ABSTRACT
Electrochemical N2 fixation is considered to be a promising alternative to Haber-Bosch technology. Inspired by the composition and structure of natural nitrogenase, Fe-doped VS2 nanosheets were prepared via one-step solvothermal method. The electron transfer system mediated by organic conductive polymer (1-AAQ-PA) was constructed to promote the electron transfer between Fe-VS2 nanosheets and the electrode in electrocatalytic N2 reduction reaction (NRR). The obtained 1-AAQ-PA-Fe-VS2 electrode converted N2 to NH3 with a yield of 31.6â µg h-1 mg-1 at -0.35â V vs. reversible hydrogen electrode and high faradaic efficiency of 23.5 %. The introduction of Fe dopants favored N2 adsorption and activation, while the Li-S bond between Fe-VS2 and Li2 SO4 effectively inhibited hydrogen evolution. The highly efficient electron utilization in the electrocatalytic NRR process was realized using the 1-AAQ-PA as the electron transfer medium. Density functional theory calculations showed that N2 was preferentially adsorbed on Fe and reduced to NH3 via both distal and alternating mechanism.
Subject(s)
Electrons , Nitrogen FixationABSTRACT
Antibacterial agents with enzyme-like properties and bacteria-binding ability have provided an alternative method to efficiently disinfect drug-resistance microorganism. Herein, a Fe3O4@MoS2-Ag nanozyme with defect-rich rough surface was constructed by a simple hydrothermal method and in-situ photodeposition of Ag nanoparticles. The nanozyme exhibited good antibacterial performance against E. coli (~69.4%) by the generated ROS and released Ag+, while the nanozyme could further achieve an excellent synergistic disinfection (~100%) by combining with the near-infrared photothermal property of Fe3O4@MoS2-Ag. The antibacterial mechanism study showed that the antibacterial process was determined by the collaborative work of peroxidase-like activity, photothermal effect and leakage of Ag+. The defect-rich rough surface of MoS2 layers facilitated the capture of bacteria, which enhanced the accurate and rapid attack of â¢OH and Ag+ to the membrane of E. coli with the assistance of local hyperthermia. This method showed broad-spectrum antibacterial performance against Gram-negative bacteria, Gram-positive bacteria, drug-resistant bacteria and fungal bacteria. Meanwhile, the magnetism of Fe3O4 was used to recycle the nanozyme. This work showed great potential of engineered nanozymes for efficient disinfection treatment.
ABSTRACT
Photocatalytic disinfection with high performance is thought to be a promising way for water purification. Herein, plasmonic Ag doped urea-derived graphitic carbon nitride (g-C3N4) composites were fabricated via in-situ photo-deposition at room temperature as the visible-light photocatalyst. Scan electron microscopy and transmission electron microscopy images showed the uniform dispersion of Ag nanoparticles on the surface of g-C3N4 sheet, which facilitated the synergistic effect of antibacterial performance from Ag and photocatalytic property from Ag/g-C3N4 composites. Photocatalytic water disinfection against Escherichia coli with visible light was performed to demonstrate the improved photocatalytic property with assistance of Ag. The 3-Ag/g-C3N4 exhibited the best bactericidal performance by inactivating all bacteria within 120â¯min with damaged cell membranes of Escherichia coli observed by scan electron microscopy and transmission electron microscopy images. Photoluminescence spectra, steady-state surface photovoltage spectra, photocurrent response, and electrochemical impedance spectra results revealed that Ag nanoparticles inhibited the recombination of photo-generated e- and h+ pairs and further reinforced the photocatalytic performance of g-C3N4. Scavenger experiments indicated that h+ produced on valence band of g-C3N4 dominated the photocatalytic disinfection process against Escherichia coli. This work further proved Ag/g-C3N4 showed great potential in photocatalytic water disinfection under visible-light irradiation.
