Abstract
Ammonia (NH3) synthesis is a critical chemical process to develop nitrogen-containing commodities which remains a significant challenge in chemistry and industry. Photocatalysis reduction has been deemed as one of the most promising strategies for N2 fixation under mild conditions. Herein, a series of Pr doped LiNbO3 (Pr3+:LiNbO3) were synthesized by a facile sol–gel method. Results showed that the Pr3+:LiNbO3 upconverted visible light into ultraviolet light and had the highest up-conversion efficiency when the molar ratio of Pr3+ was 2.5 mol%. In addition, the oxygen vacancies generated by the incorporation of Pr3+ into the LiNbO3 crystal lattice acted as active sites boosting the adsorption and activation of N2. The NH4+ production rate reached the highest of 30.72 μmol/L, attributed to the synergistic effects combining spontaneous polarization of the nonlinear optical (NLO) material LiNbO3 and up-conversion luminescence of Pr3+, which not only broaden the adsorption range of solar light but also enhance the charge separation. The up-conversion NLO material Pr3+:LiNbO3 in this study provides a novel alternative for guiding the design of ammonia synthesis photocatalyst.
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References
W. Qiu, X.Y. Xie, J. Qiu, W.H. Fang, R. Liang, X. Ren, X. Ji, G. Cui, A.M. Asiri, G. Cui, B. Tang, X. Sun, Nat Commun. 9, 3485 (2018)
T. Kandemir, M.E. Schuster, A. Senyshyn, M. Behrens, R. Schlogl, Angew. Chem Int Ed Engl. 52, 12723 (2013)
R. Li, Chin. J. Catal. 39, 1180 (2018)
X. Chen, N. Li, Z. Kong, W.J. Ong, X. Zhao, Mater. Horiz. 5, 9 (2018)
W. Zhao, H. Xi, M. Zhang, Y. Li, J. Chen, J. Zhang, X. Zhu, Chem Commun (Camb) 51, 4785 (2015)
T. Fei, L. Yu, Z. Liu, Y. Song, F. Xu, Z. Mo, C. Liu, J. Deng, H. Ji, M. Cheng, Y. Lei, H. Xu, H. Li, J Colloid Interface Sci. 557, 498 (2019)
S. Deng, Z. Yang, G. Lv, Y. Zhu, H. Li, F. Wang, X. Zhang, Appl. Phys. A. 125, (2019)
C. Shu, A. Noble, V.K. Aggarwal, Angew. Chem Int Ed Engl. 58, 3870 (2019)
F. Chen, H. Huang, L. Guo, Y. Zhang, T. Ma, Angew. Chem Int Ed Engl. 58, 10061 (2019)
K. D. Baklanova, A. V. Solnyshkin, I. L. Kislova, S. I. Gudkov, A. N. Belov, V. I. Shevyakov, R. N. Zhukov, D. A. Kiselev, M. D. Malinkovich, Physica Status Solidi (a). 215, (2018)
X. Wang, W. Yan, L. Zhang, L. Shi, H. Chen, Y. Zhang, M. Wu, P. Zhang, Opt. Mater. Express. 5, (2015)
B. Zielinska, M. Janus, R. Kalenczuk, Open Chemistry. 11, (2013)
L. Yin, Y. Li, J. Wang, Y. Zhai, Y. Kong, J. Gao, G. Han, P. Fan, J. Lumin. 132, 3010 (2012)
L. Sun, L. Li, R. Gao, K. Tang, L. Fu, X.C. Ai, J.P. Zhang, Phys Chem Chem Phys. 20, 17141 (2018)
N. Tyagi, A.A. Reddy, R. Nagarajan, Opt. Mater. 33, 42 (2010)
P. W. Jaschin, K. B. R. Varma, Journal of Applied Physics. 122, (2017)
N. Sinclair, E. Saglamyurek, M. George, R. Ricken, C. La Mela, W. Sohler, W. Tittel, J. Lumin. 130, 1586 (2010)
S. Bharathkumar, M. Sakar, N. Ponpandian, S. Balakumar, Mater. Res. Bull. 101, 107 (2018)
P. Li, Z. Zhou, Q. Wang, M. Guo, S. Chen, J. Low, R. Long, W. Liu, P. Ding, Y. Wu, Y. Xiong, J Am Chem Soc. 142, 12430 (2020)
R. Shi, Y. Zhao, G.I.N. Waterhouse, S. Zhang, T. Zhang, ACS Catal. 9, 9739 (2019)
H. Li, J. Shang, Z. Ai, L. Zhang, J. Am Chem Soc. 137, 6393 (2015)
Y. Fang, J. Lang, J. Wang, Q. Han, Z. Zhang, Q. Zhang, J. Yang, S. G. Xing, Appl. Phys. A. 124, (2018)
L. Sun, R. Gao, T. Pan, X.C. Ai, L. Fu, J.P. Zhang, Nanoscale. 11, 18150 (2019)
T. Su, Y. Yang, Y. Na, R. Fan, L. Li, L. Wei, B. Yang, W. Cao, ACS Appl Mater Interfaces. 7, 3754 (2015)
H. Xu, Y. Li, M. Ding, W. Chen, K. Wang, C. Lu, ACS Sustain. Chem. Eng. 6, 7042 (2018)
H. Huang, Y. He, Y. Guo, R. He, Z. Lin, Y. Zhang, Solid State Sci. 46, 37 (2015)
C. Hu, C. Sun, J. Li, Z. Li, H. Zhang, Z. Jiang, Chem. Phys. 325, 563 (2006)
E.L. Cates, A.P. Wilkinson, J.H. Kim, J. Lumin. 160, 202 (2015)
M.E. Lines, A.M. Glass, G. Burns, Phys. Today 31, 56 (1978)
T. Huang, S. Pan, L. Shi, A. Yu, X. Wang, Y. Fu, Nanoscale. 12, 1833 (2020)
S. Zhang, Y. Zhao, R. Shi, G. I. N. Waterhouse, T. Zhang, Energy Chem. 1, (2019)
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This work was supported by the National Natural Science Foundation of China (51674043, 51702026).
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Sun, L., Chu, X., He, C. et al. Efficient photocatalytic nitrogen fixation over up-conversion nonlinear optical material Pr3+:LiNbO3 under visible light irradiation. Appl. Phys. A 127, 35 (2021). https://doi.org/10.1007/s00339-020-04186-x
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DOI: https://doi.org/10.1007/s00339-020-04186-x