Jinyun Liu

Heterostructured cathodes are widely credited with accelerating conversion kinetics in magnesium/lithium hybrid-ion batteries (MLHBs). Here, we construct a Cu7S4/CuCo2S4 heterostructure in a single hydrothermal process, in which the two phases sharing a common Cu–S sublattice form a coherent interface within individual particles. By fixing the phase ratio independently through Rietveld refinement and benchmarking against both phase-pure constituents under identical conditions, we show that the composite exceeds the composition-weighted rule-of-mixtures prediction by a factor of 3.4 at 0.3 A g–1. Because the constituents exhibit closely comparable charge–discharge profiles, the redox chemistry itself is unchanged, and this strongly super-additive response can primarily originate from the interface rather than from composition. Elemental mapping and surface-sensitive XPS, together with the coexistence of Li2S and MgS in in situ XRD, further reveal that storage is spatially partitioned: Li+ converts the particle interior while Mg2+ reacts predominantly in the near-surface region, so that the two carriers occupy complementary regions of the same particle. Comparing APC-LiCl with APC-LiTFSI at matched salt concentration, and identical in every other respect, localizes the electrolyte effect to the electrode interface, where the chloride-containing system suppresses the progressive Mg-surface passivation that drives continuous overpotential growth in the TFSI– system. The resulting cell delivers 400 mAh g–1 at 0.3 A g–1 and retains 152.56 mAh g–1 after 330 cycles at 1.0 A g–1 at ∼100% Coulombic efficiency. DFT calculations indicate increased states near the Fermi level and a localized interfacial electrostatic gradient consistent with the measured kinetics.

Defect-engineering commonly enables improved energy-storage performance; however, how it synergizes with interfacial bond bridging to boost fast-charging capacity remains a challenge. Here, we develop a FeS2@Ga2S3 heterostructure as sodium-ion battery anode that integrates dual-phase vacancies with Fe–S–Ga bonds. Peak-force atomic force microscopy and insitu characterizations reveal that Fe–S–Ga bonds enable structural stability. Density functional theory (DFT) calculations and kinetic analyses demonstrate the tailored heterointerface exhibits moderate Na+ adsorption energy and reduced diffusion barrier. The FeS2@Ga2S3 anode delivers a capacity of 468.5 mAh g–1 after 1000 cycles at 10.0 A g–1 with nearly 100% Coulombic efficiency, an exceptional rate-performance keeping 416.8 mAh g–1 at 20.0 A g–1, and stable performance over wide temperatures from −15 to 50 °C. FeS2@Ga2S3||Na3V2(PO4)3 full cell retains 442.4 mAh g–1 after 500 cycles at 1.0 A g–1, exhibiting a good potential for applications. This dual-defects and chemical bond-bridging design could be applied for developing a broad set of battery systems.

Silicon oxide (SiOx) is a promising anode for lithium-ion batteries, yet its practical application is hindered by multistep synthesis, hazardous silane-based routes, poor scalability, and sluggish electrochemical conversion. Herein, we report a low-cost and scalable strategy for constructing graphitic carbon-confined SiOx (SiOx@GC) anodes via all-process catalysis using waste-derived superabsorbent polymers and industrial by-product SiCl4 as carbon and silicon precursors, respectively. Ni species participate throughout by catalyzing carbon graphitization, mediating confined SiOx formation, and dynamically facilitating electrochemical conversion during cycling. This integrated Ni-enabled process promotes efficient SiOx formation and its deeper, more reversible conversion into electrochemically active silicon. Consequently, the SiOx@GC anode delivers 1147 mAh g–1 after 100 cycles at 0.1 A g–1, stable cycling over 1000 cycles at 5 A g–1, and a full-cell energy density of 353 Wh kg–1 after 250 cycles. This work establishes an all-process catalytic framework for coupling scalable SiOx synthesis with reversible electrochemical conversion.

Developing high-capacity and fast reaction kinetic sodium-ion (Na-ion) battery anodes still remains a big challenge. Here, a ternary heterostructure composite of NiS2/CoS2/CuS2 with hollow cubic structure configuration is developed by sulfurizing a NiCoCu-based prussian blue analog precursor. The ternary sulfides synergistically enhance electron/ion transport, while the hollow cubic morphology improves structural stability during cycling which is confirmed through in situ studies such as in situ Raman and X-ray diffraction. The NiS2/CoS2/CuS2 anode delivers a high capacity of 671 mAh g–1 after cycling 250 times under 0.5 A g–1, and it maintains 417 mAh g–1 after 900 cycles at 1 A g–1. The NiS2/CoS2/CuS2 anode-based full cell when paired with a NVP cathode achieves 310 mAh g–1 after 1000 cycles under 0.5 A g–1, displaying a good applicability potential. It is expected these findings are of great significance to develop long-life, high-capacity Na-ion batteries.

We develop a carbon-encapsulated hollow ZnS/SnS ₂ /SnO ₂ heterojunction as an Na-ion battery anode, displaying excellent Na-storage performance with high capacity and good stability.

Solid‐state sodium‐ion batteries (SSSIBs) combining with good safety and appropriate cost are considered as a promising emerging energy‐storage system. However, poor electrochemical reversibility and sluggish kinetics of anodes remain critical bottlenecks. Here, we develop a CoS/Co ₉ S ₈ /SnS composite coated with nitrogen‐doped carbon (named as CoS/Co ₉ S ₈ /SnS@NC), where a triple‐phase‐interface heterostructure is constructed among CoS, Co ₉ S ₈ and SnS, which enables synergistically amplifying of electric field network and thus improving electron/ion transport kinetics. The CoS/Co ₉ S ₈ /SnS@NC as SSSIB anode exhibits excellent compatibility with conventional Na ₃ PS ₄ solid‐electrolyte, and delivers a large capacity of 441 mAh g ^{− 1} after 120 cycles at 0.5 A g ^{− 1} , and superior rate‐performance of 348.7 mAh g ^{− 1} at 5.0 A g ^{− 1} . Stable high‐temperature tolerance (capacity keeps 502 mAh g ^{− 1} after 50 cycles), and solid‐state full‐cells paring with Na ₃ V ₂ (PO ₄ ) ₃ cathode, are also achievable. Synergistic enhancement effect of the heterostructure is demonstrated via ex situ characterizations and in situ electrochemical impedance spectroscopy, which verifies that the triple‐phase‐interface efficiently reduces the charge transfer resistance and promotes ion diffusion. These findings provide a general strategy for engineering triple‐phase‐interface heterostructures for energy‐storage with optimal interfaces, and sheds light on the fundamental understanding of interface‐enhanced solid‐state batteries.

Silicon (Si) anodes exhibit remarkable theoretical capacity, enabling them to be attractive candidates for high-energy-density lithium-ion batteries. However, conventional surface-modification strategies on Si often fail due to insufficient adhesion between the coating and Si, thereby giving rise to interfacial degradation and poor ion/electron transport. Here, we develop a heterointerface-engineered Si@Co_0.85Se/N-doped carbon (NC) anode. Porous Si is coated by metal-organic framework (MOF)-derived Co_0.85Se, and Si@Co_0.85Se is encapsulated in an NC matrix. This design establishes robust Co-Se-Si bonding at the heterointerface, enabling highly efficient ionic and electronic transport. The Si@Co_0.85Se/NC anode delivers a large specific capacity of 1155.1 mA h g^-1 after 100 cycles at 0.2 A g^-1 and remains stable over 600 cycles at 1.0 A g^-1. As a pairing with a LiFePO₄ cathode, the full cell demonstrates exceptional cycling stability. In situ X-ray diffraction and in situ Raman spectroscopy confirm highly reversible electrochemical processes. These findings provide a heterointerface-designing strategy for Si-based anodes to achieve synergistic enhancement for high-performance energy storage.

Sodium-ion batteries face some critical anode-level barriers: sluggish Na⁺ transport, conversion-induced instability, and poor temperature adaptability. Here, we develop a vacancy-based synergy in Co₉S₈@ZnS/C synthesized by metal–organic framework-templated sulfidation. The Co–Zn–S system provides sodiophilic vacancies that lower Na⁺ diffusion barriers and further strengthen the interfacial field. This self-reinforcing synergy is validated through in situ X-ray diffraction and in situ Raman spectroscopy, demonstrating reversible conversion/alloying and interfacial reconstruction. The Co₉S₈@ZnS/C anode delivers exceptional performance, including a high capacity of 458.7 mAh g^–1 after 400 cycles at 1.0 A g^–1 and a remarkable ultralong stability of 249.1 mAh g^–1 after 4000 cycles at 15.0 A g^–1, with robust operation from −10 to 50 °C. Full cells paired with Na₃V₂(PO₄)₃ demonstrate excellent stability, validating their practical viability. This work establishes a generalizable vacancy-abundant design principle that deterministically links defect thermodynamics and electrostatics to long-term Na storage across diverse operating conditions.

Magnesium/sodium hybrid-ion batteries (MNHBs), combining dendrite-free, high-capacity Mg anodes with fast Na⁺ cathode kinetics, are appealing for post-lithium-ion storage. However, adoption is limited by sluggish Mg²⁺ diffusion and a lack of ideal electrolytes. Here we present a synergistically engineered MNHB coupling a Se-vacancy-rich FeSe₂/Bi₂Se₃ heterojunction cathode with an optimized trace water-in-oil electrolyte. The vacancy-tailored heterointerface accelerates Mg²⁺/Na⁺ migration, preserving structural integrity, supported by first-principles calculations. Molecular dynamics reveal that controlled microhydration strengthens [Mg(H₂O)_n]²⁺ coordination, weakens Mg²⁺-Na⁺ pairing, and increases the diffusivity. Electrochemical measurements reveal a high capacity 487 mAh g^-1, excellent rate capability, a high Coulombic efficiency of >99.7% after 1000 cycles at 1.0 A g^-1, and ultralong cycling stability ≥ 3500 cycles at 1.5 A g^-1. In-situ/ex-situ characterizations reveal low polarization, fast diffusion, and reversible phase transitions. These findings establish a clear mechanistic understanding and a broadly applicable strategy to overcome kinetic and interfacial limitations in secondary batteries.