N,P-co-Doped Graphdiyne as Efficient Metal-free Catalysts for Oxygen Reduction Reaction

doi:10.1007/s40242-021-1256-6

Abstract

Abstract: The carbon-based metal-free catalyst is one of the ideal alternatives to Pt as electrocatalysts for oxygen reduction reaction, which can reduce the cost of fuel cells and zinc-air batteries. Here, graphdiyne(GDY), a carbon material with uneven charge distribution, was used as substrate. By doping nitrogen and phosphorus, a N-P-GDY catalyst was prepared, which further regulated the electron structure of GDY. The sheet-like morphology of GDY was preserved in N-P-GDY. The N and P were distributed uniformly in the catalyst, whereas defects and active sites were created by doping N and P, as demonstrated by the element mapping images and Raman spectra. X-Ray photoelectron spectroscopy results indicated N and P existed in many forms in N-P-GDY. The N-P-GDY exhibited higher activity for ORR than only N or P doped GDY, due to the synergistic effect of N and P in N-P-GDY. Moreover, the activity of N-P-GDY changed little after a long time cyclic voltammetry test or injecting methanol in the electrolyte. Besides, the four electrons transfer reaction to produce water was the main process for ORR on N-P-GDY catalysts.

Key words: Graphdiyne, Oxygen reduction reaction, Metal-free catalyst

LI Meiping, WANG Kaihang, LV Qing. N,P-co-Doped Graphdiyne as Efficient Metal-free Catalysts for Oxygen Reduction Reaction[J]. Chemical Research in Chinese Universities, 2021, 37(6): 1283-1288.

References

[1] Lai L., Potts J. R., Zhan D., Wang L., Poh C. K., Tang C., Gong H., Shen Z., Lin J., Ruoff R. S., Energy Environ. Sci., 2012, 5(7), 7936
[2] Higgins D., Zamani P., Yu A., Chen Z., Energy Environ. Sci., 2016, 9(2), 357
[3] Wei W., Liang H., Parvez K., Zhuang X., Feng X., Müllen K., Angew. Chem., 2014, 126(6), 1596
[4] Chen P., Wang L.-K., Wang G., Gao M.-R., Ge J., Yuan W.-J., Shen Y.-H., Xie A.-J., Yu S.-H., Energy Environ. Sci., 2014, 7(12), 4095
[5] Wang G., Sun Y., Li D., Liang H.-W., Dong R., Feng X., Müllen K., Angew. Chem. Int. Ed., 2015, 54(50), 15191
[6] Tang J., Liu J., Li C., Li Y., Tade M. O., Dai S., Yamauchi Y., Angew. Chem. Int. Ed., 2015, 54(2), 588
[7] Li J.-C., Hou P.-X., Zhao S.-Y., Liu C., Tang D.-M., Cheng M., Zhang F., Cheng H.-M., Energy Environ. Sci., 2016, 9(10), 3079
[8] Zhao S., Wang D.-W., Amal R., Dai L., Adv. Mater., 2019, 31(9), 1801526
[9] Gong Y., Fei H., Zou X., Zhou W., Yang S., Ye G., Liu Z., Peng Z., Lou J., Vajtai R., Yakobson B. I., Tour J. M., Ajayan P. M., Chem. Mater., 2015, 27(4), 1181
[10] Chai G.-L., Qiu K., Qiao M., Titirici M.-M., Shang C., Guo Z., Energy Environ. Sci., 2017, 10(5), 1186
[11] Pei Z., Li H., Huang Y., Xue Q., Huang Y., Zhu M., Wang Z., Zhi C., Energy Environ. Sci., 2017, 10(3), 742
[12] Lu T., He J., Li R., Wang K., Yang Z., Shen X., Li Y., Xiao J., Huang C., Energy Storage Materials, 2020, 29, 131
[13] Wang F., Zuo Z., Li L., Li K., He F., Jiang Z., Li Y., Angew. Chem. Int. Ed., 2019, 58(42), 15010
[14] Yang Z., Liu R., Wang N., He J., Wang K., Li X., Shen X., Wang X., Lv Q., Zhang M., Luo J., Jiu T., Hou Z., Huang C., Carbon, 2018, 137, 442
[15] Xie C., Hu X., Guan Z., Li X., Zhao F., Song Y., Li Y., Li X., Wang N., Huang C., Angew. Chem. Int. Ed., 2020, 59(32), 13542
[16] He J., Bao K., Cui W., Yu J., Huang C., Shen X., Cui Z., Wang N., Chemistry, 2018, 24(5), 1187
[17] Li L., Zuo Z., Wang F., Gao J., Cao A., He F., Li Y., Adv. Mater., 2020, 32(14), e2000140
[18] Zuo Z., He F., Wang F., Li L., Li Y., Adv. Mater., 2020, 32(49), e2004379
[19] Lv Q., Si W., Yang Z., Wang N., Tu Z., Yi Y., Huang C., Jiang L., Zhang M., He J., Long Y., ACS Appl. Mater. Interfaces, 2017, 9(35), 29744
[20] Lv Q., Si W., He J., Sun L., Zhang C., Wang N., Yang Z., Li X., Wang X., Deng W., Long Y., Huang C., Li Y., Nat. Commun., 2018, 9(1), 3376
[21] Zhao Y., Wan J., Yao H., Zhang L., Lin K., Wang L., Yang N., Liu D., Song L., Zhu J., Gu L., Liu L., Zhao H., Li Y., Wang D., Nat. Chem., 2018, 10(9), 924
[22] Li Y., Shang H., Zuo Z., Li L., Wang F., Liu H., Li Y., Angew. Chem. Int. Ed., 2018, 57(3), 774
[23] Qiu H.-J., Du P., Hu K., Gao J., Li H., Liu P., Ina T., Ohara K., Ito Y., Chen M., Adv. Mater., 2019, 31(19), 1900843
[24] Lu X. F., Xia B. Y., Zang S.-Q., Lou X. W., Angew. Chem. Int. Ed., 2020, 59(12), 4634
[25] Wu P., Du P., Zhang H., Cai C., J. Phys. Chem. C, 2012, 116(38), 20472
[26] Lv Q., Wang N., Si W., Hou Z., Li X., Wang X., Zhao F., Yang Z., Zhang Y., Huang C., Applied Catalysis B:Environmental, 2020, 261, 118234
[27] Zion N., Cullen D. A., Zelenay P., Elbaz L., Angew. Chem. Int. Ed., 2020, 59(6), 2483
[28] Xiao M., Chen Y., Zhu J., Zhang H., Zhao X., Gao L., Wang X., Jin Z., Ge J., Jiang Z., Chen S., Liu C., Xing W., J. Am. Chem. Soc., 2019, 141(44), 17763
[29] Sanad M. F., Puente Santiago A. R., Tolba S. A., Ahsan M. A., Fernandez-Delgado O., Shawky Adly M., Hashem E. M., Mahrous Abodouh M., El-Shall M. S., Sreenivasan S. T., Allam N. K., Echegoyen L., J. Am. Chem. Soc., 2021, 143(10), 4064