摘要
为了提高TiO_(2)的光催化氧化脱硫(PODS)活性,利用负载和复合的协同作用,将TiO_(2)与g-C_(3)N_(4)复合,并负载于双介孔二氧化硅(BMMS)上,制备了TiO_(2)–g-C_(3)N_(4)/BMMS。以含二苯并噻吩(DBT)的十二烷溶液为模拟油,评价了催化剂的催化性能;优化了反应条件并提出了催化反应机理。结果表明:TiO_(2)–g-C_(3)N_(4)/BMMS具有明显的双介孔结构,TiO_(2)与g-C_(3)N_(4)已实现复合并负载于BMMS上,TiO_(2)–g-C_(3)N_(4)活性组分在载体上分散良好,与单一TiO_(2)相比对光的吸收能力增强,催化活性有明显提高,优化后的反应条件为,催化剂用量3%(质量分数),O/S摩尔比为10:1,萃取剂与模拟油体积比为1:1,此时脱硫率可达96.6%,且重复使用8次后脱硫率仍保持85%以上,PODS过程中的主要活性中间物种是·O_(2)^(–)和h^(+)。
In order to improve the photocatalytic oxidative desulfurization(PODS) activity of TiO_(2), a composite of TiO_(2) and g-C_(3)N_(4) was supported on bimodal mesoporous silica(BMMS) to synthesize TiO_(2)–g-C_(3)N_(4)/BMMS. The dodecane solution of dibenzothiophene(DBT) was used as a simulated oil to evaluate the catalytic performance of the samples. The reaction conditions were optimized and the catalytic reaction mechanism was proposed. The results show that TiO_(2)–g-C_(3)N_(4)/BMMS has a bimodal mesoporous structure. As an active composite, TiO_(2)–g-C_(3)N_(4) can be dispersed on BMMS. Compared to pure TiO_(2), the light absorption ability of TiO_(2)–g-C_(3)N_(4)/BMMS is enhanced and the catalytic activity is improved. The desulfurization rate of TiO_(2)–g-C_(3)N_(4)/BMMS obtained under optimized reaction conditions(i.e., the catalyst amount of 3%(in mass fraction), the molar ratio of O:S of 10:1, and the volume ratio of solvent to oil of 1:1) can reach 96.6%, and the desulfurization rate remains more than 85% after 8-run repeated reactions. The main active species in the PODS process are ·O_(2)^(–) and h^(+).
作者
杨丽娜
张熙
郭永成
崔莉程
李剑
YANG Lina;ZHANG Xi;GUO Yongcheng;CUI Licheng;LI Jian(School of Petrochemical Engineering,Liaoning Shihua University,Fushun 113001,Liaoning,China;Washing Plant,PetroChina Fushun Petrochemical Company,Fushun 113001,Liaoning,China;Petrochina Liaoyang Petrochemical Company,Liaoyang 111003,China)
出处
《硅酸盐学报》
EI
CAS
CSCD
北大核心
2021年第3期528-536,共9页
Journal of The Chinese Ceramic Society
基金
辽宁省高等学校杰出青年学者成长计划项目(LJQ2015062)
辽宁省科学技术厅项目(20170540585)
辽宁省教育厅项目(L2015296,L2016018)
抚顺市科技计划项目(FSKJHT201376)。
关键词
光催化氧化脱硫
二氧化钛
氮化碳
双介孔分子筛
复合
负载
photocatalytic oxidative desulfurization
titanium dioxide
graphitic carbon nitride
bimodal mesoporous molecular sieve
composites
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