Synthesis of Highly Luminescent Carbon Dots@Polyacrylate Sodium Composites with High Loading Fraction and Their Application in Light-Emitting Diodes †

doi:10.7503/cjcu20190481

Abstract

Abstract:

Luminescent materials have wide application prospects in many fields, and hence they have drawn increasing attention. In this work, carbon dots(g-CDs) and polyacrylate sodium(PAAS) were used as raw materials. By combining g-CDs aqueous solution with PAAS, a luminescent composites(g-CDs@PAAS) was obtained. Because the PAAS has a large number of carboxyl group and strong water imbibition thereof, while there are lots of carboxyl, hydroxyl and amino groups on g-CDs surface, leading to the combination of PAAS with g-CDs through hydrogen bonding interaction. In the as-prepared composites, g-CDs maintain monodisperse, which effectively overcomes the aggregation-induced solid-state luminescence quenching of g-CDs. This synthetic method is simple to operate and has no loss of raw materials during the preparation. The loading g-CDs fraction in g-CDs@PAAS is up to 30%, and its photoluminescence quantum yields could achieve 52%. In addition, the g-CDs@PAAS composites have good thermal stability, photostability, and organic solvent resistance. These advantages ensure that g-CDs@PAAS composites can be used as the color conversion layer in the manufacturing of white light-emitting diode.

Key words: Carbon dot, Polyacrylate sodium, Luminescent composite, Light-emitting diode

CLC Number:

TrendMD:

Zijie WU,Xin LI,Zhiwei LI,Di LI,Yuechen ZHAI,Ding ZHOU,Songnan QU. Synthesis of Highly Luminescent Carbon Dots@Polyacrylate Sodium Composites with High Loading Fraction and Their Application in Light-Emitting Diodes ^†[J]. Chem. J. Chinese Universities, 2019, 40(12): 2427.

Figures/Tables 9

Scheme 1 Schematics of g-CDs@PAAS composites preparation for WLED

Fig.1 Optical images for illustrating the preparation process of g-CDs@PAAS composites (A) Images of PAAS powders(left) and g-CDs aqueous solution(right) under sunlight; (B) after mixing the PAAS powders and g-CDs aqueous solution, the images of the mixtures under sunlight(left) and UV light(right); (C) after removing the solvent, the images of the g-CDs@PAAS composites under sunlight(C) and UV light(D).

Fig.2 Diffuse reflection absorption(a) and PL emission(b) spectra(A) and excitation-emission maps(B) of g-CDs@PAAS composites

Fig.3 Luminescence lifetime decay curves of g-CDs solution(a), g-CDs@PAAS composites(b) and IRF(c)

Sample	τ₁/ns	A₁(%)	τ₂/ns	A₂(%)	τ_ave/ns	χ²
g-CDs solution	5.03	74.8	10.81	25.2	6.48	1.2
g-CDs@PAAS	3.98	15.3	12.34	84.7	11.06	1.3

Fig.4 HRTEM image(A), SEM image(B), EDS pattern(C) and XRD pattern(D) of g-CDs@PAAS composites

Fig.5 Evaluation of the photostability(A), the thermal stability(B), resistance to chloroform(C) and UV light(D) of g-CDs@PAAS composites a. Fluorescent dye; b. g-CDs@PAAS.

Fig.6 Images(A, B) and PL emission spectrum(C) of luminescent bulk materials composed of g-CDs@PAAS composites and epoxy-silicone resin

Fig.7 Images(A—C) and CIE chromaticity diagram(D) of working WLEDs with different CIE coordinates and color temperatures m(g-CDs@PAAS):m(epoxy-sclicone): (A) 1:5; (B) 2:5; (C) 3:5. Insets in (A—C) are the corresponding optical images and emission spectra. (D) m(g-CDs@PAAS):m(epoxy-silicone): a. 1:5; b. 2:5; c. 3:5.

References 52

[1]	Grandjean N., Butté R ., Nat. Photonics, 2011,5(12), 714— 715 doi: 10.1038/nphoton.2011.298 URL
[2]	Huang X. Y ., Nat. Photonics, 2014,8(10), 748— 749 doi: 10.1038/nphoton.2014.221 URL
[3]	Liu B. Q., Wang L., Gao D. Y., Zou J. H., Ning H. L., Peng J. B., Cao Y ., Light: Sci. Appl., 2016,5(8), e16137 doi: 10.1038/lsa.2016.137 URL pmid: 30167184
[4]	Dai P. P., Li C., Zhang X. T., Xu J., Chen X., Wang X. L., Jia Y., Wang X. J., Liu Y. C ., Light: Sci. Appl., 2016,5(1), e16024 doi: 10.1038/lsa.2016.24 URL
[5]	Pust P., Weiler V., Hecht C., Tucks A., Wochnik A. S., Henss A. K., Wiechert D., Scheu C., Schmidt P. J., Schnick W ., Nat. Mater., 2014,13(9), 891— 896 doi: 10.1038/nmat4012 URL pmid: 24952748
[6]	Li X. F., Budai J. D., Liu F., Howe J. Y., Zhang J. H., Wang X. J., Gu Z. J., Sun C. J., Meltzer R. S., Pan Z. W ., Light: Sci. Appl., 2013,2(1), e50 doi: 10.1038/lsa.2013.6 URL
[7]	Dai Q. Q., Duty C. E., Hu M. Z ., Small, 2010,6(15), 1577— 1588 doi: 10.1002/smll.201000144 URL pmid: 20602425
[8]	Wang L., Xie R. J., Li Y. Q., Wang X. J., Ma C. G., Luo D., Takeda T., Tsai Y. T., Liu R. S., Hirosaki N ., Light: Sci. Appl., 2016,5(10), e16155 doi: 10.1038/lsa.2016.155 URL pmid: 30167122
[9]	Lim S. H., Ko Y. H., Rodriguez C., Gong S. H., Cho Y. H ., Light: Sci. Appl., 2016,5(2), e16030 doi: 10.1038/lsa.2016.30 URL pmid: 30167143
[10]	Jang E., Jun S., Jang H., Lim J., Kim B., Kim Y ., Adv. Mater., 2010,22(28), 3076— 3080 doi: 10.1002/adma.201000525 URL pmid: 20517873
[11]	Adam M., Gaponik N., Eychmuller A., Erdem T., Soran-Erdem Z., Demir H. V ., J. Phys. Chem. Lett., 2016,7, 4117— 4123 doi: 10.1021/acs.jpclett.6b01699 URL pmid: 27687584
[12]	Abe S., Joos J. J., Martin L. I. D. J., Hens Z., Smet P. F ., Light: Sci. Appl., 2017,6(6), e16271 doi: 10.1038/lsa.2016.271 URL pmid: 30167259
[13]	Sun Y. P., Zhou B., Lin Y., Wang W., Fernando K. A., Pathak P., Meziani M. J., Harruff B. A., Wang X., Wang H. F., Luo P. G., Yang H., Kose M. E., Chen B. L., Veca L. M., Xie S. Y ., J. Am. Chem. Soc., 2006,128(24), 7756— 7757 doi: 10.1021/ja062677d URL pmid: 16771487
[14]	Gong N. Q., Ma X. W., Ye X. X., Zhou Q. F., Chen X. A., Tan X. L., Yao S. K., Huo S. D., Zhang T. B., Chen S. Z., Teng X. C., Hu X. X., Yu J., Gan Y. L., Jiang H. D., Li J. H., Liang X. J ., Nat. Nanotechnol., 2019,14(4), 379— 387 doi: 10.1038/s41565-019-0373-6 URL pmid: 30778211
[15]	Song Y. B., Zhu S. J., Xiang S. Y., Zhao X. H., Zhang J. H., Zhang H., Fu Y., Yang B ., Nanoscale, 2014,6(9), 4676— 4682 doi: 10.1039/c4nr00029c URL
[16]	Jiang B. P., Yu Y. X., Guo X. L., Ding Z. Y., Zhou B., Liang H., Shen X. C ., Carbon, 2018,128, 12— 20 doi: 10.1016/j.carbon.2017.11.070 URL
[17]	Chen J., Wei J. S., Zhang P., Niu X. Q., Zhao W., Zhu Z. Y., Ding H., Xiong H. M ., ACS Appl. Mater. Interfaces, 2017,9(22), 18429— 18433 doi: 10.1021/acsami.7b03917 URL pmid: 28537370
[18]	Liu M. L., Chen B. B., Li C. M., Huang C. Z ., Green Chem., 2019,21(3), 449— 471 doi: 10.1039/C8GC02736F URL
[19]	Yang X. D., Yang X., Li Z. Y., Li S. Y., Han Y. X., Chen Y., Bu X. Y., Su C. Y., Xu H., Jiang Y. N., Lin Q ., J. Colloid Interface Sci., 2015,456, 1— 6 doi: 10.1016/j.jcis.2015.06.002 URL pmid: 26074383
[20]	Zhao P., Li X. P., Baryshnikov G., Wu B., Ågren H., Zhang J. J., Zhu L. L ., Chem. Sci., 2018,9(5), 1323— 1329 doi: 10.1039/c7sc04607c URL pmid: 29675179
[21]	Zhang Y. J., Yuan R. R., He M. L., Hu G. C., Jiang J. T., Xu T., Zhou L., Chen W., Xiang W. D., Liang X. J ., Nanoscale, 2017,9(45), 17849— 17858 doi: 10.1039/c7nr05363k URL pmid: 29116274
[22]	Liu J. C., Wang N., Yu Y., Yan Y., Zhang H. Y., Li J. Y., Yu J. H ., Sci. Adv., 2017,3(5), e1603171 doi: 10.1126/sciadv.1603171 URL pmid: 28560347
[23]	Zhu A. W., Qu Q., Shao X. L., Kong B., Tian Y ., Angew. Chem., Int. Ed., 2012,51(29), 7185— 7189 doi: 10.1002/anie.201109089 URL pmid: 22407813
[24]	Liu C., Bao L., Tang B., Zhao J. Y., Zhang Z. L., Xiong L. H., Hu J., Wu L. L., Pang D. W ., Small, 2016,12(34), 4702— 4706 doi: 10.1002/smll.201503958 URL pmid: 26972488
[25]	Wang Y. F., Hu A. G ., J. Mater. Chem. C, 2014,2(34), 6921— 6939 doi: 10.1039/C4TC00988F URL
[26]	Jiang K., Sun S., Zhang L., Lu Y., Wu A. G., Cai C. Z., Lin H. W ., Angew. Chem., Int. Ed., 2015,54(18), 5360— 5363 doi: 10.1002/anie.201501193 URL pmid: 25832292
[27]	Ge J. C., Jia Q. Y., Liu W. M., Guo L., Liu Q. Y., Lan M. H., Zhang H. Y., Meng X. M., Wang P. F ., Adv. Mater., 2015,27(28), 4169— 4177 doi: 10.1002/adma.201500323 URL pmid: 26045099
[28]	Ding H., Yu S. B., Wei J. S., Xiong H. M ., ACS Nano, 2016,10(1), 484— 491 doi: 10.1021/acsnano.5b05406 URL pmid: 26646584
[29]	Guo X., Wang C. F., Yu Z. Y., Chen L., Chen S ., Chem. Commun., 2012,48(21), 2692— 2694 doi: 10.1039/c2cc17769b URL pmid: 22306963
[30]	Liu R. L., Wu D. Q., Liu S. H., Koynov K., Knoll W., Li Q ., Angew. Chem., Int. Ed., 2009,48(25), 4598— 4601 doi: 10.1002/anie.200900652 URL pmid: 19388019
[31]	Liu J., Xiong R. H., Brans T., Lippens S., Parthoens E., Zanacchi F. C., Magrassi R., Singh S. K., Kurungot S., Szunerits S., Bove H., Ameloot M., Fraire J. C., Teirlinck E., Samal S. K., Rycke R., Houthaeve G., De Smedt S. C., Boukherroub R., Braeckmans K ., Light: Sci. Appl., 2018,7, 47 doi: 10.1038/s41377-018-0048-3 URL pmid: 30839577
[32]	Zheng D. W., Li B., Li C. X., Fan J. X., Lei Q., Li C., Xu Z. S., Zhang X. Z ., ACS Nano, 2016,10(9), 8715— 8722 doi: 10.1021/acsnano.6b04156 URL pmid: 27532320
[33]	Xu X. W., Zhang K., Zhao L., Li C., Bu W. H., Shen Y. Q., Gu Z. Y., Chang B., Zheng C. Y., Lin C. T., Sun H. C., Yang B ., ACS Appl. Mater. Interfaces, 2016,8(48), 32706— 32716 doi: 10.1021/acsami.6b12252 URL pmid: 27934165
[34]	Qu D., Zheng M., Li J., Xie Z. G., Sun Z. C ., Light: Sci. Appl., 2015,4(12), e364 doi: 10.1038/lsa.2015.137 URL
[35]	Fernando K. A., Sahu S., Liu Y., Lewis W. K., Guliants E. A., Jafariyan A., Wang P., Bunker C. E., Sun Y. P ., ACS Appl. Mater. Interfaces, 2015,7(16), 8363— 8376 doi: 10.1021/acsami.5b00448 URL pmid: 25845394
[36]	Xiao L., Sun H. D ., Nanoscale Horiz., 2018,3(6), 565— 597 doi: 10.1039/C8NH00106E URL
[37]	Li X. M., Rui M. C., Song J. Z., Shen Z. H., Zeng H. B ., Adv. Funct. Mater., 2015,25(31), 4929— 4947 doi: 10.1002/adfm.v25.31 URL
[38]	Zhou D., Jing P. T., Wang Y., Zhai Y. C., Li D., Xiong Y., Baranov A. V., Qu S. N., Rogach A. L ., Nanoscale Horiz., 2019,4(2), 388— 395 doi: 10.1039/C8NH00247A URL
[39]	Wang Y., Kalytchuk S., Wang L. Y., Zhovtiuk O., Cepe K., Zboril R., Rogach A. L ., Chem. Commun., 2015,51(14), 2950— 2953 doi: 10.1039/c4cc09589h URL pmid: 25594080
[40]	Kwon W., Do S., Lee J., Hwang S., Kim J. K., Rhee S. W ., Chem. Mater., 2013,25(9), 1893— 1899 doi: 10.1021/cm400517g URL
[41]	Chen Y. H., Zheng M. T., Xiao Y., Dong H. W., Zhang H. R., Zhuang J. L., Hu H., Lei B. F., Liu Y. L ., Adv. Mater., 2016,28(2), 312— 318 doi: 10.1002/adma.201503380 URL pmid: 26568431
[42]	Sun C., Zhang Y., Kalytchuk S., Wang Y., Zhang X. Y., Gao W. Z., Zhao J., Cepe K., Zboril R., Yu W. W., Rogach A. L ., J. Mater. Chem. C, 2015,3(26), 6613— 6615 doi: 10.1039/C5TC01379H URL
[43]	Zhou D., Zhai Y. C., Qu S. N., Li D., Jing P. T., Ji W. Y., Shen D. Z., Rogach A. L ., Small, 2017,13(6), 1602055 doi: 10.1002/smll.v13.6 URL
[44]	Zhai Y. C., Zhou D., Jing P. T., Li D., Zeng H. B., Qu S. N ., J. Colloid Interface Sci., 2017,497, 165— 171 doi: 10.1016/j.jcis.2017.03.007 URL pmid: 28284070
[45]	Sun M. Y., Qu S. N., Hao Z. D., Ji W. Y., Jing P. T., Zhang H., Zhang L. G., Zhao J. L., Shen D. Z ., Nanoscale, 2014,6(21), 13076— 13081 doi: 10.1039/c4nr04034a URL
[46]	Zhai Y. C., Shen F. Z., Zhang X. T., Jing P. T., Li D., Yang X. D., Zhou D., Xu X. W., Qu S. N ., J. Colloid Interface Sci., 2019,554, 344— 352 doi: 10.1016/j.jcis.2019.07.022 URL pmid: 31306946
[47]	Liu M. Z., Guo T. H ., J. Appl. Polym. Sci., 2001,82(6), 1515— 1520 doi: 10.1002/(ISSN)1097-4628 URL
[48]	Hua F. J., Qian M. P ., J. Mater. Sci., 2001,36(3), 731— 738 doi: 10.1023/A:1004849210718 URL
[49]	Ogawa I., Yamano H., Miyagawa K ., J. Appl. Polym. Sci., 1993,47(2), 217— 222 doi: 10.1002/app.1993.070470204 URL
[50]	Zhou D., Li D., Jing P. T., Zhai Y. C., Shen D. Z., Qu S. N., Rogach A. L ., Chem. Mater., 2017,29(4), 1779— 1787 doi: 10.1021/acs.chemmater.6b05375 URL
[51]	Qu S. N., Shen D. Z., Liu X. Y., Jing P. T., Zhang L. G., Ji W. Y., Zhao H. F., Fan X. W., Zhang H ., Part. Part. Syst. Charact., 2014,31(11), 1175— 1182 doi: 10.1002/ppsc.201400055 URL
[52]	Zou H. Y., Liu M., Zhou D., Zhang X., Liu Y., Yang B., Zhang H ., J. Phys. Chem. C, 2017,121(9), 5313— 5323 doi: 10.1021/acs.jpcc.6b12129 URL