Lignin-derived hard carbon is considered a promising anode material for sodium-ion batteries due to its low cost and high carbon content. However, severe π-π stacking of carbon layers and insufficient closed pore content limit its sodium storage performance. Herein, we propose a molecular engineering strategy involving the selective conversion of aliphatic OH in alkali lignin into side-chain acetyl groups to precisely regulate the pyrolysis behavior of alkali lignin. This modification can delay the excessive decomposition of functional groups at low temperatures, thereby alleviating the structural densification of carbon layers resulting from severe π-π stacking during high-temperature carbonization. Moreover, the cleavage of side-chain acetyl during pyrolysis triggers a pronounced self-activation effect, yielding a microporous carbon intermediate with an ultrahigh microporosity of 97.04 %. The resulting HC features wide interlayer spacing, short and thin carbon layers, and abundant closed pores (0.193 cm3/g), which collectively reduce diffusion resistance and shorten the transport path of sodium ions in the low-potential region. Consequently, the optimized HC anode achieves a reversible specific capacity of 347.6 mAh/g with an ICE of 81.2 %, maintaining a remarkable rate performance of 229.5 mAh/g even at 2 A/g. This work offers important insights for the precise structural control of HC.

Depolymerizing lignin is one of the most effective approaches for its high-valued utilization. However, the high oxygen contents in lignin depolymerized products cause the low calorific value, and hence limit their application in liquid fuels. A high efficiency 0.5 wt% Pd/WOx-ZrO2 catalyst was designed and applied in the process for the depolymerization of lignin in this work. The effect of preparation methodology of catalyst support, the molar ratio of W to Zr, and Pd loading on both the structure of catalyst and catalytic activity to lignin depolymerization were investigated. It was found that the catalyst prepared by hydrothermal method exhibited a large specific surface area, more uniform distribution of supported Pd, as well as higher acid content and oxygen vacancies, which contributed a good catalytic activity. Moreover, the lower Pd loading and higher dispersion of Pd particles were beneficial for hindering the decrease in the specific surface area of the WOx-ZrO2 support, and hence increasing the acidic sites of the catalyst, which also promoted both the cleavage of C-O bonds in lignin subunits and the alkylation of depolymerized products. When the catalyst prepared with 1:1 of W/Zr molar ratio and 0.5 wt% of Pd loading contributed to higher yields of bio-oil and aromatic monomers, achieving 83.30% and 35.49%, respectively. Among the aromatic monomers, 87.86% were demethoxylated alkylphenols, which significantly reduced the oxygen content of the depolymerization products.

Cost-effective sodium-ion battery technologies require low-cost, high-performance hard carbon anode materials. Therefore, the employment of sustainable lignocellulose as a precursor offers economic benefits. Herein, an insitu sacrificing templating strategy is proposed, and hard carbon anode materials with high closed-pore volumes are successfully synthesized using lignin as the sustainable precursor. The closed-pore structure and microscopic crystalline structures of hard carbon are regulated through the adsorption of zinc ions by the abundant oxygen containing functional groups in pristine lignin molecules, followed by the in-situ generation of ZnO nanoparticles as sacrificial templates during carbonization. Results demonstrate that the ZnO templates significantly enhance the closed-pore volume (0.258 cm3 g-1) and expand the interlayer spacing (0.374 nm). The optimized hard carbon material (HC-Z-1600) exhibits a high reversible specific capacity of 358 mAh g-1 at 0.05 A g-1. Through combined in-situ Raman spectroscopy and electrode kinetic analyses, the progressive sodium-ion storage mechanism is demonstrated as a mechanism of "surface adsorption, interlayer intercalation, closed-pore filling". This study provides an innovative strategy for the controlled synthesis of sustainable biomass-derived hard carbon materials for high-performance sodium-ion batteries.

Technical lignin valorization is fundamentally limited by the scarcity and kinetic inertia of cleavable C & horbar;O linkages in a condensed C & horbar;C/C & horbar;O network, constraining the production of aromatic monomers and other fuel-relevant intermediates. Here, we report a coordination-engineered Ni-Pd on lignin-derived Carbon (NiPd0.1/C) constructed via solvent/antisolvent assembly to enable trace Pd incorporation that electronically modulates Ni. Structural analyses suggest a uniform solid solution with interfacial charge redistribution (Ni delta+-Pd delta-), which generates polarized interfacial sites and strengthens C & horbar;O bond activation. The NiPd0.1/C boosts aromatic monomer yield from enzymatic hydrolysis lignin to 23 wt.%, outperforming commercial Pd/C (similar to 16 wt.%). Product analysis shows syringyl/guaiacyl/p-hydroxyphenyl (S/G/H)phenolics dominated by G-type units, and the catalyst remains effective for more condensed alkali lignin (similar to 16 wt.% monomers), underscoring feedstock tolerance. Model-compound and kinetic studies indicate that Ni-Pd alloying accelerates the turnover of phenoxy intermediates by lowering the apparent barrier for dehydrogenation and subsequent ether C & horbar;O bond cleavage, thereby enabling the selective cleavage of C & horbar;O bonds. This work establishes solid-solution electronic engineering as a broadly generalizable strategy to unlock cost-effective C & horbar;O activation and accelerate lignin valorization toward scalable, low-carbon aviation fuel precursors.

Biomass-based aerogels derived from polysaccharides and proteins have attracted considerable interest because of their environmental compatibility, cost-effectiveness, and inherent biodegradability. However, their carbon- and hydrogen-rich chemical structures render them intrinsically flammable, necessitating effective flame-retardant modification to satisfy stringent fire-safety requirements. Herein, an eco-sustainable strategy is reported for constructing biomass-derived composite aerogels that simultaneously integrate high mechanical strength, efficient thermal insulation, and enhanced fire safety. High-strength flame-retardant aerogels were fabricated from sodium alginate (SA), sodium lignosulphonate (LS), and hydroxyapatite (HAP) through a glucono-δ-lactone (GDL)-regulated in situ ion-release strategy. The gradual hydrolysis of GDL induces controlled acidification of the precursor system, promoting the sustained release of Ca2+ from HAP and the homogeneous ionic cross-linking of SA chains into a stable three-dimensional “egg-box” network. The mechanically optimized SL3H0.6G0.8 aerogel achieved the highest compressive modulus of 9.32 MPa, corresponding to approximately 13 times that of pristine SA aerogel (0.69 MPa). In contrast, SL3H0.9G0.8 exhibited the most balanced overall performance, retaining a lightweight porous structure and a low axial thermal conductivity of 0.04553 W m−1 K−1 while delivering superior thermal stability, flame retardancy, and smoke-suppression capability. The enhanced fire resistance originates predominantly from a synergistic condensed-phase mechanism involving LS-derived carbonaceous char formation, phosphate-assisted dehydration and carbonisation, and reinforcement by thermally stable calcium/phosphate-rich inorganic residues. The resulting organic-inorganic protective layer effectively suppresses heat transfer, volatile release, and smoke evolution during combustion. Consequently, SL3H0.9G0.8 achieved a UL-94 V-0 rating and a limiting oxygen index of 37.5%, together with a peak heat release rate of 104.56 W g−1 and a total smoke production of 0.23 m2. This work establishes a sustainable route for the green fabrication of mechanically robust, thermally insulating, and fire-safe biomass-based aerogels, offering considerable potential for energy-efficient building applications.

The strategy of coating porous carbon offers a promising pathway for constructing closed-pore architectures in hard carbon (HC) anodes. However, the coating efficiency is strongly governed by the pyrolysis behavior of the coating agent. Conventional pyrolytic treatment of glucose produces substantial volatile by-products, leading to severe mass loss and necessitating glucose dosages exceeding twice the mass of PC to achieve effective coating, which limits practical applicability. In this study, a hydrothermal carbon-coating strategy is proposed to address this challenge. During hydrothermal pretreatment, glucose molecules diffuse into the surface and pore channels of PC, where they undergo in situ polymerization to form polyfuran-derived carbon coatings. This transformation markedly mitigates mass loss during subsequent carbonization, enabling effective coating using glucose and PC at a 1 : 1 mass ratio. Moreover, the carbon formed within the pore network generates internal diffusion channels that accelerate Na+ transport and facilitate electrochemical storage. The resulting HC exhibits a high reversible capacity of 323 mAh g-1 at 0.05 A g-1, and maintains 175 mAh g-1 at 5 A g-1, demonstrating both enhanced capacity and superior rate performance. This work provides an efficient and scalable strategy for coating engineering in biomass-derived HC, offering valuable insights for the development of high-performance sodium-ion battery anodes.

Understanding the structural formation mechanism of hard carbon and the relationship between its microstructure and sodium-ion storage performance is critical for the precise fabrication of hard carbon. Herein, lignin-derived hard carbons with tunable microstructures were prepared via one-step carbonization by tuning carbonization temperatures (600 degrees C-1600 degrees C) and time (0-6 h). The graphitic microcrystalline structures in hard carbons become more ordered with increasing carbonization temperature and time, which in turn leads to the reduced interlayer spacing of graphene layers, decreased defect concentration, and increased size and volume of the closed pores. The pseudo-graphitic structures with expanded interlayer spacing and abundant defect structures contribute to enhanced slope-potential capacity, whereas the sodium-ion accessible closed pores with large pore volume contribute to improved plateau-potential capacity. A small closed-pore size is beneficial for enhancing the rate performance. The hard carbons displayed an adsorption/intercalation-dominated to a pore-filling-dominated mechanism with increasing carbonization temperature and time. The optimized hard carbon exhibited a high reversible capacity (322 mAh g-1 at 0.05 A g-1) with a plateau-potential capacity of 246 mAh g-1, and good rate performance. These findings provide fundamental insights for the structural revolution and sodium-ion storage mechanism of hard carbon anodes, which could pave the way for understanding how the structure evolves and how we precisely design high-performance hard carbon anodes.

Next-generation 5G/6G communication and high-density electronics intensifies electromagnetic interference, driving demand for thin, broadband, lightweight, low-cost, and scalable EM absorbers. Carbon-fiber absorbers often exhibit an overly strong dielectric response that causes impedance mismatch, while magnetic fillers aggregate and form weak interfaces, limiting coordinated dielectric-magnetic loss. Here we integrate electrospinning, pre-oxidation, and carbonization to fabricate magnetic lignin-based carbon fibers (Fe2CuO4/LCF). Multifunctional lignin groups coordinate and anchor Fe(acac)3 and Cu(acac)2, enabling molecular-level dispersion and confined solidification, followed by uniform in situ formation of spinel Fe2CuO4 nanoparticles. The material retains a continuous 3D fibrous network with tight nano-carbon coupling and Cu-O-C interfacial bonding. Fe-Cu electronic coupling further enhances attenuation and matching robustly. It exhibits a minimum reflection loss (RLmin) of -47.6 dB at 2.3 mm, with an effective absorption bandwidth (EAB) of 12.27 GHz, and a matching thickness of 1.3 mm across the 10-18 GHz frequency range. Defects, nano-graphitic domains, heterogeneous interfaces, conduction loss, multiple scattering, and Fe2CuO4 magnetic loss synergistically enable thin-layer broadband absorption.

ABSTRACT Electro‐oxidative lignin depolymerization is considered a promising route to renewable aromatics; however, its selectivity is often limited by competition with oxygen evolution and uncontrolled overoxidation at the anode. A CuO/Cu 0.92 Co 2.08 O 4 hetero structured catalyst was developed, with which 88% conversion of 2‐phenoxy‐1‐phenylethanol was achieved, affording benzaldehyde and phenol in 53% and 27% yields, respectively. By means of time‐resolved analysis and intermediate‐feeding experiments, a tandem pathway involving benzylic oxidation to 2‐phenoxyacetophenone followed by C α ‐C β scission was identified. In situ Raman and FTIR spectroscopy, together with EPR, revealed that the Cu─Co interface suppresses the accumulation of OER‐type CoOOH species while promoting oxygen‐centered radical chemistry under reaction conditions. Through density functional theory, it was further shown that interfacial electronic modulation strengthens substrate adsorption and lowers the barrier for bond cleavage. The same mechanistic logic was extended from the model substrate to enzymatic hydrolysis lignin, for which characteristic interunit linkages are weakened while aromatic products are retained. These findings establish interfacial control of anodic radical chemistry as a strategy for selective lignin bond editing under electrochemical conditions.

Biomass-derived hard carbon materials have broad prospects as the anodes of commercial sodium-ion batteries (SIBs) due to their advantages of low cost, renewability, and abundant resources. However, the practical application of hard carbons in SIBs is limited by their inferior rate capabilities. In this work, the rate capabilities of lignin-derived hard carbon were improved by a strategy of pre-oxidizing the lignin precursor. The lignin was slightly oxidized by hydrogen peroxide under acidic conditions. The carbonyl groups were introduced into the side chains of the structural units of lignins. The carbonyl group hindered the connection of carbocations during the assembly process of the carbon chain. The appropriate length of the carbon chain (3.3 nm) and size of closed pores (1.62 nm) were formed by the growth of the carbon chain. The closed pores with small sizes enable the hard carbon to possess a great rate capability of the plateau-potential range. The closed pores with small pore sizes enable the sodium clusters to be filled rapidly.Thus, the sodium-ion storage in the plateau-potential region exhibits excellent rate capability. The retention of plateau capacity was still as high as 59.4 % at the current density of 5.0 A g- 1, which exhibited a greater improvement than the hard carbon with big-sized closed pores. The excellent rate capability shows the tremendous potential for the oxidation of precursors in preparing fastcharging hard carbon materials.

High-voltage cathodes improve the energy density of lithium metal batteries (LMBs). However, cathodes constructed by high-nickel layered oxide severely suffer from structural degradation and interfacial instability under high-voltage condition. Herein, an alkali lignin cross-linked acrylonitrile and acrylic acid copolymer is developed as 3D cathode binder (PNAL), which effectively scavenges oxygen radicals generated under high-voltage, suppresses the irreversible dissolution of transition metal ions, and stabilizes both the electrode-electrolyte interface and the cathode structure. As a result, the PNAL-based LiNi0.8Mn0.1Co0.1O2 LMB achieve a high-capacity retention of 75.7% after 300 cycles at 4.6 V under 3C. Furthermore, an Ah-scale pouch cell fabricated by PNAL delivers an energy density of 376.5 Wh kg-1 and retains 81.7% capacity after 100 cycles at 4.6 V. This work provides a promising binder strategy to construct high-voltage cathodes for next-generation LMBs.

Eco-friendly and intelligent elastomer materials with strain-adaptive stiffening and thermo-adjustable modulus are promising for safe tire applications, yet their preparation remains challenging. Herein, inspired by the lignin role in bridging cellulose and hemicellulose in plants and the self-strengthening of skeletal muscles by physical exercise, high performance eco-friendly and intelligent elastomer composite is prepared by rearrangement of interfacial hydrogen bonds via a repetitive mechanical training process. Biomass lignin is incorporated as a bridging agent for the construction of interfacial hydrogen bonds between silica filler and bromobutyl rubber matrix. The incorporation of lignin decreases 40% usage of silane coupling agent, 25% usage of silica for elastomer biocomposite. After mechanical training, the ordered hydrogen bond networks are formed among fillers, which endow the elastomer biocomposite with excellent strain-adaptive stiffening performance (elastic modulus increasing from 1.0 MPa to 24.7 MPa during deformation) and thermally tunable modulus (reversible variations between 2.0 MPa and 3.2 MPa). In this work, we show a facile strategy for the fabrication of eco-friendly intelligent elastomer biocomposite using easily available green raw materials.

Sustainable and green materials are demanded for flexible electronics while the conventional hydrogel and organogel systems face dual challenges of environmental vulnerability such as dehydration and liquid leakage and limited multifunctionality. Here, a biomass-based ionogel with covalent-physical dual crosslinking networks by integrating lignin, poly(thioctic acid) (PTA), and a halometallate ionic liquid is reported. The optimized ionogel presents exceptional mechanical properties (75 kPa strength, 1230% elongation at break) and near infrared (NIR)-accelerated self-healing function benefiting from lignin's photothermal properties. Enabled by a decent conductivity (0.026 S/m), the ionogel manifest multi-stimuli sensing abilities, including strain, heat, and NIR light through distinct electrical signals including resistance and current changes. As a versatile multi-modal flexible sensor, it demonstrates robust human motion monitoring and accurate stimulus recognition of combined stimuli. This work advances high-value utilization of lignin and provides a green and practical strategy for fabricating multifunctional flexible sensors.

The hard carbon anode material for sodium-ion batteries consists of curved graphene sheets and cross-linked structures with abundant sp3-hybridized carbon. These randomly stacked graphene sheets form numerous closed pores. Both these closed pores and the randomly stacked graphene sheets provide abundant sodium-ion storage sites. To further enhance the sodium-ion storage performance of hard carbon, it is essential to rationally design the precursor structure of hard carbon. These precursors should endow hard carbon with larger interlayer spacing and more closed-pore structures. Alkali lignin (AL), with its high carbon content and innate 3D network molecular structure, is considered one of the most promising biomass precursors for hard carbon. However, the aggregate structure in lignin hinders the fabrication of hard carbons with large interlayer spacing and a closed-pore-rich structure during carbonization. In this study, polyaniline (PANI) was combined with AL through intermolecular interactions to form lignin-polyaniline composite (AL/PANI) as a precursor. This composite was then subjected to one-step high-temperature carbonization to prepare a lignin-polyaniline-derived hard carbon (LPHC). PANI decomposes and disrupts the inherent aromatic aggregate structure of the lignin macromolecules. Ultimately, this process results in the formation of hard carbon with a rich closed-pore structure and enlarged interlayer spacing after carbonization. LPHC delivers a high specific capacity of 360 mAh g-1 at a current density of 0.1 A g-1, with a plateau-potential capacity as high as 250 mAh g-1. This work proposes a strategy of utilizing guest molecules to regulate the composite structure of lignin via structure engineering, thereby tailoring the microstructure of lignin-derived hard carbon materials.

Silicon anodes are known for their high theoretical specific capacity, which can reach up to 4200 mAh·g-1. However, their practical application in lithium-ion batteries is limited by severe volume expansion (300–400%) during charge and discharge cycles. This expansion causes mechanical instability and degradation of the anode material over time. As an alternative to pure silicon, silicon monoxide (SiO) significantly reduces volume expansion to approximately 200%, making it a more viable option for battery anodes. Among the various anode components, the binder plays a crucial role in mitigating the expansion of active materials during cycling. Therefore, developing effective binders that maintain electrode integrity while minimizing volume changes has become a critical factor limiting the broader adoption of silicon-based anodes in lithium-ion batteries. To address this challenge, sulfonated lignin (SL) is employed as a three-dimensional (3D) framework to facilitate the creation of an aqueous composite binder. Through thermal esterification and the introduction of ionic bonds, a high-strength, 3D crosslinked network is formed, overcoming the complexities of processing and reducing the high toxicity often associated with organic solvents in conventional binders. The resulting PSZ-150 binder, featuring 3D network with synergistic covalent-ionic crosslinking, exhibits exceptional bonding strength (4.00 N) and excellent electrochemical performance, maintaining a specific capacity of 1045.30 mAh·g-1 after 250 cycles at a current density of 0.2 A·g-1. Additionally, the rate performance of the SiO electrode is significantly enhanced, underscoring the potential of this binder system for designing high-energy-density silicon-based anodes.

Lignin is second abundant component in lignocellulose which acts as a natural binder in plant cell wall. Since the utilization of phenolic and urea-formaldehyde as wood adhesive in furniture continuously releasing toxic formaldehyde gas and damaging people's health, using natural lignin as wood adhesive performs significant advantages. However, harsh reaction conditions are generally used in lignin extraction from lignocellulose to overcome the dense structure, which causes lignin structural condensation and reduces its adhesive activity. To address this issue, we employed a novel lithium bromide (LiBr) molten salt hydrate (MSH) acidified with citric acid to facilitate the rapid dissolution and hydrolysis of cellulose and hemicellulose with conversion rates of 95.7% and 98.6%, respectively, with less-condensed lignin of a purity of 95.7% isolated in solid part at mild condition at 100 degrees C for 60 min. The obtained lignin can be directly blended with water and used as a plywood adhesive without the addition of any other chemicals addition, demonstrating the dry strength of plywood reached 1.19 MPa, surpassing the industry standard at 0.7 MPa, highlighting the practical viability of the obtained lignin in adhesive applications.

Lignin, the most abundant aromatic polymer in nature, holds immense potential for sustainable chemical production. Deciphering lignin dissolution behavior is essential for suitable solvent selection and achieving efficient conversion. However, the high heterogeneity of lignin and the complex interaction between lignin and solvents increase the difficulty in understanding dissolution behavior. To address this issue, in this work, an intermolecular force quantification method was proposed to establish the correlation between microscopic adhesion force and macroscopic solubility using atomic force microscopy (AFM). By engineering a stable lignin-coated AFM probe/substrate system (thickness >100 nm) via electrostatic adsorption, a precise lignin adhesion force quantification system was successfully established. As adhesion forces decreased from 0.106 to 0.026 mN/m, the lignin solubility surged from 0.06 to 168.49 g/L, indicating a strong relevance. Therefore, the lignin solubility can be readily evaluated via adhesion force quantification. Strikingly, a universal critical adhesion force (0.43 mN/m) across diverse lignin types (enzymatic hydrolysis lignin; alkaline lignin) and solvent systems (gamma-valerolactone (GVL)/H2O, dioxane/H2O, acetone/H2O) has been identified, beyond which negligible dissolution occurs. This constant serves as a quantitative '' dissolution threshold '', offering a rapid tool to screen optimal solvents. This work bridges intermolecular force quantification with solubility prediction, advancing rational solvent design for lignin valorization.

Aldehyde oxidation-coupled hydrogen production can markedly reduce the energy demand of electrolysis while enabling hydrogen generation and collection from two compartments. However, high-current-density operation relies on catalysts that sustain fast kinetics and high selectivity under strong interfacial gradients. Electro-oxidized lignin is employed to construct a lignin-metal supramolecular framework composite, which upon carbonization yields RuNi@NOLC, a Ni-enriched RuNi alloy confined within an oxygen-enriched, nitrogen-doped lignin-derived carbon (NOLC) microenvironment. In a membrane-free flow electrolyzer using RuNi@NOLC as both cathode and anode catalysts, the coupled process achieves a specific energy consumption of 0.76 kWh Nm-3 H2, a formate Faradaic efficiency of 99.5%, and an apparent hydrogen Faradaic efficiency of 199.6% arising from dual-compartment hydrogen generation and collection. The NOLC microenvironment provides Donnan hydration with a hydration-funnel effect, enabling directional enrichment of H2O together with OH- at N-containing sites and stabilization of the transition configuration for water splitting, thereby markedly accelerating the Ni-centered Volmer step as the rate-determining process and establishing a 3-fold synergy of Ni-centered water activation, Ru-mediated hydrogen release, and NOLC-directed transport of water and hydroxide. Under formaldehyde oxidation bias, Ru-OH and RuOxH species dominate low-potential initiation. Assisted by neighboring Ni-OHads, these Ru-centered oxygenated species drive intermediates toward OCHO formation and formate production, while alloy electronic effects mitigate poisoning by strongly adsorbed intermediates before transport limitations prevail at higher potentials. This work converts the coordination-chemistry programmability of lignin into quantifiable interfacial-solvation advantages, providing a clear paradigm for understanding and designing microenvironment-dominated mechanisms in paired electrolysis.

Lignin, the most abundant aromatic biopolymer in nature, holds great promise for carbon-neutral materials development yet is limited by its inherent dark color and poor solvent stability. Transforming it into uniform lignin colloidal spheres (LCSs) with ordered arrays enables specific visible light reflection and thus presents tunable colors. However, industrial lignin-derived LCSs via self-assembly typically exhibit broad size distribution and poor solvent resistance. To address these challenges, we proposed a novel strategy combining solvent fractionation and surface covalent polymerization. Acetone/water fractionation effectively reduced lignin heterogeneity, narrowing LCSs size distribution. Bisphenol A diglycidyl ether (BADGE) was used as cross-linker to covalently polymerize hydroxyl groups, inhibiting LCSs dissolution. Two hybrid LCSs were fabricated: hy-LCSs via co-self-assembly of lignin and BADGE and hy@LCSs through subsequent surface cross-linking. Hy-LCSs20 (20 wt% BADGE) shows stability in pH 12 alkali and acetone/water, while hy@LCSs70 exhibited unprecedented alkaline resistance up to pH 14, far exceeding the highest reported value of pH 12 for lignin colloidal spheres to date. Critically, BADGE incorporation preserved monodispersity of both hy-LCSs20 and hy@LCSs70, enabling precise size control without compromising uniformity. After centrifugation to form ordered structures, both hy-LCSs20 and hy@LCSs70 reflect specific wavelengths with tunable colors, overcoming key barriers in lignin valorization.

Oxygen (O)/nitrogen (N) codoped porous carbons are promising electrode materials for supercapacitors. The simultaneous construction of the O/N functionalized sites and efficient porous structure remains challenging. Herein, a novel in situ gas exfoliation chemistry engineering, including self-assembly synthesis and NaNO3/CaC2O4 activation, is designed to construct an O/N functionalized lignosulfonate sodium (LS)-derived porous carbon nanosheet framework. Ca2+ ions first coordinate with -SO3/-OH groups to disperse LS, and then partially combine with C2O42- ions to form elliptical CaC2O4@LS. NaNO3 is precipitated within CaC2O4@LS to form uniformly mixed precursor. The uniform mixing enhances NaNO3 and CaC2O4 activation to construct a porous carbon nanosheet framework (LPCA-Ca-Na) with 0.7-0.9 and 1-2 nm micropores, 8-200 nm meso-macropores, and high C═O (6.0 at. %) and edge N (6.3 at. %) contents. LPCA-Ca-Na delivers a high capacitance of 369 F g-1 at 0.5 A g-1, good rate capability, and outstanding cycling stability, due to the high micropore volume and high C═O and edge N contents providing sufficient adsorption sites and meso-macropores accelerating kinetics. The symmetric supercapacitor achieves a high energy density of 17 Wh kg-1 at 238 W kg-1 and excellent temperature adaptability. This work demonstrates a sustainable strategy for the efficient preparation of O/N-doped lignin-derived porous carbons for supercapacitors.