高洪成,王秀艳,张晓飞,刘云鹤,祁强,宋晓静.PW11M(M=Cu、Co)@TiO2多相催化剂的制备及氧化脱硫性能[J].分子催化编辑部,2019,33(5):438-446
PW11M(M=Cu、Co)@TiO2多相催化剂的制备及氧化脱硫性能
Preparation of PW11M(M=Cu, Co)@TiO2 Heterogeneous Catalysts and Oxidative Desulfurization Performance
投稿时间:2019-08-16  修订日期:2019-09-21
DOI:
中文关键词:  过渡金属  多金属氧酸盐  TiO2  多相催化  氧化脱硫
英文关键词:transition metal  polyoxometalate  TiO2  heterogeneous catalysis  oxidative desulfurization
基金项目:河北省自然科学青年基金(B2017411009)
作者单位E-mail
高洪成 承德石油高等专科学校 化学工程系, 河北 承德 067000  
王秀艳 承德石油高等专科学校 化学工程系, 河北 承德 067000  
张晓飞 承德石油高等专科学校 化学工程系, 河北 承德 067000  
刘云鹤 承德石油高等专科学校 化学工程系, 河北 承德 067000  
祁强 承德石油高等专科学校 化学工程系, 河北 承德 067000  
宋晓静 南阳理工学院 生物与化学工程学院, 河南 南阳 473004 583087487@qq.com 
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中文摘要:
      以过渡金属(Cu,Co)取代磷钨酸为模板剂,硫酸钛为钛源,通过一步模板法合成出一类多酸基PW11M(M=Cu、Co)@TiO2材料,采用FT-IR、XRD、XPS、Raman、SEM和TEM表征手段对材料进行了结构表征.结果表明,PW11M(M=Cu、Co)被引入到TiO2中,形成了球形核壳结构.N2吸附-脱附测试表明,PW11Co@TiO2具有介孔结构:孔径大小为3.3 nm,比表面积为72.4 m2/g.在以H2O2为氧化剂,乙腈为溶剂的氧化脱硫反应体系中考察了其催化活性,结果表明:复合材料PW11M(M=Cu、Co)@TiO2表现出良好的催化性能.其中催化剂PW11Co@TiO2在投入量为40 mg,反应底物为500 ppm,反应温度60℃,反应40 min后,DBT的脱硫率达到99.7%.中断和循环实验表明,催化剂PW11Co@TiO2具有良好的稳定性,在相同的反应条件下,循环反应5次后,催化剂的催化活性没有明显下降.
英文摘要:
      A polyoxometalate-based materials has been synthesized though the one-step template using transition metal (Cu, Co) substituted phosphotungstic acid as template and titanium sulfate as titanium source, denoted as PW11M (M=Cu, Co)@TiO2. Multiple characterization methods namely FT-IR, XRD, XPS, Raman, SEM and TEM were used to characterize the resultant materials, and results indicated that PW11M (M=Cu, Co) is introduced into TiO2, forming core-shell spherical structure. N2 adsorption-desorption test showed that PW11Co@TiO2 was mesoporous material with pore size of 3.3 nm and specific surface area of 72.4 m2/g. The catalytic properties of these materials were investigated in the oxidative desulfurization reaction system with H2O2 as oxidant and acetonitrile as solvent. The results showed that the PW11M (M=Cu, Co)@TiO2 exhibited good catalytic performance. The S-removal of DBT reached 99.7% after 40 min reaction at a temperature of 60℃ when dosage of catalyst PW11Co@TiO2 was 40 mg and reaction substrate was 500 mg/kg. Leaching and recycling experiments revealed that catalyst PW11Co@TiO2 had excellent stability, and there was no significant decrease in S-removal after five cycles under same reaction conditions.
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