Synthesis, Characterization and Catalytic Fuel Ultra-Deep Desulfurization of Keggin-Type Polyoxometalates
Synthesis, Characterization and Catalytic Fuel Ultra-Deep Desulfurization of Keggin-Type Polyoxometalates
复制标题
Keggin型多金属氧酸盐的合成、表征及催化燃料超深度脱硫
DOI：
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发表时间：
2014
影响因子：
0.7
通讯作者：
王睿
中科院分区：
文献类型：
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作者：
刘日嘉;刘日嘉;刘日嘉;王睿;王睿;王睿
以六种金属盐和磷钨酸盐为原料，制备了Keggin多金属氧酸盐催化剂Mx/nH0.6PW(Zr0.6H0.6PW、Al0.8H0.6PW、Zn1.2H0.6PW、Fe0.8H0.6PW、Ti0.6H0.6PW和Sn0.6H0.6PW)和Alx/3H3-xPW(AlPW、Al0.8H0.6PW、Al0.5H1.5PW、Al0.3H2.1PW和Al0.1H2.7PW)。采用FTIR、X射线衍射仪、DSC/TGA和电感耦合等离子体对催化剂进行了表征。从催化活性筛选结果来看，Al0.5H1.5PW是最好的催化剂。以过氧化氢为氧化剂，乙腈为萃取剂，对燃料超深度脱硫催化氧化萃取进行了研究。考察了催化剂用量、O/S摩尔比、催化剂在H_2O_2溶液中的预浸时间、反应温度和初始硫含量对脱硫效率的影响。结果表明，在Al0.5H1.5PW催化剂/模拟柴油用量为0.25%(m/m)，O/S摩尔比为10，催化剂在H_2O_2溶液中预浸时间为8min，反应温度为60℃，初始硫含量为350 mg·L~(-1)的条件下，脱硫率为99.3%，脱硫率为99.3%。氧化萃取法的脱硫效率远高于纯萃取法(提高45.3%)。此外，Al0.5H1.5PW催化剂对实际汽油和柴油催化氧化脱硫均取得了很好的脱硫效果，5次循环后脱硫效率没有明显下降。
Keggin-type polyoxometalate catalysts Mx/nH0.6PW(Zr0.6H0.6PW, Al0.8H0.6PW, Zn1.2H0.6PW, Fe0.8H0.6PW, Ti0.6H0.6PW and Sn0.6H0.6PW) and Alx/3H3-xPW(AlPW, Al0.8H0.6PW, Al0.5H1.5PW, Al0.3H2.1PW and Al0.1H2.7PW) were prepared using 6 metal salts and phosphotungstate. The prepared catalysts were characterized by FTIR, XRD, DSC/ TGA and ICP. Al0.5H1.5PW is the best catalyst based on the catalytic activity screening results. The catalytic oxidation extraction for fuel ultra-deep desulfurization was studied using hydrogen peroxide as the oxidant and MeCN as the extractant. The effect of catalyst dosage, O/S molar ratio, pre-immersion time of the catalyst in H2O2solution, reaction temperature and initial sulfur content on the desulfurization efficiency was studied. The results show that the sulfur content of simulated diesel is reduced from 350 mg·L-1to 2.45 mg·L-1with a desulfurization efficiency of 99.3% at 60 min under the following operating conditions: Al0.5H1.5PW catalyst/simulated diesel, 0.25%(m/m); molar ratio of O/S= 10; pre-immersion time of the catalyst in H2O2solution, 8 min; reaction temperature, 60 ℃; initial sulfur content, 350 mg·L-1. The efficiency of the oxidation extraction desulfurization is much higher than that of extraction only(45.3% higher). Moreover, very good desulfurization efficiency is obtained for real gasoline and diesel catalytic oxidative desulfurization over Al0.5H1.5PW catalyst, and the desulfurization efficiency is not reduced obviously after 5 cycles.