Paper
Journal of Materials Chemistry A
containing functional groups in the carbon network and thus 11 Z. H. Xue, S. N. Zhang, Y. X. Lin, H. Su, G. Y. Zhai, J. T. Han,
formed –Cl and –COCl, which can tune the p orbital electrons of
carbon atoms and make them highly active sites. The catalyst
Q. Y. Yu, X. H. Li, M. Antonietti and J. S. Chen, J. Am. Chem.
Soc., 2019, 141, 14976–14980.
shows a superior NRR performance with the ammonia yielding 12 Y. T. Liu, X. Chen, J. Yu and B. Ding, Angew. Chem., Int. Ed.,
rate of 103.96 mg hÀ1 mgcat
and a faradaic efficiency of
2019, 58, 18903–18907.
À1
21.71%. Thus, this work provides a rational thought for 13 Z. Lin, Y. Yang, M. Li, H. Huang, W. Hu, L. Cheng, W. Yan,
designing a highly active metal-free catalyst for nitrogen
xation.
Z. Yu, K. Mao, G. Xia, J. Lu, P. Jiang, K. Yang, R. Zhang, P. Xu,
C. Wang, L. Hu and Q. Chen, Angew. Chem., Int. Ed., 2019, 58,
16973–16980.
14 P. Jiang, J. Chen, C. Wang, K. Yang, S. Gong, S. Liu, Z. Lin,
M. Li, G. Xia, Y. Yang, J. Su and Q. Chen, Adv. Mater.,
2018, 30, 1705324–1705333.
15 C. Ling, X. Niu, Q. Li, A. Du and J. Wang, J. Am. Chem. Soc.,
2018, 140, 14161–14168.
Conflicts of interest
The authors declare no competing nancial interest.
16 Z.-H. Sheng, H.-L. Gao, W.-J. Bao, F.-B. Wang and X.-H. Xia, J.
Mater. Chem., 2012, 22, 390–395.
Acknowledgements
17 Y. L. Liangti Qu, J.-B. Baek and L. Dai, ACS Nano, 2010, 4,
1321–1326.
18 C. Su, M. Acik, K. Takai, J. Lu, S. J. Hao, Y. Zheng, P. Wu,
Q. Bao, T. Enoki, Y. J. Chabal and K. P. Loh, Nat.
Commun., 2012, 3, 1298.
19 X. Yu, F. Yang, Y. Wu and Y. Wu, Org. Lett., 2019, 21, 1726–
1729.
20 Y. Xin, C. Wang, Y. Wang, J. Sun and Y. Gao, RSC Adv., 2017,
7, 1697–1700.
21 S. Bai, Y. Ma, R. Luo, A. Chen and D. Li, RSC Adv., 2016, 6,
2687–2694.
22 S. Banerjee, T. Hemraj-Benny, M. Balasubramanian,
D. A. Fischer, J. A. Misewich and S. S. Wong,
ChemPhysChem, 2004, 5, 1416–1422.
23 A. Ganguly, S. Sharma, P. Papakonstantinou and
J. Hamilton, J. Phys. Chem. C, 2011, 115, 17009–17019.
24 D. Ketenoglu, G. Spiekermann, M. Harder, E. Oz, C. Koz,
M. C. Yagci, E. Yilmaz, Z. Yin, C. J. Sahle, B. Detlefs and
H. Yavas, J. Synchrotron Radiat., 2018, 25, 537–542.
25 X. Liang, M. Lao, D. Pan, S. Liang, D. Huang, W. Zhou and
J. Guo, Appl. Surf. Sci., 2017, 400, 339–346.
26 P. Chen, N. Zhang, S. Wang, T. Zhou, Y. Tong, C. Ao, W. Yan,
L. Zhang, W. Chu, C. Wu and Y. Xie, Proc. Natl. Acad. Sci. U. S.
A., 2019, 116, 6635–6640.
This study was supported by the National Natural Science
Foundation (NSFC, 51772283, 21271163, 21972145), the
National Key R&D Program of China (Grant No.
2016YFA0401801), the Fundamental Research Funds for the
Central Universities (WK2060000032) and the Hong Kong
Scholars Program (XJ2019022). The calculations were
completed on the supercomputing system in the Super-
computing Center of USTC. The authors thank the so X-ray
magnetic circular dichroism end station (XMCD) of National
Synchrotron Radiation Laboratory (NSRL) for assistance with
XANES measurements.
References
1 H. M. Hiromasa Tanaka, H. Seino, M. Hidai, Y. Mizobe and
K. Yoshizawa, J. Am. Chem. Soc., 2008, 130, 9037–9047.
2 Z. Geng, Y. Liu, X. Kong, P. Li, K. Li, Z. Liu, J. Du, M. Shu,
R. Si and J. Zeng, Adv. Mater., 2018, e1803498, DOI:
10.1002/adma.201803498.
3 Y. Yang, S. Q. Wang, H. Wen, T. Ye, J. Chen, C. P. Li and
M. Du, Angew. Chem., Int. Ed., 2019, 58, 15362–15366.
4 Y. Yao, S. Zhu, H. Wang, H. Li and M. Shao, J. Am. Chem. Soc.,
2018, 140, 1496–1501.
5 J. Su, Y. Yang, G. Xia, J. Chen, P. Jiang and Q. Chen, Nat. 27 J. Li, C. W. Rochester, I. E. Jacobs, S. Friedrich, P. Stroeve,
Commun., 2017, 8, 14969.
6 Y. Chen, R. Guo, X. Peng, X. Wang, X. Liu, J. Ren, J. He,
M. Riede and A. J. Moule, ACS Appl. Mater. Interfaces, 2015,
7, 28420–28428.
L. Zhuo, J. Sun, Y. Liu, Y. Wu and J. Luo, ACS Nano, 2020, 28 S. C. Ray, Frontier Research Today, 2018, 1, 1006–1020.
14, 6938–6946.
29 A. Shaporenko, K. Heister, A. Ulman, M. Grunze and
7 L. Han, Z. Ren, P. Ou, H. Cheng, N. Rui, L. Lin, X. Liu,
M. Zharnikov, J. Phys. Chem. B, 2005, 109, 4096–4103.
L. Zhuo, J. Song, J. Sun, J. Luo and H. L. Xin, Angew. 30 H. Geng, S. Li, Y. Pan, Y. Yang, J. Zheng and H. Gu, RSC Adv.,
Chem., Int. Ed., 2021, 133, 349–354. 2015, 5, 52993–52997.
8 W. Liu, L. Han, H.-T. Wang, X. Zhao, J. A. Boscoboinik, 31 H. L. Poh, P. Simek, Z. Sofer and M. Pumera, Chemistry,
X. Liu, C.-W. Pao, J. Sun, L. Zhuo, J. Luo, J. Ren,
2013, 19, 2655–2662.
W.-F. Pong and H. L. Xin, Nano Energy, 2020, 77, 105078– 32 J. Zheng, H. T. Liu, B. Wu, C. A. Di, Y. L. Guo, T. Wu, G. Yu,
105085.
Y. Q. Liu and D. B. Zhu, Sci. Rep., 2012, 2, 662.
9 Y. Wang, A. Chen, S. Lai, X. Peng, S. Zhao, G. Hu, Y. Qiu, 33 D. Zhang, X. Han, X. Kong, F. Zhang and X. Lei, Nano-Micro
J. Ren, X. Liu and J. Luo, J. Catal., 2020, 381, 78–83. Lett., 2020, 12, 107–120.
10 M. M. Shi, D. Bao, B. R. Wulan, Y. H. Li, Y. F. Zhang, 34 L. Han, X. Liu, J. Chen, R. Lin, H. Liu, F. Lu, S. Bak, Z. Liang,
J. M. Yan and Q. Jiang, Adv. Mater., 2017, 29, 1606550–
1606555.
S. Zhao, E. Stavitski, J. Luo, R. R. Adzic and H. L. Xin, Angew.
Chem., Int. Ed., 2019, 58, 2321–2325.
This journal is © The Royal Society of Chemistry 2021
J. Mater. Chem. A, 2021, 9, 5807–5814 | 5813