Optimization of Interfacial Electrons and Compressive‐Tensile Strains at Lignin‐Derived Carbon‐Supported Multiphase Ni/Cu/MoO2 Interfaces for Boosting Large Current‐Density HER

Abstract Developing efficient pH‐universal hydrogen evolution electrocatalysts is critically needed yet challenged by pH‐dependent. Here, a lignin‐derived carbon‐supported Ni/Cu/MoO 2 heterostructure (Ni/Cu/MoO 2 @LC) through multiphase interfaces design is engineered, which displays excellent electrochemical activity, featuring low potentials of −14.4/−201.5 (acidic), −44.5/−615.7 (neutral), and −28.2/−242.3 mV (alkaline) at −10/−1000 mA cm −2 . Theoretical and experimental analysis show that the Ni/Cu/MoO 2 @LC multiphase interfaces produce a synergistic coupling of compressive‐tensile strains and interfacial electron transfer effect. This synergistic effect triggers electron redistribution, tailors the electronic configuration through d ‐band center optimization, and balances intermediate adsorption/desorption energetics. Additionally, lignin‐derived carbon self‐supported micro‐nano‐array structure enhances gas‐liquid transport and corrosion resistance, allowing Ni/Cu/MoO 2 @LC to operate stably for at least 120 h, at −500 mA cm −2 in various pH solutions. Thus, this study provides a new idea for the design of cost‐effective pH‐universal HER electrocatalysts and a new approach for applying lignin‐derived carbon in electrocatalysis.