RESUMEN
Clean production of hydrogen peroxide (H2O2) with water, oxygen, and renewable energy is considered an important green synthesis route, offering a valuable substitute for the traditional anthraquinone method. Currently, renewable energy-driven production of H2O2 mostly relies on soluble additives, such as electrolytes and sacrificial agents, inevitably compromising the purity and sustainability of H2O2. Herein, we develop a solution plasma catalysis technique that eliminates the need for soluble additives, enabling eco-friendly production of concentrated H2O2 directly from water and O2. Screening over 40 catalysts demonstrates the superior catalytic performance of carbon nitride interacting with discharge plasma in water. High-throughput density functional theory calculations for 68 models, along with machine learning using 29 descriptors, identify cyano carbon nitride (CCN) as the most efficient catalyst. Solution plasma catalysis with the CCN achieves concentrated H2O2 of 20 mmol L-1, two orders of magnitude higher than photocatalysis by the same catalyst. Plasma diagnostics, isotope labeling, and COMSOL simulations collectively validate that the interplay of solution plasma and the CCN accounts for the significantly increased production of singlet oxygen and H2O2 thereafter. Our findings offer an efficient and sustainable pathway for H2O2 production, promising wide-ranging applications across the chemical industry, public health, and environmental remediation.
RESUMEN
In this study, a series of Co nanoparticles (NPs) with different sizes and Co single-atom catalysts (SACs) with different cobalt-nitrogen coordination numbers (Co-N2, Co-N3, and Co-N4) were synthesized and applied to the synthesis of ammonia catalyzed by plasma at low temperatures and atmospheric pressures. Under the same reaction conditions, the yield of nitrogen obtained from the reduction to ammonia over a series of Co NP catalysts varies with the Co particle size. The smaller the size of the Co NPs, the greater the number of exposed active centers, and the catalytic activity is higher. Among the Co SACs, the best catalyst was Co-N2 with two coordinated nitrogen atoms, and the ammonia yield was 181 mg·h-1·gcat-1. The experimental and theoretical calculations were consistent in that a low Co-N coordination number was beneficial to the adsorption and dissociation of N2, thereby enhancing the reduction activity of N2 and promoting the increase of ammonia production.
RESUMEN
A dielectric barrier discharge (DBD) catalyst hybrid reactor with CeO2/γ-Al2O3 catalyst balls was investigated for benzene decomposition at atmospheric pressure and 30⯰C. At an energy density of 37-40â¯J/L, benzene decomposition was as high as 92.5% when using the hybrid reactor with 5.0wt%CeO2/γ-Al2O3; while it was 10%-20% when using a normal DBD reactor without a catalyst. Benzene decomposition using the hybrid reactor was almost the same as that using an O3 catalyst reactor with the same CeO2/γ-Al2O3 catalyst, indicating that O3 plays a key role in the benzene decomposition. Fourier transform infrared spectroscopy analysis showed that O3 adsorption on CeO2/γ-Al2O3 promotes the production of adsorbed O2- and O22â, which contribute benzene decomposition over heterogeneous catalysts. Nano particles as by-products (phenol and 1,4-benzoquinone) from benzene decomposition can be significantly reduced using the CeO2/γ-Al2O3 catalyst. H2O inhibits benzene decomposition; however, it improves CO2 selectivity. The deactivated CeO2/γ-Al2O3 catalyst can be regenerated by performing discharges at 100⯰C and 192-204â¯J/L. The decomposition mechanism of benzene over CeO2/γ-Al2O3 catalyst was proposed.
RESUMEN
Non-thermal plasma (NTP) an emerging technology to treat volatile organic compounds (VOCs) present in unhygienic point source air streams. In present study, double dielectric barrier discharge (DDBD) reactors were used for the first time to evaluate the removal efficiency of VOCs mixture of different nature at constant experimental conditions (input power 16-65.8â¯W, VOCs mixture feeding rate 1-6â¯L/min, 100-101â¯ppm inlet concentration of individual VOC). Reactor A and B with discharge gap at 6â¯mm and 3â¯mm respectively, were used in current study. When treated at an input power of 53.7â¯W with gas feeding rate of 1â¯L/min in DDBD reactor A, removal efficiency of the VOCs were: tetrachloroethylene (100%), toluene (100%), trichloroethylene (100%), benzene (100%), ethyl acetate (100%) and carbon disulfide (88.30%); whereas in reactor B, the removal efficiency of all VOCs were 100%. Plasma-catalyst (Pt-Sn/Al2O3, BaTiO3 and HZSM-5) synergistic effect on VOCs removal efficiency was also investigated. Highest removal efficiency i.e 100% was observed for each compound with BaTiO3 and HZSM-5 at an input power 65.8â¯W. However, integrating NTP with BaTiO3 and HZSM-5 leads to enhanced removal performance of VOCs mixture with high activity, increase in energy efficiency and suppression of unwanted byproducts.
RESUMEN
The paper reports the use of atmospheric non-thermal plasma torch as a catalyst for degradation of various organic pollutants dissolved in water. A flow of He mixed with air was used to produce the dielectric barrier discharge (DBD), at the tip of the torch, using pulsed electric excitation at 12 kV. The torch, operated at a power of 750 mW/mm2, was seen to completely degrade the aqueous solutions of the pollutants namely methylene blue (MB), methyl orange (MO) and rhodamine-B (RB), at around 10-4 M concentrations, the concentration of polluants is one order higher than of routinely used heterogeneous photocatalytic reactions, within 10 min of irradiation time at room temperature. UV Visible spectra of the organic dye molecules, monitored after different intervals of plasma-irradiation, ranging between 1 and 10 min, have been used as tools to quantify their sequential degradation. Further, instead of using He, only air was used to form plasma plume and used for degradation of organic dye which follow similar trend as that of He plasma. Further, Liquid Chromatography Mass Spectroscopy (LCMS) technique has been used to understand degradation pathway of methylene blue (MB) as a representative case. Total organic carbon (TOC) measurements indicates significant decrease in its content as a function of duration of plasma exposure onto methylene blue as a representative case. Toxicity studies were carried out onto Gram negative Escherichia coli. This indicated that methylene blue, without plasma treatment, shows growth inhibition, whereas with plasma treatment no inhibition was observed.