Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

Spatially coupled adsorption and catalysis for sustainable lithium–sulfur batteries

Nature Sustainability (2026)Cite this article

Subjects

Abstract

Lithium–sulfur batteries have been considered a promising energy storage technology for maximizing sustainability, owing to their ultrahigh theoretical energy density and the abundant supply of low-cost sulfur. However, their high-energy advantage is often compromised in practice by the heavy, voluminous host materials and catalysts required to mitigate the polysulfide shuttle effect and sluggish redox kinetics. Here we address this dilemma by spatially coupling adsorption and catalytic sites within an sp-nitrogen-doped graphdiyne multishelled architecture. This design enables an exceptional sulfur loading of 93.9%, achieving a close-to-theoretical capacity of 1,462 mAh g(S+host)−1 and a pouch-cell energy density of ~457 Wh kg−1. Even at a high rate of 10C, the system maintains an energy density of 1,384.5 Wh kg(S+host)−1 over 600 cycles. In situ spectroscopic characterizations and theoretical calculations reveal that the favourable orbital overlapping between sp-nitrogen and neighbouring carbon facilitates rapid electron transfer and optimized charge redistribution, thus simultaneously promoting the adsorption and redox reaction of polysulfides. By minimizing inactive mass, this work provides a scalable blueprint for high-performance, resource-efficient battery chemistries.

This is a preview of subscription content, access via your institution

Access options

Buy this article

  • Purchase on SpringerLink
  • Instant access to the full article PDF.

USD 39.95

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Material characterization.
Fig. 2: Electrochemical performance of Li–S coin cells.
Fig. 3: Chemical adsorption of polysulfides and in situ characterization.
Fig. 4: DFT calculations.
Fig. 5: Electrochemical performance of Li–S pouch cells.

Similar content being viewed by others

Data availability

All data are available in the main text or the Supplementary Information and are also available from the corresponding authors upon request. Source data are provided with this paper.

References

  1. Liao, M. et al. Hybrid polymer network cathode-enabled soluble-polysulfide-free lithium–sulfur batteries. Nat. Sustain. 7, 1709–1718 (2024).

    Article  Google Scholar 

  2. Song, H. et al. All-solid-state Li–S batteries with fast solid–solid sulfur reaction. Nature 637, 846–853 (2025).

    Article  CAS  Google Scholar 

  3. Bauer, C. et al. Charging sustainable batteries. Nat. Sustain. 5, 176–178 (2022).

    Article  Google Scholar 

  4. Zhou, G. et al. Formulating energy density for designing practical lithium-sulfur batteries. Nat. Energy 7, 312–319 (2022).

    Article  CAS  Google Scholar 

  5. Raza, H. et al. Li-S batteries: challenges, achievements and opportunities. Electrochem. Energy Rev. 6, 29 (2023).

    Article  CAS  Google Scholar 

  6. Wang, D. et al. Overcoming the conversion reaction limitation at three-phase interfaces using mixed conductors towards energy-dense solid-state Li–S batteries. Nat. Mater. 24, 243–251 (2025).

    Article  CAS  Google Scholar 

  7. She, Z. et al. Designing high-energy lithium-sulfur batteries. Chem. Soc. Rev. 45, 5605–5634 (2016).

    Article  Google Scholar 

  8. Zhou, F. et al. Strutted graphene foam loading sulfur for high-rate long-lifetime Li-S batteries. Nano Energy 127, 109755 (2024).

    Article  CAS  Google Scholar 

  9. Huang, L. et al. Synergistic interfacial bonding in reduced graphene oxide fiber cathodes containing polypyrrole@sulfur nanospheres for flexible energy storage. Angew. Chem. Int. Ed. 61, e202212151 (2022).

    Article  CAS  Google Scholar 

  10. Qi, F. et al. Tunable interaction between metal-organic frameworks and electroactive components in lithium-sulfur batteries: status and perspectives. Adv. Energy Mater. 11, 2100387 (2021).

    Article  CAS  Google Scholar 

  11. Liu, W. et al. Conjugated three-dimensional high-connected covalent organic frameworks for lithium-sulfur batteries. J. Am. Chem. Soc. 144, 17209–17218 (2022).

    Article  CAS  Google Scholar 

  12. Zhong, Y. et al. Surface chemistry in cobalt phosphide-stabilized lithium-sulfur batteries. J. Am. Chem. Soc. 140, 1455–1459 (2018).

    Article  CAS  Google Scholar 

  13. Luo, D. et al. Synergistic engineering of defects and architecture in binary metal chalcogenide toward fast and reliable lithium-sulfur batteries. Adv. Energy Mater. 9, 1900228 (2019).

    Article  Google Scholar 

  14. Wang, J. et al. Multi-shelled metal oxides prepared via an anion-adsorption mechanism for lithium-ion batteries. Nat. Energy 1, 16050 (2016).

    Article  CAS  Google Scholar 

  15. Zhang, X. et al. Delicate co-control of shell structure and sulfur vacancies in interlayer-expanded tungsten disulfide hollow ephere for fast and stable sodium storage. Adv. Mater. 35, 2209354 (2023).

    Article  CAS  Google Scholar 

  16. Wei, Y. et al. Steering hollow multishelled structures in photocatalysis: optimizing surface and mass transport. Adv. Mater. 32, 2002556 (2020).

    Article  CAS  Google Scholar 

  17. Wei, Y. et al. Heterogeneous hollow multi-shelled structures with amorphous-crystalline outer-shells for sequentially photoreduction of CO2. Angew. Chem. Int. Ed. 61, 202212049 (2022).

    Article  Google Scholar 

  18. Wei, Y. et al. Efficient sequential harvesting of solar light by heterogeneous hollow shells with hierarchical pores. Natl Sci. Rev. 7, 1638–1646 (2020).

    Article  CAS  Google Scholar 

  19. Zhao, D. et al. Sequential drug release via chemical diffusion and physical barriers enabled by hollow multishelled structures. Nat. Commun. 11, 4450 (2020).

    Article  CAS  Google Scholar 

  20. Xu, W. et al. Hollow multishelled structural TiN as multi-functional catalytic host for high-performance lithium-sulfur batteries. Nano Res. 16, 12745–12752 (2023).

    Article  CAS  Google Scholar 

  21. Salhabi, E. et al. Hollow multi-shelled structural TiO2-x with multiple spatial confinement for long-life lithium-sulfur batteries. Angew. Chem. Int. Ed. 58, 9078–9082 (2019).

    Article  CAS  Google Scholar 

  22. Zhu, Y. et al. V2O5 textile cathodes with high capacity and stability for flexible lithium-ion batteries. Adv. Mater. 32, 1906205 (2020).

    Article  CAS  Google Scholar 

  23. Ye, C. et al. The role of electrocatalytic materials for developing post-lithium metal||sulfur batteries. Nat. Commun. 15, 4797 (2024).

    Article  CAS  Google Scholar 

  24. Wang, Z. et al. Conductive CoOOH as carbon-free sulfur immobilizer to fabricate sulfur-based composite for lithium-sulfur battery. Adv. Funct. Mater. 29, 190105 (2019).

    Google Scholar 

  25. Yao, Y. et al. A dual-functional conductive framework embedded with TiN-VN heterostructures for highly efficient polysulfide and lithium regulation toward stable Li-S full batteries. Adv. Mater. 32, 1905658 (2019).

    Article  Google Scholar 

  26. Wang, Z. et al. Self-supported and flexible sulfur cathode enabled via synergistic confinement for high-energy-density lithium-sulfur batteries. Adv. Mater. 31, 1902228 (2019).

    Article  Google Scholar 

  27. Shen, Z. et al. Cation-doped ZnS catalysts for polysulfide conversion in lithium-sulfur batteries. Nat. Catal. 5, 555–563 (2022).

    Article  CAS  Google Scholar 

  28. Zhang, B. et al. Optimized catalytic WS2-WO3 heterostructure design for accelerated polysulfide conversion in lithium-sulfur batteries. Adv. Energy Mater. 10, 2000091 (2020).

    Article  CAS  Google Scholar 

  29. Zhang, H. et al. Long-life lithium-sulfur batteries with high areal capacity based on coaxial CNTs@TiN-TiO2 sponge. Nat. Commun. 12, 4738 (2021).

    Article  CAS  Google Scholar 

  30. Zuo, Z. et al. Emerging electrochemical energy applications of graphdiyne. Joule 3, 899–907 (2019).

    Article  Google Scholar 

  31. He, F. et al. Advances on theory and experiments of the energy applications in graphdiyne. CCS Chem. 5, 72–94 (2023).

    Article  CAS  Google Scholar 

  32. Zheng, X. et al. Two-dimensional carbon graphdiyne: advances in fundamental and application research. ACS Nano 17, 14309–14346 (2023).

    Article  CAS  Google Scholar 

  33. Mao, D. et al. Sequential templating approach: a groundbreaking strategy to create hollow multishelled structures. Adv. Mater. 31, 1802874 (2019).

    Article  Google Scholar 

  34. Mao, D. et al. Hollow multishelled structure: synthesis chemistry and application. Chem. Res. Chin. Univ. 40, 346–393 (2024).

    Article  CAS  Google Scholar 

  35. Qi, J. et al. Multi-shelled hollow micro-/nanostructures. Chem. Soc. Rev. 44, 6749–6773 (2015).

    Article  CAS  Google Scholar 

  36. Wang, J. et al. Hollow multishell structures exercise temporal-spatial ordering and dynamic smart behavior. Nat. Rev. Chem. 4, 159–168 (2020).

    Article  CAS  Google Scholar 

  37. Wang, J. et al. The development of hollow multishelled structure: from the innovation of synthetic method to the discovery of new characteristics. Sci. China Chem. 65, 7–19 (2022).

    Article  CAS  Google Scholar 

  38. Zhan, S. et al. Hollow multishelled structured graphdiyne realized radioactive water safe-discharging. Nano Today 47, 101626 (2022).

    Article  CAS  Google Scholar 

  39. Gao, X. et al. Ultrathin graphdiyne film on graphene through solution-phase van der Waals epitaxy. Sci. Adv. 4, eaat6378 (2018).

    Article  Google Scholar 

  40. Zhao, Y. et al. Few-layer graphdiyne doped with sp-hybridized nitrogen atoms at acetylenic sites for oxygen reduction electrocatalysis. Nat. Chem. 10, 924–931 (2018).

    Article  CAS  Google Scholar 

  41. Zhao, Y. et al. Stereodefined codoping of sp-N and S atoms in few-layer graphdiyne for oxygen evolution reaction. J. Am. Chem. Soc. 141, 7240–7244 (2019).

    Article  CAS  Google Scholar 

  42. Liu, B. et al. Revealing the mechanism of sp-N doping in graphdiyne for developing site-defined metal-free catalysts. Adv. Mater. 32, 2206450 (2022).

    Google Scholar 

  43. Zhao, Y. et al. Boosting hydrogen evolution reaction on few-layer graphdiyne by sp-N and B codoping. APL Mater. 9, 071102 (2021).

    Article  CAS  Google Scholar 

  44. Li, M. et al. Sp-hybridized nitrogen as new anchoring sites of iron single atoms to boost the oxygen reduction reaction. Angew. Chem. Int. Ed. 61, 202208238 (2022).

    Article  Google Scholar 

  45. Wu, R. et al. Hierarchically porous nitrogen-doped carbon as cathode for lithium-sulfur batteries. J. Energy Chem. 27, 1661–1667 (2018).

    Article  Google Scholar 

  46. Liu, S. et al. Crepe cake structured layered double hydroxide/sulfur/graphene as a positive electrode material for Li-S batteries. ACS Nano 14, 8220–8231 (2020).

    Article  CAS  Google Scholar 

  47. Li, Y. et al. Manipulating redox kinetics of sulfur species using Mott-Schottky electrocatalysts for advanced lithium-sulfur batteries. Nano Lett. 21, 6656–6663 (2021).

    Article  CAS  Google Scholar 

  48. Zou, K. et al. A highly efficient sulfur host enabled by nitrogen/oxygen dual-doped honeycomb-like carbon for advanced lithium-sulfur batteries. Small 18, 2107380 (2022).

    Article  CAS  Google Scholar 

  49. Xu, H. et al. Discarded cigarette filter-derived hierarchically porous carbon@graphene composites for lithium-sulfur batteries. J. Mater. Chem. A 7, 3558–3562 (2019).

    Article  CAS  Google Scholar 

  50. Gu, Z. et al. Synergistic effect of Co3Fe7 alloy and N-doped hollow carbon spheres with high activity and stability for high-performance lithium-sulfur batteries. Nano Energy 86, 106111 (2021).

    Article  CAS  Google Scholar 

  51. Du, Z. et al. Cobalt in nitrogen-doped graphene as single-atom catalyst for high-sulfur content lithium-sulfur batteries. J. Am. Chem. Soc. 141, 3977–3985 (2019).

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by the Natural Science Foundation of China (grant nos. 52025028 to L.L., 52372170 to R.Y., 92572205 to D.W., 52261160573 and 52301296 to J. Wang), the National Key R&D Program (grant nos. 2024YFA1509400 and 2022YFA1204500 to D.W., 2022YFA1504101 to J. Wang, 2021YFB2400300 to Z.L.), Shenzhen University 2035 Program for Excellent Research (grant no. 2024B005 to R.Y. and D.W.), the Zhongke-Yuneng Joint R&D Center Program (grant no. ZKYN2022008 to D.W.), Hebei Provincial Department of Science and Technology - Basic Research Cooperation Project of Beijing-Tianjin-Hebei Region (grant no. B2024204027 to R.Y.), the Beijing Natural Science Foundation (grant no. Z230019 to J. Wang) and the Institute of Process Engineering (IPE) Project for Frontier Basic Research grant no. QYJC-2022-008 to J. Wang. D.W. thanks the Financial Support for Outstanding scientific and technological innovation Talents Training Fund in Shenzhen. We thank Y. Li and H. Liu from Institute of Chemistry, Chinese Academy of Sciences, for their help with the HEB-TMS chemical. We thank H. Pang and Y. Su from Yangzhou University for their help with in situ UV–vis test. We thank K. Zhang and H. Zhu from Nankai University for their help with in situ FTIR test.

Author information

Authors and Affiliations

  1. State Key Laboratory of Intelligent Construction and Healthy Operation and Maintenance of Deep Underground Engineering, College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, China

    Ruyi Bi, Ranbo Yu & Dan Wang

  2. School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing, China

    Ruyi Bi & Ranbo Yu

  3. State Key Laboratory of Biopharmaceutical Preparation and Delivery, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, China

    Ruyi Bi, Jiangyan Wang, Jiawei Wan, Lijuan Zhang, Yasong Zhao & Dan Wang

  4. School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing, China

    Jiangyan Wang, Jiawei Wan, Lijuan Zhang & Dan Wang

  5. Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, China

    Mingzi Sun & Bolong Huang

  6. Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing, China

    Boquan Li

  7. Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, China

    Zheng Liang

  8. Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong University, Shanghai, China

    Zheng Liang

  9. School of Physical Science and Technology, Jiangsu Key Laboratory of Frontier Material Physics and Devices, Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou, China

    Liang Li

Authors
  1. Ruyi Bi
    View author publications

    Search author on:PubMed Google Scholar

  2. Jiangyan Wang
    View author publications

    Search author on:PubMed Google Scholar

  3. Jiawei Wan
    View author publications

    Search author on:PubMed Google Scholar

  4. Lijuan Zhang
    View author publications

    Search author on:PubMed Google Scholar

  5. Mingzi Sun
    View author publications

    Search author on:PubMed Google Scholar

  6. Bolong Huang
    View author publications

    Search author on:PubMed Google Scholar

  7. Boquan Li
    View author publications

    Search author on:PubMed Google Scholar

  8. Zheng Liang
    View author publications

    Search author on:PubMed Google Scholar

  9. Yasong Zhao
    View author publications

    Search author on:PubMed Google Scholar

  10. Liang Li
    View author publications

    Search author on:PubMed Google Scholar

  11. Ranbo Yu
    View author publications

    Search author on:PubMed Google Scholar

  12. Dan Wang
    View author publications

    Search author on:PubMed Google Scholar

Contributions

D.W. conceived the idea and supervised the research. R.Y. and J. Wang supervised the research. R.B. performed experiments and basic characterizations. D.W., R.Y., J. Wang, R.B., Z.L. and L.L. analysed and discussed the experimental data. J. Wan helped with the XANES experiments. L.Z., M.S. and B.H. carried out the DFT calculations. B.L. helped with the pouch-cell assembly and tests. Y.Z. helped with XPS experiments. R.B. and J. Wang drafted the manuscript. D.W., R.Y., Z.L. and L.L. revised and improved the manuscript. All authors read and approved the final manuscript.

Corresponding authors

Correspondence to Jiangyan Wang, Zheng Liang, Liang Li, Ranbo Yu or Dan Wang.

Ethics declarations

Competing interests

The authors declare no competing interests.

Peer review

Peer review information

Nature Sustainability thanks Shizhang Qiao and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

Additional information

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information (download PDF )

Supplementary Figs. 1–29, Tables 1–6, Data 1 and 2 and References.

Reporting Summary (download PDF )

Source data

Source Data Fig. 1 (download ZIP )

Statistical source data for Fig. 1c–h,j–l. Unprocessed source data for Fig. 1a,b,i.

Source Data Fig. 2 (download XLSX )

Statistical source data for Fig. 2.

Source Data Fig. 3 (download ZIP )

Statistical source data for Fig. 3. Unprocessed source data for Fig. 3a.

Source Data Fig. 4 (download ZIP )

Statistical source data for Fig. 4b,c. Unprocessed source data for Fig. 4a,b.

Source Data Fig. 5 (download ZIP )

Statistical source data for Fig. 5. Unprocessed source data for Fig. 5c.

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Bi, R., Wang, J., Wan, J. et al. Spatially coupled adsorption and catalysis for sustainable lithium–sulfur batteries. Nat Sustain (2026). https://doi.org/10.1038/s41893-026-01794-y

Download citation

  • Received:

  • Accepted:

  • Published:

  • Version of record:

  • DOI: https://doi.org/10.1038/s41893-026-01794-y

Search

Advanced search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing