Precise and controllable tandem strategy triggering boosted oxygen reduction activity

doi:10.1016/S1872-2067(21)63966-9

Abstract

Abstract:

The development of efficient and cost-effective metal-free electrocatalysts for oxygen reduction reaction (ORR) has become crucial for electrochemical energy systems. However, reasonably validating and precisely regulating the active sites for designing optimized materials are still challenging. Herein, we report a precise and controllable tandem strategy to boost the ORR activity based on metal-free covalent organic frameworks (MFCOFs) comprising imine-N, thiophene-S, or triazine-N. Among these MFCOFs, post-tandem BTT-TAT-COF structure displayed a more positive catalytic capability and excellent electrochemical stability, indicating that the synergistic catalysis of multiple active sites induced the ORR catalytic activity through the conjugated skeleton of the structure. Density-functional theory calculations suggest that the series-connected backbone contained highly effective electrocatalytic active centers and provided synergistic catalysis. More importantly, this strategy highlights new opportunities for the advancement of efficient COF-based metal-free ORR catalysts.

Key words: Covalent organic frameworks, Metal-free electrocatalyst, Tandem strategy, Synergistic catalysis, Oxygen reduction reaction

Guoxing Jiang, Longhai Zhang, Wenwu Zou, Weifeng Zhang, Xiujun Wang, Huiyu Song, Zhiming Cui, Li Du*. Precise and controllable tandem strategy triggering boosted oxygen reduction activity[J]. Chinese Journal of Catalysis, 2022, 43(4): 1042-1048.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63966-9

https://www.cjcatal.com/EN/Y2022/V43/I4/1042

Figures/Tables 5

Scheme 1. Schematic of the (a) tandem synthetic procedure of the MFCOFs and (b) ORR process induced by BTT-TAT-COF.

Fig. 1. Probable chemical structures (left) and reconstructed structures of one hexagonal macrocycle (right) for TFPB-TAPB-COF (a), BTT-TAPB-COF (b), and BTT-TAT-COF (c) (gray, blue, and red spheres represent C, N, and S atoms, respectively); PXRD patterns of TFPB-TAPB-COF (d), BTT-TAPB-COF (e), and BTT-TAT-COF (f).

Fig. 2. (a) N2 adsorption-desorption isotherms of TFPB-TAPB-COF (pink), BTT-TAPB-COF (blue), and BTT-TAT-COF (red); (b) PXRD spectra of BTT-TAT-COF after treatment under different conditions; SEM images of TFPB-TAPB-COF (c), BTT-TAPB-COF (d), and BTT-TAT-COF (e); (f) TEM image and EDS maps for C, N, and S of BTT-TAT-COF.

Fig. 3. Electrochemical ORR performance. Comparison of LSV curves in O2-saturated 0.1 mol/L aqueous KOH at 1600 r min-1(a), Tafel plots (b), electron transfer number (n) and H2O2 yield (c), and mass activities and TOFs (d) for TFPB-TAPB-COF, BTT-TAPB-COF, and BTT-TAT-COF; Long-term stability test (e) and methanol tolerance (f) of BTT-TAT-COF; (g) Galvanostatic discharge curve when BTT-TAT-COF was used as electrodes in 6 mol/L KOH at a current density of 5 mA cm-2(without iR correction) and images of a “SCUT” LED panel powered by three series-connected ZABs.

Fig. 4. Optimized structures of TFPB-TAPB-COF (a), BTT-TAPB-COF (b), and BTT-TAT-COF (c). Gray, blue, red, and white balls represent C, N, S, and H atoms, respectively. Calculated density of states (d) and Kohn-Sham LUMOs, HOMOs, and LUMO-HOMO gaps based on the DFT methods with B3LYP/6-31G* (e) for TFPB-TAPB-COF, BTT-TAPB-COF, and BTT-TAT-COF; (f) Calculated free energy diagrams for TFPB-TAPB-COF (at site 1), BTT-TAPB-COF (at site 4), and BTT-TAT-COF (at site 5).

References

[1]	J. W. Chen, Z. Q. Ou, H. X. Chen, S. Q. Song, K. Wang, Y. Wang, Chin. J. Catal., 2021, 42, 1297-1326.
[2]	L. J. Li, A. Manthiram, Adv. Energy Mater., 2016, 6, 1502054.
[3]	J. F. Kong, W. L. Cheng, Chin. J. Catal., 2017, 38, 951-969.
[4]	I. Katsounaros, S. Cherevko, A. R. Zeradjanin, K. J. J. Mayrhofer, Angew. Chem. Int. Ed., 2014, 53, 102-121.
[5]	M. K. Debe, Nature, 2012, 486, 43-51.
[6]	A. C. Chen, P. Holt-Hindle, Chem. Rev., 2010, 110, 3767-3804.
[7]	Z. Y. Yan, B. Li, D.J. Yang, J. X. Ma, Chin. J. Catal., 2013, 34, 1471-1481.
[8]	S. Y. Ding, W. Wang, Chem. Soc. Rev., 2013, 42, 548-568.
[9]	X. Y. Chen, K. Y. Geng, R. Y. Liu, K. T. Tan, Y. F. Gong, Z. P. Li, S. S. Tao, Q. H. Jiang, D. L. Jiang, Angew. Chem. Int. Ed., 2020, 59, 5050-5091.
[10]	A. P. Cote, A. I. Benin, N. W. Ockwig, M. O'Keeffe, A. J. Matzger, O. M. Yaghi, Science, 2005, 310, 1166-1170.
[11]	T. Q. Ma, E. A. Kapustin, S. X. Yin, L. Liang, Z. Y. Zhou, J. Niu, L. H. Li, Y. Y. Wang, J. Su, J. Li, W. D. Wang, W. Wang, J.L Sun, O. M. Yaghi, Science, 2018, 361, 48-52.
[12]	J. Li, X. C. Jing, Q. Q. Li, S. W. Li, X. Gao, X. Feng, B. Wang, Chem. Soc. Rev., 2020, 49, 3565-3604.
[13]	C. Y. Lin, D. T. Zhang, Z. H. Zhao, Z. H Xia, Adv. Mater., 2018, 30, 1703646.
[14]	X. J. Zhao, P. Pachfule, A. Thomas, Chem. Soc. Rev., 2021, 50, 6871-6913.
[15]	M. H. Yu, R. H. Dong, X. L. Feng, J. Am. Chem. Soc., 2020, 142, 12903-12915.
[16]	P. Pachfule, V. M. Dhavale, S. Kandambeth, S. Kurungot, R. Banerjee, Chem. Eur. J., 2013, 19, 974-980.
[17]	Q. Xu, Y. P. Tang, X. B. Zhang, Y. Oshima, Q. H. Chen, D. L. Jiang, Adv. Mater., 2018, 30, 1706330.
[18]	X. Cui, S. Lei, A. C. Wang, L. K. Gao, Q. Zhang, Y. K. Yang, Z. Q. Lin, Nano Energy, 2020, 70, 104525.
[19]	P. Peng, Z. H. Zhou, J. N. Guo, Z. H. Xiang, ACS Energy Lett., 2017, 2, 1308-1314.
[20]	D. H. Guo, R. Shibuya, C. Akiba, S. Saji, T. Kondo, J. Nakamura, Science, 2016, 351, 361-365.
[21]	K. H. Wu, D. W. Wang, D. S. Su, L. R. Gentle, Chemsuschem, 2015, 8, 2772-2788.
[22]	Y. Zheng, S. Chen, H. Song, H. L. Guo, K. A. Zhang, C. Zhang, T. X. Liu, Nanoscale, 2020, 12, 14441-14447.
[23]	J. D. Yi, R. Xu, Q. Wu, T. Zhang, K. T. Zang, J. Luo, Y. L. Liang, Y. B. Huang, R. Cao, ACS Energy Lett., 2018, 3, 883-889.
[24]	E. Tavakoli, A. Kakekhani, S. Kaviani, P. Tan, M. M. Ghaleni, M. A. Zaeem, A. M. Rappe, S. Nejati, J. Am. Chem. Soc., 2019, 141, 19560-19564.
[25]	B. Q. Li, S. Y. Zhang, X. Chen, C. Y. Chen, Z. J. Xia, Q. Zhang, Adv. Funct. Mater., 2019, 29, 1901301.
[26]	Y. Pan, S. J. Liu, K. A. Sun, X. Chen, B. Wang, K. L. Wu, X. Cao, W. C. Cheong, R. A Shen, A. J. Han, Z. Chen, L. R. Zheng, J. Luo, Y. Lin, Y. Q. Liu, D. S. Wang, Q. Peng, Q. Zhang, C. Chen, Y. D. Li, Angew. Chem. Int. Ed., 2018, 57, 8614-8618.
[27]	P. Peng, L. Shi, F. Huo, C. X. Mi, X. H. Wu, S. J. Zhang, Z. H. Xiang, Sci. Adv., 2019, 5, eaaw2322.
[28]	L. J. Kong, M. Zhong, W. Shuang, Y. H. Xu, X. H. Bu, Chem. Soc. Rev., 2020, 49, 2378-2407.
[29]	J. L. Liu, Y. J. Hu, J. J. Cao, Catal. Commun., 2015, 66, 91-94.
[30]	D. H. Li, C. Y. Li, L. J. Zhang, H. Li, L. K. Zhu, D. J. Yang, Q. R. Fang, S. L. Qiu, X. D. Yao, J. Am. Chem. Soc., 2020, 142, 8104-8108.
[31]	Z. H. Zhao, M. T. Li, L. P. Zhang, L. M. Dai, Z. H. Xia, Adv. Mater., 2015, 27, 6834-6840.
[32]	L. P. Zhang, Z. H. Xia, J. Phys. Chem. C, 2011, 115, 11170-11176.
[33]	M. Kaukonen, R. Kujala, E. Kauppinen, J. Phys. Chem. C, 2012, 116, 632-636.
[34]	K. P. Gong, F. Du, Z. H. Xia, M. Durstock, L. M. Dai, Science, 2009, 323, 760-764.
[35]	R Liu, D. Li, D. Q. Wu, X. L. Feng, K. Muellen, Angew. Chem. Int. Ed., 2010, 49, 2565-2569.
[36]	X. J. Long, D. H. Li, B. B. Wang, Z. J. Jiang, W. J. Xu, B. B. Wang, D. J. Yang, Y. Z. Xia, Angew. Chem. Int. Ed., 2019, 58, 11369-11373.
[37]	L. P. Zhai, N. Huang, H. Xu, Q. H. Chen, D. L. Jiang, Chem. Commun., 2017, 53, 4242-4245.
[38]	T. P. Zhou, N. Zhang, C. Z. Wu, Y. Xie, Energy Environ. Sci., 2020, 13, 1132-1153.
[39]	T. Sick, J. M. Rotter, S. Reuter, S. Kandambeth, N. N. Bach, M. Doeblinger, J. Merz, T. Clark, T. B. Marder, T. Bein, D. D. Medina, J. Am. Chem. Soc., 2019, 141, 12570-12581.
[40]	G. Kresse, J. Furthmüller, Phys. Rev. B, 1996, 54, 11169-11186.
[41]	W. J. Hehre, R. Ditchfield, J. A. Pople, J. Chem. Phys., 1972, 56, 2257-2261.
[42]	R. Ditchfield, W. J. Hehre, J. A. Pople, J. Chem. Phys., 1971, 54, 724-728.
[43]	Z. C. Ding, X. J. Long, C. D. Dou, J. Liu, L. X. Wang, Chem. Sci., 2016, 7, 6197-6202.
[44]	X. Chen, Q. A. Qiao, L. An, D. G. Xia, J. Phys. Chem. C, 2015, 119, 11493-11498.