Catalytic Oxidative Desulfurization of Diesel Fuel Catalyzed by Quaternary Ammonium Phosphomolybdate
首发时间:2009-09-07
Abstract:Phosphomolybdic acid mixed with hexadecyl trimethyl ammonium chloride as the catalyst was prepared and evaluated for the oxidative desulfurization of straight-run diesel using hydrogen peroxide as an oxidant. Results of the FT-IR and SEM analyses indicated that the catalyst keeps the entire Keggin structure of phosphomolybdic acid. The catalyst can oxidize the sulfur-containing molecules into sulfones with desulfurization rate of 84.6% and diesel recovery rate of 98.1% in 2 h. Orthogonal test and single factor analysis showed that the catalyst dosage, hydrogen peroxide dosage, reaction temperature and reaction time are the main influential factors for oxidative desulfurization, and the influential factors order is: reaction time > reaction temperature > hydrogen peroxide dosage > catalyst dosage. Increasing extraction times, the desulfurization rates increased, but the recovery rates of diesel declined notably. The proposed catalytic oxidative mechanism of organosulfur compounds contains two steps, the active center Mo(Ⅵ) attacked by hydrogen peroxide catalyzes sulfide to form sulfoxide and subsequent oxidation of sulfoxide to produce sulfone.
keywords: Oxidative desulfurization diesel fuel quaternary ammonium salts phosphomolybdic acid mechanism
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磷钼酸季铵盐催化柴油氧化脱硫研究
摘要:以磷钼酸掺杂十六烷基三甲基氯化铵作为催化剂,以过氧化氢作为氧化剂,研究了直馏柴油的催化氧化脱硫反应。FT-IR 和 SEM结果显示磷钼酸掺杂季铵盐后保持了其Keggin结构。催化反应2小时后柴油的脱硫率达到84.6%,收率为98.1%。正交试验和单因素分析显示,各反应条件对直馏柴油脱硫率的影响顺序为:反应时间 > 反应温度 > 氧化剂用量 > 催化剂用量。提高萃取次数,柴油的脱硫率提高了,但回收率却明显下降.在氧化脱硫过程中,首先过氧化氢亲核进攻催化剂的活性中心Mo(VI),然后氧化噻吩类形成亚砜,最后亚砜进一步被氧化生成砜.
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No.3497649013012523****
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