A series of highly dispersed platinum‐deposited porous g‐C3N4 (Pt/pg‐C3N4) were successfully fabricated by a simple in situ photoreduction strategy using chloroplatinic acid and porous g‐C3N4 as precursors. Porou...A series of highly dispersed platinum‐deposited porous g‐C3N4 (Pt/pg‐C3N4) were successfully fabricated by a simple in situ photoreduction strategy using chloroplatinic acid and porous g‐C3N4 as precursors. Porous g‐C3N4 was fabricated by a pretreatment strategy using melamine as a raw material.The morphology, porosity, phase, chemical structure, and optical and electronic properties ofas‐prepared Pt/pg‐C3N4 were characterized. The photocatalytic activity of as‐prepared Pt/pg‐C3N4was preliminarily evaluated by the degradation of aqueous azo dyes methyl orange under visible light irradiation. The as‐prepared Pt/pg‐C3N4 were further applied to the degradation and mineralization of aqueous 4‐fluorophenol. The recyclability of Pt/pg‐C3N4 was evaluated under four consecutive photocatalytic runs.展开更多
Fluorine-containing halogenated fluorophenol may have effect as intermediate species involved in the formation of polyfluorinated dibenzo-p-dioxin/dibenzofurans （PFDDs/Fs）. The mechanism for the atomic H initiated r...Fluorine-containing halogenated fluorophenol may have effect as intermediate species involved in the formation of polyfluorinated dibenzo-p-dioxin/dibenzofurans （PFDDs/Fs）. The mechanism for the atomic H initiated reactions with complete series of nineteen fluorophenol congeners was studies using the density functional theory. At the MPWB1K,/6-31＋G（d,p） level, the geometries and frequencies of reactants, transition states, and products were obtained, and the accurate energetic values were acquired at the MPWB 1K/6-311 ＋G（3df,2p） level. The rate constants were evaluated by the canonical variational transition-state theory with the small curvature tunneling contribution over a wide temperature range of 600-1000 K. The study shows that the intramolecular hydrogen-bond in the ortho-substituted FPs as well as the inductive effect of the electron-withdrawing fluorine and steric repulsion of multiple substitutions may ultimately be responsible for the relative strength of the O-H bonds in FPs. The results can be used for further studies on PFDD/Fs formation mechanism.展开更多
By measuring the respiratory oxygen consumption, a study on the aerobic biodegradability of 2-fluorophenol, 3- fluorophenol and 4-fluorophenol was conducted using activated sludge acclimated by themselves respectively...By measuring the respiratory oxygen consumption, a study on the aerobic biodegradability of 2-fluorophenol, 3- fluorophenol and 4-fluorophenol was conducted using activated sludge acclimated by themselves respectively. The experimental results showed that bio-oxidation ratios of 2- fluorophenol, 3- fluorophenol and 4- fluorophenol were 25.30%, 35.28% and 36.60% respectively, and the constmdng rate constants were 0.009 3, 0.013 3 and 0.014 5 L/ gSS. h respect/vdy. The aerobic biodegradability of the mono-fluorophenols decreased in the order of 4- fluorop- henol〉3 - fluorophenol 〉2 - fluorophenol, resulting mainly from the different octanol/water partition coefficient and the different steric parameter of the fluorophenols which can affect the penetration of fluorophenol into cell membrane.展开更多
The ultrafast dynamics of o-fluorophenol via the excited states has been studied by femtosecond time-resolved photoelectron imaging. The photoion and photoelectron spectra taken with a time delay between 267 nm pump l...The ultrafast dynamics of o-fluorophenol via the excited states has been studied by femtosecond time-resolved photoelectron imaging. The photoion and photoelectron spectra taken with a time delay between 267 nm pump laser and 800 nm probe laser provide a longer-lived S1 electronic state of about ns timescale. In comparison,the spectra obtained by exciting the S2 state with femtosecond laser pulses at 400 nm and ionizing with pulses at 800 nm suggest that the S2 state has an ultrashort lifetime about 102 fs and reflects the internal conversion dynamics of the S2 state to the S1 state.展开更多
基金supported by the National Natural Science Foundation of China (51568049, 51208248, 51468043, 21366024)the National Science Fund for Excellent Young Scholars (51422807)+1 种基金the Natural Science Foundation of Jiangxi Province, China (20161BAB206118, 20114BAB213015)the Natural Science Foundation of Jiangxi Provincial Department of Education, China (GJJ14515, GJJ12456)~~
文摘A series of highly dispersed platinum‐deposited porous g‐C3N4 (Pt/pg‐C3N4) were successfully fabricated by a simple in situ photoreduction strategy using chloroplatinic acid and porous g‐C3N4 as precursors. Porous g‐C3N4 was fabricated by a pretreatment strategy using melamine as a raw material.The morphology, porosity, phase, chemical structure, and optical and electronic properties ofas‐prepared Pt/pg‐C3N4 were characterized. The photocatalytic activity of as‐prepared Pt/pg‐C3N4was preliminarily evaluated by the degradation of aqueous azo dyes methyl orange under visible light irradiation. The as‐prepared Pt/pg‐C3N4 were further applied to the degradation and mineralization of aqueous 4‐fluorophenol. The recyclability of Pt/pg‐C3N4 was evaluated under four consecutive photocatalytic runs.
基金supported by the National Natural Science Foundation of China(No.21177077,21177076)the Independent Innovation Foundation of Shandong University(No.2012JC030)
文摘Fluorine-containing halogenated fluorophenol may have effect as intermediate species involved in the formation of polyfluorinated dibenzo-p-dioxin/dibenzofurans （PFDDs/Fs）. The mechanism for the atomic H initiated reactions with complete series of nineteen fluorophenol congeners was studies using the density functional theory. At the MPWB1K,/6-31＋G（d,p） level, the geometries and frequencies of reactants, transition states, and products were obtained, and the accurate energetic values were acquired at the MPWB 1K/6-311 ＋G（3df,2p） level. The rate constants were evaluated by the canonical variational transition-state theory with the small curvature tunneling contribution over a wide temperature range of 600-1000 K. The study shows that the intramolecular hydrogen-bond in the ortho-substituted FPs as well as the inductive effect of the electron-withdrawing fluorine and steric repulsion of multiple substitutions may ultimately be responsible for the relative strength of the O-H bonds in FPs. The results can be used for further studies on PFDD/Fs formation mechanism.
基金Supported by State Key Laboratory of Pollution Control and Resource Reuse ( No. PCRRF06007and PCRRYSF06001) and ShanghaiScience and Technology Commission (No.05JC14059and05DZ22330)
文摘By measuring the respiratory oxygen consumption, a study on the aerobic biodegradability of 2-fluorophenol, 3- fluorophenol and 4-fluorophenol was conducted using activated sludge acclimated by themselves respectively. The experimental results showed that bio-oxidation ratios of 2- fluorophenol, 3- fluorophenol and 4- fluorophenol were 25.30%, 35.28% and 36.60% respectively, and the constmdng rate constants were 0.009 3, 0.013 3 and 0.014 5 L/ gSS. h respect/vdy. The aerobic biodegradability of the mono-fluorophenols decreased in the order of 4- fluorop- henol〉3 - fluorophenol 〉2 - fluorophenol, resulting mainly from the different octanol/water partition coefficient and the different steric parameter of the fluorophenols which can affect the penetration of fluorophenol into cell membrane.
基金supported by the National Natural Science Foundation of China (Grant No.10704083)
文摘The ultrafast dynamics of o-fluorophenol via the excited states has been studied by femtosecond time-resolved photoelectron imaging. The photoion and photoelectron spectra taken with a time delay between 267 nm pump laser and 800 nm probe laser provide a longer-lived S1 electronic state of about ns timescale. In comparison,the spectra obtained by exciting the S2 state with femtosecond laser pulses at 400 nm and ionizing with pulses at 800 nm suggest that the S2 state has an ultrashort lifetime about 102 fs and reflects the internal conversion dynamics of the S2 state to the S1 state.
