bonding view. • Water content of 5 wt% promotes products aggregation in favor of phase change. Ionic liquids-based anhydrous biphasic absorbents have the potential to lower the energy consumption for CO 2 capture. Recent experimental studies have revealed that the presence of water in [N 1111 ][Gly]/EtOH system leads to generation of a new CO 2 -product – bicarbonate and affects the phase change behavior. However, the reaction pathway for bicarbonate formation remains unclear. In this work, the reaction pathways were investigated in depth through quantum chemical calculations employing density functional theory, with reaction rate constants determined via transition state theory. Among the three possible reaction pathways, the base-catalyzed CO 2 hydration reaction prevailed, i.e. a one-step reaction involving [Gly]-, H 2 O, and CO 2. An H atom in H 2 O was transferred to [Gly]-'s amino group, forming protonated [Gly]-, and hydroxide combined with CO 2 to generate bicarbonate. Additionally, molecular dynamics simulations were conducted to understand the phase change behaviors with varying water content. When water content exceeded 5 wt%, an increased water content led to reduced hydrogen bonding among products and enhanced hydrogen bonding of products-solvent with the solvent, diminishing product self-aggregation. No phase change behavior were observed at water contents up to 80 wt%. This study could well explain the experimental phenomena of water effect on CO 2 absorption in [N 1111 ][Gly]/EtOH, providing theoretical references for application of ILs-based anhydrous biphasic absorbent. [ABSTRACT FROM AUTHOR]

[Display omitted] • Mo-based MXene is first applied as a cathode catalyst for Li-CO 2 batteries. • An innovative surface modification strategy, mild oxidation by CO 2 , is employed. • The catalyst optimizes the growth and decomposition of discharge products. • This MoO 2 @Mo 2 C-based Li-CO 2 battery outperforms most other MXene-based catalysts. The lithium-carbon dioxide (Li-CO 2) batteries hold promise for energy storage, given their capacity to capture and convert carbon dioxide (CO 2). However, the practical application of Li-CO 2 batteries continues to face substantial obstacles caused by sluggish CO 2 reduction/evolution kinetics, resulting in high overpotential and short lifespan. This work presents the fabrication of a highly effective MoO 2 @Mo 2 C heterostructure hybrid catalyst using a CO 2 oxidation strategy. This strategy integrated (in-situ) MoO 2 onto the surface of two-dimensional (2D) Mo 2 C MXene, enhancing catalytic activity while preserving 2D electron/ion pathways. As a result, the MoO 2 @Mo 2 C, when used as a catalyst in Li-CO 2 battery showcased a discharge capacity of 20790.8 mAh g−1 at a current density of 200 mA g−1. Notably, it achieved a long cycling life of 230 cycles at a cutoff capacity of 1000 mAh g−1 with a voltage gap as low as 1.85 V, which was significantly superior to that of a pristine Mo 2 CT x catalyst (3.61 V after twenty cycles). This work provides critical insights into the design of MXenes-based high-performance catalysts for advanced Li-CO 2 batteries. [ABSTRACT FROM AUTHOR]

[Display omitted] • MXene was used as conductive substrate to reinforce the structural stability of Sb@C. • The MXene and carbon can spatially confine the Sb particles during cycling. • The MXene-Sb@C shows better lithium storage properties than the Sb@C composite. • The assembled Li ion full cell delivers a maximum energy density of 381.2 Wh kg−1. Antimony (Sb) is recognized as a potential anode material for lithium-ion batteries due to its high theoretical capacity and adequate working potential. However, its application is hindered by the significant volume expansion during lithiation and low intrinsic conductivity, leading to considerable capacity fading and reduced rate capability. Herein, a unique MXene-reinforced Sb@C (MSC) nanocomposite is constructed via in-situ growing Sb-MOF over the conductive MXene substrate, followed by annealing. MXene substrate and MOF-derived carbon layer coupling effectively creates a continuous and conductive framework, encapsulating Sb nanoparticles. This unique architecture mitigates volume expansion, prevents particle aggregation, and enhances interfacial charge transfer, significantly improving the lithium storage performance of the MSC nanocomposite over its Sb@C (SC) counterpart. The MSC nanocomposite achieves a high capacity of 625 mAh g−1 at 100 mA g−1, superior rate capability of 305 mAh g−1 at 10 A g−1, as well as excellent cycling stability with a capacity retention of 84.4 % over 2000 continuous cycles. Additionally, a lithium-ion full batteries with MSC anode and LiFePO 4 cathode demonstrates a capacity of 168.9 mAh g−1 at 100 mA g−1 and a maximum energy density of 381.2 Wh kg−1 based on the cathode mass, illustrating its promising potential for constructing high-performance lithium ion batteries. [ABSTRACT FROM AUTHOR]

[Display omitted] • Both laser/chlorine and laser/PS systems could efficiently degrade CBZ. • HO·, Cl· and ClO· were dominant for CBZ degradation in laser/chlorine system. • CBZ degradation in laser/PS system was primarily attributed to HO· and SO 4. -. • The degradation pathways of CBZ were proposed based on DFT analysis. Residual carbamazepine (CBZ) in water is difficult to remove through conventional treatment processes, threatening the safety of drinking water. Ultraviolet-based advanced oxidation processes (UV-AOPs) have shown promise in removing refractory organic pollutants, while the low energy and efficiency of traditional mercury lamps hinder their practical applications. In this study, the performance and mechanism of an intensive-energy light source, UV laser, were systematically explored in UV-AOPs (laser/chlorine, laser/persulfate (PS)). It was found that UV laser exhibited a significantly activating ability for chlorine and PS due to its precise wavelength and high pulse energy. When exposed to UV laser (266 nm, 4.2 mW/cm2) combined with 200 μM chlorine and PS, the kinetic rate constants for the degradation of 10 μM CBZ were determined to be 3.160 × 10-3 and 1.227 × 10-3 s−1, respectively. The degradation of CBZ was dominated by hydroxyl radicals (60.98 %) and sulfate radicals (23.15 %) in laser/PS system, while in laser/chlorine system, hydroxyl radicals (54.90 %), chlorine radicals (27.43 %), and chlorine oxide radicals (13.81 %) were primary reactive species. Furthermore, both the laser/chlorine and laser/PS systems demonstrated compatibility with a wide pH range of 5.0–9.0 and high resistance to anionic interference. Moreover, the electrophilic and nucleophilic sites of CBZ and energy barrier of the initial reaction were calculated based on the density functional theory (DFT). Additionally, the degradation pathways of CBZ and the toxicity of transformation products in laser/chlorine and laser/PS processes were proposed and evaluated. These results demonstrated that the UV laser-based processes exhibited promising prospects in eliminating refractory organic pollutants in water treatment. [ABSTRACT FROM AUTHOR]

[Display omitted] • Excellent activity and selectivity of CO 2 -to-CH 4 conversion is realized by MIS. • The ultrathin insulator layer significantly expedites the interfacial electrons tunneling. • The MIS promotes rate-determining step from *COOH to *CO to produce CH 4. A metal–insulator-semiconductor (MIS) ternary photo-system was intricately crafted through precise amalgamation polyvinylpyrrolidone (PVP)-capped metal Cu with typical covalent triazine framework CTF-1 via electrostatic self-assembly. The 2 % Cu-PVP-CTF exhibited an impressive CH 4 yield of 80.7 μmol·g−1·h−1 with selectivity of 96.8 % under visible light, representing a 2.3-fold and 112-fold improvement over Schottky-type Cu-CTF and pristine CTF-1, respectively. In-situ XPS and VASP-diff calculations unfolded that the ultrathin PVP insulating layer significantly expedited interfacial charges tunneling, corroborated by smaller lifetime τ 2 determined via femtosecond transient absorption spectroscopy. The intermediates of paramount importance in CO 2 reduction like *COOH and *HCHO were meticulously monitored by in-situ Fourier infrared spectroscopy. DFT calculations elucidated that Cu-PVP-CTF was notably more adept at facillitating the rate-determining step (*COOH → *CO) to produce CH 4 than Cu-CTF. This work tamps the groundwork for conceptional roadmap in designing novel MIS photo-system for CO 2 conversion. [ABSTRACT FROM AUTHOR]