双助剂促进g-C3N4光解水制氢性能

doi:10.1016/S1872-2067(18)63189-4

催化学报 ›› 2019, Vol. 40 ›› Issue (3): 434-445.DOI: 10.1016/S1872-2067(18)63189-4

双助剂促进g-C₃N₄光解水制氢性能

李纵^a, 马永宁^a, 胡晓云^b, 刘恩周^a,b,c, 樊君^a

a 西北大学化工学院, 陕西西安 710069;
b 西北大学物理学院, 陕西西安 710127;
c 西北大学现代物理研究所, 陕西西安 710069

收稿日期:2018-08-30 修回日期:2018-10-13 出版日期:2019-03-18 发布日期:2019-02-22
通讯作者: 刘恩周, 樊君
基金资助:
国家自然科学基金（21676213，21476183，51372201）；中国博士后科学基金（2016M600809）；中国陕西省自然科学基础研究计划（2017JM2026）.

Enhanced photocatalytic H₂ production over dual-cocatalyst-modified g-C₃N₄ heterojunctions

Zong Li^a, Yongning Ma^a, Xiaoyun Hu^b, Enzhou Liu^a,b,c, Jun Fan^a

a School of Chemical Engineering, Northwest University, Xi'an 710069, Shaanxi, China;
b School of Physics, Northwest University, Xi'an 710069, Shaanxi, China;
c Institute of Modern Physics, Northwest University, Xi'an 710069, Shaanxi, China

Received:2018-08-30 Revised:2018-10-13 Online:2019-03-18 Published:2019-02-22
Supported by:
This work was supported by the National Natural Science Foundation of China (21676213, 21476183, 51372201), the China Postdoctoral Science Foundation (2016M600809), and the Natural Science Basic Research Plan in Shaanxi Province of China (2017JM2026).

摘要/Abstract

摘要：

氢能是最具应用前景的清洁能源之一，利用太阳能作为驱动力光催化水分解制取氢气已被广泛研究.作为非金属半导体光催化剂，g-C₃N₄具有合适的能带结构（2.71eV），良好的可见光捕获能力和物理化学稳定性，因而有一定的光催化产氢能力；但是它具有可见光吸收能力（<470nm）不够、光生电子空穴容易复合等缺点，使其光催化制氢能力受到了极大限制.通过助剂修饰可有效促进载流子分离，增加反应活性位点及加速产氢动力学.因此，本文采用双助剂改性以提高g-C₃N₄的光催化制氢性能.
本文首先采用原位煅烧法将银纳米粒子（Ag NPs）沉积在g-C₃N₄表面（Ag/g-C₃N₄），随后利用水热法成功地将硫化镍（NiS）负载在Ag/g-C₃N₄复合材料表面.XRD，FT-IR，XPS和TEM结果表明，通过原位煅烧和水热合成法可以成功地将Ag和NiS均匀、稳定沉积在g-C₃N₄表面，并且g-C₃N₄保持原有结构不变.紫外可见吸收光谱（UV-Vis）、瞬态光电流、阻抗（EIS）和光致发光谱（PL）分析表明，Ag NPs和NiS的引入不仅改善了体系的光吸收范围和强度，而且显著提高了体系光生电子和空穴的产生、分离性能，有助于提高光子利用效率.其中三元样品的最高光电流可以达到2.94x 10^-7A·cm^-2，是纯g-C₃N₄的3.1倍.
对系列光催化剂的分解水制氢性能测试发现（采用300W氙灯作为光源，三乙醇胺作为牺牲剂），10 wt%-NiS/1.0 wt%-Ag/CN样品具有最优异的光催化分解水制氢性能，产氢速率可达9.728mmol·g^-1·h^-1，是纯g-C₃N₄的10.82倍，二元10 wt%-NiS/CN的3.45倍，1.0 wt%-Ag/CN的2.77倍.三元样品反应前后的XRD特征峰位置没有发生变化，循环四次后样品仍具有83%的催化活性，证明其具有良好的制氢稳定性.10 wt%-NiS/1.0 wt%-Ag/CN样品在可见光下（λ > 420nm）的制氢量子效率为1.21%.三元体系光催化产氢性能增强的原因在于：（1）Ag纳米颗粒的局域表面等离子体效应使得三元体系的光捕获能力得到提高；（2）Ag NPs和NiS负载在g-C₃N₄上共同促进了光生电子空穴的产生和分离；（3）Ag NPs和NiS作为优良的析氢助催化剂沉积在g-C₃N₄表面上可以有效地提高产氢动力学.本文构建的NiS/Ag/g-C₃N₄复合体系为g-C₃N₄基复合光催化剂的设计及制备提供了新的思路.

关键词: 光催化, 光催化制氢, 氮化碳, 银, 硫化镍

Abstract:

Ag nanoparticles (NPs) were deposited on the surface of g-C₃N₄ (CN) by an in situ calcination method. NiS was successfully loaded onto the composites by a hydrothermal method. The results showed that the 10 wt%-NiS/1.0 wt%-Ag/CN composite exhibits excellent photocatalytic H₂ generation performance under solar-light irradiation. An H₂ production rate of 9.728 mmol·g^-1·h^-1 was achieved, which is 10.82-, 3.45-, and 2.77-times higher than those of pure g-C₃N₄, 10 wt%-NiS/CN, and 1.0 wt%-Ag/CN composites, respectively. This enhanced photocatalytic H₂ generation can be ascribed to the co-decoration of Ag and NiS on the surface of g-C₃N₄, which efficiently improves light harvesting capacity, photogenerated charge carrier separation, and photocatalytic H₂ production kinetics. Thus, this study demonstrates an effective strategy for constructing excellent g-C₃N₄-related composite photocatalysts for H₂ production by using different co-catalysts.

Key words: Photocatalysis, Photocatalytic H₂ generation, g-C₃N₄, Ag, NiS

李纵, 马永宁, 胡晓云, 刘恩周, 樊君. 双助剂促进g-C₃N₄光解水制氢性能[J]. 催化学报, 2019, 40(3): 434-445.

Zong Li, Yongning Ma, Xiaoyun Hu, Enzhou Liu, Jun Fan. Enhanced photocatalytic H₂ production over dual-cocatalyst-modified g-C₃N₄ heterojunctions[J]. Chinese Journal of Catalysis, 2019, 40(3): 434-445.

×
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(18)63189-4

https://www.cjcatal.com/CN/Y2019/V40/I3/434

参考文献

[1] C. L. Muhich, B. D. Ehrhart, I. Al-Shankiti, B. J. Ward, C. B. Musgrave, A. W. Weimer, Wires Wiley Interdis. Rev. Energy Environ., 2016, 5, 261-287.
[2] X. Li, J. G. Yu, J. X. Low, Y. P. Fang, J. Xiao, X. B. Chen, J. Mater. Chem. A, 2015, 3, 2485-2534.
[3] W. J. Ong, L. L. Tan, Y. H. Ng, S. T. Yong, S. P. Chai, Chem. Rev., 2016, 116, 7159-7329.
[4] K. Chen, Z. G. Chai, C. Li, L. R. Shi, M. X. Liu, Q. Xie, Y. F. Zhang, D. S. Xu, A. Manivannan, Z. F. Liu, ACS Nano, 2016, 10, 3665-3673.
[5] Q. Li, X. Li, S. Wageh, A. A. Al-Ghamdi, J. G. Yu, Adv. Energy. Mater., 2015, 5, 1500010.
[6] J. Q. Wen, J. Xie, X. B. Chen, X. Li, Appl. Surf. Sci., 2017, 391, 72-123.
[7] S. W. Cao, H. Li, Y. Li, B. C. Zhu, J. G. Yu, ACS Sustain. Chem. Eng., 2018, 6, 6478-6487.
[8] W. H. Xue, X. Y. Hu, E. Z. Liu, J. Fan, Appl. Surf. Sci., 2018, 447, 783-794.
[9] X. C Wang, K. Maeda, A. Thomas, K. Takanabe, G. Xin, J. M. Carlsson, K. Domen, M. Antonietti, Nat. Mater., 2008, 8, 76-80.
[10] J. Zhang, X. H. Mao, W. Xiao, Y. F. Zhuang, Chin. J. Catal., 2017, 38, 2009-2020.
[11] P. Kumar, R. Boukherroub, K. Shankar, J. Mater. Chem. A, 2018, 6, 12876-12931.
[12] Z. Zhao, Y. Sun, F. Dong, Nanoscale, 2015, 7, 15-37.
[13] J. Luo, X. Zhang, J. Zhang, ACS Catal., 2015, 5, 2250-2254.
[14] M. Marszewski, S. W. Cao, J. G. Yu, M. Jaroniec, Mater. Horiz., 2015, 2, 261-278.
[15] D. Xu, B. Cheng, W. K. Wang, C. J. Jiang, J. G. Yu, Appl. Catal. B, 2018, 231, 368-380.
[16] N. Nie, L. Y. Zhang, J. W. Fu, B. Cheng, J. G. Yu, Appl. Surf. Sci., 2018, 441, 12-22.
[17] S. Chandrasekaran, C. Bowen, P. X. Zhang, Z. L. Li, Q. H. Yuan, X. Z. Ren, L. B. Deng, J. Mater. Chem. A., 2018, 6, 11078-11104.
[18] J. W. Fu, J. G. Yu, C. J. Jiang, B. Cheng, Adv. Energy. Mater., 2018, 8, 1701503.
[19] J. B. Fei, J. B. Li, Adv. Mater., 2015, 27, 314-319.
[20] C. Liu, F. Raziq, Z. J. Li, Y. Qu, A. Zada, L. Q. Jing, Chin. J. Catal., 2017, 38, 1072-1078.
[21] J. X. Low, L. Y. Zhang, T. Tong, B. J. Shen, J. G. Yu, J. Catal., 2018, 361, 255-266.
[22] S. Wang, P. Y. Kuang, B. Cheng, J. G. Yu, C. J. Jiang, J. Alloys Compd., 2018, 741, 622-632.
[23] J. J. Yu, D. P. Sun, T. H. Wang, F. Li, Chem. Eng. J., 2018, 334, 225-236.
[24] J. Cheng, Y. Shen, K. Chen, X. Wang, Y. F. Guo, X. J. Zhou, R. B. Bai, Chin. J. Catal., 2018, 39, 810-820.
[25] P. Zhang, T. Wang, J. Gong, Adv. Mater., 2015, 27, 5328-5342.
[26] R. O. Reithmeier, S. Meister, A. Siebel, B. Rieger, Dalton Trans., 2015, 44, 6466-6472.
[27] Q. Sun, P. Wang, H. G. Yu, X. F. Wang, J. Mol. Catal. A, 2016, 424, 369-376.
[28] Z. Wang, W. Guan, Y. Sun, F. Dong, Y. Zhou, W. K. Ho, Nanoscale, 2015, 7, 2471-2479.
[29] Z. L. Fang, H. F. Rong, Z. L. Ya, P. Qi, J. Mater. Sci., 2015, 50, 3057-3064.
[30] W. Mao, T. Y. Wang, H. Y. Wang, S. Zou, S. X. Liu, J. Mater. Sci-Mater. El., 2018, 29, 15174-15182.
[31] M. Ou, Q. Zhong, S. L. Zhang, L. M. Yu, J. Alloys Compd., 2015, 626, 401-409.
[32] G. Miao, D. S. Huang, X. L. Ren, X. Li, Z. Li, J. Xiao, Appl. Catal. B, 2016, 192, 72-79.
[33] S. Patnaik, G. Swain, K. M. Parida, Nanoscale, 2018, 10, 5950-5964.
[34] W. L. Shi, F. Guo, J. B. Chen, G. B. Che, X. Lin, J Alloys Compd., 2014, 612, 143-148.
[35] J. X. Low, C. J. Jiang, B. Cheng, S. Wageh, A. A. Al-Ghamdi, J. G. Yu, Small Methods, 2017, 1, 1700080/1-1700080/21.
[36] X. T. Xu, Y. Z. Liu, Y. Z. Zhu, X. B. Fan, Y. Li, F. B. Zhang, G. L. Zhang, W. C. Peng, ChemElectroChem, 2017, 4, 1498-1502.
[37] H. G. Yu, P. Xiao, P. Wang, J. G. Yu, Appl. Catal. B, 2016, 193, 217-225.
[38] Y. H. Fu, Z. J. Li, Q. Q. Liu, X. F. Yang, H. Tang, Chin. J. Catal., 2017, 38, 2160-2170.
[39] K. He, J. Xie, M. L. Li, X. Li, Appl. Surf. Sci., 2018, 430, 208-217.
[40] H. Zhu, F. Lyu, M. Du, M. Zhang, Q. Wang, J. Yao, B. Guo, ACS Appl. Mater. Interfaces, 2014, 6, 22126-22137.
[41] J. W. Fu, C. B. Bie, B. Cheng, C. J. Jiang, J. G. Yu, ACS Sustain. Chem. Eng., 2018, 6, 2767-2779.
[42] X. J. Lu, Y. Wang, X. Y. Zhang, G. Q. Xu, D. M. Wang, J. Lv, Z. X. Zheng, Y. C. Wu, J. Hazard. Mater., 2018, 341, 10-19.
[43] J. Wen, J. Xie, H. Zhang, A. Zhang, Y. Liu, X. Chen, X. Li, ACS Appl. Mater. Interfaces, 2017, 9, 14031-14042.
[44] J. Q. Wen, X. Li, H. Q. Li, S. Ma, K. He, Y. H. Xu, Y. P. Fang, W. Liu, Q. Z. Gao, Appl. Surf. Sci., 2015, 358, 204-212.
[45] K. He, J. Xie, X. Y. Luo, J. Q. Wen, S. Ma, X. Li, Y. P. Fang, X. C. Zhang, Chin. J. Catal., 2017, 38, 240-252.
[46] T. Tong, B. C. Zhu, C. J. Jiang, B. Cheng, J. G. Yu, Appl. Surf. Sci., 2018, 433, 1175-1183.
[47] X. F. Wang, D. Liao, H. G. Yu, J. G. Yu, Dalton Trans., 2018, 47, 6370-6377.
[48] F. Chen, H. Yang, W. Luo, P. Wang, H. G. Yu, Chin. J. Catal., 2017, 38, 1990-1998.
[49] Z. Zhu, Z. Y. Lu, D. D. Wang, X. Tang, Y. S. Yan, W. D. Shi, Y. Wang, N. L. Gao, X. Yao, H. J. Dong, Appl. Catal. B, 2016, 182, 115-122.
[50] Y. Chen, W. Huang, D. He, Y. Situ, H. Huang, ACS Appl. Mater. Interfaces, 2014, 6, 14405-14414.
[51] F. Chen, H. Yang, W. Luo, P. Wang, H. G. Yu, Chin. J. Catal., 2017, 38, 1990-1998.
[52] X. L. Luo, G. L. He, Y. P. Fang, Y. H. Xu, J. Colloid Interface Sci., 2018, 518, 184-191.
[53] H. G. Yu, W. Y. Chen, X. F. Wang, Y. Xu, J. G. Yu, Appl. Catal. B, 2016, 187, 163-170.
[54] W. Zhao, Y. Guo, S. M. Wang, H. He, C. Sun, S. G. Yang, Appl. Catal. B, 2015, 165, 335-343.
[55] F. F. Liang, Y. F. Zhu, Appl. Catal. B, 2016, 180, 324-329.
[56] R. C. Shen, J. Xie, H. D. Zhang, A. P. Zhang, X. B. Chen, X. Li, ACS Sustain. Chem. Eng., 2017, 6, 816-826.
[57] X. Du, G. Zou, Z. Wang, X. Wang, Nanoscale, 2015, 7, 8701-8706.
[58] Y. N. Ma, J. Li, E. Z. Liu, J. Wan, X. Y. Hu, J. Fan, Appl. Catal. B, 2017, 219, 467-478.
[59] J. Chen, S. H. Shen, P. H. Guo, M. Wang, P. Wu, X. X. Wang, L. J. Guo, Appl. Catal. B, 2014, 152-153, 335-341.
[60] Z. H. Chen, P. Sun, B. Fan, Z. Zhang, X. M. Fang, J. Phys. Chem. C, 2014, 118, 7801-7807.
[61] J. Wang, H. Xu, S. M. Li, B. Yan, Y. T. Shi, C. Q. Wang, Y. K. Du, Ana-lyst, 2017, 142, 4852-4861.
[62] J. X. Low, J. G. Yu, M. Jaroniec, S. Wageh, A. A. Al-Ghamdi, Adv. Mater., 2017, 29, 1601694.
[63] Z. Mo, X. J. She, Y. P. Li, L. Liu, L. Y. Huang, Z. G. Chen, Q. Zhang, H. Xu, H. M. Li, RSC Adv., 2015, 5, 101552-101562.
[64] S. Patnaik, D. P. Sahoo, K. Parida, Renew. Sust. Energy Rev., 2018, 82, 1297-1312.
[65] Y. F. Ma, L. L. Yang, Y. Yang, Y. S. Peng, Y. Q. Wei, Z. R. Huang, RSC Adv., 2018, 8, 22095-22102.
[66] D. Z. Lu, H. M. Wang, X. N. Zhao, K. K. Kondamareddy, J. Q. Ding, C. H. Li, P. F. Fang, ACS Sustainable Chem. Eng., 2017, 5, 1436-1445.
[67] J. Qin, J. Huo, P. Zhang, J. Zeng, T. Wang, H. Zeng, Nanoscale, 2016, 8, 2249-2259.
[68] J. Q. Wen, J. Xie, Z. H. Yang, R. C. Shen, H. Y. Li, X. Y. Luo, X. B. Chen, X. Li, ACS Sustain. Chem. Eng., 2017, 5, 2224-2236.
[69] T. Xiong, W. G. Cen, Y. X. Zhang, F. Dong, ACS Catal., 2016, 6, 2462-2472.
[70] H. G. Yu, G. Q. Cao, F. Chen, X. F. Wang, J. G. Yu, M. Lei, Appl. Catal. B, 2014, 160-161, 658-665.
[71] J. Fei, J. Li, Adv. Mater., 2015, 27, 314-319.
[72] S. Patnaik, D. P. Sahoo, K. Parida, Renew. Sust. Energ. Rev., 2018, 82, 1297-1312.
[73] W. Zhang, Y. Wang, Z. Wang, Z. Zhong, R. Xu, Chem. Commun., 2010, 46, 7631-7633.
[74] Y. Zhong, J. Yuan, J. Wen, X. Li, Y. Xu, W. Liu, S. Zhang, Y. Fang, Dal-ton Trans., 2015, 44, 18260-18269.

双助剂促进g-C₃N₄光解水制氢性能

Enhanced photocatalytic H₂ production over dual-cocatalyst-modified g-C₃N₄ heterojunctions

PDF

Supporting Information

可视化

摘要/Abstract

引用本文

使用本文

扫码分享

参考文献

相关文章 15

编辑推荐

Metrics

[1]	赵彬彬, 钟威, 陈峰, 王苹, 别传彪, 余火根. 高晶化g-C₃N₄光催化剂: 合成、结构调控和光催化产氢[J]. 催化学报, 2023, 52(9): 127-143.
[2]	唐小龙, 李锋, 李方, 江燕斌, 余长林. 单原子催化剂在光催化和电催化合成过氧化氢中的研究进展[J]. 催化学报, 2023, 52(9): 79-98.
[3]	蔡铭洁, 刘艳萍, 董珂欣, 陈晓波, 李世杰. 漂浮型Bi₂WO₆/C₃N₄/碳布S型异质结光催化材料用于高效净化水体环境[J]. 催化学报, 2023, 52(9): 239-251.
[4]	王思恺, 闵祥婷, 乔波涛, 颜宁, 张涛. 单原子催化: 追寻催化领域的“圣杯”[J]. 催化学报, 2023, 52(9): 1-13.
[5]	江梓聪, 程蓓, 张留洋, 张振翼, 别传彪. 氧化锌基梯型异质结光催化剂[J]. 催化学报, 2023, 52(9): 32-49.
[6]	刘博文, 蔡家杰, 张建军, 谭海燕, 程蓓, 许景三. MOF/CdS梯型光催化剂同时进行苯甲醇氧化和析氢反应及其机理研究[J]. 催化学报, 2023, 51(8): 204-215.
[7]	宋明明, 宋相海, 刘鑫, 周伟强, 霍鹏伟. ZnIn₂S₄/MOF-808微球结构S型异质结光催化剂的制备及其光还原CO₂性能研究[J]. 催化学报, 2023, 51(8): 180-192.
[8]	邵秀丽, 李可, 李静萍, 程强, 王国宏, 王楷. 揭示NiS@Ta₂O₅纳米纤维中梯型电荷转移路径及光催化CO₂转化性能[J]. 催化学报, 2023, 51(8): 193-203.
[9]	李嘉明, 李源, 王小田, 杨直雄, 张高科. TiO₂上原子分散的Fe位点促进光催化CO₂还原: 增强的催化活性、 DFT计算和机制洞察[J]. 催化学报, 2023, 51(8): 145-156.
[10]	阎菲, 张由子, 刘思碧, 邹睿卿, Jahan B Ghasemi, 李炫华. 供体-受体型卟啉基金属有机框架实现有效电荷分离高效光催化析氢[J]. 催化学报, 2023, 51(8): 124-134.
[11]	孙利娟, 王伟康, 路平, 刘芹芹, 王乐乐, 唐华. 纳米高熵合金实现光催化剂肖特基势垒的调控用于光催化制氢与苯甲醇氧化耦合反应[J]. 催化学报, 2023, 51(8): 90-100.
[12]	刘海峰, 黄祥, 陈加藏. 电子态调控促进氢气无损耗纯化中CO的光致富集和氧化[J]. 催化学报, 2023, 51(8): 49-54.
[13]	袁鑫, 范海滨, 刘杰, 覃龙州, 王剑, 段秀, 邱江凯, 郭凯. 连续流技术在光氧化还原催化转化的最新进展[J]. 催化学报, 2023, 50(7): 175-194.
[14]	刘德法, 孙彬, 白硕杰, 高婷婷, 周国伟. 双助催化剂Ag/Ti₃C₂/TiO₂分层花状微球用于增强光催化产氢活性[J]. 催化学报, 2023, 50(7): 273-283.
[15]	肖汉至, 于博, 颜思顺, 章炜, 李茜茜, 鲍莹, 罗书平, 叶剑衡, 余达刚. 可见光催化二氧化碳参与非活化烯烃1,3-双羧基化反应[J]. 催化学报, 2023, 50(7): 222-228.