Synthesis of Z-scheme Ag3PO4/MIL-125(Ti) Heterojunction and Its Performance in Photocatalytic Reduction of Cr(VI)

doi:10.11901/1005.3093.2022.669

Chinese Journal of Materials Research

2023, Vol. 37

Issue (11): 871-880 DOI: 10.11901/1005.3093.2022.669

ARTICLES

Current Issue | Archive | Adv Search

Synthesis of Z-scheme Ag₃PO₄/MIL-125(Ti) Heterojunction and Its Performance in Photocatalytic Reduction of Cr(VI)

SUN Yuwei¹^,², CHEN Chou¹, QI Xin¹, REN Chuqi¹, TANG Qian¹^,², TENG Honghui¹^,²(

), REN Baixiang¹^,²

^1.College of Engineering, Jilin Normal University, Siping 136000, China
^2.Key Laboratory of Environmental Materials and Pollution Control, Education Department of Jilin Province, Siping 136000, China

Cite this article:

SUN Yuwei, CHEN Chou, QI Xin, REN Chuqi, TANG Qian, TENG Honghui, REN Baixiang. Synthesis of Z-scheme Ag₃PO₄/MIL-125(Ti) Heterojunction and Its Performance in Photocatalytic Reduction of Cr(VI). Chinese Journal of Materials Research, 2023, 37(11): 871-880.

Download:

HTML

PDF(7889KB)
Export: BibTeX | EndNote (RIS)

Abstract

A composite of Z-scheme Ag₃PO₄/MIL-125(Ti) heterojunction was synthesized by loading Ag₃PO₄ nano particles on the surface of round-shaped MIL-125(Ti). The Ag₃PO₄/MIL-125(Ti) composite can effectively improve the utilization of light and charge separation efficiency. The crystal-structure, morphology, optical absorption, valence band structure and charge separation efficiency of the prepared Ag₃PO₄/MIL-125(Ti) composite were characterized by XRD、SEM、EDS、UV-vis、FTIR、EIS and PL testing methods. Under a simulated solar irradiation, the performance of Cr(VI) reduction by Ag₃PO₄/MIL125(Ti) composite with different deposition amounts of Ag₃PO₄ was studied. Furthermore, the effect of solution pH and catalyst dosage in the photocatalytic reduction process was also discussed. The photocatalytic test results indicated that the deposition of Ag₃PO₄ effectively improved the photocatalytic reduction performance of MIL-125(Ti). When the concentration of Cr(VI) solution was 10mg/L and pH was 2, the reduction rate of Cr(VI) by Ag₃PO₄/MIL-125(Ti)-2 could reach to 96.9%. The results of bandgap structure calculation and free radical trapping experiments show that photon-generated carriers in Ag₃PO₄/MIL-125(Ti) are conformed to Z-scheme mechanism.

Key words: inorganic non-metallic materials MIL-125 (Ti) Ag₃PO₄ Z-scheme heterojunction photocatalytic reduction of Cr(VI)

Received: 19 December 2022

ZTFLH:

X703.1

Fund: Department of Science and Technology of Jilin Province(YDZJ202201ZYTS368);Department of Science and Technology of Jilin Province(20210101391JC);Department of Education of Jilin Province(JJKH20220451KJ);Department of Education of Jilin Province(JJKH20230517KJ)

Corresponding Authors: TENG Honghui, Tel: 13944400855, E-mail: hhteng2022@163.com

	Service

	E-mail this article
	Add to citation manager
	E-mail Alert
	RSS
	（）
	Articles by authors
	SUN Yuwei
	CHEN Chou
	QI Xin
	REN Chuqi
	TANG Qian
	TENG Honghui
	REN Baixiang

URL:

https://www.cjmr.org/EN/10.11901/1005.3093.2022.669 OR https://www.cjmr.org/EN/Y2023/V37/I11/871

Fig.1 XRD patterns of different samples

Fig.2 SEM of MIL125(Ti) (a), Ag₃PO₄(b), Ag₃PO₄/MIL125(Ti)-2 (c) and EDS spectrum of Ag₃PO₄/MIL125(Ti)-2 (d~g)

Fig.3 UV-vis spectrum (a), (αhv)^1/2 vs. hv curves of different samples (b), VB profiles of MIL-125(Ti) and Ag₃PO₄ (c) and the band structure diagrams of MIL125(Ti) and Ag₃PO₄ (d)

Fig.4 Infrared spectrum of different samples

Fig.5 EIS (a) and PL spectrum (b) of different samples

Fig.6 Photocatalytic reduction performance of different samples (a) and the first-order kinetic curves (b) of the photoca-talytic reduction of Cr(VI)

Fig.7 Effects of different initial pH values on the photocatalytic reduction performance (a, b), the effects of different dosage on the photocatalytic reduction performance (c, d), the effects of different organic acids on the photocatalytic reduction performance (e, f)

Table1 Comparison of photocatalytic Cr(VI) removal activities of various MOFs-based photocatalysts

Fig.8 4 cycles of photocatalytic reduction experiment (a) and XRD patterns (b) of Ag₃PO₄/MIL-125(Ti)-2 before and after 6 cycles

Fig.9 Experimental results of active species capture

Fig.10 Mechanism of photocatalytic reduction of Cr(VI) by Ag₃PO₄/MIL-125(Ti)

1	Li Y X, WANG X, WANG C C, et al. S-TiO₂/UiO-66-NH₂ composite for boosted photocatalytic Cr(VI) reduction and bisphenol A degradation under LED visible light [J]. J. Hazaed. Mater., 2020, 399: 123085
2	Ma J, Chen K Z. Designing porous nickel architectures for adsorptive removal of Cr(VI) to achieve drinking water standard [J]. Sep. Purif. Technol., 2020, 241: 116705 doi: 10.1016/j.seppur.2020.116705
3	Zhang L X, Li P, Feng L P, et al. Controllable fabrication of visible-light-driven CoS _x /CdS photocatalysts with direct Z-scheme heterojunctions for photocatalytic Cr(VI) reduction with high efficiency [J]. Chem. Eng. J., 2020, 397: 125464 doi: 10.1016/j.cej.2020.125464
4	Wang M, Zeng Y B, Dong G H, et al. Br-doping of g-C₃N₄ towards enhanced photocatalytic performance in Cr(VI) reduction [J]. Chin. J. Catal., 2020, 41(10): 1498 doi: 10.1016/S1872-2067(19)63435-2
5	Hu Q S, Di J, Wang B, et al. In-situ preparation of NH₂-MIL-125(Ti)/BiOCl composite with accelerating charge carriers for boosting visible light photocatalytic activity [J]. Appl. Surf. Sci., 2019, 466: 525 doi: 10.1016/j.apsusc.2018.10.020
6	Guo J Y, Fu Y J, Zhang K J, et al. Preparation and visible light catalytic performance of g-C₃N₄/POPs heterojunction [J]. Acta Mater. Compos. Sin, 2023, 40: 904
	郭佳允, 傅炀杰, 张柯杰等. g-C₃N₄/POPs异质结制备及其可见光催化性能 [J]. 复合材料学报, 2023, 40: 904
7	Haroon H, Majid K. MnO₂ nanosheets supported metal-organic framework MIL-125(Ti) towards efficient visible light photocatalysis: Kinetic and mechanistic study [J]. Chem. Phys. Lett., 2020, 745: 137283 doi: 10.1016/j.cplett.2020.137283
8	Zhang X Y, Zhang Q Y, Tang T, et al. Fabrication of composite material based on MOFs and its adsorption properties for methylene blue dyes [J]. Chin. J. Mater. Res., 2021, 35: 866 doi: 10.11901/1005.3093.2021.002
	张向阳, 章奇羊, 汤涛等. 基于MOFs的复合材料制备及其对亚甲基蓝染料的吸附性能 [J]. 材料研究学报, 2021, 35: 866 doi: 10.11901/1005.3093.2021.002
9	Yue K, Zhang X D, Jiang S T, et al. Recent advances in strategies to modify MIL-125(Ti) and its environmental applications [J]. J. Mol. Liq., 2021, 335: 116108 doi: 10.1016/j.molliq.2021.116108
10	Ao D, Zhang J, Liu H. Visible-light-driven photocatalytic degradation of pollutants over Cu-doped NH₂-MIL-125(Ti) [J]. J. Photoch. Photobio., 2018, 364A: 524
11	Cui W C, Shang J P, Bai H Y, et al. In-situ implantation of plasmonic Ag into metal-organic frameworks for constructing efficient Ag/NH₂-MIL-125/TiO₂ photoanode [J]. Chem. Eng. J., 2020, 388: 124206 doi: 10.1016/j.cej.2020.124206
12	Abdelhameed R M, Abu-Elghait M, El-Shahat M. Hybrid three MOFs composites (ZIF-67@ZIF-8@MIL-125-NH₂): Enhancement the biological and visible-light photocatalytic activity [J]. J. Environ. Chem. Eng., 2020, 8(5): 104107 doi: 10.1016/j.jece.2020.104107
13	Wang Z C, Liu Y, Li J H, et al. Efficient immobilization of enzymes on amino functionalized MIL-125-NH₂ metal organic framework [J]. Biotechnol. Bioproc. Eng., 2022, 27(1): 135 doi: 10.1007/s12257-020-0393-y
14	Xu Y F, Zhou Y, Deng Y H, et al. Synthesis of Bi₂WO₆@NH₂-MIL-125(Ti): A S-scheme photocatalyst with enhanced visible light catalytic activity [J]. Catal. Lett., 2020, 150(12): 3470 doi: 10.1007/s10562-020-03258-0
15	Li Y X, Wang C C, Fu H F, et al. Marigold-flower-like TiO₂/MIL-125 core-shell composite for enhanced photocatalytic Cr(VI) reduction [J]. J. Environ. Chem. Eng., 2021, 9(4): 105451 doi: 10.1016/j.jece.2021.105451
16	Hu Q S, Yin S, Chen Y, et al. Construction of MIL-125(Ti)/ZnIn₂S₄ composites with accelerated interfacial charge transfer for boosting visible light photoreactivity [J]. Colloids Surf., 2020, 585A: 124078
17	Han L, Zhang X M, Wu D Y. MoS₂ quantum dots decorated NH₂-MIL-125 heterojunction: preparation and visible light photocatalytic performance [J]. J. Inorg. Mater., 2019, 34(11): 1205
	韩丽, 张晓敏, 吴德勇. 具有可见光催化活性的MoS₂量子点/NH₂-MIL-125复合材料的制备及性能表征 [J]. 无机材料学报, 2019, 34(11): 1205
18	Promnopas S, Promnopas W, Maisang W, et al. One-step microwave-hydrothermal synthesis of visible-light-driven Ag₃PO₄/LaPO₄ photocatalyst induced by visible light irradiation [J]. Chem. Phys. Lett., 2021, 779: 138883 doi: 10.1016/j.cplett.2021.138883
19	Cui C, Wang Y P, Liang D Y, et al. Photo-assisted synthesis of Ag₃PO₄/reduced graphene oxide/Ag heterostructure photocatalyst with enhanced photocatalytic activity and stability under visible light [J]. Appl. Catal., 2014, 158-159B: 150
20	Liu J H, Li X, Liu F, et al. The stabilization effect of surface capping on photocatalytic activity and recyclable stability of Ag₃PO₄ [J]. Catal. Commun., 2014, 46: 138 doi: 10.1016/j.catcom.2013.12.005
21	Sofi F A, Majid K. Enhancement of the photocatalytic performance and thermal stability of an iron based metal–organic-framework functionalised by Ag/Ag₃PO₄ [J]. Mater. Chem. Front., 2018, 2: 942 doi: 10.1039/C8QM00051D
22	Zhou T H, Zhang G Z, Zhang H W, et al. Highly efficient visible-light-driven photocatalytic degradation of rhodamine B by a novel Z-scheme Ag₃PO₄/MIL-101/NiFe₂O₄ composite [J]. Catal. Sci. Technol., 2018, 8: 2402 doi: 10.1039/C8CY00182K
23	Liang Y H, Shang R, Lu J R, et al. Ag₃PO₄@UMOFNs core–shell structure: two-dimensional MOFs promoted photoinduced charge separation and Photocatalysis [J]. ACS Appl. Mater. Interfaces, 2018, 10: 8758 doi: 10.1021/acsami.8b00198
24	Han X, Yang X B, Liu G B, et al. Boosting visible light photocatalytic activity via impregnation-induced RhB-sensitized MIL-125(Ti) [J]. Chem. Eng. Res. Des., 2019, 143: 90 doi: 10.1016/j.cherd.2019.01.010
25	Liu L, Ding L, Liu Y G, et al. A stable Ag₃PO₄@PANI core@shell hybrid: Enrichment photocatalytic degradation with π-π conjugation [J]. Appl. Catal., 2017, 201B: 92
26	Xie L C, Yang Z H, Xiong W P, et al. Construction of MIL-53(Fe) metal-organic framework modified by silver phosphate nanoparticles as a novel Z-scheme photocatalyst: Visible-light photocatalytic performance and mechanism investigation [J]. Appl. Surf. Sci., 2019, 465: 103 doi: 10.1016/j.apsusc.2018.09.144
27	Hu Z, He Q B, Ge M. Photocatalytic degradation of organic contaminants by magnetic Ag₃PO₄/MFe₂O₄ (M = Zn, Ni, Co) composites: a comparative study and a new insight into mechanism [J]. J. Mater. Sci. Mater. Electron., 2021, 32(1): 827 doi: 10.1007/s10854-020-04861-y
28	Yang X M, Gu W H, Ma Y W, et al. Interface electron transfer of Bi₂MoO₆/MIL-125 and the visible-light performance for pollutant degradation [J]. Colloids Surf., 2020, 597A: 124748
29	Abdelhameed R M, Simões M M Q, Silva A M S, et al. Enhanced photocatalytic activity of MIL-125 by post-synthetic modification with Cr^III and Ag nanoparticles [J]. Chem. Eur. J., 2015, 21(31): 11072 doi: 10.1002/chem.v21.31
30	George P, Chowdhury P. NH₂-MIL-125(Ti) and its emeraldine functionalized derivative as a chemical sensor for effective detection of dopamine [J]. Micropor. Mesopor. Mat., 2019, 288: 109591 doi: 10.1016/j.micromeso.2019.109591
31	Zhu S R, Liu R F, Wu M K, et al. Enhanced photocatalytic performance of BiOBr/NH₂-MIL-125(Ti) composite for dye degradation under visible light [J]. Dalton Trans., 2016, 45(43): 17521 doi: 10.1039/C6DT02912D
32	Chen S, Huang D L, Zeng G M, et al. In-situ synthesis of facet-dependent BiVO₄/Ag₃PO₄/PANI photocatalyst with enhanced visible-light-induced photocatalytic degradation performance: synergism of interfacial coupling and hole-transfer [J]. Chem. Eng. J., 2020, 382: 122840 doi: 10.1016/j.cej.2019.122840
33	Lv Y H, Liu H Y, Jin D X, et al. Effective degradation of norfloxacin on Ag₃PO₄/CNTs photoanode: Z-scheme mechanism, reaction pathway, and toxicity assessment [J]. Chem. Eng. J., 2022, 429: 132092 doi: 10.1016/j.cej.2021.132092
34	Wang F H, Liu X Z, Xu L, et al. One-pot synthesis of CeO₂/Mg-Al layered double oxide nanosheets for efficient visible-light induced photo-reduction of Cr(VI) [J]. Colloids Surf., 2020, 601A: 125044
35	Deng Y C, Tang L, Zeng G M, et al. Insight into highly efficient simultaneous photocatalytic removal of Cr(VI) and 2,4-diclorophenol under visible light irradiation by phosphorus doped porous ultrathin g-C₃N₄ nanosheets from aqueous media: Performance and reaction mechanism [J]. Appl. Catal., 2017, 203B: 343
36	Ma N, Qiu Y W, Zhang Y C, et al. Reduced graphene oxide enwrapped pinecone-liked Ag₃PO₄/TiO₂ composites with enhanced photocatalytic activity and stability under visible light [J]. J. Alloys Compd., 2015, 648: 818 doi: 10.1016/j.jallcom.2015.07.070
37	Yu C F, Yang P Y, Tie L N, et al. One-pot fabrication of β-Bi₂O₃@Bi₂S₃ hierarchical hollow spheres with advanced sunlight photocatalytic RhB oxidation and Cr(VI) reduction activities [J]. Appl. Surf. Sci., 2018, 455: 8 doi: 10.1016/j.apsusc.2018.04.201
38	Song X L, Wang Y, Zhu T, et al. Facile synthesis a novel core-shell amino functionalized MIL-125(Ti) micro-photocatalyst for enhanced degradation of tetracycline hydrochloride under visible light [J]. Chem. Eng. J., 2021, 416: 129126 doi: 10.1016/j.cej.2021.129126
39	Yi X H, Wang F X, Du X D, et al. Facile fabrication of BUC-21/g-C₃N₄ composites and their enhanced photocatalytic Cr(VI) reduction performances under simulated sunlight [J]. Appl. Organomet. Chem., 2019, 33: e4621 doi: 10.1002/aoc.v33.1
40	Qiu J H, Yang L Y, Li M, et al. Metal nanoparticles decorated MIL-125-NH₂ and MIL-125 for efficient photocatalysis [J]. Mater. Res. Bull., 2019, 112: 297 doi: 10.1016/j.materresbull.2018.12.038
41	Wang M H, Yang L Y, Yuan J Y, et al. Heterostructured Bi₂S₃@NH₂-MIL-125(Ti) nanocomposite as a bifunctional photocatalyst for Cr(vi) reduction and rhodamine B degradation under visible light [J]. RSC Adv., 2018, 8: 12459 doi: 10.1039/C8RA00882E
42	Wang H, Yuan X Z, Wu Y, et al. Photodeposition of metal sulfides on titanium metal-organic frameworks for excellent visible-light-driven photocatalytic Cr(vi) reduction [J]. RSC Adv., 2015, 5: 32531 doi: 10.1039/C5RA01283J
43	Liu S J, Zhou X F, Wei C H, et al. Spatial directional separation and synergetic treatment of Cr(VI) and Rhodamine B mixed pollutants on three-layered Pd@MIL-101/P25 photocatalyst [J]. Sci. Total. Environ., 2022, 842: 156836 doi: 10.1016/j.scitotenv.2022.156836
44	Gao K, Chen J, Liu Z, et al. Intensified redox co-conversion of As(III) and Cr(VI) with MIL-125(Ti)-derived COOH functionalized TiO₂: performance and mechanism [J]. Chem. Eng. J., 2019, 360: 1223 doi: 10.1016/j.cej.2018.09.134
45	Shi C, Qi H J, Sun Z, et al. Carbon dot-sensitized urchin-like Ti³⁺ self-doped TiO₂ photocatalysts with enhanced photoredox ability for highly efficient removal of Cr⁶⁺ and RhB [J]. J. Mater. Chem., 2020, 8C: 2238
46	Meng X F, Zhuang Y, Tang H, et al. Hierarchical structured ZnFe₂O₄@SiO₂@TiO₂ composite for enhanced visible-light photocatalytic activity [J]. J. Alloys Compd., 2018, 761: 15 doi: 10.1016/j.jallcom.2018.05.150
47	Wang Y H, Kang C L, Li X Y, et al. Ag NPs decorated C-TiO₂/Cd_0.5Zn_0.5S Z-scheme heterojunction for simultaneous RhB degradation and Cr(VI) reduction [J]. Environ. Pollut., 2021, 286: 117305 doi: 10.1016/j.envpol.2021.117305
48	Wang J C, Ren J, Yao H C, et al. Synergistic photocatalysis of Cr(VI) reduction and 4-Chlorophenol degradation over hydroxylated α-Fe₂O₃ under visible light irradiation [J]. J. Hazard. Mater., 2016, 311: 11 doi: 10.1016/j.jhazmat.2016.02.055
49	Hu X F, Ji H H, Chang F, et al. Simultaneous photocatalytic Cr(VI) reduction and 2,4,6-TCP oxidation over g-C₃N₄ under visible light irradiation [J]. Catal. Today, 2014, 224: 34 doi: 10.1016/j.cattod.2013.11.038
50	Yi X H, Ma S Q, Du X D, et al. The facile fabrication of 2D/3D Z-scheme g-C₃N₄/UiO-66 heterojunction with enhanced photocatalytic Cr(VI) reduction performance under white light [J]. Chem. Eng. J., 2019, 375: 121944 doi: 10.1016/j.cej.2019.121944

[1]	SONG Lifang, YAN Jiahao, ZHANG Diankang, XUE Cheng, XIA Huiyun, NIU Yanhui. Carbon Dioxide Adsorption Capacity of Alkali-metal Cation Dopped MIL125[J]. 材料研究学报, 2023, 37(9): 649-654.
[2]	SHAO Hongmei, CUI Yong, XU Wendi, ZHANG Wei, SHEN Xiaoyi, ZHAI Yuchun. Template-free Hydrothermal Preparation and Adsorption Capacity of Hollow Spherical AlOOH[J]. 材料研究学报, 2023, 37(9): 675-684.
[3]	REN Fuyan, OUYANG Erming. Photocatalytic Degradation of Tetracycline Hydrochloride by g-C₃N₄ Modified Bi₂O₃[J]. 材料研究学报, 2023, 37(8): 633-640.
[4]	LIU Mingzhu, FAN Rao, ZHANG Xiaoyu, MA Zeyuan, LIANG Chengyang, CAO Ying, GENG Shitong, LI Ling. Effect of Photoanode Film Thickness of SnO₂ as Scattering Layer on the Photovoltaic Performance of Quantum Dot Dye-sensitized Solar Cells[J]. 材料研究学报, 2023, 37(7): 554-560.
[5]	LI Yanwei, LUO Kang, YAO Jinhuan. Lithium Ions Storage Properties of Ni(OH)₂ Anode Materials Prepared with Sodium Dodecyl Sulfate as Accessory Ingredient[J]. 材料研究学报, 2023, 37(6): 453-462.
[6]	YU Moxin, ZHANG Shuhai, ZHU Bowen, ZHANG Chen, WANG Xiaoting, BAO Jiamin, WU Xiang. Preparation of Nitrogen-doped Biochar and its Adsorption Capacity for Co²⁺[J]. 材料研究学报, 2023, 37(4): 291-300.
[7]	ZHU Mingxing, DAI Zhonghua. Study on Energy Storage Properties of SrSC_0.5Nb_0.5O₃ Modified BNT-based Lead-free Ceramics[J]. 材料研究学报, 2023, 37(3): 228-234.
[8]	WANG Sheng, ZHOU Qiaoting, ZHAN Huimin, CHEN Jingjing. Atomic Analysis of Contact-induced Subsurface Damage Behavior of Single Crystal SiC Based on Molecular Simulation[J]. 材料研究学报, 2023, 37(12): 943-951.
[9]	WANG Yue, FU Boyan, CHEN Shuanglong, ZOU Binglin, WANG Chunjie. Thermophysical Properties of Ln₂(Zr_0.7Ce_0.3)₂O₇ (Ln=La, Nd, Sm, Gd) Nanomaterials for Thermal Barrier Coatings[J]. 材料研究学报, 2023, 37(11): 855-861.
[10]	LIU Zhihua, YUE Yuanchao, QIU Yifan, BU Xiang, YANG Tao. Preparation of g-C₃N₄/Ag/BiOBr Composite and Photocatalytic Reduction of Nitrate[J]. 材料研究学报, 2023, 37(10): 781-790.
[11]	ZHOU Yi, TU Qiang, MI Zhonghua. Effect of Preparing Methods on Structure and Properties of Phosphate Glass-ceramics[J]. 材料研究学报, 2023, 37(10): 739-746.
[12]	XIE Feng, GUO Jianfeng, WANG Haitao, CHANG Na. Construction of ZnO/CdS/Ag Composite Photocatalyst and Its Catalytic and Antibacterial Performance[J]. 材料研究学报, 2023, 37(1): 10-20.
[13]	FANG Xiangming, REN Shuai, RONG Ping, LIU Shuo, GAO Shiyong. Fabrication and Infrared Detection Performance of Ag-modified SnSe Nanotubes[J]. 材料研究学报, 2022, 36(8): 591-596.
[14]	LI Fulu, HAN Chunmiao, GAO Jiawang, JIANG Jian, XU Hui, LI Bing. Temperature Dependent Luminescence Properties of Graphene Oxide[J]. 材料研究学报, 2022, 36(8): 597-601.
[15]	ZHU Xiaodong, XIA Yangwen, YU Qiang, Yang Daixiong, HE Lili, FENG Wei. Preparation and Characterization of Cu Doped Rutile TiO₂ and Photocatalytic Property[J]. 材料研究学报, 2022, 36(8): 635-640.

No Suggested Reading articles found!

Viewed

Full text

Abstract

Cited

Shared

Discussed