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Common precursors for carbon materials typically include petroleum‐based polymers or MOF materials. However, these materials often encounter challenges such as metal aggregation, high cost, and metals leaching. In this work, a novel of approach lignin‐metal supramolecular framework complex (MSF@Lignin) is introduced. These complexes are formed through oxidative ammonolysis of lignin (OAL) to synthesize a nitrogen‐doped carbon‐encapsulated CoRu nanocatalyst (CoRu@OALC) via in situ carbonization. CoRu@OALC exhibited exceptional performance in both HER (90 mV) and OER (200 mV) at the current density of 10 mA cm−2, with an overall water splitting voltage of 1.5 V and outstanding stability under high density. During the pyrolysis process, metal became encapsulated by lignin‐derived carbon, occurring within the temperature range of 600–700 °C. In the catalytic process, active sites are primarily located within the defects in lignin‐derived carbon, showcasing a unique "self‐healing" phenomenon within the carbon layer. Oxygen‐containing intermediates (*OH, *O, and *OOH) facilitated the reconstruction of defects on the carbon layer, while the hydrogen‐containing intermediates (*H) contributed to the reappearance of a defect‐rich structure. [ABSTRACT FROM AUTHOR]

The utilization of plant polyphenols as catalyst carriers holds promise for environmentally friendly catalysis. However, challenges such as the inhomogeneous distribution of organic ligands often hinder their effectiveness. In this study, lignin–metal supramolecular framework were formed through ionic coordination self-assembly, achieved by oxidative ammonolysis modified lignin. The specific spatial domain-limiting effect of lignin–metal supramolecular framework ensures the dispersion and stability of catalyst active sites. Carbon-coated trimetallic catalysts (Ru–FeNi@OALC) derived from lignin–metal supramolecules exhibit promising performance, with low overpotentials for the oxygen evolution reaction (OER, η10 = 290 mV) and the hydrogen evolution reaction (HER, η10 = 52 mV), surpassing commercial noble metal catalysts. Additionally, these catalysts demonstrate long-lasting water-splitting performance, highlighting their potential for sustainable catalytic reactions. Molecular simulations and DFT theoretical calculations elucidate the feasibility of lignin oxidative ammonolysis modification and reveal the coordination mechanism. Furthermore, the abundant defects and disorder in the coordination polymer-derived carbon materials optimize electron transfer processes and accelerate reaction kinetics. This construction strategy towards designable polyphenol–metal supramolecular framework presents a promising avenue for the green synthesis of a variety of metal/carbon composite catalysts, contributing to sustainable catalysis and environmental protection. [ABSTRACT FROM AUTHOR]

Rechargeable sodium‐ion batteries usually suffer from accelerated electrode destruction at high temperatures and high synthesis costs of electrode materials. Therefore, it is highly desirable to explore novel organic electrodes considering their cost‐effectiveness and large adaptability to volume changes. Herein, natural biomass, pristine lignin, is employed as the sodium‐ion battery anodes, and their sodium storage performance is investigated at room temperature and 60 °C. The lignin anodes exhibit excellent high‐temperature sodium‐ion battery performance. This mainly results from the generation of abundant reactive sites (C=O) due to the high temperature‐induced homogeneous cleavage of the Cβ–O bond in the lignin macromolecule. This work can inspire researchers to explore other natural organic materials for large‐scale applications and high‐value utilization in advanced energy storage devices. [ABSTRACT FROM AUTHOR]

The development of inexpensive and robust bifunctional electrocatalysts for hydrogen evolution reactions (HER) and oxygen evolution reactions (OER) was crucial for renewable energy systems. Herein, a novel strategy for preparing CoNiRu alloy nano‐electrocatalyst capsulated by nitrogen‐doped biochar (CoNiRu@NLC) using carboxymethylated lignin macromolecules was proposed. CoNiRu@NLC exhibited excellent HER and OER performance, and the overall water splitting voltage was only 1.47 V at 10 mA/cm2 with excellent catalytic stability, which was superior to the noble metal catalysts Pt/C ‖ RuO2. Theoretical calculations confirmed the strong electron interaction between CoNiRu alloy and carbon layer, and XPS patterns proved that the electrons transfer from Ru to CoNi, significantly boosted the electrocatalytic activity. This study demonstrated the importance of lignin‐driven alloying on enhancing catalytic performance and provided a concept for the development of high‐efficiency catalysts and high‐value utilization of polyphenol biomass. [ABSTRACT FROM AUTHOR]