Bismuth-Based Free-Standing Electrodes for Ambient-Condition Ammonia Production in Neutral Media
Corresponding Author: Tianyi Ma
Nano-Micro Letters,
Vol. 12 (2020), Article Number: 133
Abstract
Electrocatalytic nitrogen reduction reaction is a carbon-free and energy-saving strategy for efficient synthesis of ammonia under ambient conditions. Here, we report the synthesis of nanosized Bi2O3 particles grown on functionalized exfoliated graphene (Bi2O3/FEG) via a facile electrochemical deposition method. The obtained free-standing Bi2O3/FEG achieves a high Faradaic efficiency of 11.2% and a large NH3 yield of 4.21 ± 0.14 μgNH3 h−1 cm−2 at − 0.5 V versus reversible hydrogen electrode in 0.1 M Na2SO4, better than that in the strong acidic and basic media. Benefiting from its strong interaction of Bi 6p band with the N 2p orbitals, binder-free characteristic, and facile electron transfer, Bi2O3/FEG achieves superior catalytic performance and excellent long-term stability as compared with most of the previous reported catalysts. This study is significant to design low-cost, high-efficient Bi-based electrocatalysts for electrochemical ammonia synthesis.
Highlights:
1 The Bi2O3 nanoplates homogeneously decorated free-standing exfoliated graphene (Bi2O3/FEG) was prepared by a facile electrochemical deposition method.
2 The Bi2O3/FEG first used as nitrogen reduction electrocatalyst exhibits excellent electrocatalysis performance and stability for nitrogen reduction reaction in neutral media.
3 The superior electrocatalytic nitrogen reduction activity is attributed to the strong interaction of the Bi 6p band with the N 2p orbitals, binder-free nature of the electrodes, and facile electron transfer through the graphene nanosheets.
Keywords
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References
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M.G. Wu, J.Q. Liao, L.X. Yu, R.T. Lv, P. Li et al., 2020 Roadmap on carbon materials for energy storage and conversion. Chem. Asian J. 15(7), 995–1013 (2020). https://doi.org/10.1002/asia.201901802
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H.J. Wang, Y.H. Li, C.J. Li, K. Deng, Z.Q. Wang, Y. Xu, X.N. Li, H.R. Xue, L. Wang, One-pot synthesis of bi-metallic PdRu tripods as an efficient catalyst for electrocatalytic nitrogen reduction to ammonia. J. Mater. Chem. A 2, 801–805 (2019). https://doi.org/10.1039/C8TA09482A
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H.T. Du, X.X. Guo, R.M. Kong, F.L. Qu, Cr2O3 nanofiber: a high-performance electrocatalyst toward artificial N2 fixation to NH3 under ambient conditions. Chem. Commun. 91, 12848–12851 (2018). https://doi.org/10.1039/C8CC07186A
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H.Y. Jin, L.Q. Li, X. Liu, C. Tang, W.J. Xu et al., Nitrogen vacancies on 2D layered W2N3: a stable and efficient active site for nitrogen reduction reaction. Adv. Mater. 32, 1902709 (2019). https://doi.org/10.1002/adma.201902709
G.F. Chen, S.Y. Ren, L.L. Zhang, H. Cheng, Y.R. Luo, K.H. Zhu, L.X. Ding, H.H. Wang, Nitrogen reduction reactions: advances in electrocatalytic N2 reduction—strategies to tackle the selectivity challenge. Small Methods 6, 1970016 (2019). https://doi.org/10.1002/smtd.201970016
J.H. Montoya, C. Tsai, A. Vojvodic, J.K. Nørskov, The challenge of electrochemical ammonia synthesis: a new perspective on the role of nitrogen scaling relations. Chemsuschem 13, 2180–2186 (2015). https://doi.org/10.1002/cssc.201500322
Z. Wang, F. Gong, L. Zhang, R. Wang, L. Ji et al., Electrocatalytic hydrogenation of N2 to NH3 by MnO: experimental and theoretical investigations. Adv. Sci. 1, 1801182 (2019). https://doi.org/10.1002/advs.201801182
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F.Y. Wang, X. Lv, X.J. Zhu, J. Du, S.Y. Lu et al., Bi nanodendrites for efficient electrocatalytic N2 fixation to NH3 under ambient conditions. Chem. Commun. 14, 2107–2110 (2020). https://doi.org/10.1039/C9CC09803H
L.Q. Li, C. Tang, B.Q. Xia, H.Y. Jin, Y. Zheng, S.Z. Qiao, Two-dimensional mosaic bismuth nanosheets for highly selective ambient electrocatalytic nitrogen reduction. ACS Catal. 4, 2902–2908 (2019). https://doi.org/10.1021/acscatal.9b00366
Y. Peng, M. Yan, Q.G. Chen, C.M. Fan, H.Y. Zhou, A.W. Xu, Novel one-dimensional Bi2O3–Bi2WO6 p–n hierarchical heterojunction with enhanced photocatalytic activity. J. Mater. Chem. A 22, 8517–8524 (2014). https://doi.org/10.1039/C4TA00274A
H.J. Lu, Q. Hao, T. Chen, L.H. Zhang, D.M. Chen, C. Ma, W.Q. Yao, Y.F. Zhu, A high-performance Bi2O3/Bi2SiO5 p–n heterojunction photocatalyst induced by phase transition of Bi2O3. Appl. Catal. B-Environ. (2018). https://doi.org/10.1016/j.apcatb.2018.05.069
S. Sanna, V. Esposito, J.W. Andreasen, J. Hjelm, W. Zhang et al., Enhancement of the chemical stability in confined δ-Bi2O3. Nat. Mater. 5, 500–504 (2015). https://doi.org/10.1038/nmat4266
Y. Song, X. Cai, X.X. Xu, X.X. Liu, Integration of nickel–cobalt double hydroxide nanosheets and polypyrrole films with functionalized partially exfoliated graphite for asymmetric supercapacitors with improved rate capability. J. Mater. Chem. A 28, 14712–14720 (2015). https://doi.org/10.1039/C5TA02810H
J.H. Cao, K.X. Wang, J.Y. Chen, C.J. Lei, B. Yang, Z.J. Li, L.C. Lei, Y. Hou, K. Ostrikov, Nitrogen-doped carbon-encased bimetallic selenide for high-performance water electrolysis. Nano-Micro Lett. 11, 67 (2019). https://doi.org/10.1007/s40820-019-0299-4
Y.L. Yang, Y. Tang, H.M. Jiang, Y.M. Chen, P.Y. Wan et al., 2020 Roadmap on gas-involved photo- and electro-catalysis. Chin. Chem. Lett. 12, 2089–2109 (2019). https://doi.org/10.1016/j.cclet.2019.10.041
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