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针对传统α-Fe_2O3光催化剂比表面积有限、氧空位(OVs)浓度偏低、光生载流子易复合等问题,通过引入一定量的SiO32-制备出具有高比表面积和丰富OVs的SiO32--α-Fe_2O3(SF)纳米片,并采用水热法构建了不同质量比的SF/CeO2异质结复合光催化剂.实验结果表明,SiO32-的引入有效提升了α-Fe_2O3的表面活性,异质结的构筑显著促进了光生载流子的分离与迁移.其中,m(SF)∶m(CeO2)=2:1的SF/CeO2-2复合物在可见光下活化过一硫酸氢钾(PMS)降解四环素(TC)的性能最优.机理分析证实,异质结、OVs和PMS活化的协同作用,可促进复合物降解体系中活性氧物种(reactive oxygen species,ROS)中的生成,从而实现了TC高效降解.本研究为高效可见光催化剂的设计及水环境中抗生素类污染物降解提供了新思路.
Abstract：Conventional α-Fe2 O3 photocatalysts are constrained by inherent limitations,including limited specific surface area,low oxygen vacancy(OVs) concentration,and rapid recombination of photogenerated charge carriers.To address these issues,SiO32- was introduced to fabricate SiO32--α-Fe2 O3(SF) nanosheets with enlarged specific surface area and abundant OVs.Subsequently,a series of SF/CeO2 heterojunction composite photocatalysts with varying mass ratios were constructed via a hydrothermal method.The experimental results showed that the surface activity of α-Fe2 O3 was effectively enhanced by the incorporation of SiO32- and the separation and interfacial migration of photogenerated electron-hole pairs were substantially facilitated by the construction of heterojunctions.The SF/CeO2-2 sample with a mass ratio of 2:1 for SF to CeO2 exhibited the optimal photocatalytic performance toward tetracycline(TC) degradation in a visiblelight-activated peroxymonosulfate(PMS) system.Mechanistic analysis confirmed that the generation of reactive oxygen species(ROS) was significantly promoted by the synergistic effect involving heterojunction interfacial charge transfer,OVs trapping,and PMS activation,thereby enabling efficient TC degradation.This work provides a new perspective for the rational design of highly efficient visible-light-responsive photocatalysts and the remediation of antibiotic-contaminated water environments.
[1] Chen Z J,Guo H,Liu H Y,et al.Construction of dual S-scheme Ag_2CO_3/Bi_4O_5I_2/g-C_3N_4 heterostructure photocatalyst with enhanced visible-light photocatalytic degradation for tetracycline[J].Chemical Engineering Journal,2022,438:135471.DOI:10.1016/j.cej.2022.135471.
[2]Ren X F,Wang Y B,Hu G C,et al.Improved PMS activation by natural sepiolite/Fe_3O_4 composite for effective tetracycline degradation:performance,mechanism and degradation pathway[J].Journal of Environmental Chemical Engineering,2024,12(1):111878.DOI:10.1016/j.jece.2024.111878.
[3] Wang A W,Ni J X,Wang W,et al.MOF Derived Co-Fe nitrogen doped graphite carbon@crosslinked magnetic chitosan Micro-nanoreactor for environmental applications:synergy enhancement effect of adsorption-PMS activation[J].Applied Catalysis B:Environmental,2022,319:121926.DOI:10.1016/j.apcatb.2022.121926.
[4]Yao C H,Wang Z H,Xu Z,et al.2D/2Dα-Fe_2O_3/single-layer MXene Schottky photocatalysis-PMS activation bidirectionally enhanced coupling system for environmental remediation[J].Journal of Alloys and Compounds,2023, 941:168920.DOI:10.1016/j.jallcom.2023.168 920.
[5] Chen P,Cheng Z L,Zhang X Z,et al.Fe-Mn bimetallic catalyst to activate peroxymonosulfate(PMS)for efficient degrada-tion of tetracycline:mechanism insights and application for pharmaceutical wastewater[J].Journal of Cleaner Production,2024,445:141365.DOI:10.1016/j.j clepro.2024.141365.
[6] Xu M H,Yang J J,Wang Y,et al.Novel urchin-like Co_5 Mn-LDH hierarchical nanoarrays:formation mechanism and its performance in PMS activation and norfloxacin degradation[J].Separation and Purification Technology,2022,300:121822.DOI:10.1016/j.seppur.2022.121822.
[7]Tang Q Y,Luo X L,Yang S Y,et al.Novel Z-scheme In_2S_3/BiVO_4 composites with improved visible-light photocatalytic performance and stability for glyphosate degradation[J].Separation and Purification Technology,2020,248:117039.DOI:10.1016/j.seppur.2020.117039.
[8] Liu J F,Zhang Y,Dong Y B,et al.Highly efficient photo-degradation for tetracycline elimination in pharmaceutical wastewater byα-Fe_2O_3/V_2O_5/BC assisted peroxy monosulfate activation[J].Separation and Purification Technology,2024,328:125034.DOI:10.1016/j.seppur.2023.125034.
[9] Wang Y Q,Li K,Shang M Y,et al.A novel partially carbonized Fe_3O_4@PANI-p catalyst for tetracycline degradation via peroxymonosulfate activation[J].Chemical Engineering Journal, 2023,451:138655.DOI:10.1016/j.cej.2022.138655.
[10] Huang F,Wang W L,Li G,et al.Exceptional degradation of organic pollutant through piezoelectric photocatalysis and peroxymonosulfate activation in the designed Bi_4O_5Br_2/BCZT S-scheme heteroj unction[J].Rare Metals,2025,44(6):3981-3994.DOI:10.1007/s12598-024-03203-9.
[11]Lin H G,Han X R,Tang Y H,et al.Tannic acid-mediated oxygen vacancies in broccoli-like CeO_2@carbon for enhanced photocatalytic peroxymonosulfate activation toward tetracycline degradation[J].Environmental Research,2026,288:123268.DOI:10.1016/j.envres.2025.123268.
[12] Zhang H L,Li M,Zhu C X,et al.Preparation of magneticα-Fe_2O_3/ZnFe_2O_4@Ti_3C_2 MXene with excellent photocatalytic performance[J].Ceramics International,2020,46(1):81-88.DOI:10.1016/j.ceramint.2019.08.236.
[13]Liu H T,Tong M L,Zhu K L,et al.Preparation and photo-Fenton degradation activity ofα-Fe_2O_3 nanorings obtained by adding H_2PO_4~-,SO_4~(2-),and citric acid[J].Chemical Engineering Journal,2020, 382:123010.DOI:10.1016/j.cej.2019.123010.
[14]Shao P H,Ren Z J,Tian J Y,et al.Silica hydrogel-mediated dissolution-recrystallization strategy for synthesis of ultrathinα-Fe_2O_3 nanosheets with highly exposed(110)facets:a superior photocatalyst for degradation of bisphenol S[J].Chemical Engineering Journal,2017,323:64-73.DOI:10.1016/j.cej.2017.04.069.
[15] Su W T,Liu X M,Tan L,et al.Rapid sterilization by photocatalytic Ag_3PO_4/α-Fe_2O_3 composites using visible light[J].ACS Sustainable Chemistry&Engineering,2020,8(6):2577-2585.DOI:10.1021/acssuschemeng.9b07615.
[16]刘祎涵,申紫玉,陈汝芬.高活性α-Fe_2O_3/BiOI复合物的制备及其光催化降解性能[J].河北师范大学学报(自然科学版),2025,49(5):487-495.DOI:10.13763/j.cnki.jhebnu.nse.202503014.Liu Yihan,Shen Ziyu,Chen Rufen.Preparation and photocatalytic degradation performance of highly activeα-Fe_2O_3/BiOI composites[J].Journal of Hebei Normal University(Natural Science),2025,49(5):487-495.
[17]Li Z,Zhang J F,Lv J L,et al.Sustainable synthesis of CeO_2/CdS-diethylenetriamine composites for enhanced photocatalytic hydrogen evolution under visible light[J].Journal of Alloys and Compounds,2018,758:162-170.DOI:10.1016/j.jallcom.2018.05.115.
[18] Shen J Y,Shen J,Zhang W J,et al.Built-in electric field induced CeO_2/Ti_3C_2-MXene Schottky-junction for coupled photocatalytic tetracycline degradation and CO2 reduction[J].Ceramics International,2019,45(18):24146-24153.DOI:10.1016/j.ceramint.2019.08.123.
[19]Krishnan A,Vishwanathan P V,Mohan A C,et al.Tuning of photocatalytic performance of CeO_2-Fe_2O_3 composite by Sn-doping for the effective degradation of methlene blue(MB)and methyl orange(MO)dyes[J].Surfaces and Interfaces,2021,22:100808.DOI:10.1016/j.surfin.2020.100808.
[20] He S,Yan C,Chen X Z,et al.Construction of core-shell heteroj unction regulatingα-Fe_2O_3 layer on CeO_2 nanotube arrays enables highly efficient Z-scheme photoelectrocatalysis[J].Applied Catalysis B:Environmental,2020, 276:119138.DOI:10.1016/j.apcatb.2020.119138.
[21] Lee B H,Park S,Kim M,et al.Reversible and cooperative photoactivation of single-atom Cu/TiO_2 photocatalysts[J].Nature Materials,2019,18(6):620-626.DOI:10.1038/s41563-019-0344-1.
[22]Zhu Y K,Lv C X,Yin Z C,et al.A[001]-oriented Hittorf's phosphorus nanorods/polymeric carbon nitride heterostruc-ture for boosting wide-spectrum-responsive photocatalytic hydrogen evolution from pure water[J].Angewandte Chemie International Edition,2020,59(2):868-873.DOI:10.1002/anie.201911503.
[23]Zhang P,Liu Y,Tian B Z,et al.Synthesis of core-shell structured CdS@CeO_2 and CdS@TiO_2 composites and comparison of their photocatalytic activities for the selective oxidation of benzyl alcohol to benzaldehyde[J].Catalysis Today,2017,281:181-188.DOI:10.1016/j.cattod.2016.05.042.
[24]Jia L M,Zhang Y,Wang C,et al.Defect-enriched(H_2PO_4~-,Cr~(3+))-α-Fe_2O_3/β-In_2S_3 composites for visible light degradation of 4-nitrophenol[J].Journal of Colloid and Interface Science,2023,643:528-540.DOI:10.1016/j.jcis.2023.03.092.
[25]Zhong Q,Sun Y,Wu S X,et al.Uniformed core-shell FeSe_(2+x)@C nanocube superlattices for Fenton-like reaction:coordinative roles of cation and anion[J].Applied Catalysis B:Environmental,2023,325:122357.DOI:10.1016/j.apcatb.2022.122357.
[26] Chen L,Xu Y M,Chen B L.In situ photochemical fabrication of CdS/g-C_3N_4 nanocomposites with high performance for hydrogen evolution under visible light[J].Applied Catalysis B:Environmental,2019,256:117848.DOI:10.1016/j.apcatb.2019.117848.
[27] Tan M X,Yu C Y,Luan Q J,et al.The Mott-Schottky heteroj unction MoC@NG@ZIS with enhanced kinetic response for promoting photocatalytic hydrogen production[J].Journal of Materials Chemistry A,2022,10(40):21465-21473.
[28] Ishikawa A,Takata T,Kondo J N,et al.Oxysulfide Sm_2Ti_2S_2O_5 as a stable photocatalyst for water oxidation and reduction under visible light irradiation(λ≤650 nm)[J].Journal of the American Chemical Society,2002,124(45):13547-13553.DOI:10.1021/ja0269643.
[29]Sun S M,Wang W Z,Li D Z,et al.Solar light driven pure water splitting on quantum sized BiVO_4 without any cocatalyst[J].ACS Catalysis,2014,4(10):3498-3503.DOI:10.1021/cs501076a.
[30] Liu D D,Chen D Q,Hao Z K,et al.Efficient degradation of Rhodamine B in water by CoFe_2O_4/H2O_2 and CoFe_2O_4/PMS systems:a comparative study[J].Chemosphere,2022,307:135935.DOI:10.1016/j.chemosphere.2022.135935.
基本信息:
DOI：10.13763/j.cnki.jhebnu.nse.202603013
中图分类号:O643.36;O644.1;X703
引用信息:
[1]申紫玉,刘祎涵,杨立盼,等.高活性SiO_3~(2-)-α-Fe_2O_3/CeO_2复合物的制备及其光催化降解四环素性能[J].河北师范大学学报(自然科学版)().DOI:10.13763/j.cnki.jhebnu.nse.202603013.
基金信息:
国家自然科学基金(21477032); 河北师范大学技术创新项目(L2021K02)
2026-07-20
2026-07-20
2026-07-20