• Highly efficient debromination of BDE-47 was achieved in the ZVZ/AA system.• BDE-47 debromination by the ZVZ/AA can be applied to a wide range of pH.• AA inhibits the formation of (hydr)oxide and accelerates the corrosion of ZVZ.• Reduction mechanism of BDE-47 debromination by the ZVZ/AA system was proposed. A new technique of zero-valent zinc coupled with ascorbic acid (ZVZ/AA) was developed and applied to debrominate the 2,2′,4,4′-Tetrabromodiphenyl ether (BDE-47), which achieved high conversion and rapid debromination of BDE-47 to less- or non-toxic forms. The reaction conditions were optimized by the addition of 100 mg/L ZVZ particles and 3 mmol/L AA at original solution pH= 4.00 using the solvent of methanol/H2O (v:v= 4:6), which could convert approximately 94% of 5 mg/L BDE-47 into lower-brominated diphenyl ethers within a 90 min at the ZVZ/AA system. The high debromination of BDE-47 was mainly attributed to the effect of AA that inhibits the formation of Zn(II)(hydr)oxide passivation layers and promotes the corrosion of ZVZ, which leads to increase the reactivity of ZVZ. Additionally, ion chromatography and gas chromatography mass spectrometry analyses revealed that bromine ion and lower-debromination diphenyl ethers formed during the reduction of BDE-47. Furthermore, based on the generation of the intermediates products, and its concentration changes over time, it was proposed that the dominant pathway for conversion of BDE-47 was sequential debromination and the final products were diphenyl ethers. These results suggested that the ZVZ/AA system has the potential for highly efficient debromination of BDE-47 from wastewater. 相似文献
• Sulfidation significantly enhanced As(V) immobilization in soil by zerovalent iron.• S-ZVI promoted the conversion of exchangeable As to less mobile Fe-Mn bound As.• Column test further confirmed the feasibility of sulfidated ZVI on As retention.• S-ZVI amendment and magnetic separation markedly reduced TCLP leachability of As. In this study, the influences of sulfidation on zero-valent iron (ZVI) performance toward As(V) immobilization in soil were systemically investigated. It was found that, compared to unamended ZVI, sulfidated ZVI (S-ZVI) is more favorable to immobilize As(V) in soil and promote the conversion of water soluble As to less mobile Fe-Mn bound As. Specifically, under the optimal S/Fe molar ratio of 0.05, almost all of the leached As could be sequestrated by>0.5 wt.% S-ZVI within 3 h. Although the presence of HA could decrease the desorption of As from soil, HA inhibited the reactivity of S-ZVI to a greater extent. Column experiments further proved the feasibility of applying S-ZVI on soil As(V) immobilization. More importantly, to achieve a good As retention performance, S-ZVI should be fully mixed with soil or located on the downstream side of As migration. The test simulating the flooding conditions in rice culture revealed there was also a good long-term stability of soil As(V) after S-ZVI remediation, where only 0.7% of As was desorbed after 30 days of incubation. Magnetic separation was employed to separate the immobilized As(V) from soil after S-ZVI amendment, where the separation efficiency was found to be dependent of the iron dosage, liquid to soil ratio, and reaction time. Toxicity characteristic leaching procedure (TCLP) tests revealed that the leachability of As from soil was significantly reduced after the S-ZVI amendment and magnetic separation treatment. All these findings provided some insights into the remediation of As(V)-polluted soil by ZVI. 相似文献
• N-doped activated carbon was prepared for catalytic pyrolysis of walnut shell.• Alkylphenols were selectively produced from catalytic pyrolysis process.• The alkylphenols yield increased by 8.5 times under the optimal conditions.• Formation mechanism of alkylphenols was proposed. Alkylphenols are a group of valuable phenolic compounds that can be derived from lignocellulosic biomass. In this study, three activated carbons (ACs) were prepared for catalytic fast pyrolysis (CFP) of walnut shell to produce alkylphenols, including nitrogen-doped walnut shell-derived activated carbon (N/WSAC), nitrogen-doped rice husk-derived activated carbon (N/RHAC) and walnut shell-derived activated carbon (WSAC). Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) experiments were carried out to reveal the influences of AC type, pyrolytic temperature, and AC-to-walnut shell (AC-to-WS) ratio on the product distributions. Results showed that with nitrogen doping, the N/WSAC possessed stronger capability than WSAC toward the alkylphenols production, and moreover, the N/WSAC also exhibited better effects than N/RHAC to prepare alkylphenols. Under the catalysis of N/WSAC, yields of alkylphenols were significantly increased, especially phenol, cresol and 4-ethylphenol. As the increase of pyrolytic temperature, the alkylphenols yield first increased and then decreased, while high selectivity could be obtained at low pyrolytic temperatures. Such a trend was also observed as the AC-to-WS ratio continuously increased. The alkylphenols production achieved a maximal yield of 44.19 mg/g with the corresponding selectivity of 34.7% at the pyrolytic temperature of 400°C and AC-to-WS ratio of 3, compared with those of only 4.67 mg/g and 6.1% without catalyst. In addition, the possible formation mechanism of alkylphenols was also proposed with the catalysis of N/WSAC. 相似文献