张丹^1,2,赵振涛²,王宁²,尚润梅²,邢锦娟²,李君华^1,2

• 1:辽宁石油化工大学 石油化工学院，辽宁 抚顺 113001
• 2:渤海大学 化学与材料工程学院，辽宁 锦州 121013

摘要(Abstract)：

为了研究ZSM-5分子筛中硅铝物质的量比变化对TiO₂/ZSM-5光催化性能的影响，通过水热合成法制备了5种不同硅铝比的ZSM-5分子筛，并以此为载体通过浸渍-煅烧法制备了TiO₂/ZSM-5复合材料。对制备材料的物化性能以及光电学性能进行了分析，并对光催化实验中的活性组分进行了研究。结果表明：当ZSM-5分子筛中硅铝物质的量比为120时，制备的TiO₂/ZSM-5复合材料吸附性较好，负载TiO₂后光响应程度最高，光生电子(e^-)和空穴(h⁺)复合率低且电阻最小， 紫外光照100 min时罗丹明B(Rh-B)的降解率为99.6%，TOC去除率为60.4%。同时，实验发现羟基自由基(·O₂^-)是光催化反应过程中的主要活性组分。

关键词(KeyWords)： 硅铝比;光催化;TiO₂/ZSM-5;罗丹明B

Abstract:

Keywords:

基金项目(Foundation): 国家自然科学基金(21606117)；辽宁省重点研发计划(2020JH2/10100008)。

作者(Author): 张丹^1,2,赵振涛²,王宁²,尚润梅²,邢锦娟²,李君华^1,2

DOI: 10.3969/j.issn.1003-9015.2023.02.011

参考文献(References)：

• [1] SHAYEGAN Z, HAGHIGHAT F, LEE C S. Carbon-doped TiO₂ film to enhance visible and UV light photocatalytic degradation of indoor environment volatile organic compounds[J]. Journal of Environmental Chemical Engineering, 2020, 8(5):104162.
  [2] AKBARI A, SABOURI Z, HOSSEINI H A, et al. Effect of nickel oxide nanoparticles as a photocatalyst in dyes degradation and evaluation of effective parameters in their removal from aqueous environments[J]. Inorganic Chemistry Communications, 2020, 115:107867.
  [3] HOU H L, ZHANG X W. Rational design of 1D/2D heterostructured photocatalyst for energy and environmental applications[J]. Chemical Engineering Journal, 2020, 395:125030.
  [4] 张翠平, 刘娟. C-PANI/Ag/Ag₃PO₄复合材料增强可见光光催化性能[J]. 高校化学工程学报, 2017, 31(3):618-625. ZHANG C P, LIU J. Preparation of C-PANI/Ag/Ag₃PO₄ with enhanced visible light photocatalytic activity[J]. Journal of Chemical Engineering of Chinese Universities, 2017, 31 (3):618-625.
  [5] ZAINUDIN N F, ABDULLAH A Z, MOHAMED A R. Characteristics of supported nano-TiO₂/ZSM-5/silica gel(SNTZS):photocatalytic degradation of phenol[J]. Journal of Hazardous Materials, 2010, 174(1/2/3):299-306.
  [6] REN L, LI Y Z, MAO M Y, et al. Significant improvement in photocatalytic activity by forming homojunction between anatase TiO₂ nanosheets and anatase TiO₂ nanoparticles[J]. Applied Surface Science, 2019, 490:283-292.
  [7] CHEN R, YANG C J, ZHANG Q Q, et al. Visible-light-driven selective oxidation of glucose in water with H-ZSM-5 zeolite supported biomimetic photocatalyst[J]. Journal of Catalysis, 2019, 374:297-305.
  [8] 郭鹏. TiO₂/ZSM-5复合光催化剂的制备及性能研究[D]. 大连:大连理工大学, 2010. GUO P. Study on the preparation and performance of TiO₂/ZSM-5 composite photocatalyst[D]. Dalian: Dalian University of Technology, 2010.
  [9] 刘粤, 车庆丰, 易为, 等. 微介孔Ni/ZSM-5分子筛对甲苯催化重整的影响[J]. 可再生能源, 2021, 39(4):427-433. LIU Y, CHE Q F, YI W, et al. Effect of micro-mesoporous Ni/ZSM-5 zeolites on catalytic reforming of toluene[J]. Renewable Energy Resources, 2021, 39(4):427-433.
  [10] 袁亚伟, 李勇. ZSM-5分子筛吸附剂应用于污染治理的研究进展[J]. 无机盐工业, 2019, 51(10):18-21. YUAN Y W, LI Y. Research progress of ZSM-5 molecular sieve adsorbents used in pollution control[J]. Inorganic Chemicals Industry, 2019, 51(10):18-21.
  [11] WAN Z J, WU W, LI G, et al. Effect of SiO₂/Al₂O₃ ratio on the performance of nanocrystal ZSM-5 zeolite catalysts in methanol to gasoline conversion[J]. Applied Catalysis A:General, 2016, 523:312-320.
  [12] 周梦雪, 肖永厚, 焉晓明, 等. 硅铝比和金属离子对ZSM-5吸附CO₂/N₂的Monte Carlo模拟的影响[J]. 现代化工, 2020, 40(11):87-91. ZHOU M X, XIAO Y H, YAN X M, et al. Influences of Si/Al ratio and metal ions on Monte Carlo simulation to adsorption of CO₂/N₂ by ZSM-5[J]. Modern Chemical Industry, 2020, 40(11):87-91.
  [13] ZHANG G, ZHANG T, LI B, et al. An ingenious strategy of preparing TiO₂/g-C₃N₄ heterojunction photocatalyst:In situ growth of TiO₂ nanocrystals on g-C₃N₄ nanosheets via impregnation-calcination method[J]. Applied Surface Science, 2018, 433:963-974.
  [14] XIN M D, XING E H, YANG Y Q, et al. Insight into interactions among P, Zn and ZSM-5 during bi-component modification on ZSM-5[J]. New Journal of Chemistry, 2020, 44(47):20785-20796.
  [15] WANG J, ZHANG R Z, HAN L N, et al. Seed-assisted synthesis and characterization of nano and micron ZSM-5 molecular sieves in template-free system[J]. Journal of Solid State Chemistry, 2020, 290:121536.
  [16] 刘军. 邻菲罗啉/TiO₂复合光催化材料的性能研究[D]. 南昌:南昌航空大学, 2018. LIU J. Performance study of the photocatalyst of phenanthroline/TiO₂[D]. Nanchang:Nanchang Hangkong University, 2018.
  [17] BALAKRISHNAN M, JOHN R. Properties of sol-gel synthesized multiphase TiO₂(AB)-ZnO(ZW) semiconductor nanostructure:An effective catalyst for methylene blue dye degradation[J]. Iranian Journal of Catalysis, 2020, 10(1):1-16.
  [18] BADVI K, JAVANBAKHT V. Enhanced photocatalytic degradation of dye contaminants with TiO₂ immobilized on ZSM-5 zeolite modified with nickel nanoparticles[J]. Journal of Cleaner Production, 2021, 280:124518.
  [19] FARGHALI A A, KHEDR M H, EL-DEK S I, et al. Synthesis and multifunctionality of (CeO₂-NiO) nanocomposites synthesized via sonochemical technique[J]. Ultrasonics Sonochemistry, 2018, 42:556-566.
  [20] 王宇航. NiFe₂O₄@TiO₂/RGO光催化剂的制备及催化性能研究[J]. 化学与生物工程, 2018, 35(8):45-49. WANG Y H. Preparation and photocatalytic performance of NiFe₂O₄@TiO₂/RGO and photocatalyst[J]. Chemistry & Bioengineering, 2018, 35(8):45-49.
  [21] LIN L, YANG Y, MEN L, et al. A highly efficient TiO₂@ZnO n-p-n heterojunction nanorod photocatalyst[J]. Nanoscale, 2013, 5(2):588-593.
  [22] 郭鹏, 刘春燕, 高敏, 等. ZSM-5晶粒度对其负载的TiO₂光催化剂性能的影响[J]. 催化学报, 2010, 31(5):573-578. GUO P, LIU C Y, GAO M, et al. Effect of ZSM-5 crystal size on properties of supported TiO₂ photocatalyst[J]. Chinese Journal of Catalysis, 2010, 31(5):573-578.
  [23] 余海湖, 余丁山, 李小甫, 等. 二氧化钛胶体及其自组装薄膜的光谱分析[J]. 光学学报, 2005, 25(10):131-134. YU H H, YU D S, LI X F, et al. Spectroscopic studies of colloidal TiO₂ and its self-assembled composite films[J]. Acta Optica Sinica, 2005, 25(10):131-134.
  [24] KHAN S, SINGH K. Structural, optical, thermal and conducting properties of V_2-xLi_xO_5-δ (0.15 ≤ x ≤ 0.30) systems[J]. Scientific Reports, 2020, 10(1):1089.
  [25] GUPTA N M, KELKAR S, KORAKE P. The quenching effect of uranyl species in the photoluminescence emission and visible-light-driven water dissociation activity of CdS and TiO₂ photocatalysts[J]. Photochemical & Photobiological Sciences, 2016, 15(6):758-766.
  [26] RAWOOL S A, PAI M R, BANERJEE A M, et al. pn Heterojunctions in NiO:TiO₂ composites with type-II band alignment assisting sunlight driven photocatalytic H₂ generation[J]. Applied Catalysis B:Environmental, 2018, 221:443-458.
  [27] ALSAIARI M. Biomass-derived active carbon (AC) modified TiO₂ photocatalyst for efficient photocatalytic reduction of chromium (VI)under visible light[J]. Arabian Journal of Chemistry, 2021, 14(8):103258.
  [28] 胡玉林, 李永进, 谢燕春, 等. 掺Ni铁酸铋纳米粉的制备及光催化性能[J]. 材料导报, 2020, 34(18):18009-18013. HU Y L, LI Y J, XIE Y C, et al. Preparation and photocatalytic properties of bismuth ferrite nano-powder doped with Ni[J]. Materials Review, 2020, 34(18):18009-18013.
  [29] LIU G, WANG G, HU Z, et al. Ag₂O nanoparticles decorated TiO₂ nanofibers as a p-n heterojunction for enhanced photocatalytic decomposition of RhB under visible light irradiation[J]. Applied Surface Science, 2019, 465:902-910.
  [30] ENDO-KIMURA M, JANCZAREK M, BIELAN Z, et al. Photocatalytic and antimicrobial properties of Ag₂O/TiO₂ heterojunction[J]. ChemEngineering, 2019, 3(1):3-20.