CeO2-ZnO/KIT-6催化剂在光催化吸附脱硫中的应用
收稿日期: 2022-03-25
网络出版日期: 2022-09-22
基金资助
国家自然科学基金(21503152);武汉工程大学科学研究基金(K201640);武汉工程大学科学研究基金(K201760)
Application of CeO2-ZnO/KIT-6 catalyst in photocatalytic adsorption desulfurization
Received date: 2022-03-25
Online published: 2022-09-22
光催化吸附脱硫技术在油品脱硫领域引起了极大的关注，具有高光催化活性和有机硫化物吸附能力的双功能材料的开发是关键。首次合成了3D介孔二氧化铈-氧化锌/KIT-6（CeO2-ZnO/KIT-6）催化剂，并应用于二苯并噻吩（DBT）的光催化吸附脱硫。通过X射线衍射（XRD）、氮气吸附-脱附和透射电子显微镜（TEM）等手段对催化剂进行表征，并研究了催化剂在光照下对DBT的转化性能。实验结果表明，在没有额外添加氧化剂（例如氧气、过氧化氢或有机氧化剂）的情况下，CeO2-ZnO/KIT-6具有很好的光催化脱硫能力，当二氧化铈质量分数为10%、氧化锌质量分数为15%时，催化剂CeO2-ZnO/KIT-6对DBT的转化率可达90%，最大吸附量（以硫计）为8.1 mg/g。无氧化剂体系对于燃料的后续处理非常有利，并且可以明显降低脱硫成本。
张哲 , 廖明宇 , 陈铭 , 喻珊珊 , 周康帝 , 李佳纯 , 张林锋 , 吴华东 , 郭嘉 . CeO2-ZnO/KIT-6催化剂在光催化吸附脱硫中的应用[J]. 无机盐工业, 2022 , 54(9) : 143 -149 . DOI: 10.19964/j.issn.1006-4990.2022-0142
Photocatalytic adsorption desulfurization technology has attracted great attention in the field of oil desulfurization.The development of bifunctional materials with high photocatalytic activity and organic sulfide adsorption capacity is the key.3D mesoporous ceria oxide-zinc oxide/KIT-6（CeO2-ZnO/KIT-6） catalyst was synthesized for the first time and applied to the photocatalytic adsorption desulfurization of dibenzothiophene（DBT）.The catalyst was characterized by X-ray diffraction（XRD），nitrogen adsorption desorption and transmission electron microscope（TEM），and the conversion performance of the catalyst to DBT under light was studied.The experimental results showed that CeO2-ZnO/KIT-6 had good photocatalytic desulfurization ability without adding additional oxidants（such as oxygen，hydrogen peroxide or organic oxidants）.When the mass fraction of cerium dioxide was 10% and the mass fraction of zinc oxide was 15%，the conversion of DBT by CeO2-ZnO/KIT-6 catalyst could reach 90%，and the maximum adsorption capacity（calculated by sulfur） was 8.1 mg/g.The oxidant free system was very beneficial to the subsequent treatment of fuel and could significantly reduce the desulfurization cost.
Key words： photocatalysis; desulfurization; KIT-6; ZnO; CeO2
| [1] | 杨闯闯，杨清河，孙谦.加氢脱硫催化剂制备方法研究进展[J].工业催化，2021，29（8）:1-6. |
| [1] | YANG Chuangchuang， YANG Qinghe， SUN Qian.Research progress on preparation methods of hydrodesulfurization catalysts[J].Industrial Catalysis，2021，29（8）:1-6. |
| [2] | ZENG Xingye， XIAO Xinyan， LI Yang， et al.Deep desulfurization of liquid fuels with molecular oxygen through graphene photocatalytic oxidation[J].Applied Catalysis B:Environmental，2017，209:98-109. |
| [3] | 岳源源，郑晓桂，康颖，等.基于镁铝水滑石的Mo/Al2O3-MgO催化剂制备及其加氢脱硫性能[J].化工学报，2018，69（1）:405-413. |
| [3] | YUE Yuanyuan， ZHENG Xiaogui， KANG Ying， et al.Mo/Al2O3-MgO catalyst preparation from MgAl-hydrotalcite and their hydrogenation desulfurization performance[J].CIESC Journal，2018，69（1）:405-413. |
| [4] | 杨丽娜，张熙，郭永成，等.TiO2-g-C3N4/BMMS光催化氧化脱硫催化剂[J].硅酸盐学报，2021，49（3）:528-536. |
| [4] | YANG Lina， ZHANG Xi， GUO Yongcheng， et al.TiO2-g-C3N4/BMMS photocatalytic oxidation desulfurization catalyst[J].Journal of the Chinese Ceramic Society，2021，49（3）:528-536. |
| [5] | EBADI M， ASRI M， BESHKAR F.Novel Mo/Bi2MoO6/Bi3ClO4 heterojunction photocatalyst for ultra?deep desulfurization of thiophene under simulated sunlight irradiation[J].Advanced Powder Technology，2021，32（7）:2160-2170. |
| [6] | GUO Guoqing， GUO Haiyang， WANG Feng， et al.Dye-sensitized TiO2@SBA-15 composites:Preparation and their application in photocatalytic desulfurization[J].Green Energy & Environment，2020，5（1）:114-120. |
| [7] | 李剑，王雪莹，黄鑫，等.CuWO4/SBA-15催化剂的制备及其光催化氧化脱硫性能[J].燃料化学学报，2020，48（5）:632-640. |
| [7] | LI Jian， WANG Xueying， HUANG Xin， et al.Preparation of the CuWO4/SBA-15 catalyst and its performance in the photocatalytic oxidation desulfurization[J].Journal of Fuel Chemistry and Technology，2020，48（5）:632-640. |
| [8] | 李飞虹，李霞章，陆晓旺，等.钒掺杂磷酸铋/蒙脱石复合材料的制备及可见光催化脱硫性能[J].硅酸盐学报，2018，46（2）:275-280. |
| [8] | LI Feihong， LI Xiazhang， LU Xiaowang， et al.Preparation of vanadium doped bismuth phosphate/montmoril lonite nanocomposites for visible light photocatalytic desulfurization[J].Journal of the Chinese Ceramic Society，2018，46（2）:275-280. |
| [9] | KLEITZ F， CHOI S H， RYOO R.Cubic Ia3-d large mesoporous silica:Synthesis and replication to platinum nanowires，carbon nanorods and carbon nanotubes[J].Chemical Communications:Cambridge，England，2003（17）:2136-2137. |
| [10] | HUSSAIN M， AKHTER P， SARACCO G， et al.Nanostructured TiO2/KIT-6 catalysts for improved photocatalytic reduction of CO2 to tunable energy products[J].Applied Catalysis B:Environmental，2015，170/171:53-65. |
| [11] | SUBHAN F， ASLAM S， YAN Zifeng， et al.Size regulation and dispersion of ceria using confined spaces for adsorptive desulfurization[J].Chemical Engineering Journal，2018，348:319-326. |
| [12] | SUBHAN F， ASLAM S， YAN Zifeng， et al.Facile functionalization of 3-D ordered KIT-6 with cuprous oxide for deep desulfurization[J].Chemical Engineering Journal，2017，330:372-382. |
| [13] | 左士祥，吴红叶，刘文杰，等.凹凸棒石/g-C3N4/LaCoO3复合材料的制备及其光催化脱硫性能[J].硅酸盐学报，2020，48（5）:753-760. |
| [13] | ZUO Shixiang， WU Hongye， LIU Wenjie， et al.Preparation of attapulgite/g-C3N4/LaCoO3 composites and their performance of photocatalytic desulfurization[J].Journal of the Chinese Ceramic Society，2020，48（5）:753-760. |
| [14] | ZHANG Juan， ZHAO Dishun， MA Zhen， et al.Phase-boundary photocatalytic oxidation of dibenzothiophene over amphiphilic Ti-MCM-41 molecular sieve[J].Catalysis Letters，2010，138（1/2）:111-115. |
| [15] | ONG C B， NG L Y， MOHAMMAD A W.A review of ZnO nanoparticles as solar photocatalysts:Synthesis，mechanisms and applications[J].Renewable and Sustainable Energy Reviews，2018，81:536-551. |
| [16] | 胡敏，郭嘉，吴华东，等.N-Zn/TiO2光催化氧化脱硫废液中亚硫酸钠的研究[J].无机盐工业，2020，52（10）:151-156. |
| [16] | HU Min， GUO Jia， WU Huadong， et al.Photocatalytic oxidation of sodium sulfite in desulfurization wastewater by N-Zn/TiO2 [J].Inorganic Chemicals Industry，2020，52（10）:151-156. |
| [17] | ZHANG Qian， ZHAO Xiaoru， DUAN Libing， et al.Controlling oxygen vacancies and enhanced visible light photocatalysis of CeO2/ZnO nanocomposites[J].Journal of Photochemistry and Photobiology A:Chemistry ，2020，392.Doi:10.1016/j.jphotochem.2019.112156. |
| [18] | VISUVAMITHIRAN P， PALANICHAMY M， SHANTHI K， et al.Selective epoxidation of olefins over Co（Ⅱ）-Schiff base immobilised on KIT-6[J].Applied Catalysis A:General，2013，462/463:31-38. |
| [19] | WANG Quan， XIE Wenlei， GUO Lihong.Molybdenum and zirconium oxides supported on KIT-6 silica:A recyclable composite catalyst for one?pot biodiesel production from simulated low?quality oils[J].Renewable Energy，2022，187:907-922. |
| [20] | SUBHAN F， ASLAM S， YAN Zifeng， et al.Enhanced desulfurization characteristics of Cu-KIT-6 for thiophene[J].Microporous and Mesoporous Materials，2014，199:108-116. |
| [21] | LIU Yang， LI Peng， XUE Ruiting， et al.Research on catalytic performance and mechanism of Ag2O/ZnO heterostructure under UV and visible light[J].Chemical Physics Letters，2020，746.Doi:10.1016/j.cplett.2020.137301. |
| [22] | 岳明月，朱佳，李天保，等.CeO2/CuBi2O4异质结的制备及其光催化性能研究[J].功能材料，2021，52（8）:8001-8007. |
| [22] | YUE Mingyue， ZHU Jia， LI Tianbao， et al.Preparation of CeO2/CuBi2O4 heterojunctions and their photocatalytic properties[J].Journal of Functional Materials，2021，52（8）:8001-8007. |
| [23] | 刘同慧，刘宏乾，褚格，等.CaO/KIT-6固体碱催化剂的制备及其在酯交换反应中的催化性能[J].燃料化学学报，2021，49（3）:321-328. |
| [23] | LIU Tonghui， LIU Hongqian， CHU Ge， et al.Preparation of CaO/KIT-6 solid base catalyst and its catalytic performance in transesterification[J].Journal of Fuel Chemistry and Technology，2021，49（3）:321-328. |
| [24] | 史亚卜，张国强，孙宇辰，等.KIT-6负载CeO2催化CO2和甲醇合成碳酸二甲酯[J].无机化学学报，2021，37（6）:1004-1016. |
| [24] | SHI Yabo， ZHANG Guoqiang， SUN Yuchen， et al.KIT-6 supported CeO2 for catalytic synthesis of dimethyl carbonate from CO2 and methanol[J].Chinese Journal of Inorganic Chemistry，2021，37（6）:1004-1016. |
| [25] | MUNAWAR T， MUKHTAR F， NADEEM M S， et al.Novel photocatalyst and antibacterial agent；direct dual Z-scheme ZnO-CeO2-Yb2O3 heterostructured nanocomposite[J].Solid State Sciences，2020，109.Doi:10.1016/j.solidstatesciences.2020.106446. |
| [26] | SIRAJ Z， MAAFA I M， SHAFIQ I， et al.KIT-6 induced mesostructured TiO2 for photocatalytic degradation of methyl blue[J].Environmental Science and Pollution Research International，2021，28（38）:53340-53352. |
| [27] | WANG Sihua， ZU Yun， QIN Yucai， et al.Fabrication of effective desulfurization species active sites in the CeY zeolites and the adsorption desulfurization mechanisms[J].Journal of Fuel Chemistry and Technology，2020，48（1）:52-62. |
| [28] | MIAO Guang， HUANG Dishun， REN Xiaoling， et al.Visible-light induced photocatalytic oxidative desulfurization using BiVO4/C3N4@SiO2 with air/cumene hydroperoxide under ambient conditions[J].Applied Catalysis B:Environmental，2016，192:72-79. |
| [29] | LI Xin， XU Yilin， ZHANG Chen， et al.H2O2-assisted hydrothermal synthesis of TiO2-SiO2 and its enhanced photocatalytic?adsorptive desulfurization performance for model fuel[J].Fuel， 2018，226:527-535. |
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