CdS修饰的一维g-C<sub>3</sub>N<sub>4</sub>多孔纳米管在光催化降解污染物和产氢中的应用

引用本文: 种奔, 陈雷, 韩德志, 王亮, 冯丽娟, 李勤, 李春虎, 王文泰. CdS修饰的一维g-C₃N₄多孔纳米管在光催化降解污染物和产氢中的应用[J]. 催化学报, 2019, 40(6): 959-968. doi: S1872-2067(19)63355-3 shu

Citation: Ben Chong, Lei Chen, Dezhi Han, Liang Wang, Lijuan Feng, Qin Li, Chunhu Li, Wentai Wang. CdS-modified one-dimensional g-C₃N₄ porous nanotubes for efficient visible-light photocatalytic conversion[J]. Chinese Journal of Catalysis, 2019, 40(6): 959-968. doi: S1872-2067(19)63355-3 shu

CdS修饰的一维g-C₃N₄多孔纳米管在光催化降解污染物和产氢中的应用

种奔 ^a, ,
陈雷 ^a, ,
韩德志 ^b, ,
王亮 ^a, ,
冯丽娟 ^a, ,
李勤 ^c, ,
李春虎 ^a, ,
王文泰 ^a,

a 中国海洋大学海洋化学理论与技术教育部重点实验室, 化学化工学院, 山东青岛 266100, 中国;
b 青岛科技大学化工学院, 山东青岛 266042, 中国;
c 格里菲斯大学昆士兰微米纳米技术中心, 布里斯班, 澳大利亚
基金项目:
国家自然科学基金（51602297，U1510109）；山东省重点研发计划（重大关键技术）（2016ZDJS11A04）；中央高校基本科研业务费（201612007）；山东省博后创新项目（201603043）；澳大利亚研究理事会（ARC）项目（DP160104089）；青岛科技大学引进人才科研启动基金（010022919）.

摘要: 利用太阳光在光催化材料作用下将低能量密度的太阳能转化成化学能储存在氢气和一氧化碳等清洁能源中，有利于能量的存储、运输和使用，具有广阔的前景.光催化技术的关键在于催化剂，以TiO₂为代表的传统半导体光催化剂存在着电子与空穴复合率高、禁带宽度过大和无法吸收可见光等缺点，这些因素限制了其在光催化领域的进一步发展和应用.因此，寻找优秀的光催化材料是科研工作者的不懈追求.
石墨相氮化碳是一种仅由C和N两种元素组成的有机半导体材料，具有良好的热稳定、耐腐蚀性和生物相容性，这些优点使得石墨相氮化碳在多个领域都极具应用前景.在光催化领域，石墨相氮化碳独特的电子结构、稳定的物理化学性质，以及其导带位置（约–1.12eV）远小于氢离子的还原电势（0eV），使其能够很好地应用于光解化降解污染物和光解水产氢.
目前，石墨相氮化碳光催化技术的研究重点在于如何解决石墨相氮化碳比表面积过小和光量子效率低的问题.针对这些问题，我们对石墨相氮化碳光催化材料的结构进行了设计，构建出CdS修饰的一维g-C₃N₄多孔纳米管.以三聚氰胺为原料，通过质子化处理，得到表面光滑、质地均匀、拥有超高长径比的三聚氰胺纳米纤维（MNFs），然后对其进行煅烧处理得到多孔纳米管状g-C₃N₄催化剂.随后，在纳米管的基础上通过水热法与CdS颗粒复合，成功制备出多孔管状g-C₃N₄/CdS复合异质结型催化剂.利用多种表征手段对所合成的新型光催化剂的形貌、结构、光学性质及光电性质进行了表征，并评估了其光催化降解罗丹明B和光解水产氢性能，考察了催化剂的循环利用及稳定性.
SEM和TEM结果表明，管状的石墨相氮化碳拥有丰富的孔道结构，其增大的比表面积有利于暴露更多的活性位点，从而提高了光催化性能.光催化降解罗丹明B实验表明，多孔管状g-C₃N₄的催化性能较体相g-C₃N₄有明显提高.当管状g-C₃N₄与适量CdS复合形成异质结型光催化剂时，光催化效果得到进一步提升，其中当CdS负载量为10 mol%时，复合物的催化效果最好，在60min内可完全降解罗丹明B.在光催化分解水产氢实验中，5h内管状g-C₃N₄/CdS复合物产氢量高达362.7μmol，分别是体相g-C₃N₄的16.3倍和管状g-C₃N₄的4.6倍.

关键词:

English

CdS-modified one-dimensional g-C₃N₄ porous nanotubes for efficient visible-light photocatalytic conversion

a Key Laboratory of Marine Chemistry Theory and Technology, Ministry of Education, College of Chemistry and Chemical Engineering, Ocean University of China, Qingdao 266100, Shandong, China;
b College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China;
c Queensland Micro- and Nanotechnology Centre, Griffith University Nathan Campus, Brisbane, QLD 4111, Australia
Received Date: 19 December 2018
Revised Date: 12 March 2019
Fund Project:
The authors acknowledge the financial support from the National Natural Science Foundation of China (51602297 and U1510109), Major Research Project of Shandong Province (2016ZDJS11A04), Fundamental Research Funds for the Central Universities (201612007), Postdoctoral Innovation Program of Shandong Province (201603043), Australia Research Council (ARC) under the Project DP160104089, and Start-up Foundation for Advanced Talents of Qingdao University of Science and Technology (010022919).

Abstract: A heterojunction photocatalyst based on porous tubular g-C₃N₄ decorated with CdS nanoparticles was fabricated by a facile hydrothermal co-deposition method. The one-dimensional porous structure of g-C₃N₄ provides a higher specific surface area, enhanced light absorption, and better separation and transport performance of charge carriers along the longitudinal direction, all of which synergistically contribute to the superior photocatalytic activity observed. The significantly enhanced catalytic efficiency is also a benefit originating from the fast transfer of photogenerated electrons and holes between g-C₃N₄ and CdS through a built-in electric field, which was confirmed by investigating the morphology, structure, optical properties, electrochemical properties, and photocatalytic activities. Photocatalytic degradation of rhodamine B (RhB) and photocatalytic hydrogen evolution reaction were also carried out to investigate its photocatalytic performance. RhB can be degraded completely within 60 min, and the optimum H₂ evolution rate of tubular g-C₃N₄/CdS composite is as high as 71.6 μmol h^-1, which is about 16.3 times higher than that of pure bulk g-C₃N₄. The as-prepared nanostructure would be suitable for treating environmental pollutants as well as for water splitting.

Key words:

1. [1] Y. Zheng, Y. Jiao, Y. Zhu, L. H. Li, Y. Han, Y. Chen, A. Du, M. Jaroniec, S. Z. Qiao, Nat. Commun., 2014, 5, 3783/1-3783/8.
2. [2] W. J. Ong, L. L. Tan, Y. H. Ng, S. T. Yong, S. P. Chai, Chem. Rev., 2016, 116, 7159-7329.
3. [3] S. Ye, R. Wang, M. Z. Wu, Y. P. Yuan, Appl. Surf. Sci., 2015, 358, 15-27.
4. [4] S. Yin, J. Han, T. Zhou, R. Xu, Catal. Sci. Technol., 2015, 5, 5048-5061.
5. [5] X. Ma, Y. Lv, J. Xu, Y. Liu, R. Zhang, Y. Zhu, J. Phys. Chem. C, 2012, 116, 23485-23493.
6. [6] Y. Zhou, L. Zhang, W. Huang, Q. Kong, X. Fan, M. Wang, J. Shi, Carbon, 2016, 99, 111-117.
7. [7] S. Tonda, S. Kumar, S. Kandula, V. Shanker, J. Mater. Chem. A, 2014, 2, 6772-6780.
8. [8] X. Wu, F. Chen, X. Wang, H. Yu, Appl. Surf. Sci., 2018, 427, 645-653.
9. [9] Z. Zhu, M. Murugananthan, J. Gu, Y. Zhang, Catalysts, 2018, 8, 112/1-112/16.
10. [10] J. Yu, S. Wang, J. Low, W. Xiao, Phys. Chem. Chem. Phys., 2013, 15, 16883-16890.
11. [11] L. Ge, C. Han, X. Xiao, L. Guo, Int. J. Hydrogen Energy, 2013, 38, 6960-6969.
12. [12] B. Chong, L. Chen, W. Wang, D. Han, L. Wang, L. Feng, Q. Li, C. Li, Mater. Lett., 2017, 204, 149-153.
13. [13] L. Liu, Y. Qi, J. Lu, S. Lin, W. An, Y. Liang, W. Cui, Appl. Catal. B, 2016, 183, 133-141.
14. [14] F. Wang, Y. Wang, Y. Feng, Y. Zeng, Z. Xie, Q. Zhang, Y. Su, P. Chen, Y. Liu, K. Yao, W. Lv, G. Liu, Appl. Catal. B, 2018, 221, 510-520.
15. [15] F. Chen, H. Yang, X. Wang, H. Yu, Chin. J. Catal., 2017, 38, 296-304.
16. [16] J. Zhang, Y. Wang, J. Jin, J. Zhang, Z. Lin, F. Huang, J. Yu, ACS Appl. Mater. Interfaces, 2013, 5, 10317-10324.
17. [17] L. Cheng, Q. Xiang, Y. Liao, H. Zhang, Energy Environ. Sci., 2018, 11, 1362-1391.
18. [18] H. Zhao, M. Wu, J. Liu, Z. Deng, Y. Li, B. L. Su, Appl. Catal. B, 2016, 184, 182-190.
19. [19] F. Ye, H. Li, H. Yu, S. Chen, X. Quan, Appl. Catal. B, 2018, 227, 258-265.
20. [20] D. Barpuzary, Z. Khan, N. Vinothkumar, M. De, M. Qureshi, J. Phys. Chem. C, 2011, 116, 150-156.
21. [21] Y. Shi, H. Li, L. Wang, W. Shen, H. Chen, ACS Appl. Mater. Interfaces, 2012, 4, 4800-4806.
22. [22] H. Huang, K. Xiao, N. Tian, F. Dong, T. Zhang, X. Du, Y. Zhang, J. Mater. Chem. A, 2017, 5, 17452-17463.
23. [23] F. Jiang, T. Yan, H. Chen, A. Sun, C. Xu, X. Wang, Appl. Surf. Sci., 2014, 295, 164-172.
24. [24] F. Cheng, H. Yin, Q. Xiang, Appl. Surf. Sci., 2017, 391, 432-439.
25. [25] L. Ge, F. Zuo, J. Liu, Q. Ma, C. Wang, D. Sun, L. Bartels, P. Feng, J. Phys. Chem. C, 2012, 116, 13708-13714.
26. [26] N. Wu, J. Wang, D. N. Tafen, H. Wang, J. G. Zheng, J. P. Lewis, X. Liu, S. S. Leonard, A. Manivannan, J. Am. Chem. Soc., 2010, 132, 6679-6685.
27. [27] K. Wu, H. Zhu, Z. Liu, W. Rodriguez-Cordoba, T. Lian, J. Am. Chem. Soc., 2012, 134, 10337-10340.
28. [28] X. Pan, Y. Zhao, S. Liu, C. L. Korzeniewski, S. Wang, Z. Fan, ACS Appl. Mater. Interfaces, 2012, 4, 3944-3950.
29. [29] J. Gao, Y. Zhou, Z. Li, S. Yan, N. Wang, Z. Zou, Nanoscale, 2012, 4, 3687-3692.
30. [30] Y. Zheng, Y. Jiao, Y. Zhu, Q. Cai, A. Vasileff, L. H. Li, Y. Han, Y. Chen, S. Z. Qiao, J. Am. Chem. Soc., 2017, 139, 3336-3339.
31. [31] G. Dong, Y. Zhang, Q. Pan, J. Qiu, J. Photochem. Photobiol. C, 2014, 20, 33-50.
32. [32] X. Yang, F. Qian, G. Zou, M. Li, J. Lu, Y. Li, M. Bao, Appl. Catal. B, 2016, 193, 22-35.
33. [33] C. Liu, Y. Zhang, F. Dong, X. Du, H. Huang, J. Phys. Chem. C, 2016, 120, 10381-10389.
34. [34] J. Xu, G. Wang, J. Fan, B. Liu, S. Cao, J. Yu, J. Power Sources, 2015, 274, 77-84.
35. [35] X. Wu, J. Zhao, L. Wang, M. Han, M. Zhang, H. Wang, H. Huang, Y. Liu, Z. Kang, Appl. Catal. B, 2017, 206, 501-509.
36. [36] P. Dalvand, M. R. Mohammadi, D. J. Fray, Mater. Lett., 2011, 65, 1291-1294.
37. [37] K. He, J. Xie, X. Luo, J. Wen, S. Ma, X. Li, Y. Fang, X. Zhang, Chin. J. Catal., 2017, 38, 240-252.

扫一扫看文章

计量

PDF下载量: 7
文章访问数: 1913
HTML全文浏览量: 137

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

CdS修饰的一维g-C₃N₄多孔纳米管在光催化降解污染物和产氢中的应用

English

CdS-modified one-dimensional g-C₃N₄ porous nanotubes for efficient visible-light photocatalytic conversion

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

CdS修饰的一维g-C3N4多孔纳米管在光催化降解污染物和产氢中的应用

English

CdS-modified one-dimensional g-C3N4 porous nanotubes for efficient visible-light photocatalytic conversion

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

文章相关

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

CdS修饰的一维g-C₃N₄多孔纳米管在光催化降解污染物和产氢中的应用

CdS-modified one-dimensional g-C₃N₄ porous nanotubes for efficient visible-light photocatalytic conversion

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs