盐酸介导策略合成的具有优异光催化能力的ZnFe2O4小颗粒点缀一维苝二酰亚胺S型异质结

doi:10.1016/S1872-2067(21)63930-X

催化学报 ›› 2022, Vol. 43 ›› Issue (4): 1111-1122.DOI: 10.1016/S1872-2067(21)63930-X

盐酸介导策略合成的具有优异光催化能力的ZnFe₂O₄小颗粒点缀一维苝二酰亚胺S型异质结

徐阳锐^a, 朱晓蝶^a, 颜欢^a, 王盼盼^a, 宋旼珊^b, 马长畅^c, 陈自然^g, 储金宇^a, 刘馨琳^d^,^e^,^*(), 逯子扬^a^,^f^,^h^,^*()

^a江苏大学环境与安全工程学院, 环境健康与生态安全研究院, 江苏镇江212013, 中国
^b江苏科技大学理学院, 江苏镇江212003, 中国
^c东京大学化学系, 首尔04620, 韩国
^d江苏大学能源与动力工程学院, 江苏镇江212013, 中国
^e美国波特兰州立大学机械与材料工程系, 波特兰, 美国
^f美国田纳西州大学化学系, 诺克斯维尔37996, 美国
^g四川职业技术学院建筑与环境工程系, 四川遂宁629000, 中国
^h苏州科技大学江苏水处理技术与材料协同创新中心, 江苏苏州215009, 中国

收稿日期:2021-07-18 接受日期:2021-07-18 出版日期:2022-03-05 发布日期:2022-03-01
通讯作者: 刘馨琳,逯子扬
基金资助:
国家自然科学基金(21908080);江苏省自然科学基金(BK20180884);镇江市重点研发计划-社会发展项目(SH2018021);江苏省政府海外留学基金项目(JS-2018-243);江苏省政府海外留学基金项目(JS-2018-241);江苏水处理技术与材料协同创新中心

Hydrochloric acid-mediated synthesis of ZnFe₂O₄ small particle decorated one-dimensional Perylene Diimide S-scheme heterojunction with excellent photocatalytic ability

Yangrui Xu^a, Xiaodie Zhu^a, Huan Yan^a, Panpan Wang^a, Minshan Song^b, Changchang Ma^c, Ziran Chen^g, Jinyu Chu^a, Xinlin Liu^d^,^e^,^*(), Ziyang Lu^a^,^f^,^h^,^*()

^aInstitute of Environmental Health and Ecological Security, School of the Environment and Safety Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu, China
^bSchool of Science, Jiangsu University of Science and Technology, Zhenjiang 212003, Jiangsu, China
^cDepartment of Chemistry, Dongguk University, Seoul 04620, South Korea
^dSchool of Energy and Power Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu, China
^eDepartment of Mechanical & Materials Engineering, Portland State University, Portland, OR, USA
^fDepartment of Chemistry, University of Tennessee, Tennessee, Knoxville 37996, USA
^gDepartment of Architecture and Environment Engineering, Sichuan Vocational and Technical College, Suining 629000, Sichuan, China
^hJiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, Suzhou University of Science and Technology, Suzhou 215009, Jiangsu, China

Received:2021-07-18 Accepted:2021-07-18 Online:2022-03-05 Published:2022-03-01
Contact: Xinlin Liu, Ziyang Lu
Supported by:
National Natural Science Foundation of China(21908080);Natural Science Foundation of Jiangsu Province(BK20180884);Zhenjiang Key Research & Development Project(SH2018021);Jiangsu Government Scholarship for Overseas Studies(JS-2018-243);Jiangsu Government Scholarship for Overseas Studies(JS-2018-241);Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment

摘要/Abstract

摘要：

由于有机材料的结构多样性, 越来越多的研究者选择有机材料作为光催化剂. 典型的n型有机半导体苝二酰亚胺(PDI)不仅在可见光照射下有较强的光响应能力, 而且有合适的带隙和负导带, 使得光激发电子具有较强的还原能力. 半导体光催化剂的适用性受到光生载流子复合的限制, 而构建S型异质结可有效保证电荷分离, 也可保证空穴和电子的强氧化能力和强还原能力. 此外, 由于普通光催化剂分离回收困难, 可以将PDI与磁性半导体ZnFe₂O₄相结合来构建复合光催化剂, 该复合光催化剂可以通过外加磁场进行回收以降低成本, 在提高复合光催化剂性能的基础上保证回收率, 并且具有较好的光化学稳定性. 然而, 不同方法制得不同粒径和形貌的PDI或ZnFe₂O₄的光催化性能也不同. 因此控制PDI和ZnFe₂O₄的形貌对增强光催化活性起着至关重要的作用. 本文采用盐酸-介导策略制备了ZnFe₂O₄小颗粒点缀的一维PDI的S型异质结(1D PDI/ZnFe₂O₄). 实验发现, 用盐酸介导策略调控二者的形貌可以使其具有更好的光催化能力. 采用透射电镜(TEM)、X射线衍射、X射线光电子能谱等对1D PDI/ZnFe₂O₄进行表征, 通过光降解四环素溶液评价1D PDI/ZnFe₂O₄的光催化能力和稳定性, 并利用DFT理论计算和ESR方法等对1D PDI/ZnFe₂O₄的光催化机理进行深入的探讨.
扫描电子显微镜和TEM结果表明, 盐酸介导可有效调控1D PDI/ZnFe₂O₄的形貌, 经过盐酸介导, PDI变成均匀的棒状结构, ZnFe₂O₄变成均匀的小颗粒, 并点缀在PDI上; 而未引入盐酸的PDI仍呈不规则块状, 其ZnFe₂O₄仍为小颗粒团聚的大球状结构. XPS结合能的偏移及DFT理论计算结果表明, 材料间形成了内部电场. 当PDI和ZnFe₂O₄接触时, 为了使PDI和ZnFe₂O₄的费米能级相同, PDI中的e^‒通过界面转移到ZnFe₂O₄中, 导致界面处产生了内部电场. 同时, 由于e^‒的流失, PDI的带边向上弯曲, 而ZnFe₂O₄的带边向下弯曲. 在光照射下, PDI和ZnFe₂O₄的e^‒从VB激发到CB. 内电场、带边弯曲和库仑相互作用加速了PDI CB上e^‒和ZnFe₂O₄ VB上h⁺的复合, 也抑制了PDI CB上e^‒和VB上h⁺的复合. 综上, 1D PDI/ZnFe₂O₄的电子传递机理与S型异质结光催化反应机理一致. 光催化剂催化四环素溶液降解性能结果表明, 1D PDI/ZnFe₂O₄催化四环素溶液的降解率分别是PDI和ZnFe₂O₄的9.18倍和9.73倍. 说明通过盐酸介导策略可以有效地调控1D PDI/ZnFe₂O₄的形貌, 使其具有良好的光催化性能和回收再利用性. 本文为磁性有机-无机S型异质结光催化剂的组装提供了新思路.

关键词: 盐酸介导策略, 形貌调控, PDI/ZnFe₂O₄, S型异质结, 光催化能力

Abstract:

The recyclable and stable ZnFe₂O₄ small particle decorated one-dimensional perylene diimide (PDI) S-scheme heterojunction (1D PDI/ZnFe₂O₄) is prepared by the hydrochloric acid-mediated (HCl-mediated) strategy, interestingly, the morphology of the 1D PDI/ZnFe₂O₄ can also be effectively regulated by HCl-mediated process, the existence of HCl can regulate PDI into a uniform rod structure, while the co-existence of HCl and PDI can limit ZnFe₂O₄ to become the uniform small particles. More importantly, based on the 1D rod structure of PDI and the small size effect of ZnFe₂O₄, carriers can migrate to the surface more easily, which can improve the photocatalytic activity. Meanwhile, due to the appropriate energy level structure, the S-scheme heterojunction structure is formed between PDI and ZnFe₂O₄, which eliminates meaningless photo-generated charge carriers through recombination and introduces strong redox to further enhance the photodegradation effect, thereby, 1D PDI/ZnFe₂O₄ exhibits excellent photocatalytic ability, under the visible light irradiation, the degradation rate of tetracycline (TC) with 1D PDI/ZnFe₂O₄ (66.67%) is 9.18 times that with PDI (7.26%) and 9.73 times that with ZnFe₂O₄ (6.85%). This work proposes new ideas for the assembly of magnetic organic-inorganic S-scheme heterojunction photocatalysts.

Key words: Hydrochloric acid-mediated strategy, Morphology regulation, Perylene diimide/ZnFe₂O₄, S-scheme heterojunction, Photocatalytic ability

徐阳锐, 朱晓蝶, 颜欢, 王盼盼, 宋旼珊, 马长畅, 陈自然, 储金宇, 刘馨琳, 逯子扬. 盐酸介导策略合成的具有优异光催化能力的ZnFe₂O₄小颗粒点缀一维苝二酰亚胺S型异质结[J]. 催化学报, 2022, 43(4): 1111-1122.

Yangrui Xu, Xiaodie Zhu, Huan Yan, Panpan Wang, Minshan Song, Changchang Ma, Ziran Chen, Jinyu Chu, Xinlin Liu, Ziyang Lu. Hydrochloric acid-mediated synthesis of ZnFe₂O₄ small particle decorated one-dimensional Perylene Diimide S-scheme heterojunction with excellent photocatalytic ability[J]. Chinese Journal of Catalysis, 2022, 43(4): 1111-1122.

×
扫码分享

导出引用管理器 EndNote|Ris|BibTeX

链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(21)63930-X

https://www.cjcatal.com/CN/Y2022/V43/I4/1111

图/表 18

Scheme 1. The synthesis process of 1D PDI/ZnFe2O4 by the HCl-mediated strategy.

Fig. 1. TEM images of PDI (a), ZnFe2O4 (b), 1D PDI/ZnFe2O4 (c and d), PDI/ZnFe2O4 (e) and HCl-ZnFe2O4 (f).

Fig. 2. N2 adsorption-desorption isotherm of the PDI (a), ZnFe2O4(b) and 1D PDI/ZnFe2O4(c).

Fig. 3. XRD patterns (a) and FTIR spectra (b) of different samples.

Fig. 4. XPS spectra of 1D PDI/ZnFe2O4. (a) The survey spectra; (b) C 1s; (c) N 1s; (d) O 1s; (e) Zn 2p; (f) Fe 2p.

Fig. 5. Magnetization patterns at room temperature (a) and UV-vis diffuse reflectance spectrum of different samples (b). (inset in a is the photograph of 1D PDI/ZnFe2O4 separated from solution under a magnet).

Fig. 6. Degradation rates (a), the pseudo-first-order kinetics fitting data (b), degradation rates and error analysis of three repeated experiments at 60 min (c), the pseudo-first-order kinetics fitting data and error analysis of three repeated experiments at 60 min (d) for photodegradation of TC over different samples.

Table 1 Degradation rates and apparent rate constants for degradation of TC with different samples at 60 min and the corresponding error analysis of three repeated experiments.

Sample	Degradation rate (%)	Apparent rate constant (min^-1)
No sample	4.55 ± 0.25	0.065 ± 0.002
PDI	7.26 ± 0.35	0.16 ± 0.004
ZnFe₂O₄	6.85 ± 0.45	0.19 ± 0.004
1D PDI/ZnFe₂O₄	66.67 ± 1.8	1.10 ± 0.03
PDI/ZnFe₂O₄	7.98 ± 0.67	0.08 ± 0.007
HCl-ZnFe₂O₄	7.55 ± 0.56	0.08 ± 0.007

Fig. 7. Degradation rates and error analysis of three repeated experiments at 60 min for TC degradation with 1D PDI/ZnFe2O4 under different cycle times.

Fig. 8. The EIS plots (a) and photocurrent response (b) of different samples.

Fig. 9. Mott-Schottky plots of PDI (a) and ZnFe2O4 (b).

Fig. 10. The tauc plots of PDI (a) and ZnFe2O4 (b).

Fig. 11. Work function of PDI (a) and ZnFe2O4 (b), the structural models for DFT calculation (Inset).

Fig. 12. The effect of degradation of TC in existence of different quenchers and error analysis of three repeated experiments at 60 min over 1D PDI/ZnFe2O4 (a), and the corresponding time-change UV-vis UV-vis absorption spectrum (b-d).

Fig. 13. ESR of •O2-(a) and •OH (b) for PDI, ZnFe2O4 and 1D PDI/ZnFe2O4.

Fig. 14. The electron transfer mechanism near the interface of 1D PDI/ZnFe2O4. (a) PDI and ZnFe2O4 before contact; (b) PDI and ZnFe2O4 after contact; (c) PDI/ZnFe2O4 under light irradiation.

Fig. 15. The proposed photocatalytic mechanism of degradation of TC by 1D PDI/ZnFe2O4.

Fig. 16. The possible intermediates products on degradation of TC.

参考文献

[1]	H. Wu, J. Wang, R. Chen, C. Yuan, J. Zhang, Y. Zhang, J. Sheng, F. Dong, Chin. J. Catal., 2021, 42, 1195-1204.
[2]	R. Chen, H. Wang, H. Wu, J. Sheng, J. Li, W. Cui, F. Dong, Chin. J. Catal., 2020, 41, 710-718.
[3]	W. Zeng, C. Tao, Y. Liu, L. Wang, W. Dong, H. Chen, X. Xia, Chem. Eng. J., 2019, 381, 122691.
[4]	Q. Ji, Z. Xu, W. Xiang, Y. Wu, X. Cheng, C. Xu, C. Qi, H. He, J. Hu, S. Yang, S. Li, L. Zhang, Chemosphere, 2020, 253, 126751.
[5]	J. Shang, H. Tang, H. Ji, W. Ma, C. Chen, J. Zhao, Chin. J. Catal., 2017, 38, 2094-2101.
[6]	F. Shao, Y. Wang, Y. Mao, T. Shao, J. Shang, Chemosphere, 2020, 261, 127844.
[7]	Z. Lu, G. Zhou, M. Song, D. Wang, P. Huo, W. Fan, H. Dong, H. Tang, F. Yan, G. Xing, J. Mater. Chem. A, 2019, 7, 13986-14000.
[8]	A. Xu, W. Tu, S. Shen, Z. Lin, N. Gao, W. Zhong, Appl. Surf. Sci., 2020, 528, 146949.
[9]	Q. Xie, W. He, S. Liu, C. Li, J. Zhang, P. Wong, Chin. J. Catal., 2020, 41, 140-153.
[10]	Q. Xu, L. Zhang, B. Cheng, J. Fan, J. Yu, Chem, 2020, 6, 1543-1559.
[11]	X. Jia, Q. Han, H. Liu, S. Li, H. Bi, Chem. Eng. J., 2020, 399, 125701.
[12]	H. Ge, F. Xu, B. Cheng, J. Yu, W. Ho, ChemCatChem, 2019, 11 : 6301-6309.
[13]	W. Wang, W. Zhao, H. Zhang, X. Dou, H. Shi, Chin. J. Catal., 2021, 42, 97-106.
[14]	J. Wei, Y. Chen, H. Zhang, Z. Zhuang, Y. Yu, Chin. J. Catal., 2021, 42, 78-86.
[15]	J. Wang, G. Wang, B. Cheng, J. Yu, J. Fan, Chin. J. Catal., 2021, 42, 56-68.
[16]	F. He, Z. Lu, M. Song, X. Liu, H. Tang, P. Huo, W. Fan, H. Dong, X. Wu, S. Han, Chem. Eng. J., 2019, 360, 750-761.
[17]	N. Chnadel, K. Sharma, A. Sudahiak, P. Raizada, A. Hosseini-Bandegharaei, V. K. Thakur, P. Singh, Arab. J. Chem., 2020, 13, 4324-4340.
[18]	F. He, Z. Lu, M. Song, X. Liu, H. Tang, P. Huo, W. Fan, H. Dong, X. Wu, G. Xing, Appl. Surf. Sci., 2019, 483, 453-462.
[19]	Z. Lu, G. Zhou, M. Song, X. Liu, H. Tang, H. Dong, P. Huo, F. Yan, P. Du, G. Xing, Appl. Catal. B, 2020, 268, 118433.
[20]	D. Qin, Y. Xia, Q. Li, C. Yang, Y. Qin, K. Lv, J. Mater. Sci. Technol., 2020, 56, 206-215.
[21]	Y. Huang, D. Zhu, Q. Zhang, Y. Zhang, J. Cao, Z. Shen, W. Ho, S. C. Lee, Appl. Catal. B, 2018, 234, 70-78.
[22]	Y. Li, Y. Fang, Z. Cao, N. Li, D. Chen, Q. Xu, J. Lu, Appl. Catal. B, 2019, 250, 150-162.
[23]	T. Cai, W. Zeng, Y. Liu, L. Wang, W. Dong, H. Chen, X. Xia, Appl. Catal. B, 2020, 263, 118327.
[24]	Z. Zhang, X. Chen, H. Zhang, W. Liu, W. Zhu, Y. Zhu, Adv. Mater., 2020, 32, 1907746.
[25]	Q. Zhang, L. Jiang, J. Wang, Y. Zhu, Y. Pu, W. Dai, Appl. Catal. B, 2020, 277, 119122.
[26]	A. Meng, B. Cheng, H. Tan, J. Fan, C. Su, J. Yu, Appl. Catal. B, 2021, 289, 120039.
[27]	Q. Gao, J. Xu, Z. Wang, Y. Zhu, Y. Zhu,, Appl. Catal. B, 2020, 271, 118933.
[28]	Z. Lu, X. Zhao, Z. Zhu, Y. Yan, W. Shi, H. Dong, Z. Ma, N. Gao, Y. Wang, H. Huang, Chem. Eur. J., 2015, 21, 18528-18533.
[29]	A. Habibi-Yangjeh, M. Shekofteh-Gohari, D. O. Chemistry, F. O. Science, Prog. Nat. Sci., Mater. Int., 2019, 29, 145-155.
[30]	Z. Lu, Z. Yu, J. Dong, M. Song, Y. Liu, X. Liu, Z. Ma, H. Su, Y. Yan, P. Huo, Chem. Eng. J., 2018, 337, 228-241.
[31]	F. J. Zhao, G. Zhang, Z. Ju, Y. X. Tan, D. Yuan, Inorg. Chem., 2020, 59, 3297-3303.
[32]	H. Zhang, Y. Song, L. Nengzi, J. Gou, B. Li, X. Cheng, Chem. Eng. J., 2020, 379, 122362.
[33]	J. Wang, Q. Zhang, F. Deng, X. Luo, D. D. Dionysiou, Chem. Eng. J., 2020, 379, 122264.
[34]	M. Zangiabadi, A. Saljooqi, T. Shamspur, A. Mostafavi, Ceram. Int., 2020, 46, 6124-6128.
[35]	D. Lei, J. Xue, X. Peng, S. Li, Q. Bi, C. Tang, L. Zhang, Appl. Catal. B, 2021, 282,119578.
[36]	F. Mei, Z. Li, K. Dai, J. Zhang, C. Liang, Chin. J. Catal., 2020, 41, 41-49.
[37]	A. H. Mady, M. L. Baynosa, D. Tuma, J.-J. Shim, Appl. Catal. B, 2017, 203, 416-427.
[38]	Z. Lu, W. Zhou, P. Huo, Y. Luo, M. He, J. Pan, C. Li, Y. Yan, Chem. Eng. J., 2013, 225, 34-42.
[39]	H. Zhou, S. Zhou, M. Shen, Y. Yao, Ceram. Int., 2019, 45, 15036-15047.
[40]	Z. Lu, J. Peng, M. Song, Y. Liu, X. Liu, P. Huo, H. Dong, S. Yuan, Z. Ma, S. Han, Chem. Eng. J., 2019, 360, 1262-1276.
[41]	Y. Zhou, S. Fang, M. Zhou, G. Wang, S. Xue, Z. Li, S. Xu, C. Yao, J. Alloys Compd., 2017, 696, 353-361.
[42]	M. Hong, J. Yang, Y. Wei, W. Li, Y. Zhu, Appl. Catal. B, 2018, 239, 61-67.
[43]	Z. Lu, Y. Xu, Y. Ren, G. Zhou, H. Yan, M. Song, P. Wang, C. Ma, S. Han, X. Liu, Appl. Surf. Sci., 2021, 569, 151027.
[44]	I. Benyamina, K. Manseri, M. Mansour, B. Benalioua, A. Bentouami, B. Boury, Appl. Surf. Sci., 2019, 483, 859-869.
[45]	X. Li, J. Zhang, Y. Huo, K. Dai, S. Li, S. Chen, Appl. Catal. B, 2021, 280, 119452.
[46]	T. Yan, H. Liu, Z. Jin, ACS Appl. Mater. Interfaces, 2021, 13, 24896-24906.
[47]	J. Xu, X. Li, J. Niu, M. Chen, J. Yue, J. Alloys Compd., 2020, 834, 155061.
[48]	A. Serra, P. Pip, E. Gómez, L. Philippe, Appl. Catal. B, 2020, 268, 118745.
[49]	Z. Lu, F. Chen, M. He, M. Song, Z. Ma, W. Shi, Y. Yan, J. Lan, F. Li, P. Xiao, Chem. Eng. J., 2014, 249, 15-26.
[50]	W. Zhao, Z. Wei, X. Zhang, M. Ding, S. Huang, S. Yang, Appl. Catal. A, 2020, 593, 117443.
[51]	Z. Zhu, C. Ma, K. Yu, Z. Lu, Z. Liu, P. Huo, T. Xu, Y. Yan, Appl. Catal. B, 2020, 268, 118432.
[52]	M. Tahir, N. Manzoor, M. Sagir, M. B. Tahir, T. Nawaz, Fuel, 2021, 285, 119206.
[53]	J. Yang, H. Miao, J. Jing, Y. Zhu, W. Choi, Appl. Catal. B, 2021, 281, 119547.
[54]	S. Wageh, A. A. Al-Ghamdi, R. Jafer, X. Li, P. Zhang, Chin. J. Catal., 2021, 42, 667-669.
[55]	C. Cheng, B. He, J. Fan, B. Cheng, S. Cao, J. Yu, Adv. Mater., 2021, 33, 2100317.
[56]	J. Mu, F. Teng, H. Miao, Y. Wang, X. Hu, Appl. Surf. Sci., 2020, 501, 143974.
[57]	J. Fu, Q. Xu, J. Low, C. Jiang, J. Yu, Appl. Catal. B, 2019, 243, 556-565.
[58]	T. Yan, H. Liu, Z. L. Jin, ACS Appl. Mater. Interfaces, 2021, 13, 24896-24906.
[59]	H. Wu, S. Meng, J. Zhang, X. Zheng, Y. Wang, S. Chen, G. Qi, X. Fu, Appl. Surf. Sci., 2020, 505, 144638.
[60]	Y. Sun, X. Qi, R. Li, Y. Xie, Q. Tang, B. Ren, Opt. Mater., 2020, 108, 110170.
[61]	S. Tang, M. Zhao, D. Yuan, X. Li, Z. Wang, X. Zhang, T. Jiao, J. Ke, Chemosphere, 2020, 268, 129315.

编辑推荐

Metrics

阅读次数

全文

492

HTML			PDF

最新录用	在线预览	正式出版	最新录用	在线预览	正式出版
0	0	7	19	0	466

来源	本网站	其他网站

次数	479	13
比例	97%	3%

摘要

175

最新录用	在线预览	正式出版

22	0	153

	来源	本网站

	次数	175
	比例	100%

盐酸介导策略合成的具有优异光催化能力的ZnFe₂O₄小颗粒点缀一维苝二酰亚胺S型异质结

Hydrochloric acid-mediated synthesis of ZnFe₂O₄ small particle decorated one-dimensional Perylene Diimide S-scheme heterojunction with excellent photocatalytic ability

RichHTML

PDF

Supporting Information