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Research Article

Simultaneous diffusion of cation and anion to access N, S co-coordinated Bi-sites for enhanced CO2 electroreduction

Zhiyuan Wang1, Chun Wang2, Yidong Hu1, Shuai Yang4, Jia Yang1,6, Wenxing Chen5, Huang Zhou1, Fangyao Zhou1, Lingxiao Wang1, Junyi Du1, Yafei Li2( ), Yuen Wu1,3( )
School of Chemistry and Materials Science, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China
Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, Jiangsu Key Laboratory of New Power Batteries, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, China
Dalian National Laboratory for Clean Energy, Dalian 116023, China
Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201210, China
Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Institutes of Physical Science and Information Technology, Key Laboratory of Structure and Functional Regulation of Hybrid Materials, Ministry of Education, Anhui Graphene Engineering Laboratory, Anhui University, Hefei 230601, China
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Graphical Abstract

Abstract

Developing highly active single-atom sites catalysts for electrochemical reduction of CO2 is an effective and environmental-friendly strategy to promote carbon-neutral energy cycle and ameliorate global climate issues. Herein, we develop an atomically dispersed N, S co-coordinated bismuth atom sites catalyst (Bi-SAs-NS/C) via a cation and anion simultaneous diffusion strategy for electrocatalytic CO2 reduction. In this strategy, the bonded Bi cation and S anion are simultaneously diffused into the nitrogen-doped carbon layer in the form of Bi2S3. Then Bi is captured by the abundant N-rich vacancies and S is bonded with carbons support at high temperature, formed the N, S co-coordinated Bi sites. Benefiting from the simultaneous diffusion of Bi and S, different electronegative N and S can be effectively co-coordinated with Bi, forming the uniform Bi-N3S/C sites. The synthesized Bi-SAs-NS/C exhibits a high selectivity towards CO with over 88% Faradaic efficiency in a wide potential range, and achieves a maximum FECO of 98.3% at -0.8 V vs. RHE with a current density of 10.24 mA·cm-2, which can keep constant with negligible degradation in 24 h continuous electrolysis. Experimental results and theoretical calculations reveal that the significantly improved catalytic performance of Bi-SAs-NS/C than Bi-SAs-N/C is ascribed to the replacement of one coordinated-N with low electronegative S in Bi-N4C center, which can greatly reduce the energy barrier of the intermediate formation in rate-limiting step and increase the reaction kinetics. This work provides an effective strategy for rationally designing highly active single-atom sites catalysts for efficient electrocatalysis with optimized electronic structure.

Keywords

SN-co-doped carbon nanotubesingle bismuth siteselectronic structure modulationelectrochemical CO2 reduction

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References

[1]
Wang, Y. H.; Wang, Z. Y.; Dinh, C. T.; Li, J.; Ozden, A.; Kibria, M. G.; Seifitokaldani, A.; Tan, C. S.; Gabardo, C. M.; Luo, M. C. et al. Catalyst synthesis under CO2 electroreduction favours faceting and promotes renewable fuels electrosynthesis. Nat. Catal. 2020, 3, 98-106.
Google Scholar
[2]
Jiao, Y.; Zheng, Y.; Chen, P.; Jaroniec, M.; Qiao, S. Z. Molecular scaffolding strategy with synergistic active centers to facilitate electrocatalytic CO2 reduction to hydrocarbon/alcohol. J. Am. Chem. Soc. 2017, 139, 18093-18100.
Google Scholar
[3]
Ross, M. B.; De Luna, P.; Li, Y. F.; Dinh, C. T.; Kim, D.; Yang, P. D.; Sargent, E. H. Designing materials for electrochemical carbon dioxide recycling. Nat. Catal. 2019, 2, 648-658.
Google Scholar
[4]
Zheng, T. T.; Jiang, K.; Wang, H. T. Recent advances in electrochemical CO2-to-CO conversion on heterogeneous catalysts. Adv. Mater. 2018, 30, 1802066.
Google Scholar
[5]
Li, F. W.; Chen, L.; Knowles, G. P.; MacFarlane, D. R.; Zhang, J. Hierarchical mesoporous SnO2 nanosheets on carbon cloth: A robust and flexible electrocatalyst for CO2 reduction with high efficiency and selectivity. Angew. Chem., Int. Ed. 2017, 56, 505-509.
Google Scholar
[6]
Varela, A. S.; Ju, W.; Bagger, A.; Franco, P.; Rossmeisl, J.; Strasser, P. Electrochemical reduction of CO2 on metal-nitrogen-doped carbon catalysts. ACS Catal. 2019, 9, 7270-7284.
Google Scholar
[7]
Wang, Y. F.; Han, P.; Lv, X. M.; Zhang, L. J.; Zheng, G. F. Defect and interface engineering for aqueous electrocatalytic CO2 reduction. Joule 2018, 2, 2551-2582.
Google Scholar
[8]
Qiao, J. L.; Liu, Y. Y.; Hong, F.; Zhang, J. J. A review of catalysts for the electroreduction of carbon dioxide to produce low-carbon fuels. Chem. Soc. Rev. 2014, 43, 631-675.
Google Scholar
[9]
Zhang, L.; Zhao, Z. J.; Gong, J. L. Nanostructured materials for heterogeneous electrocatalytic CO2 reduction and their related reaction mechanisms. Angew. Chem., Int. Ed. 2017, 56, 11326-11353.
Google Scholar
[10]
Sun, Z. Y.; Ma, T.; Tao, H. C.; Fan, Q.; Han, B. X. Fundamentals and challenges of electrochemical CO2 reduction using two-dimensional materials. Chem 2017, 3, 560-587.
Google Scholar
[11]
Li, M. H.; Wang, H. F.; Luo, W.; Sherrell, P. C.; Chen, J.; Yang, J. P. Heterogeneous single-atom catalysts for electrochemical CO2 reduction reaction. Adv. Mater. 2020, 32, 2001848.
Google Scholar
[12]
Lin, L.; Li, H. B.; Yan, C. C.; Li, H. F.; Si, R.; Li, M. R.; Xiao, J. P.; Wang, G. X.; Bao, X. H. Synergistic catalysis over iron-nitrogen sites anchored with cobalt phthalocyanine for efficient CO2 electroreduction. Adv. Mater. 2019, 31, 1903470.
Google Scholar
[13]
Zhu, D. D.; Liu, J. L.; Qiao, S. Z. Recent advances in inorganic heterogeneous electrocatalysts for reduction of carbon dioxide. Adv. Mater. 2016, 28, 3423-3452.
Google Scholar
[14]
Zhang, N. Q.; Ye, C. L.; Yan, H.; Li, L. C.; He, H.; Wang, D. S.; Li, Y. D. Single-atom site catalysts for environmental catalysis. Nano Res. 2020, 13, 3165-3182.
Google Scholar
[15]
Li, X. Y.; Rong, H. P.; Zhang, J. T.; Wang, D. S.; Li, Y. D. Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance. Nano Res. 2020, 13, 1842-1855.
Google Scholar
[16]
Yang, F.; Song, P.; Liu, X. Z.; Mei, B. B.; Xing, W.; Jiang, Z.; Gu, L.; Xu, W. L. Highly efficient CO2 electroreduction on ZnN4-based single-atom catalyst. Angew. Chem., Int. Ed. 2018, 57, 12303-12307.
Google Scholar
[17]
Wang, X. Q.; Chen, Z.; Zhao, X. Y.; Yao, T.; Chen, W. X.; You, R.; Zhao, C. M.; Wu, G.; Wang, J.; Huang, W. X. et al. Regulation of coordination number over single Co sites: Triggering the efficient electroreduction of CO2. Angew. Chem., Int. Ed. 2018, 130, 1962-1966.
Google Scholar
[18]
Zhang, M.; Hu, Z.; Gu, L.; Zhang, Q. H.; Zhang, L. H.; Song, Q.; Zhou, W.; Hu, S. Electrochemical conversion of CO2 to syngas with a wide range of CO/H2 ratio over Ni/Fe binary single-atom catalysts. Nano Res. 2020, 13, 3206-3211.
Google Scholar
[19]
Sun, T. T.; Xu, L. B.; Wang, D. S.; Li, Y. D. Metal organic frameworks derived single atom catalysts for electrocatalytic energy conversion. Nano Res. 2019, 12, 2067-2080.
Google Scholar
[20]
Zhuang, Z. C.; Kang, Q.; Wang, D. S.; Li, Y. D. Single-atom catalysis enables long-life, high-energy lithium-sulfur batteries. Nano Res. 2020, 13, 1856-1866.
Google Scholar
[21]
Yang, J. R.; Li, W. H.; Wang, D. S.; Li, Y. D. Single-atom materials: Small structures determine macroproperties. Small Struct., in press, .
Crossref Google Scholar
[22]
Zhang, J.; Zheng, G. Y.; Zhang, M. L.; Qiu, Y. J.; Xu, Q.; Cheong, W. C.; Chen, W. X.; Zheng, L. R.; Gu, L.; Hu, Z. P. et al. Controlling N-doping type in carbon to boost single-atom site Cu catalyzed transfer hydrogenation of quinoline. Nano Res. 2020, 13, 3082-3087.
Google Scholar
[23]
Jiang, K.; Siahrostami, S.; Zheng, T. T.; Hu, Y. F.; Hwang, S.; Stavitski, E.; Peng, Y. D.; Dynes, J.; Gangisetty, M.; Su, D. et al. Isolated Ni single atoms in graphene nanosheets for high-performance CO2 reduction. Energy Environ. Sci. 2018, 11, 893-903.
Google Scholar
[24]
Zhang, Z.; Ma, C.; Tu, Y. C.; Si, R.; Wei, J.; Zhang, S. H.; Wang, Z.; Li, J. F.; Wang, Y.; Deng, D. H. Multiscale carbon foam confining single iron atoms for efficient electrocatalytic CO2 reduction to CO. Nano Res. 2019, 12, 2313-2317.
Google Scholar
[25]
Liu, S.; Yang, H. B.; Hung, S. F.; Ding, J.; Cai, W. Z.; Liu, L. H.; Gao, J. J.; Li, X. N.; Ren, X. Y.; Kuang, Z. C. et al. Elucidating the electrocatalytic CO2 reduction reaction over a model single-atom nickel catalyst. Angew. Chem., Int. Ed. 2020, 59, 798-803.
Google Scholar
[26]
Jiang, Z. L.; Wang, T.; Pei, J. J.; Shang, H. S.; Zhou, D. N.; Li, H. J.; Dong, J. C.; Wang, Y.; Cao, R.; Zhuang, Z. B. et al. Discovery of main group single Sb-N4 active sites for CO2 electroreduction to formate with high efficiency. Energy Environ. Sci. 2020, 13, 2856-2863.
Google Scholar
[27]
Shang, H. S.; Wang, T.; Pei, J. J.; Jiang, Z. L.; Zhou, D. N.; Wang, Y.; Li, H. J.; Dong, J. C.; Zhuang, Z. B.; Chen, W. X. et al. Design of a single-atom indiumδ+-N4 interface for efficient electroreduction of CO2 to formate. Angew. Chem., Int. Ed. 2020, 59, 22465-22469.
Google Scholar
[28]
Shang, H. S.; Zhou, X. Y.; Dong, J. C.; Li, A.; Zhao, X.; Liu, Q. H.; Lin, Y.; Pei, J. J.; Li, Z.; Jiang, Z. L. et al. Engineering unsymmetrically coordinated Cu-S1N3 single atom sites with enhanced oxygen reduction activity. Nat. Commun. 2020, 11, 3049.
Google Scholar
[29]
Ramaswamy, N.; Tylus, U.; Jia, Q. Y.; Mukerjee, S. Activity descriptor identification for oxygen reduction on nonprecious electrocatalysts: Linking surface science to coordination chemistry. J. Am. Chem. Soc. 2013, 135, 15443-15449.
Google Scholar
[30]
Osmieri, L.; Videla, A.; Ocon, P.; Specchia, S. Kinetics of oxygen electroreduction on Me-N-C (Me = Fe, Co, Cu) catalysts in acidic medium: Insights on the effect of the transition metal. J. Phys. Chem. C 2017, 121, 17796-17817.
Google Scholar
[31]
Hou, Y.; Qiu, M.; Kim, M. G.; Liu, P.; Nam, G.; Zhang, T.; Zhuang, X. D.; Yang, B.; Cho, J.; Chen, M. W. et al. Atomically dispersed nickel-nitrogen-sulfur species anchored on porous carbon nanosheets for efficient water oxidation. Nat. Commun. 2019, 10, 1392.
Google Scholar
[32]
Zhang, J. Q.; Zhao, Y. F.; Chen, C.; Huang, Y. C.; Dong, C. L.; Chen, C. J.; Liu, R. S.; Wang, C. Y.; Yan, K.; Li, Y. D. et al. Tuning the coordination environment in single-atom catalysts to achieve highly efficient oxygen reduction reactions. J. Am. Chem. Soc. 2019, 141, 20118-20126.
Google Scholar
[33]
Chen, Y. Q.; Yao, Y. J.; Xia, Y. J.; Mao, K.; Tang, G. A.; Wu, Q.; Yang, L. J.; Wang, X. Z.; Sun, X. H.; Hu, Z. Advanced Ni-Nx-C single-site catalysts for CO2 electroreduction to CO based on hierarchical carbon nanocages and S-doping. Nano Res. 2020, 13, 2777-2783.
Google Scholar
[34]
Li, Q. H.; Chen, W. X.; Xiao, H.; Gong, Y.; Li, Z.; Zheng, L. R.; Zheng, X. S.; Yan, W. S.; Cheong, W. C.; Shen, R. et al. Fe isolated single atoms on S, N codoped carbon by copolymer pyrolysis strategy for highly efficient oxygen reduction reaction. Adv. Mater. 2018, 30, 1800588.
Google Scholar
[35]
Xue, P.; Wang, N. N.; Fang, Z. W.; Lu, Z. X.; Xu, X.; Wang, L.; Du, Y.; Ren, X. C.; Bai, Z. C.; Dou, S. X. et al. Rayleigh-instability-induced bismuth nanorod @ nitrogen-doped carbon nanotubes as a long cycling and high rate anode for sodium-ion batteries. Nano Lett. 2019, 19, 1998-2004.
Google Scholar
[36]
Wang, Z. Y.; Yang, J.; Cao, J. B.; Chen, W. X.; Wang, G.; Liao, F.; Zhou, X.; Zhou, F. Y.; Li, R. L.; Yu, Z. Q. et al. Room-temperature synthesis of single iron site by electrofiltration for photoreduction of CO2 into tunable syngas. ACS Nano 2020, 14, 6164-6172.
Google Scholar
[37]
Ferrari, A. C.; Basko, D. M. Raman spectroscopy as a versatile tool for studying the properties of graphene. Nat. Nanotechnol. 2013, 8, 235-246.
Google Scholar
[38]
Ye, L.; Ying, Y. R.; Sun, D. R.; Zhang, Z. Y.; Fei, L. F.; Wen, Z. H.; Qiao, J. L.; Huang, H. T. Highly efficient porous carbon electrocatalyst with controllable N-species content for selective CO2 reduction. Angew. Chem., Int. Ed. 2020, 59, 3244-3251.
Google Scholar
[39]
Ito, Y.; Cong, W. T.; Fujita, T.; Tang, Z.; Chen, M. W. High catalytic activity of nitrogen and sulfur co-doped nanoporous graphene in the hydrogen evolution reaction. Angew. Chem., Int. Ed. 2015, 54, 2131-2136.
Google Scholar
[40]
Zhang, E. H.; Wang, T.; Yu, K.; Liu, J.; Chen, W. X.; Li, A.; Rong, H. P.; Lin, R.; Ji, S. F.; Zheng, X. S. et al. Bismuth single atoms resulting from transformation of metal-organic frameworks and their use as electrocatalysts for CO2 reduction. J. Am. Chem. Soc. 2019, 141, 16569-16573.
Google Scholar
[41]
Shang, H. S.; Sun, W. M.; Sui, R.; Pei, J. J.; Zheng, L. R.; Dong, J. C.; Jiang, Z. L.; Zhou, D. N.; Zhuang, Z. B.; Chen, W. X. et al. Engineering isolated Mn-N2C2 atomic interface sites for efficient bifunctional oxygen reduction and evolution reaction. Nano Lett. 2020, 20, 5443-5450.
Google Scholar
[42]
Zhong, H. X.; Meng, F. L.; Zhang, Q.; Liu, K. H.; Zhang, X. B. Highly efficient and selective CO2 electro-reduction with atomic Fe-C-N hybrid coordination on porous carbon nematosphere. Nano Res. 2019, 12, 2318-2323.
Google Scholar
[43]
Liu, J. Y.; Kong, X.; Zheng, L. R.; Guo, X.; Liu, X. F.; Shui, J. L. Rare earth single-atom catalysts for nitrogen and carbon dioxide reduction. ACS Nano 2020, 14, 1093-1101.
Google Scholar
[44]
Zhang, B. X.; Zhang, J. L.; Shi, J. B.; Tan, D. X.; Liu, L. F.; Zhang, F. Y.; Lu, C.; Su, Z. Z.; Tan, X. N.; Cheng, X. Y. et al. Manganese acting as a high-performance heterogeneous electrocatalyst in carbon dioxide reduction. Nat. Commun. 2019, 10, 2980.
Google Scholar
[45]
Rong, X.; Wang, H. J.; Lu, X. L.; Si, R.; Lu, T. B. Controlled synthesis of a vacancy-defect single-atom catalyst for boosting CO2 electroreduction. Angew. Chem., Int. Ed. 2020, 59, 1961-1965.
Google Scholar
Nano Research
Volume 14 Issue 8,
August 2021
Pages 2790-2796
DOI: 10.1007/s12274-021-3287-1
Cite this article:
Wang Z, Wang C, Hu Y, et al. Simultaneous diffusion of cation and anion to access N, S co-coordinated Bi-sites for enhanced CO2 electroreduction. Nano Research, 2021, 14(8): 2790-2796. https://doi.org/10.1007/s12274-021-3287-1
Topics:
Bismuth compoundsCarbonCarbon dioxideCatalystsDoping (additives)Electrocatalysis Electrolytic reduction Electronic structureLayered semiconductorsPositive ionsReaction intermediates

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Received: 15 November 2020
Revised: 06 December 2020
Accepted: 07 December 2020
Published: 05 January 2021
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021
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