Hexachloroethane dechlorination in sulfide-containing aqueous solutions catalyzed by nitrogen-doped carbon materials
This study demonstrated that nitrogen-doped carbon materials (NCMs) could effectively catalyze the chlorine elimination process in hexachloroethane (HCA) declorination in sulfide-containing environments for the first time. The kobs values of HCA dechlorination by sulfide in the presence of 10 mg/L N...
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Veröffentlicht in: | Environmental pollution (1987) 2021-07, Vol.281, p.116915-116915, Article 116915 |
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Sprache: | eng |
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Zusammenfassung: | This study demonstrated that nitrogen-doped carbon materials (NCMs) could effectively catalyze the chlorine elimination process in hexachloroethane (HCA) declorination in sulfide-containing environments for the first time. The kobs values of HCA dechlorination by sulfide in the presence of 10 mg/L NCMs were higher than that of no mediator at pH 7.3 by one or two orders of magnitude. The catalytic capabilities of NCMs on HCA dechlorination were evident in common ranges of natural pH (5.3–8.9) and it could be accelerated by the increase of pH but be suppressed by the presence of dissolved humic acid. Moreover, NCMs exhibited much better catalytic capability on HCA dechlorination compared to the carbon materials, mainly owing to the combined contributions of pyridine N, including enhanced nucleophilic attack to HCA molecule by generating newborn C–S–S and activation of HCA molecule by elongating C–Cl bonds. The functions of pyridine N in micron-sized NCMs with mesopores were better than in nano-sized NCMs on HCA dechlorination. These findings displayed the potential of NCMs, when released into sulfide-containing environments, may significantly increase the dechlorination of chlorinated aliphatic hydrocarbons.
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•N-doped carbon materials have great catalytic ability on chlorine elimination process.•Catalytic effects evident under all natural pH ranges from 5.3 to 8.9.•N-doped carbon materials exhibit much better catalytic ability than carbon materials.•Pyridinic-N is responsible for the better catalytic capability.
NCMs have great catalytic abilities of chlorine elimination process in hexachloroethane dechlorination and their catalytic abilities are much better than that of CMs. |
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ISSN: | 0269-7491 1873-6424 |
DOI: | 10.1016/j.envpol.2021.116915 |