Phenolate-Mediated Structural Evolution of Lignin toward Hard Carbon Anodes for Sodium-Ion Batteries

Abstract

Hard carbon (HC) anodes are typically described in terms of their final structure. However, this structure is influenced by multiple competing factors, and precursor-level chemical interactions can play an important role in directing its eventual evolution. Here, metal coordination is used to direct lignin precursor organization and control the evolution of lignin-derived HCs. Magnesium gluconate (MgGlu2) introduced into alkaline lignin promotes selective Mg2+ coordination with oxygen-containing functional groups, enabling reorganization of the lignin network prior to carbonization. Density functional theory (DFT) calculations show a thermodynamic preference of Mg2+ for phenolate (Ph–)-rich environments over gluconate ligands and β–O–4 linkages, consistent with the formation of cross-linked precursor configurations. This coordination is preserved during freeze-drying and translates into a distinct carbon microstructure upon pyrolysis. The resulting carbon exhibits a more accessible pore structure and improved cycling stability, retaining 93.6% of its post-solid electrolyte interphase (SEI) capacity after 400 cycles, compared to 8.7% for the pristine counterpart. These results demonstrate that phenolate-directed Mg2+ coordination governs precursor organization and contributes to the structural stability of lignin-derived HCs. More broadly, this work establishes precursor-level coordination as a route to control structure–performance relationships in HC anodes.

Solvation-mediated electrostatic shielding of Li anodes by Na+ for durable lithium–oxygen batteries
Zhuo Yang, Yichao Cai, Shuo Xu +2
Chemical science4 Nov 2026Peer-reviewedCC BYFull textOrganic chemistryEurope PMC
Cross-Dataset Assessment of Electrical Loading, Thermal-Domain Evolution, and Abuse-Domain Separation in UAV-Relevant Lithium-Ion Batteries
Yuanzhe Li, Ningning Wei, Minghai Li +1
Batteries27 Oct 2026Peer-reviewedCC BY 4.0Electrochemistry & energyCrossref
Cellulose Coating Altered the Electro-Chemo-Mechanical Evolution of Sodium Thioantimonate Electrolyte in Solid-state Sodium Batteries: An Operando Raman Study
Geng Xie, Xuehai Tan, Shu Dong +3
ChemRxiv21 Oct 2026PreprintCC BYFull textGeneral chemistryChemRxiv
Operando Cross-Sectional Nanoscale Imaging of Na Anode Formation in Zero-Excess Solid-State Batteries: Coupled Phase–Stress Evolution and X-ray Beam Effects
Henrik Rotvær Bratlie, Verena Reisecker, François Lienard +6
ChemRxiv8 Sep 2026PreprintCC BYFull textGeneral chemistryChemRxiv
Fast State-of-Health Estimation of Lithium-Ion Batteries Using Short-Term Relaxation-Voltage Features Integrated with a Differential Evolution-Optimized Extreme Learning Machine Algorithm
Zeyang Liu, Xiankui Wen, Qingxu Guo +3
Batteries5 Nov 2026Peer-reviewedCC BY 4.0Electrochemistry & energyCrossref

Cite

BibTeX RIS

BibTeX

@article{robinos2026phenolatemediated,
  title = {{Phenolate-Mediated Structural Evolution of Lignin toward Hard Carbon Anodes for Sodium-Ion Batteries}},
  author = {Angelo Robiños and Ville Yrjänä and Jerwin Jay Taping and Hao Zhang and Najeeb ur Rehman Lashari and Inge Schlapp-Hackl and Jan-Henrik Smått and Chunlin Xu and Johan Bobacka},
  journal = {ACS Omega},
  year = {2026},
  month = nov,
  doi = {10.1021/acsomega.6c06946},
  url = {https://pubs.acs.org/acsodf/article/doi/10.1021/acsomega.6c06946/5463992/Phenolate-Mediated-Structural-Evolution-of-Lignin},
  note = {CC BY 4.0},
}

RIS

TY  - JOUR
TI  - Phenolate-Mediated Structural Evolution of Lignin toward Hard Carbon Anodes for Sodium-Ion Batteries
AU  - Angelo Robiños
AU  - Ville Yrjänä
AU  - Jerwin Jay Taping
AU  - Hao Zhang
AU  - Najeeb ur Rehman Lashari
AU  - Inge Schlapp-Hackl
AU  - Jan-Henrik Smått
AU  - Chunlin Xu
AU  - Johan Bobacka
PY  - 2026
DA  - 2026/11/04
JO  - ACS Omega
DO  - 10.1021/acsomega.6c06946
UR  - https://pubs.acs.org/acsodf/article/doi/10.1021/acsomega.6c06946/5463992/Phenolate-Mediated-Structural-Evolution-of-Lignin
AB  - Hard carbon (HC) anodes are typically described in terms of their final structure. However, this structure is influenced by multiple competing factors, and precursor-level chemical interactions can play an important role in directing its eventual evolution. Here, metal coordination is used to direct lignin precursor organization and control the evolution of lignin-derived HCs. Magnesium gluconate (MgGlu2) introduced into alkaline lignin promotes selective Mg2+ coordination with oxygen-containing functional groups, enabling reorganization of the lignin network prior to carbonization. Density functional theory (DFT) calculations show a thermodynamic preference of Mg2+ for phenolate (Ph–)-rich environments over gluconate ligands and β–O–4 linkages, consistent with the formation of cross-linked precursor configurations. This coordination is preserved during freeze-drying and translates into a distinct carbon microstructure upon pyrolysis. The resulting carbon exhibits a more accessible pore structure and improved cycling stability, retaining 93.6% of its post-solid electrolyte interphase (SEI) capacity after 400 cycles, compared to 8.7% for the pristine counterpart. These results demonstrate that phenolate-directed Mg2+ coordination governs precursor organization and contributes to the structural stability of lignin-derived HCs. More broadly, this work establishes precursor-level coordination as a route to control structure–performance relationships in HC anodes.
SN  - 2470-1343
ER  -

Abstract

Related

Cite