Citation: Saifei Yuan, Beixi Xu, Shujuan Li, Wenbiao Zhu, Shulai Lei, Wenyue Guo, Hao Ren. Highly efficient photocatalytic reduction of nitrogen into ammonia by single Ru atom catalyst supported by BeO monolayer[J]. Chinese Chemical Letters, ;2022, 33(1): 399-403. doi: 10.1016/j.cclet.2021.06.077 shu

Highly efficient photocatalytic reduction of nitrogen into ammonia by single Ru atom catalyst supported by BeO monolayer

Saifei Yuan ^a ,
Beixi Xu ^a ,
Shujuan Li ^{b, c} ,
Wenbiao Zhu ^b ,
Shulai Lei ^{b, *,} ,
Wenyue Guo ^{a, *,} ,
Hao Ren ^a

a.
School of Materials Science and Engineering, China University of Petroleum (East China), Qingdao 266580, China
b.
Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices, Hubei University of Arts and Science, Xiangyang 441053, China
c.
Institute of Mathematics, Free University of Berlin, Arnimallee 6, D-14195 Berlin, Germany

sllei@hbuas.edu.cn

wyguo@upc.edu.cn

Received Date: 23 May 2021
Revised Date: 19 June 2021
Accepted Date: 27 June 2021
Available Online: 5 July 2021

Figures(4)

Ammonia (NH₃) is one of the most important building blocks of the chemical industry and a promising sustainable energy carrier. Conventional production of NH₃ via the Haber-Bosch process requires high temperature and high pressure, which is energy demanding and suffers safety issues. Photocatalytic nitrogen reduction reaction (NRR) is a green and sustainable route for NH₃ production, and has been expected to be an alternative for NH₃ production under mild conditions. However, solar-driven N₂ activated has appeared as the bottleneck for photocatalytic NRR. In this work, we propose that single Ru atom supported by BeO monolayer is a promising photocatalytic single atom catalyst (SAC) for efficient N₂ activation with visible illumination. The high efficiency originates from the enhanced absorption in the visible range, as well as the back-donation mechanism when N₂ were adsorbed on the SAC. Our results show that N₂ can be efficiently activated by the Ru/BeO SAC and be reduced to NH₃ with extremely low limiting potential of −0.41 V. The NRR process also exhibits dominate selectivity respect to hydrogen evolution.
- Nitrogen reduction reaction,
- Single atom catalyst,
- Monolayer,
- Ab initio,
- Optical absorption spectra
1. [1]
  G. Qing, R. Ghazfar, S.T. Jackowski, et al., Chem. Rev. 120 (2020) 5437–5516. doi: 10.1021/acs.chemrev.9b00659
2. [2]
  L. Shi, Y. Yin, S. Wang, H. Sun, et al., ACS Catal. 10 (2020) 6870–6899. doi: 10.1021/acscatal.0c01081
3. [3]
  W. Guo, K. Zhang, Z. Liang, R. Zou, Q. Xu, Chem. Soc. Rev. 48 (2019) 5658–5716. doi: 10.1039/c9cs00159j
4. [4]
  C. Tang, S.Z. Qiao, Chem. Soc. Rev. 48 (2019) 3166–3180. doi: 10.1039/c9cs00280d
5. [5]
  J. Lee, L.L. Tan, S.P. Chai, Nanoscale. 13 (2021) 7011–7033. doi: 10.1039/d1nr00783a
6. [6]
  L.W. Chen, Y.C. Hao, Y. Guo, et al., J. Am. Chem. Soc. 143 (2021) 5727–5736. doi: 10.1021/jacs.0c13342
7. [7]
  C. Ling, X. Niu, Q. Li, A. Du, J. Wang, et al., J. Am. Chem. Soc. 140 (2018) 14161–14168. doi: 10.1021/jacs.8b07472
8. [8]
  M.A. Légaré, G. Bélanger-Chabot, R.D. Dewhurst, et al., Science359 (2018) 896–900. doi: 10.1126/science.aaq1684
9. [9]
  Y. Gong, J. Wu, M. Kitano, et al., Nat. Catal. 1 (2018) 178–185. doi: 10.1038/s41929-017-0022-0
10. [10]
  R. Guan, D. Wang, Y. Zhang, et al., Appl. Catal. B: Environ. 282 (2021) 119580. doi: 10.1016/j.apcatb.2020.119580
11. [11]
  T.N. Ye, S.W. Park, Y. Lu, et al., Nature583 (2020) 391–395. doi: 10.1038/s41586-020-2464-9
12. [12]
  K.Q. Hu, P.X. Qiu, L.W. Zeng, et al., Angew. Chem. Int. Ed. 59 (2020) 20666–20671. doi: 10.1002/anie.202009630
13. [13]
  H.K. Lee, C.S.L. Koh, Y.H. Lee, et al., Sci. Adv. 4 (2018) eaar3208. doi: 10.1126/sciadv.aar3208
14. [14]
  Z. Zhao, D. Wang, R. Gao, et al., Angew. Chem. Int. Ed. 60 (2021) 11910–11918. doi: 10.1002/anie.202100726
15. [15]
  L. Hui, Y. Xue, H. Yu, et al., J. Am. Chem. Soc. 141 (2019) 10677–10683. doi: 10.1021/jacs.9b03004
16. [16]
  C. Liu, Q. Li, C. Wu, et al., J. Am. Chem. Soc. 141 (2019) 2884–2888. doi: 10.1021/jacs.8b13165
17. [17]
  S. Tang, Q. Dang, T. Liu, et al., J. Am. Chem. Soc. 142 (2020) 19308–19315. doi: 10.1021/jacs.0c09527
18. [18]
  S. Yuan, H. Ren, G. Meng, et al., Appl. Surf. Sci. 555 (2021) 149682. doi: 10.1016/j.apsusc.2021.149682
19. [19]
  J. Zhao, Z. Chen, J. Am. Chem. Soc. 139 (2017) 12480–12487. doi: 10.1021/jacs.7b05213
20. [20]
  X. Lv, W. Wei, F. Li, B. Huang, Y. Dai, Nano Lett. 19 (2019) 6391–6399. doi: 10.1021/acs.nanolett.9b02572
21. [21]
  X. Liu, Y. Jiao, Y. Zheng, et al., J. Am. Chem. Soc. 141 (2019) 9664–9672. doi: 10.1021/jacs.9b03811
22. [22]
  W. Zhao, L. Zhang, Q. Luo, et al., ACS Catal. 9 (2019) 3419–3425. doi: 10.1021/acscatal.8b05061
23. [23]
  M. Miao, X. Gong, S. Lei, et al., Chem. Phys. 548 (2021) 111249. doi: 10.1016/j.chemphys.2021.111249
24. [24]
  L. Zhao, Y. Li, G. Zhou, et al., Chin. Chem. Lett. 32 (2021) 900–905. doi: 10.1016/j.cclet.2020.07.016
25. [25]
  B. Tian, S. Li, S. Lei, et al., Chin. Chem. Lett. (2021) 10.1016/j.cclet.2021.02.011. doi: 10.1016/j.cclet.2021.02.011
26. [26]
  W. Song, J. Wang, L. Fu, et al., Chin. Chem. Lett. (2021) 10.1016/j.cclet.2021.02.043. doi: 10.1016/j.cclet.2021.02.043
27. [27]
  H. Yang, C. He, L. Fu, et al., Chin. Chem. Lett. (2021) 10.1016/j.cclet.2021.03.038. doi: 10.1016/j.cclet.2021.03.038
28. [28]
  R. Wang, C. He, W. Chen, C. Zhao, J. Huo, Chin. Chem. Lett. (2021)), doi:10.1016/j.cclet.2021.05.024. doi: 10.1016/j.cclet.2021.05.024
29. [29]
  A.R. Singh, B.A. Rohr, J.A. Schwalbe, et al., ACS Catal. 7 (2017) 706–709. doi: 10.1021/acscatal.6b03035
30. [30]
  R. Lang, X. Du, Y. Huang, et al., Chem. Rev. 120 (2020) 11986–12043. doi: 10.1021/acs.chemrev.0c00797
31. [31]
  H.Y. Zhuo, X. Zhang, J.X. Liang, et al., Chem. Rev. 120 (2020) 12315–12341. doi: 10.1021/acs.chemrev.0c00818
32. [32]
  D. De Faoite, D.J. Browne, F.R. Chang-Díaz, K.T. Stanton, J. Mater. Sci. 47 (2012) 4211–4235. doi: 10.1007/s10853-011-6140-1
33. [33]
  L. Wang, L. Liu, J. Chen, et al., Angew. Chem. Int. Ed. 59 (2020) 15734–15740. doi: 10.1002/anie.202007244
34. [34]
  H. Zhang, M. Holbrook, F. Cheng, et al., ACS Nano15 (2021) 2497–2505. doi: 10.1021/acsnano.0c06596
35. [35]
  W. Wu, P. Lu, Z. Zhang, W. Guo, ACS Appl. Mater. Interfaces3 (2011) 4787–4795. doi: 10.1021/am201271j
36. [36]
  N.H. Song, Y.S. Wang, L.Y. Zhang, Y.Y. Yang, Y. Jia, et al., J. Magn. Magn. Mater. 468 (2018) 252–258. doi: 10.1016/j.jmmm.2018.08.019
37. [37]
  W. Sukkabot, Chin. J. Phys. 62 (2019) 335–341. doi: 10.1016/j.cjph.2019.10.009
38. [38]
  X. Chen, X. Sun, J. Jiang, et al., J. Phys. Chem. C120 (2016) 20350–20356. doi: 10.1021/acs.jpcc.6b06161
39. [39]
  L. Teitz, M.C. Toroker, Adv. Funct. Mater. 30 (2020) 1808544. doi: 10.1002/adfm.201808544
40. [40]
  J. Yu, C. He, C. Pu, et al., Chin. Chem. Lett. (2021) 10.1016/j.cclet.2021.02.046. doi: 10.1016/j.cclet.2021.02.046
41. [41]
  J. Wang, C. He, J. Huo, L. Fu, C. Zhao, Adv. Theory Simulations. 4 (2021) 2100003. doi: 10.1002/adts.202100003
42. [42]
  L. Fu, R. Wang, C. Zhao, et al., Chem. Eng. J. 414 (2021) 128857. doi: 10.1016/j.cej.2021.128857
43. [43]
  G. Kresse, D. Joubert, Phys. Rev. B59 (1999) 1758–1775.
44. [44]
  P.E. Blöchl, Phys. Rev. B50 (1994) 17953–17979. doi: 10.1103/PhysRevB.50.17953
45. [45]
  S. Grimme, J. Antony, S. Ehrlich, H. Krieg, J. Chem. Phys. 132 (2010) 154104. doi: 10.1063/1.3382344
46. [46]
  J.K. Nørskov, T. Bligaard, A. Logadottir, et al., J. Electrochem. Soc. 152 (2005) J23. doi: 10.1149/1.1856988
47. [47]
  Computational Chemistry Comparison and Benchmark Database, https://cccbdb.nist.gov/.
48. [48]
  M. Gajdoš, K. Hummer, G. Kresse, J. Furthmüller, F. Bechstedt, Phys. Rev. B: Condens. Matter Mater. Phys. 73 (2006) 045112. doi: 10.1103/PhysRevB.73.045112
49. [49]
  P. Pyykkö, M. Atsumi, Chem. Eur. J. 15 (2009) 186–197. doi: 10.1002/chem.200800987
50. [50]
  T. He, A.R. Puente Santiago, A. Du, J. Catal. 388 (2020) 77–83. doi: 10.1016/j.jcat.2020.05.009
51. [51]
  Z. Ma, Z. Cui, C. Xiao, et al., Nanoscale. 12 (2020) 1541–1550. doi: 10.1039/c9nr08969a
52. [52]
  C. Ling, Y. Ouyang, Q. Li, et al., Small Methods3 (2019) 1800376. doi: 10.1002/smtd.201800376
53. [53]
  H. Liu, L. Wei, F. Liu, et al., ACS Catal. 9 (2019) 5245–5267. doi: 10.1021/acscatal.9b00994
54. [54]
  E. Skúlason, T. Bligaard, S. Gudmundsdóttir, et al., Phys. Chem. Chem. Phys. 14 (2012) 1235–1245. doi: 10.1039/C1CP22271F
55. [55]
  Z. Geng, Y. Liu, X. Kong, et al., Adv. Mater. 30 (2018) 1803498. doi: 10.1002/adma.201803498
56. [56]
  Y. Ge, W. Wan, Y. Ren, F. Li, Y. Liu, Appl. Phys. Lett. 117 (2020) 123101. doi: 10.1063/5.0022426
57. [57]
  W. Zhang, W. Ji, Y. Ma, Mater. Today Commun. 24 (2020) 101344. doi: 10.1016/j.mtcomm.2020.101344
58. [58]
  C. Xia, W. Li, D. Ma, L. Zhang, Nanotechnology31 (2020) 375705. doi: 10.1088/1361-6528/ab97d0
59. [59]
  H. Zheng, X.B. Li, N.K. Chen, et al., Phys. Rev. B: Condens. Matter Mater. Phys. 92 (2015) 115307. doi: 10.1103/PhysRevB.92.115307
60. [60]
  S. Wang, L. Shi, X. Bai, et al., ACS Cent. Sci. 6 (2020) 1762–1771. doi: 10.1021/acscentsci.0c00552
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