Bi4O5Br2/Ti3C2-Ru复合光催化剂的合成及其对磺胺甲噁唑药物废水降解性能研究

摘要/Abstract

摘要： Bi_xO_yBr_z光催化剂在有机药物废水处理领域有着非常广阔的潜在应用价值,但光生电子-空穴对的快速复合限制了其应用。本文选用具有优良电子传递性能的Ti₃C₂作为助催化剂,首先利用Ti₃C₂表面丰富的Ti空位缺陷和高还原能力,制备了Ti₃C₂-Ru助催化剂,接着利用Ti₃C₂表面官能团与Bi³⁺的离子键合力实现了Bi₄O₅Br₂在Ti₃C₂-Ru表面的原位生长,得到Bi₄O₅Br₂/Ti₃C₂-Ru复合光催化剂,从而实现了电子由Bi₄O₅Br₂到Ti₃C₂再到反应活性位点Ru的定向传递,最终使催化剂具有较高的光生载流子分离率和较低的界面电荷转移阻力,有效抑制了光生电子-空穴对的复合。同时以磺胺甲噁唑(SMX)为模拟药物污染物进行了光催化性能测试,结果表明所制备的Bi₄O₅Br₂/Ti₃C₂-Ru复合光催化剂展示出了优异的光催化降解SMX性能,在可见光下照射75 min,SMX的降解率达到95.1%,相较于纯的Bi₄O₅Br₂和Bi₄O₅Br₂/Ti₃C₂催化剂,其降解率分别提升了36.9个百分点和25.3个百分点。最后基于自由基捕获实验和催化剂能带结构分析提出了所制催化剂的降解机理。研究结果可为构建具有药物废水净化功能的光催化剂提供设计思路。

关键词: Bi₄O₅Br₂/Ti₃C₂-Ru, 复合光催化剂, 磺胺甲噁唑, 电子-空穴-分离效率, 电子定向转移, 光催化降解

Abstract: Bi_xO_yBr_z photocatalysts display great application potential in the field of organic pharmaceutical wastewater treatment, but the high recombination rate of photogenerated electron-hole pairs limits their application. In this work, Ti₃C₂ with excellent electron transfer performance was selected as a cocatalyst. Firstly, Ti₃C₂-Ru cocatalyst was prepared by taking full use of abundant surface Ti vacancy defects and high reduction ability of Ti₃C₂, then Bi₄O₅Br₂/Ti₃C₂-Ru composite photocatalysts were prepared by realizing in-situ growth of Bi₄O₅Br₂ on Ti₃C₂-Ru surface through the ionic bonding force between Ti₃C₂ surface functional groups and Bi³⁺. This special structure ensures the directional transfer of electrons from Bi₄O₅Br₂ to Ti₃C₂ and then to the reaction active site of Ru, thereby the composite catalysts exhibit higher photogenerated carrier separation rate and lower interfacial charge transfer resistance, which effectively inhibit the recombination rate of photogenerated electron-hole pairs. The photocatalytic performance of composite photocatalysts were evaluated by the sulfamethoxazole (SMX) degradation efficiency. The results reveal that the Bi₄O₅Br₂/Ti₃C₂-Ru composite photocatalysts exhibit excellent photocatalytic performance on SMX degradation. The optimum removal efficiency of SMX reaches 95.1% under 75 min visible-light irradiation, which increase 36.9 percentage points of pure Bi₄O₅Br₂ and 25.3 percentage points of Bi₄O₅Br₂/Ti₃C₂, respectively. Finally, the underlying photocatalytic mechanism was elucidated based on the radical scavenging experiments and catalyst band structure. This results will provide a novel design idea for the construction of photocatalyst with pharmaceutical wastewater treatment capability.

Key words: Bi₄O₅Br₂/Ti₃C₂-Ru, composite photocatalyst, sulfamethoxazole, separation efficiency of electron-hole pair, electron directional transfer, photocatalytic degradation

中图分类号:

X131
X703.1

张雷, 李瑞, 樊彩梅. Bi₄O₅Br₂/Ti₃C₂-Ru复合光催化剂的合成及其对磺胺甲噁唑药物废水降解性能研究[J]. 人工晶体学报, 2022, 51(7): 1248-1256.

ZHANG Lei, LI Rui, FAN Caimei. Preparation of Bi₄O₅Br₂/Ti₃C₂-Ru Composite Photocatalysts and Their Degradation Performances for Sulfamethoxazole[J]. JOURNAL OF SYNTHETIC CRYSTALS, 2022, 51(7): 1248-1256.

参考文献

[1] 张文海,吉庆华,兰华春,等.BiOCl-(NH₄)₃PW₁₂O₄₀复合光催化剂制备及其光催化降解污染物机制[J].环境科学,2019,40(3):1295-1301.
ZHANG W H, JI Q H, LAN H C, et al. Preparation of BiOCl-(NH₄)₃PW₁₂O₄₀ photocatalyst and a mechanism for photocatalytic degradation of organic pollutants[J]. Environmental Science, 2019, 40(3): 1295-1301(in Chinese).
[2] LI R, LIU J X, ZHANG X F, et al. Iodide-modified Bi₄O₅Br₂ photocatalyst with tunable conduction band position for efficient visible-light decontamination of pollutants[J]. Chemical Engineering Journal, 2018, 339: 42-50.
[3] DI J, XIA J X, JI M X, et al. Controllable synthesis of Bi₄O₅Br₂ ultrathin nanosheets for photocatalytic removal of ciprofloxacin and mechanism insight[J]. Journal of Materials Chemistry A, 2015, 3(29): 15108-15118.
[4] CHEN Y Y, LI R P, GU Y, et al. Green and efficient degradation of cefoperazone sodium by Bi₄O₅Br₂ leading to the production of non-toxic products: performance and degradation pathway[J]. Journal of Environmental Sciences, 2021, 100: 203-215.
[5] YI F T, MA J Q, LIN C W, et al. Insights into the enhanced adsorption/photocatalysis mechanism of a Bi₄O₅Br₂/g-C₃N₄ nanosheet[J]. Journal of Alloys and Compounds, 2020, 821: 153557.
[6] LIAN W W, WANG L B, WANG X L, et al. Facile preparation of BiOCl/Ti₃C₂ hybrid photocatalyst with enhanced visible-light photocatalytic activity[J]. Functional Materials Letters, 2019, 12(1): 1850100.
[7] JIANG N, DU Y, JI P H, et al. Enhanced photocatalytic activity of novel TiO₂/Ag/MoS₂/Ag nanocomposites for water-treatment[J]. Ceramics International, 2020, 46(4): 4889-4896.
[8] AN X Q, WANG W, WANG J P, et al. The synergetic effects of Ti₃C₂ MXene and Pt as co-catalysts for highly efficient photocatalytic hydrogen evolution over g-C₃N₄[J]. Physical Chemistry Chemical Physics: PCCP, 2018, 20(16): 11405-11411.
[9] XUE Q, ZHANG H J, ZHU M S, et al. Photoluminescent Ti₃C₂ MXene quantum dots for multicolor cellular imaging[J]. Advanced Materials, 2017, 29(15): 1604847.
[10] WU X H, WANG Z Y, YU M Z, et al. Stabilizing the MXenes by carbon nanoplating for developing hierarchical nanohybrids with efficient lithium storage and hydrogen evolution capability[J]. Advanced Materials, 2017, 29(24): 1607017.
[11] ZHAO D, CHEN Z, YANG W J, et al. MXene (Ti₃C₂) vacancy-confined single-atom catalyst for efficient functionalization of CO₂[J]. Journal of the American Chemical Society, 2019, 141(9): 4086-4093.
[12] CAO S W, SHEN B J, TONG T, et al. 2D/2D heterojunction of ultrathin MXene/Bi₂WO₆ nanosheets for improved photocatalytic CO₂ reduction[J]. Advanced Functional Materials, 2018, 28(21): 1800136.
[13] BAI Y, YANG P, WANG L, et al. Ultrathin Bi₄O₅Br₂ nanosheets for selective photocatalytic CO₂ conversion into CO[J]. Chemical Engineering Journal, 2019, 360: 473-482.
[14] LIU Y P, LI Y H, LI X Y, et al. Regulating electron-hole separation to promote photocatalytic H₂ evolution activity of nanoconfined Ru/MXene/TiO₂ catalysts[J]. ACS Nano, 2020, 14(10): 14181-14189.
[15] ZHANG W B, XIAO X, WU Q F, et al. Facile synthesis of novel Mn-doped Bi₄O₅Br₂ for enhanced photocatalytic NO removal activity[J]. Journal of Alloys and Compounds, 2020, 826: 154204.
[16] ZHANG R R, JIN J Y, JIA L M, et al. Fabrication of CdS/Ti₃C₂/g-C₃N₄NS Z-scheme composites with enhanced visible light-driven photocatalytic activity[J]. Environmental Science and Pollution Research International, 2022, 29(11): 16371-16382.
[17] BHARATH G, RAMBABU K, HAI A, et al. Highly selective etherification of fructose and 5-hydroxymethylfurfural over a novel Pd-Ru/MXene catalyst for sustainable liquid fuel production[J]. International Journal of Energy Research, 2021, 45(10): 14680-14691.
[18] XI Q, YUE X P, FENG J Q, et al. Facile synthesis of 2D Bi₄O₅Br₂/2D thin layer-Ti₃C₂ for improved visible-light photocatalytic hydrogen evolution[J]. Journal of Solid State Chemistry, 2020, 289: 121470.
[19] HUANG H, DAI Q G, WANG X Y. Morphology effect of Ru/CeO₂ catalysts for the catalytic combustion of chlorobenzene[J]. Applied Catalysis B: Environmental, 2014, 158/159: 96-105.
[20] TU X M, LUO S L, CHEN G X, et al. One-pot synthesis, characterization, and enhanced photocatalytic activity of a BiOBr-graphene composite[J]. Chemistry-A European Journal, 2012, 18(45): 14359-14366.
[21] ZHANG X, YANG P, YANG B, et al. Synthesis of novel Bi/Bi₄O₅Br₂ via a UV light irradiation for decomposing the oil field pollutants[J]. Inorganic Chemistry Communications, 2020, 122: 108297.
[22] RAN J R, GAO G P, LI F T, et al. Ti₃C₂ MXene co-catalyst on metal sulfide photo-absorbers for enhanced visible-light photocatalytic hydrogen production[J]. Nature Communications, 2017, 8: 13907.
[23] BAI Y, CHEN T, WANG P Q, et al. Bismuth-rich Bi₄O₅X₂ (X=Br, and I) nanosheets with dominant{101}facets exposure for photocatalytic H₂ evolution[J]. Chemical Engineering Journal, 2016, 304: 454-460.
[24] LI J Y, DONG X A, SUN Y J, et al. Facet-dependent interfacial charge separation and transfer in plasmonic photocatalysts[J]. Applied Catalysis B: Environmental, 2018, 226: 269-277.
[25] LOU X, SHANG J, WANG L, et al. Enhanced photocatalytic activity of Bi₂₄O₃₁Br₁₀: constructing heterojunction with BiOI[J]. Journal of Materials Science & Technology, 2017, 33(3): 281-284.
[26] LI R, FENG J Q, ZHANG X C, et al. In situ reorganization of Bi₃O₄Br nanosheet on the Bi₂₄O₃₁Br₁₀ ribbon structure for superior visible-light photocatalytic capability[J]. Separation and Purification Technology, 2020, 247: 117007.

Bi₄O₅Br₂/Ti₃C₂-Ru复合光催化剂的合成及其对磺胺甲噁唑药物废水降解性能研究

Preparation of Bi₄O₅Br₂/Ti₃C₂-Ru Composite Photocatalysts and Their Degradation Performances for Sulfamethoxazole

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

编辑推荐

Metrics

本文评价

[1]	王静怡, 张众, 王梓兰, 于鑫颖, 由君颐, 朱君怡, 杨琳. 吡啶鎓盐配体构筑的多钼酸基配合物的合成、结构及光催化性能[J]. 人工晶体学报, 2022, 51(7): 1227-1232.
[2]	李瑞, 张潇, 张璐璐, 谢芳霞, 张小超, 王雅文, 樊彩梅. 原位合成Bi₃O₄Br/Bi₁₂O₁₇Br₂光催化剂及其对磺胺甲噁唑降解性能[J]. 人工晶体学报, 2021, 50(9): 1735-1744.
[3]	闵涛, 马国华, 刘桂君, 郑玉婷. TiO₂/Ni₃[Ge₂O₅](OH)₄复合材料的制备及光催化性能[J]. 人工晶体学报, 2021, 50(11): 2086-2092.
[4]	潘睿, 傅敏, 陈正波, 胡雪利. ZnSn(OH)₆/SrSn(OH)₆光催化降解甲苯的性能研究[J]. 人工晶体学报, 2021, 50(1): 122-129.
[5]	闫哲;李国强;李东昶;刘建新;樊彩梅. PtO-Pt-BiOCl Z-型异质结光催化剂的制备及其性能研究[J]. 人工晶体学报, 2019, 48(9): 1660-1666.
[6]	刘永明. 不同形貌WO3的制备及其可见光催化性能研究[J]. 人工晶体学报, 2019, 48(5): 867-872.
[7]	李朋娜;王留昌;刘欢;李芮;蒋勇;张璐. Fe@Fe2O3/g-C3N4复合光催化剂的制备及其性能[J]. 人工晶体学报, 2018, 47(6): 1142-1147.
[8]	李燕;张克华;孙宝;王爱国;耿春东. CdS/沸石分子筛复合光催化剂的制备及光催化性能[J]. 人工晶体学报, 2018, 47(6): 1182-1186.
[9]	王竹梅;张天峰;李月明;沈宗洋;左建林. 溶胶-凝胶法制备S掺杂TiO2纳米粉体的光催化性能[J]. 人工晶体学报, 2018, 47(4): 765-769.
[10]	王爱民;白妮;王金玺;范晓勇;亢玉红;马向荣. ZnTiO3/TiO2异质复合材料的制备及光催化性能[J]. 人工晶体学报, 2018, 47(2): 382-388.
[11]	潘会;胡轶;兀晓文;苏巧红. Mn掺杂ZnO的制备、表征及光催化性能[J]. 人工晶体学报, 2018, 47(12): 2498-2503.
[12]	刘少友;左成钢;陈远道;周诗彪. Fe掺杂TiO2超细粉体的能带隙调控与光催化性能[J]. 人工晶体学报, 2017, 46(8): 1552-1558.
[13]	郝艳艳;张影;赵琳. ZnO-SiO2的制备及其光催化降解罗丹明B[J]. 人工晶体学报, 2017, 46(7): 1379-1384.
[14]	王瑞琪;徐海燕;吴四维;傅敏. Bi3Ti4O12/α-Bi2O3/TiO2复合光催化剂的制备及其可见光催化活性研究[J]. 人工晶体学报, 2017, 46(12): 2386-2392.
[15]	李余杰;朱翔;张智;卢鹏;蔡松柏;李俊辉;彭竹葳;魏婷. g-C3N4/TiO2可见光催化降解磺胺二甲基嘧啶的研究[J]. 人工晶体学报, 2017, 46(11): 2190-2196.