Synergistic Pre-Oxidation and CVD Engineering for Precise Closed-Pore Construction in Coffee Grounds-Derived Hard...

Upcycling biomass waste into value-added battery materials is crucial for sustainable energy storage. Here, we transform coffee grounds into high-performance hard carbon (HC) anodes for sodium-ion batteries (SIBs) via a synergistic pre-oxidation and acetylene chemical vapor deposition (CVD) strategy, which effectively reduces open pores and promotes structural stabilization. The resulting material exhibits features consistent with a closed-pore architecture. Pre-oxidation incorporates oxygen-containing functional groups that template accessible pores and expand the interlayer spacing during carbonization. Subsequent CVD covers surface pores and contributes to the stabilization of the pore structure. The optimized HC (COF300&1300@C) exhibits a balanced set of structural features, including a low specific surface area (2.1 m² g^-1), expanded interlayer distance (0.391 nm), and a well-regulated pore system with reduced surface area and controlled pore size. As a result, it delivers a reversible capacity of 298 mAh g^-1 with an ICE of 70%, and remarkable cycling stability (97% capacity retention after 500 cycles at 1C). This study elucidates the synergistic mechanism of pre-oxidation and CVD in reducing open pores and stabilizing the pore architecture, thereby yielding characteristics indicative of closed-pore behavior, and providing a novel and efficient approach for designing high-performance biomass-derived hard carbons for energy storage.