Fe2O3/g-C3N4光催化降解罗丹明B性能研究

doi:10.3969/j.issn.1000-5641.2021.03.015

摘要/Abstract

摘要：

为了改善g-C₃N₄比表面积低等缺点, 通过高温热聚合法制备了三维(3D)多孔g-C₃N₄, 并通过与Fe₂O₃复合得到Fe₂O₃/g-C₃N₄催化剂, 提高其可见光响应. Fe₂O₃/g-C₃N₄在g-C₃N₄含量为900 mg、罗丹明B(Rhodamine B, RhB)浓度为20 mg·L^–1、H₂O₂为15 mmol时脱色速率最快, 30 min可达到100%. 同时Fe₂O₃/g-C₃N₄对其他有机物也表现出较好的降解性能, 在30 min内对甲基橙(Methyl orange, MO)、四环素(Tetracycline, TC)的降解率分别达到80%和90%. 通过活性基团捕获实验探究Fe₂O₃/g-C₃N₄的光催化降解机制, 实验结果表明h⁺和·OH在Fe₂O₃/g-C₃N₄光催化降解有机物过程中起到主要作用.

关键词: g-C₃N₄, 氧化铁, 罗丹明B, 光催化

Abstract:

In order to improve the low specific surface area of g-C₃N₄, three-dimensional (3D) porous g-C₃N₄ was prepared using high temperature thermal polymerization. Fe₂O₃/g-C₃N₄ catalyst was prepared by compositing the g-C₃N₄ with Fe₂O₃ to improve its visible light response. The decolorization rate of the Fe₂O₃/g-C₃N₄ catalyst reached 100% in 30 minutes with a g-C₃N₄ content of 900 mg, Rhodamine B (RhB) concentration of 20 mg·L^–1, and H₂O₂ content of 15 mmol. The Fe₂O₃/g-C₃N₄ catalyst also demonstrated good performance in degrading other organics; the degradation rates of Methyl orange (MO) and Tetracycline (TC) reached 80% and 90%, respectively, in 30 minutes. This photocatalytic mechanism was explored by active group capture experiments, and the results show that h⁺ and ·OH play an important role in the progress of photocatalysis.

Key words: g-C₃N₄, Fe₂O₃, Rhodamine B(RhB), photocatalytic

中图分类号:

O469

席清华, 黄宜强, 陈加祥, 聂耳, 孙卓. Fe₂O₃/g-C₃N₄光催化降解罗丹明B性能研究[J]. 华东师范大学学报（自然科学版）, 2021, 2021(3): 151-160.

Qinghua XI, Yiqiang HUANG, Jiaxiang CHEN, Er NIE, Zhuo SUN. Study on Fe₂O₃/g-C₃N₄ photocatalytic degradation of Rhodamine B[J]. Journal of East China Normal University(Natural Science), 2021, 2021(3): 151-160.

图/表 11

图1

图2

图3

图4

图5

表1

图6

图7

图8

图9

图10

参考文献 29

1	TIAN S Y, GUO J H, ZHAO C, et al. Preparation of cellulose/graphene oxide composite membranes and their application in removing organic contaminants in wastewater. Journal of Nanoscience and Nanotechnology, 2019, 19 (4): 2147- 2153. doi: 10.1166/jnn.2019.15808
2	LIU D, ZHOU J, WANG J, et al. Enhanced visible light photoelectrocatalytic degradation of organic contaminants by F and Sn co-doped TiO₂ photoelectrode . Chemical Engineering Journal, 2018, 344, 332- 341. doi: 10.1016/j.cej.2018.03.103
3	GARCIA-SEGURA S, BRILLAS E. Applied photoelectrocatalysis on the degradation of organic pollutants in wastewaters. Journal of Photochemistry and Photobiology C: Photochemistry Reviews, 2017, 31, 1- 35. doi: 10.1016/j.jphotochemrev.2017.01.005
4	CORCORAN E B, MCMULLEN J P, LÉVESQUE F, et al. Photon equivalents as a parameter for scaling photoredox reactions in flow: Translation of photocatalytic C−N cross-coupling from lab scale to multikilogram scale. Angewandte Chemie, 2020, 132 (29): 11964- 11968. doi: 10.1002/ange.202004090
5	FARES A, RAHUL B, MOAYYED S. Solar oxidation of toluene over Co doped nano-catalyst. Chemosphere, 2020, 255, 126878. doi: 10.1016/j.chemosphere.2020.126878
6	DENG H, WANG X C, WANG L, et al. Enhanced photocatalytic reduction of aqueous Re(Ⅶ) in ambient air by amorphous TiO₂/g-C₃N₄ photocatalysts: Implications for Tc(Ⅶ) elimination . Chemical Engineering Journal, 2020, 401, 125977. doi: 10.1016/j.cej.2020.125977
7	DUAN B, MEI L. A Z-scheme Fe₂O₃ /g-C₃N₄ heterojunction for carbon dioxide to hydrocarbon fuel under visible illuminance . Journal of Colloid And Interface Science, 2020, 575, 265- 273. doi: 10.1016/j.jcis.2020.04.112
8	CHAUHAN D K, JAIN S, BATTULA V R, et al. Organic motif's functionalization via covalent linkage in carbon nitride: An exemplification in photocatalysis. Carbon, 2019, 152, 40- 58. doi: 10.1016/j.carbon.2019.05.079
9	KADI M W, MOHAMED R M, ISMAIL A A, et al. Decoration of g-C₃N₄ nanosheets by mesoporous CoFe₂O₄ nanoparticles for promoting visible-light photocatalytic Hg(Ⅱ) reduction . Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2020, 603, 125306.
10	LI Y, WANG S, CHANG W, et al. Co-monomer engineering optimized electron delocalization system in carbon-bridging modified g-C₃N₄ nanosheets with efficient visible-light photocatalytic performance . Applied Catalysis B: Environmental, 2020, 274, 119116. doi: 10.1016/j.apcatb.2020.119116
11	LU M, SUN Z, ZHANG Y, et al. Construction of cobalt phthalocyanine sensitized SnIn₄S₈/g-C₃N₄ composites with enhanced photocatalytic degradation and hydrogen production performance . Synthetic Metals, 2020, 268, 116480. doi: 10.1016/j.synthmet.2020.116480
12	HE J, YANG J, JIANG F, et al. Photo-assisted peroxymonosulfate activation via 2D/2D heterostructure of Ti₃C₂/g-C₃N₄ for degradation of diclofenac . Chemosphere, 2020, 258, 127339. doi: 10.1016/j.chemosphere.2020.127339
13	CHENG J, HU Z, LI Q, et al. Fabrication of high photoreactive carbon nitride nanosheets by polymerization of amidinourea for hydrogen production. Applied Catalysis B: Environmental, 2019, 245, 197- 206. doi: 10.1016/j.apcatb.2018.12.044
14	AI M, ZHANG J W, GAO R, et al. MnOx-decorated 3D porous C₃N₄ with internal donor–acceptor motifs for efficient photocatalytic hydrogen production . Applied Catalysis B: Environmental, 2019, 256, 117805. doi: 10.1016/j.apcatb.2019.117805
15	HU X, VATANKHAH-VARNOOSFADERANI M, ZHOU J, et al. Weak hydrogen bonding enables hard, strong, tough, and elastic hydrogels. Adv Mater, 2015, 27 (43): 6899- 6905. doi: 10.1002/adma.201503724
16	TIAN R, LIU D, WANG J, et al. Three-dimensional BiOI/TiO₂ heterostructures with photocatalytic activity under visible light irradiation . Journal of Porous Materials, 2018, 25 (6): 1805- 1812. doi: 10.1007/s10934-018-0594-3
17	WANG Y, ZHONG K, HUANG Z, et al. Novel g-C₃N₄ assisted metal organic frameworks derived high efficiency oxygen reduction catalyst in microbial fuel cells . Journal of Power Sources, 2020, 450, 227681. doi: 10.1016/j.jpowsour.2019.227681
18	ZHANG Y, TIAN P, LI K, et al. C₃N₄ coordinated metal-organic-framework-derived network as air-cathode for high performance of microbial fuel cell . Journal of Power Sources, 2018, 408, 74- 81. doi: 10.1016/j.jpowsour.2018.10.036
19	JIANG J, WANG X, ZHANG C, et al. Porous 0D/3D NiCo₂O₄/g-C₃N₄ accelerate emerging pollutant degradation in PMS/vis system: Degradation mechanism, pathway and toxicity assessment . Chemical Engineering Journal, 2020, 397, 125356. doi: 10.1016/j.cej.2020.125356
20	WU X, LI S, WANG B, et al. Free-standing 3D network-like cathode based on biomass-derived N-doped carbon/graphene/g-C₃N₄ hybrid ultrathin sheets as sulfur host for high-rate Li-S battery . Renewable Energy, 2020, 158, 509- 519. doi: 10.1016/j.renene.2020.05.098
21	ZHANG L, JIN Z, LI Y, et al. Zn–Ni–P nanoparticles decorated g-C₃N₄ nanosheets applicated as photoanode in photovoltaic fuel cells . Catalysis Letters, 2019, 149 (9): 2397- 2407. doi: 10.1007/s10562-019-02859-8
22	GAO H, YANG H, XU J, et al. Strongly coupled g-C₃N₄ nanosheets-Co₃O₄ quantum dots as 2D/0D heterostructure composite for peroxymonosulfate activation . Small, 2018, 14, 1801353. doi: 10.1002/smll.201801353
23	XI J, XIA H, NING X, et al. Carbon-intercalated 0D/2D hybrid of hematite quantum dots/graphitic carbon nitride nanosheets as superior catalyst for advanced oxidation. Small, 2019, 15 (43): 1902744. doi: 10.1002/smll.201902744
24	SHENG Y, WEI Z, MIAO H, et al. Enhanced organic pollutant photodegradation via adsorption/photocatalysis synergy using a 3D g-C₃N₄/TiO₂ free-separation photocatalyst . Chemical Engineering Journal, 2019, 370, 287- 294. doi: 10.1016/j.cej.2019.03.197
25	RODRIGUEZ J, THIVEL P X, PUZENAT E. Photocatalytic hydrogen production for PEMFC supply: A new issue. International Journal of Hydrogen Energy, 2013, 38 (15): 6344- 6348. doi: 10.1016/j.ijhydene.2013.03.026
26	WANG Y, HUANG Y, HO W, et al. Biomolecule-controlled hydrothermal synthesis of C-N-S-tridoped TiO₂ nanocrystalline photocatalysts for NO removal under simulated solar light irradiation . J Hazard Mater, 2009, 169 (1/2/3): 77- 87.
27	LIU G, DONG G, ZENG Y, et al. The photocatalytic performance and active sites of g-C3N4 effected by the coordination doping of Fe(III). Chinese Journal of Catalysis, 2020, 41 (10): 1564- 1572. doi: 10.1016/S1872-2067(19)63518-7
28	QIN Y, SONG F, AI Z, et al. Protocatechuic acid promoted alachlor degradation in Fe(Ⅲ)/H₂O₂ fenton system . Environ Sci Technol, 2015, 49 (13): 7948- 7956. doi: 10.1021/es506110w
29	QIN Y, ZHANG L, AN T. Hydrothermal carbon-mediated fenton-like reaction mechanism in the degradation of alachlor: Direct electron transfer from hydrothermal carbon to Fe(Ⅲ). ACS Appl Mater Interfaces, 2017, 9 (20): 17115- 17124. doi: 10.1021/acsami.7b03310

样品	比表面积/(m²·g^–1)	孔容/(cm³·g^–1)	孔径/nm
CN-1	61	0.35	2.98
CN-2	72	0.36	3.84
CN-3	72	0.36	3.84
CN-4	74	0.35	3.82
CN-5	74	0.35	3.83

[1]	周君, 席清华, 黄宜强, 聂耳, 孙卓. I掺杂TiO₂纳米管阵列平面光催化燃料电池的性能研究[J]. 华东师范大学学报（自然科学版）, 2021, 2021(1): 165-175.
[2]	王剑桥, 刘冬, 周君, 席清华, 聂耳, 孙卓. TiO₂纳米管阵列双极光催化燃料电池的应用研究[J]. 华东师范大学学报（自然科学版）, 2020, 2020(1): 93-102.
[3]	黄贤智, 朴贤卿, 蔡亚果. 光催化材料MIL-125(Ti)/BiOI的制备及光催化性能研究[J]. 华东师范大学学报(自然科学版), 2019, 2019(1): 93-104,114.
[4]	朱培娟，陈薇，李春艳，赵雅萍. 溴化氧铋（BiOBr）光催化降解亚甲基蓝的研究[J]. 华东师范大学学报(自然科学版), 2014, 2014(4): 122-131.
[5]	章丹, 徐斌, 朱培娟, 连正豪, 赵雅萍. TiO₂光催化降解亚甲基蓝机理的研究[J]. 华东师范大学学报(自然科学版), 2013, 2013(5): 35-42.
[6]	董鹏飞;韩婧;邵启伟;成荣明. ZnO纳米棒/PVC复合材料的光催化性能研究[J]. 华东师范大学学报(自然科学版), 2009, 2009(5): 29-39,8.
[7]	丁洪流;赵婷;施国跃;金利通. 罗丹明B掺杂ZnQ₂的电致发光器件及其性能研究[J]. 华东师范大学学报(自然科学版), 2008, 2008(4): 88-95.
[8]	陆华;曲云鹤;周天舒;郑蕾;施国跃. 纳米ZnO膜光催化氧化测定化学需氧量的应用研究[J]. 华东师范大学学报(自然科学版), 2007, 2007(6): 62-68,9.
[9]	艾仕云;杨娅;鲜跃仲;李嘉庆;李洛平;金利通. 纳米TiO₂光诱导产生羟基自由基的ESR研究[J]. 华东师范大学学报(自然科学版), 2004, 2004(3): 76-81.
[10]	艾仕云;鲜跃仲;陈俊水;蔡琪;金利通. 纳米CuO/TiO₂的光催化降解及其应用[J]. 华东师范大学学报(自然科学版), 2003, 2003(1): 62-67.

Fe₂O₃/g-C₃N₄光催化降解罗丹明B性能研究

Study on Fe₂O₃/g-C₃N₄ photocatalytic degradation of Rhodamine B

RichHTML

PDF

可视化

摘要/Abstract

引用本文

使用本文

图/表 11

参考文献 29

相关文章 10

编辑推荐

Metrics

本文评价