Skip to content
Licensed Unlicensed Requires Authentication Published by De Gruyter March 4, 2022

Three-dimensional carbon architectures with O doping and rich defects for catalytic conversion of polysulfides

  • Xue Yang , Zhiming Du , Zhiping Lei EMAIL logo , Hengfu Shui , Song Han , Honglei Yan , Jingchong Yan , Zhanku Li , Zhicai Wang , Shibiao Ren , Ying Kong and Shigang Kang

Abstract

To deal with the notorious shuttle behavior and sluggish conversion of lithium polysulfides (LiPSs), heteroatoms doping and defects creating are practical strategies for improving capture and catalytic conversion of LiPSs. In this work, O doped porous carbon materials (OPC) with a 3D hierarchical structure, consisting of 2–4 μm carbon sheets decorated with macrospores of 0.2–0.4 μm, was fabricated with MgO template. It is found that the increasing the carbonization temperature and the amount of MgO will make OPC rich in oxygen functional groups and defect sites. Electrochemical measures show that the OPC12–800 achieves reversible capacity (an initial discharge specific capacity of 1448.4 mAh g−1 at current density of 0.1 C) and cycling performance (717.7 mAh g−1 at 2 C over 200 cycles). The excellent electrochemical performance is attributed to the hierarchical porous structure, abundant C–O/C=O and defects, which effectively adsorbs polysulfides and promote faster redox reaction of LiPSs. This study provides an alternative to improve the performance of carbon materials as host of Li–S batteries by regulating the types of oxygen-containing functional groups and defects on carbon surface.


Corresponding author: Zhiping Lei, Institute of Material Science & Engineering, School of Chemistry & Chemical Engineering, Anhui Province Key Laboratory of Coal Clean Conversion and High Valued Utilization, Anhui University of Technology, Ma’anshan, 243002, Anhui Province, P. R. China, E-mail:

Funding source: Natural Scientific Foundation of China

Award Identifier / Grant number: 22078002

Award Identifier / Grant number: 21878001

Award Identifier / Grant number: 21875001

Award Identifier / Grant number: 21978002

Award Identifier / Grant number: 22008001

Award Identifier / Grant number: 21978002

Funding source: Provincial Innovative Group for Processing & Clean Utilization of Coal Resource

  1. Author contributions: All authors have accepted responsibility for the entire content of this manuscript and approved its submission.

  2. Research funding: This work was supported by the Natural Scientific Foundation of China (Grants: 22078002, 21878001, 21875001, 21978002, 22008001, and 21978002). The Authors are appreciative of the financial support from the Provincial Innovative Group for Processing & Clean Utilization of Coal Resource.

  3. Conflict of interest statement: The authors declare no conflicts of interest regarding this article.

References

Balach, J., H. K. Singh, S. Gomoll, T. Jaumann, M. Klose, S. Oswald, M. Richter, J. Eckert, and L. Giebeler. 2016. “Synergistically Enhanced Polysulfide Chemisorption Using a Flexible Hybrid Separator with N and S Dual-Doped Mesoporous Carbon Coating for Advanced Lithium–Sulfur Batteries.” ACS Applied Materials & Interfaces 8: 14586–95, https://doi.org/10.1021/acsami.6b03642.Search in Google Scholar PubMed

Chen, X., X. R. Chen, T. Z. Hou, B. Q. Li, X. B. Cheng, R. Zhang, and Q. Zhang. 2019. “Lithiophilicity Chemistry of Heteroatom-Doped Carbon to Guide Uniform Lithium Nucleation in Lithium Metal Anodes.” Science Advances 5: eaau7728, doi:https://doi.org/10.1126/sciadv.aau7728.Search in Google Scholar PubMed PubMed Central

Chung, S.-H., and A. Manthiram. 2018. “Designing Lithium–Sulfur Cells with Practically Necessary Parameters.” Joule 2: 710–24, https://doi.org/10.1016/j.joule.2018.01.002.Search in Google Scholar

Fang, R., S. Zhao, Z. Sun, D. Wang, H. Cheng, and F. Li. 2017. “More Reliable Lithium–Sulfur Batteries: Status, Solutions and Prospects.” Advanced Materials (Deerfield Beach, Fla.) 29: 1606823, doi:https://doi.org/10.1002/adma.201606823.Search in Google Scholar PubMed

Fang, R., C. Liang, Y. Xia, Z. Xiao, H. Huang, Y. Gan, J. Zhang, X. Tao, and W. Zhang. 2018. “Supercritical CO2 Mediated Incorporation of Sulfur into Carbon Matrix as Cathode Materials towards High-Performance Lithium–Sulfur Batteries.” Journal of Materials Chemistry A 6: 212–22, https://doi.org/10.1039/c7ta08768c.Search in Google Scholar

Gao, X., Y. Huang, Z. Zhang, S. Batool, X. Li, and T. Li. 2020. “Porous Hollow Carbon Aerogel-Assembled Core@Polypyrrole Nanoparticle Shell as an Efficient Sulfur Host Through a Tunable Molecular Self-Assembly Method for Rechargeable Lithium/Sulfur Batteries.” ACS Sustainable Chemistry & Engineering 8: 15822–33, https://doi.org/10.1021/acssuschemeng.0c02456.Search in Google Scholar

Guan, L., H. Hu, L. Li, Y. Pan, Y. Zhu, Q. Li, H. Guo, K. Wang, Y. Huang, M. Zhang, Y. Yan, Z. Li, X. Teng, J. Yang, J. Xiao, Y. Zhang, X. Wang, and M. Wu. 2020. “Intrinsic Defect-Rich Hierarchically Porous Carbon Architectures Enabling Enhanced Capture and Catalytic Conversion of Polysulfides.” ACS Nano 14: 6222–31, https://doi.org/10.1021/acsnano.0c02294.Search in Google Scholar PubMed

He, G., S. Evers, X. Liang, M. Cuisinier, A. Garsuch, and L. F. Nazar. 2013. “Tailoring Porosity in Carbon Nanospheres for Lithium–Sulfur Battery Cathodes.” ACS Nano 7: 10920–30, https://doi.org/10.1021/nn404439r.Search in Google Scholar PubMed

Hou, T. Z., X. Chen, H. J. Peng, J. Q. Huang, B. Q. Li, Q. Zhang, and B. Li. 2016. “Design Principles for Heteroatom-Doped Nanocarbon to Achieve Strong Anchoring of Polysulfides for Lithium–Sulfur Batteries.” Small 12: 3283–91, https://doi.org/10.1002/smll.201600809.Search in Google Scholar PubMed

Kim, P. J. H., J. Seo, K. Fu, J. Choi, Z. Liu, J. Kwon, L. Hu, and U. Paik. 2017. “Synergistic Protective Effect of a BN-Carbon Separator for Highly Stable Lithium Sulfur Batteries.” NPG Asia Materials 9: e375, https://doi.org/10.1038/am.2017.51.Search in Google Scholar

Li, Z., Y. Jiang, L. Yuan, Z. Yi, C. Wu, Y. Liu, P. Strasser, and Y. Huang. 2014. “A Highly Ordered Meso@Microporous Carbon-Supported Sulfur@Smaller Sulfur Core–Shell Structured Cathode for Li–S Batteries.” ACS Nano 8: 9295–303, https://doi.org/10.1021/nn503220h.Search in Google Scholar PubMed

Li, Y., J. Fan, J. Zhang, J. Yang, R. Yuan, J. Chang, M. Zheng, and Q. Dong. 2017. “A Honeycomb-Like Co@N–C Composite for Ultrahigh Sulfur Loading Li–S Batteries.” ACS Nano 11: 11417–24, https://doi.org/10.1021/acsnano.7b06061.Search in Google Scholar PubMed

Lu, Y., S. Gu, J. Guo, K. Rui, C. Chen, S. Zhang, J. Jin, J. Yang, and Z. Wen. 2017. “Sulfonic Groups Originated Dual-Functional Interlayer for High Performance Lithium–Sulfur Battery.” ACS Applied Materials & Interfaces 9: 14878–88, https://doi.org/10.1021/acsami.7b02142.Search in Google Scholar PubMed

Liu, M., X. Qin, Y.-B. He, B. Li, and F. Kang. 2017a. “Recent Innovative Configurations in High-Energy Lithium–Sulfur Batteries.” Journal of Materials Chemistry A 5: 5222–34, https://doi.org/10.1039/c7ta00290d.Search in Google Scholar

Liu, M., Q. Li, X. Qin, G. Liang, W. Han, D. Zhou, Y. B. He, B. Li, and F. Kang. 2017b. “Suppressing Self-Discharge and Shuttle Effect of Lithium–Sulfur Batteries with V2 O5-Decorated Carbon Nanofiber Interlayer.” Small 13: 1602539, https://doi.org/10.1002/smll.201602539.Search in Google Scholar PubMed

Pang, Q., J. Tang, H. Huang, X. Liang, C. Hart, K. C. Tam, and L. F. Nazar. 2015. “A Nitrogen and Sulfur Dual-Doped Carbon Derived from Polyrhodanine@Cellulose for Advanced Lithium–Sulfur Batteries.” Advanced Materials 27: 6021–8, https://doi.org/10.1002/adma.201502467.Search in Google Scholar PubMed

Qin, X., J. Wu, Z.-L. Xu, W. G. Chong, J.-Q. Huang, G. Liang, B. Li, F. Kang, and J.-K. Kim. 2019. “Electrosprayed Multiscale Porous Carbon Microspheres as Sulfur Hosts for Long-Life Lithium–Sulfur Batteries.” Carbon 141: 16–24, https://doi.org/10.1016/j.carbon.2018.09.048.Search in Google Scholar

Quan, P., T. Juntao, H. He, L. Xiao, H. Connor, K. C. Tam, and L. F. Nazar. 2020. “A Nitrogen and Sulfur Dual-Doped Carbon Derived from Polyrhodanine@Cellulose for Advanced Lithium–Sulfur Batteries.” Advanced materials (Deerfield Beach, Fla.) 27: 6021–8.10.1002/adma.201502467Search in Google Scholar

Ren, J., Y. Zhou, H. Wu, F. Xie, C. Xu, and D. Lin. 2019. “Sulfur-Encapsulated in Heteroatom-Doped Hierarchical Porous Carbon Derived from Goat Hair for High Performance Lithium–Sulfur Batteries.” Journal of Energy Chemistry 30: 121–31, https://doi.org/10.1016/j.jechem.2018.01.015.Search in Google Scholar

Rehman, S., T. Tang, Z. Ali, X. Huang, and Y. Hou. 2017. “’Integrated Design of MnO2@Carbon Hollow Nanoboxes to Synergistically Encapsulate Polysulfides for Empowering Lithium Sulfur Batteries.” Small 13: 1700087, doi:https://doi.org/10.1002/smll.201700087.Search in Google Scholar PubMed

Seh, Z. W., Y. Sun, Q. Zhang, and Y. Cui. 2016. “Designing High-Energy Lithium–Sulfur Batteries.” Chemical Society Reviews 45: 5605–34, https://doi.org/10.1039/c5cs00410a.Search in Google Scholar PubMed

Su, Y. S., and A. Manthiram. 2012. “Lithium–sulphur Batteries with a Microporous Carbon Paper as a Bifunctional Interlayer.” Nature Communications 3: 1166, https://doi.org/10.1038/ncomms2163.Search in Google Scholar PubMed

Su, D., M. Cortie, and G. Wang. 2017. “Fabrication of N-Doped Graphene-Carbon Nanotube Hybrids from Prussian Blue for Lithium–Sulfur Batteries.” Advanced Energy Materials 7: 1602014, https://doi.org/10.1002/aenm.201602014.Search in Google Scholar

Sun, J., Y. Sun, M. Pasta, G. Zhou, Y. Li, W. Liu, F. Xiong, and Y. Cui. 2016a. “Entrapment of Polysulfides by a Black-Phosphorus-Modified Separator for Lithium–Sulfur Batteries.” Advanced Materials 28: 9797–803, https://doi.org/10.1002/adma.201602172.Search in Google Scholar PubMed

Sun, Y. M., Q. F. Zhang, Z. Seh, Y. Wei, and Y. Cui. 2016b. “Designing High-Energy Lithium–Sulfur Batteries.” Chemical Society Reviews 45: 5605–34, https://doi.org/10.1039/c5cs00410a.Search in Google Scholar PubMed

Tu, S., X. Chen, X. Zhao, M. Cheng, P. Xiong, Y. He, Q. Zhang, and Y. Xu. 2018. “A Polysulfide-Immobilizing Polymer Retards the Shuttling of Polysulfide Intermediates in Lithium–Sulfur Batteries.” Advanced Materials 30: e1804581, https://doi.org/10.1002/adma.201804581.Search in Google Scholar PubMed

Wang, H., Z. Xu, H. Yi, H. Wei, Z. Guo, and X. Wang. 2014. “One-Step Preparation of Single-Crystalline Fe2O3 Particles/Graphene Composite Hydrogels as High Performance Anode Materials for Supercapacitors.” Nano Energy 7: 86–96, https://doi.org/10.1016/j.nanoen.2014.04.009.Search in Google Scholar

Wang, H., W. Zhang, J. Xu, and Z. Guo. 2018. “Advances in Polar Materials for Lithium–Sulfur Batteries.” Advanced Functional Materials 28: 1707520, https://doi.org/10.1002/adfm.201707520.Search in Google Scholar

Wu, P., L. H. Chen, S. S. Xiao, S. Yu, Z. Wang, Y. Li, and B. L. Su. 2018. “Insight into the Positive Effect of Porous Hierarchy in S/C Cathodes on the Electrochemical Performance of Li–S Batteries.” Nanoscale 10: 11861–8, https://doi.org/10.1039/c8nr03290d.Search in Google Scholar PubMed

Wu, Q., Z. Yao, A. Du, H. Wu, M. Huang, J. Xu, F. Cao, and C. Li. 2021. “Oxygen-Defect-Rich Coating with Nanoporous Texture as Both Anode Host and Artificial SEI for Dendrite-Mitigated Lithium–Metal Batteries.” Journal of Materials Chemistry A 9: 5606–18, https://doi.org/10.1039/d0ta08782c.Search in Google Scholar

Xu, J., D. Su, W. Zhang, W. Bao, and G. Wang. 2016. “A Nitrogen–Sulfur Co-Doped Porous Graphene Matrix as a Sulfur Immobilizer for High Performance Lithium–Sulfur Batteries.” Journal of Materials Chemistry A 4: 17381–93, https://doi.org/10.1039/c6ta05878g.Search in Google Scholar

Yao, S., C. Zhang, F. Xie, S. Xue, K. Gao, R. Guo, X. Shen, T. Li, and S. Qin. 2020a. “Hybrid Membrane with SnS2 Nanoplates Decorated Nitrogen-Doped Carbon Nanofibers as Binder-Free Electrodes with Ultrahigh Sulfur Loading for Lithium Sulfur Batteries.” ACS Sustainable Chemistry & Engineering 8: 2707–15, https://doi.org/10.1021/acssuschemeng.9b06064.Search in Google Scholar

Yao, S., C. Zhang, Y. He, Y. Li, and J. Xiang. 2020b. “Functionalization of Nitrogen-Doped Carbon Nanofibers with Polyamidoamine Dendrimer as a Freestanding Electrode with High Sulfur Loading for Lithium–Polysulfides Batteries.” ACS Sustainable Chemistry & Engineering 8: 7815–24, https://doi.org/10.1021/acssuschemeng.0c00300.Search in Google Scholar

Zhang, C., H. B. Wu, C. Yuan, Z. Guo, and X. W. Lou. 2012. “Confining Sulfur in Double-Shelled Hollow Carbon Spheres for Lithium–Sulfur Batteries.” Angewandte Chemie International Edition 51: 9592–5, https://doi.org/10.1002/anie.201205292.Search in Google Scholar PubMed

Zhang, Z., G. Wang, Y. Lai, J. Li, Z. Zhang, and W. Chen. 2015. “Nitrogen-Doped Porous Hollow Carbon Sphere-Decorated Separators for Advanced Lithium–Sulfur Batteries.” Journal of Power Sources 300: 157–63, https://doi.org/10.1016/j.jpowsour.2015.09.067.Search in Google Scholar

Zhang, J. P., X. H. Qiang, J. Y. Zhan, X. L. Wang, and D. W. Yang. 2018a. “Popcorn Inspired Porous Macrocellular Carbon: Rapid Puffing Fabrication from Rice and its Applications in Lithium–Sulfur Batteries.” Advanced Energy Materials 8: 1701110.10.1002/aenm.201701110Search in Google Scholar

Zhang, Y. Z., Z. Zhang, S. Liu, G. R. Li, and X. P. Gao. 2018b. “Free-Standing Porous Carbon Nanofiber/Carbon Nanotube Film as Sulfur Immobilizer with High Areal Capacity for Lithium–Sulfur Battery.” ACS Applied Materials & Interfaces 10: 8749–57, https://doi.org/10.1021/acsami.8b00190.Search in Google Scholar PubMed

Zhang, Z., Y. Huang, X. Li, and Z. Zhou. 2021a. “Rational Construction of Hollow Nanoboxes for Long Cycle Life Alkali Metal Ion Batteries.” Journal of Materials Science and Technology 102: 46–55.10.1016/j.jmst.2021.07.007Search in Google Scholar

Zhang, Z., Y. Huang, X. Li, X. Gao, P. Liu, and T. Li. 2021b. “Rationally Designed Polyhedral Carbon Framework from Solid to Hollow for Long Cycle Life Secondary Batteries.” Journal of Materials Chemistry A 9: 6284–97, https://doi.org/10.1039/d0ta11264j.Search in Google Scholar

Zhong, Y., X. Xia, S. Deng, J. Zhan, R. Fang, Y. Xia, X. Wang, Q. Zhang, and J. Tu. 2018. “Popcorn Inspired Porous Macrocellular Carbon: Rapid Puffing Fabrication from Rice and its Applications in Lithium–Sulfur Batteries.” Advanced Energy Materials 8: 1701110, https://doi.org/10.1002/aenm.201701110.Search in Google Scholar

Zhou, G., E. Paek, G. S. Hwang, and A. Manthiram. 2015. “Long-Life Li/Polysulphide Batteries with High Sulphur Loading Enabled by Lightweight Three-Dimensional Nitrogen/sulphur-Codoped Graphene Sponge.” Nature Communications 6: 7760, https://doi.org/10.1038/ncomms8760.Search in Google Scholar PubMed PubMed Central


Supplementary Material

The online version of this article offers supplementary material (https://doi.org/10.1515/ijcre-2021-0256).


Received: 2021-10-15
Accepted: 2022-02-08
Published Online: 2022-03-04

© 2022 Walter de Gruyter GmbH, Berlin/Boston

Downloaded on 26.4.2024 from https://www.degruyter.com/document/doi/10.1515/ijcre-2021-0256/html
Scroll to top button