高效可见光响应Zn0.11Sn0.12Cd0.84S1.12/g-C3N4异质结光催化剂的制备及性能

doi:10.7503/cjcu20150721

摘要/Abstract

摘要：

以双氰胺、醋酸锌、四氯化锡、醋酸镉和硫化钠为原料, 采用水热法制备了三元金属复合硫化物Zn_0.11Sn_0.12Cd_0.84S_1.12(ZnSnCdS)及一系列异质结催化剂ZnSnCdS/g-C₃N₄. 采用X射线衍射仪(XRD)、扫描电子显微镜(SEM)、紫外-可见光谱仪(UV-Vis)、傅里叶变换红外光谱仪(FTIR)、电感耦合等离子体-质谱仪(ICP-MS)、荧光光谱仪(PL)和X射线光电子能谱仪(XPS)等对催化剂进行了表征. 结果表明, ZnSnCdS与g-C₃N₄之间以C—S键紧密结合, 构筑了异质结, 促进了界面电荷迁移, 抑制了光生电子-空穴对的复合. 可见光下降解染料罗丹明B(RhB)的结果表明, ZnSnCdS/g-C₃N₄异质结催化剂的光催化性能与单纯g-C₃N₄, ZnSnCdS及双组分硫化物/g-C₃N₄异质结催化剂相比均有大幅度提高, ZnSnCdS与g-C₃N₄质量比为4∶1时异质结催化剂表现出最大的速率常数(0.1508 min^-1), 是单纯g-C₃N₄和ZnSnCdS的32.3倍和4.9倍. 其它三元金属复合硫化物如ZnMoCdS, MoNiCdS和NiSnCdS与g-C₃N₄之间也能有效形成异质结, 促进电子-空穴对的分离和催化性能的提升.

关键词: 石墨型氮化碳, 三元金属硫化物, 异质结催化剂, 光催化, 可见光

Abstract:

Visible light responsive ZnSnCdS/g-C₃N₄ heterojunction photocatalysts were synthesized via a simple hydrothermal treatment. X-ray diffraction(XRD), scanning electron microscopy(SEM), UV-Vis spectroscopy, Fourier transform infrared spectroscopy(FTIR), inductively coupled plasma-mass spectrometry(ICP-MS), photoluminescence(PL) spectroscopy, and X-ray photoelectron spectroscopy(XPS) were used to characterize the prepared catalysts. The results indicated that the heterojunctions were formed by the formation of C—S bond across the g-C₃N₄/ZnSnCdS interface, which facilitates interfacial charge transfer and improves the separation efficiency of electron-hole pairs. The activities of catalysts were tested in photocatalytic rhodamine B(RhB) degradation under visible light. The results indicated that the ZnSnCdS/g-C₃N₄ heterojunction photocatalysts show obvious higher photocatalytic activity than the single g-C₃N₄ or ZnSnCdS. With the optimal g-C₃N₄ mass fraction of 20%, the as-prepared heterojunction photocatalyst displays the highest RhB degradation rate, which is 32.3 and 4.9 times that of single g-C₃N₄ and ZnSnCdS, respectively. Not only ZnSnCdS but other ternary metal sulfides, ZnMoCdS, MoNiCdS and NiSnCdS, can combine with g-C₃N₄ to form the heterojunction catalyst to promote the separation rate of electrons-holes.

Key words: g-C3N4, Ternary metal sulfide, Heterojunction catalyst, Photocatalysis, Visible light

中图分类号:

O644

TrendMD:

张倩, 胡绍争, 李法云, 范志平, 王琼, 王菲, 李薇, 刘道胜. 高效可见光响应Zn_0.11Sn_0.12Cd_0.84S_1.12/g-C₃N₄异质结光催化剂的制备及性能. 高等学校化学学报, 2016, 37(3): 521.

ZHANG Qian, HU Shaozheng, LI Fayun, FAN Zhiping, WANG Qiong, WANG Fei, LI Wei, LIU Daosheng. Preparation of Zn_0.11Sn_0.12Cd_0.84S_1.12/g-C₃N₄ Heterojunctions and Their Photocatalytic Performance Under Visible Light^†. Chem. J. Chinese Universities, 2016, 37(3): 521.

图/表 10

Fig.1 XRD patterns of CN, ZnSnCdS and ZnSnCdS-CN(x)a. CN; b. ZnSnCdS; c. ZnSnCdS-CN(10%); d. ZnSnCdS-CN(20%); e. ZnSnCdS-CN(50%).

Fig.2 SEM images of synthesized CN(A), ZnSnCdS(B, C) and ZnSnCdS-CN(20%)(D)

Fig.3 FTIR spectra of CN(a), ZnSnCdS(b) and ZnSnCdS-CN(20%)(c)

Fig.4 UV-Vis spectra of CN, ZnSnCdS and ZnSnCdS-CN(x)a. CN; b. ZnSnCdS-CN(80%); c. ZnSnCdS-CN(50%);

Fig.5 Schematic illustration of electron-hole separation and transport at the g-C3N4/ZnSnCdS heterojunction interface

Fig.6 XPS spectra of as-prepared catalysts in the region of C1s(A), N1s(B), Zn2p(C), Sn2p(D), Cd2p(E) and S2p(F)(A), (B) a. CN; b. ZnSnCdS-CN(20%). (C)—(F) a. ZnSnCdS; b. ZnSnCdS(20%)-CN.

Fig.7 Photoluminescence(PL) emission spectra of as-prepared catalystsa. CN; b. ZnSnCdS; c. ZnSnCdS-CN(80%); d. ZnSnCdS- CN(50%); e. ZnSnCdS-CN(10%); f. ZnSnCdS-CN(20%).

Fig.8 Photocatalytic RhB degradation performances of as-prepared catalysts under visible light irradation

Fig.9 Photocatalytic stability of ZnSnCdS-CN(20%) for RhB degradation under visible light

Fig.10 Photocatalytic RhB degradation performance over other three ternary metal sulfide/g-C3N4 catalystsa. NiSnCdS; b. g-C3N4; c. MoNiCdS; d. ZnMoCdS; e. NiSnCdS-CN(20%); f. MoNiCdS-CN(20%); g. ZnMoCdS-CN(20%).

参考文献 42

[1]	Kondo K., Murakami N., Ye C., Tsubota T., Ohno T., Appl. Catal. B: Environ., 2013, 142/143(1), 362—367
[2]	HARI Bala, Guo J. Y., Aruna., Yuan G. Y., Zhang Z. Y., Liu Z. R., Chem. J. Chinese Univeisities, 2012, 33(12), 2716—2721
	(哈日巴拉, 郭金毓, 阿茹娜 ,原光瑜 , 张占营 , 刘宗瑞 . 高等学校化学学报, 2012, 33(12), 2716—2721)
[3]	Zhang G. G., Zhang M. W., Ye X. X., Qiu X. Q., Lin S., Wang X. C., Adv. Mater., 2014, 26(5), 805—809
[4]	Xu J., Wu H. T., Wang X., Xue B., Li Y. X., Cao Y., Phys. Chem. Chem. Phys., 2013, 15(13), 4510—4517
[5]	Ge L., Mater Lett., 2011, 65(17/18), 2652—2654
[6]	Niu P., Zhang L., Liu G., Cheng H., Adv. Funct. Mater., 2012, 22(22), 4763—4770
[7]	Zhang Q., Wang H. Y., Hu S. Z., Lu G., Bai J., Liu D., Gui J. G., RSC Adv., 2015, 5(1), 42736—42743
[8]	Hu J. S., Ren L. L., Guo Y. G., Liang H. P., Cao A. M., Wan L. J., Bai C. L., Angew. Chem. Int. Ed., 2012, 44(8), 1269—1273
[9]	Yan H. J., Yang J. H., Ma G. J., Wu G. P., Zong X., Lei Z. B., Shi J. Y., Li C., J. Catal., 2009, 266(2), 165—168
[10]	Huo Y. N., Yang X. L., Zhu J., Li H. X., Appl. Catal. B: Environ., 2011, 106(1/2), 69—75
[11]	Mei Z., Ouyang S., Tang D. M., Kako T., Golberg D., Ye J., Dalton Trans., 2013, 42(8), 2687—2690
[12]	Fan Y. H., Luo Q., Liu G. X., Wang J. X., Dong X. T., Yu W. S., Sun D., Chin. J. Inorg. Chem., 2014, 30(3), 627—632
	(范英华, 雒琴, 刘桂霞, 王进贤, 董相廷, 于文生, 孙德. 无机化学学报, 2014, 30(3), 627—632)
[13]	Lu Y. H., Wu P. X., Huang J. Y., Chen L. X., Zhu N. W., Dang Z., Chem. J. Chinese Universities, 2015, 36(8), 1563—1569
	(卢勇宏, 吴平宵, 黄俊毅, 陈理想, 朱能武, 党志. 高等学校化学学报, 2015, 36(8), 1563—1569)
[14]	Xia S., Lei W., Yang Y. L., Nanoscale Res. Lett., 2011, 6(40), 562—567
[15]	Yong X., Schoonen M. A. A., Am. Mineral., 2000, 85(3/4), 543—556
[16]	Ge L., Han C. C., Xiao X. L., Guo L. L., Int. J. Hydrogen Energy, 2013, 38(17), 6960—6969
[17]	Sun M., Yan T., Yan Q, Liu H. Y., Yan L. G., Zhang Y. F., Du B., RSC Adv., 2014, 4(38), 19980—19986
[18]	Hu S. Z., Li F. Y., Fan Z. P., Wang F., Zhao Y. F., Lv Z. B., Dalton Trans., 2015, 44(1), 1084—1092
[19]	Li D., Wu Z. D., Xing C. S., Jiang D. L., Chen M., Shi W. D., Yuan S. Q., J. Mol. Catal. A: Chem., 2014, 395(1), 261—268
[20]	Chen W., Chen Z. L., Liu T. Y., Jia Z. M., Liu X. H., J. Environ. Chem. Eng., 2014, 2(3), 1889—1897
[21]	Wang D. S., Duan Y. D., Luo Q. Z., Li X. Y., Bao L. L., Desalination,2011, 270(1—3), 174—180
[22]	Lu M. L., Pei Z. X., Weng S. X., Feng W. H., Fang Z. B., Zheng Z. Y., Huang M. L., Liu P., Phys. Chem. Chem. Phys., 2014, 16(39), 21280—21288
[23]	Sun M., Yan Q., Yan T., Li M. M., Wei D., Wang Z. P., Wei Q., Du B., RSC Adv., 2014, 4(1), 31019—31027
[24]	Liu L. Y., Yang L., Pu Y. T., Xiao D. Q., Zhu J. G., Mater. Lett., 2012, 66(1), 121—124
[25]	Ge L., Han C. C., Liu J., Appl. Catal. B: Environ., 2011, 108109(1), 100—107
[26]	Joyce S. R., Thirumala R. G., Pushpa M. V., Babu B., Rama K. C., Ravikumar R. V. S. S. N.,J. Alloys Comp., 2015, 628(1), 39—45
[27]	Kiruthigaa G., Manoharan C., Raju C., Dhanapandian S., Thanikachalam V., Mater. Sci. Semicon. Proc., 2014, 26(1), 533—539
[28]	GÄrd R., Sun Z. X., Forsling W., J. Alloys Comp., 1995, 169(2), 393—399
[29]	Ma D. K., Zhou H. Y., Zhang J. H., Qian Y. T., J. Mater. Chem. Phys., 2008, 111(2/3), 391—395
[30]	Liu H., Su Y., Chen P., Wang Y., J. Mol. Catal. A: Chem., 2013, 378(1), 285—292
[31]	Liu H., Jin Z. T., Xu Z. Z., Dalton Trans., 2015, 44(1), 14368—14375
[32]	Dong F., Zhao Z. W., Xiong T., Ni Z. L., Zhang W. D., Sun Y. J., Ho W. K., ACS Appl. Mater. Interf., 2013, 5(21), 11392—11401
[33]	Cao J., Luo B. D., Lin H. L., Xu B. Y., Chen S. F., J. Hazard. Mater., 2012, 217218(1), 107—115
[34]	Wang Y., Wang X. C., Antonietti M., Angew. Chem. Int. Ed., 2012, 51(1), 68—89
[35]	Ge L., Han C., Appl. Catal. B: Environ., 2012, 117118(1), 268—274
[36]	Zhu Y. P., Li J., Ma T. Y., Liu Y. P., Du G. H., Yuan Z. Y., J. Mater. Chem. A, 2014, 2(1), 1093—1101
[37]	Zhang K., Kim W. J., Ma M., Shi X. J., Park J. H., J. Mater. Chem. A, 2015, 3(1), 4803—4810
[38]	Li Y. G., Wei X. L., Li H. J., Wang R. R., Feng J., Yun H., Zhou A. N., RSC Adv., 2015, 5(1), 14074—14080
[39]	Liu G., Niu P., Sun C. H., Smith S. C., Chen Z. G., Lu G. Q., Cheng H. M., J. Am. Chem. Soc., 2010, 132(33), 11642—11648
[40]	Jin R. R., You J. G., Zhang Q., Liu D., Hu S. Z., Gui J. Z., Acta Phys-Chim. Sin., 2014, 30(9), 1706—1712
	(金瑞瑞, 游继光, 张倩, 刘丹, 胡绍争, 桂建舟. 物理化学学报,2014, 30(9), 1706—1712)
[41]	Zhang J., Wang Y. J., Hu S. Z., Acta Phys-Chim. Sin., 2015, 31(1), 159—165
	(张健, 王彦娟, 胡绍争. 物理化学学报,2015, 31(1), 159—165)
[42]	Ji L., Wang H. R., Yu R. M., Chem. J. Chinese Universities, 2014, 35(10), 2170—2176
	(姬磊, 王浩人, 于瑞敏. 高等学校化学学报,2014, 35(10), 2170—2176)

高效可见光响应Zn_0.11Sn_0.12Cd_0.84S_1.12/g-C₃N₄异质结光催化剂的制备及性能

Preparation of Zn_0.11Sn_0.12Cd_0.84S_1.12/g-C₃N₄ Heterojunctions and Their Photocatalytic Performance Under Visible Light^†

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