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Phosphides with high theoretical capacity are considered ideal anode materials for lithium‐ion capacitors (LICs), but poor electronic conductivity as well as unsatisfied cyclic stability limits the performance of the phosphides. Here a covalently bonded CoP@C heterostructure is reported, which consists of 5 nm CoP quantum dots (QDs) like pomegranate seeds pinned in carbon polyhedron through interfacial Co─P─C bonding. The ultrafine size of CoP QDs provides more reactive sites and a shorten electrons/ions diffusion path, boosting the specific capacity. The Co─P─C bond induces the energy band variation of CoP and increases the interfacial charge density, bringing about fast kinetics. Besides, the Co─P─C bond introduces a robust pining effect among CoP QDs and carbon polyhedra, greatly improving the structure stability of 5 nm CoP QDs. The CoP@C heterostructure electrode exhibits high capacity (nearly 1000 mAh g−1) and superior cycling stability. It is worth noting that a prototyped LIC full‐cell of YP80//CoP@C presents an impressive high energy density of 172 Wh kg−1 and a power density of 10.8 kW kg−1. Moreover, the LIC possesses an ultra‐long life, retaining 80% after 20,000 cycles. This study offers an effective design for phosphides achieving fast kinetics and superior structure stability through an interfacial bonding approach. [ABSTRACT FROM AUTHOR]

Graphene/metal oxide (rGO/MOx) heterostructures hold great promise for energy storage, yet a full understanding of their synthesis remains elusive. Herein, a general, efficient, and scalable synthesis strategy is designed for the preparation of various rGO/MOx heterostructure materials featuring robust interfacial interactions. The heterogeneous nucleation growth mechanism of metal oxides on graphene is elucidated through ex situ characterization and theoretical simulation. The surface of graphene oxide (GO) is enriched with reactive oxygen‐containing functional groups, serving as potent nucleation sites that facilitate the rapid and heterogeneous nucleation of MOx grains. Simultaneously, a stable interface (C−O−M bond) is in situ formed between graphene and adsorbed metal ions during heat treatment, producing rGO/MOx heterostructure materials. Notably, the resultant rGO/CoO heterostructure material is employed as an anode and LiCoO2 as a cathode to assemble a soft packaging quasi‐solid‐state battery, which has demonstrated an impressive energy density of 341.4 Wh kg−1 and maintains outstanding capacity retention at 93.4% after 300 cycles at a 1C current. These findings provide valuable insights into the preparation and potential applications of rGO/MOx heterostructure materials for energy storage. [ABSTRACT FROM AUTHOR]

Lignin‐derived porous carbon (LPC) shows great potential as electrode material for supercapacitors. However, precise control over the pore structure during the conventional carbonization–activation process remains challenging. Here, a molecular‐level strategy to tailor the pore structure through tuning inter‐/intra‐molecular bonding of lignin in a pre‐carbonization process is shown. Based on operando pyrolysis analysis, a molecular evolution model is proposed to elucidate the relationship between pre‐carbonization and the resulting porosity of LPC. Lignin undergoes a condensation process with an increase of sp2‐hybridized carbon bonding during pre‐carbonization, causing the extension of polycyclic aromatic structure and leading to an increased mesopore volume in the final porous carbon. The variation in the content ratio of sp2‐ and sp3‐hybridized carbon bonding provides insights into the spatial structure evolution of pre‐carbonized lignin, which correlates well with changes in the porous structure of LPC. The LPCs show ultrahigh specific surface area up to 3219 m2 g−1 and tailored meso‐/micropore distribution. The lithium‐ion capacitor full‐cell tests demonstrate the great potential of LPCs in energy storage applications with superior energy density and power density. This work provides a feasible strategy to precisely design the microstructure of LPC, offering promising prospects for energy storage technologies. [ABSTRACT FROM AUTHOR]

The coassembly of primary particles into heterostructures represents a significant strategy for advanced fabrication of multi‐functional materials or devices, and templated assembly has shown remarkable advantage for deterministic placement of particles and the efficient integration with substrates. However, template induced particles coassembly, which is significant for integrating multicomponents at desired positions, is still challenging. Herein, a facile strategy of embossed templateinduced particles coassembly for diverse superstructures and precise patterns is reported. Tunable region selective assembly of particles is demonstrated by controlling the resistance force via designing the embossed edge and surface roughness of the template. Through regulating the template morphologies and particles composition, well‐controlled coassembly of "flower" shaped heterostructure and chiral superstructure arrays are realized. Furthermore, the printable nanomaterials self‐assembly template is employed to achieve totally bottom‐up fabrication of excitation responsive heterostructure arrays, in which the multi‐photons process based energy transfer is studied to show the application in high‐secure encryption. With the advantage of accurate position and compatible to different materials, this strategy is expected to provide a promising platform for fabricating micro/nanoscale advanced devices. [ABSTRACT FROM AUTHOR]

2D 1T phase MoS2 (1T‐MoS2) nanosheet with metallic conductivity and expanded interlayer spacing is considered as a highly potential lithium storage electrode material but remains thermodynamic instability in aqueous media, seriously hindering the electrochemical performance. Herein, a versatile strategy is proposed for the preparation of thermodynamically stable 1T‐MoS2/MXene heterostructures with the aid of delaminated Ti3C2Tx MXene (d‐Ti3C2Tx) dispersion containing tetrabutylammonium hydroxide. The 2D d‐Ti3C2Tx provides more uniform nucleation sites for MoS2, and the TBA+ ions can intercalate into MoS2 to induce the phase conversion from semiconducting 2H to 1T. Moreover, the electrochemical advantages of 1T‐MoS2 and d‐Ti3C2Tx can be united by the construction of a well‐organized heterostructure. Outstanding rate performance is realized because of extra‐large interlayer space of 1T MoS2 with TBA+ intercalation and decreased energy barrier for fast Li+ diffusion. Subsequently, a lithium‐ion capacitor (LIC) is assembled based on 1T‐MoS2/d‐Ti3C2Tx as anode and hierarchically porous graphene nanocomposite with micro/mesoporous structure as a cathode. The LIC exhibits a large energy density up to 188 Wh kg−1, an ultra‐high power density of 13 kW kg−1, together with remarkable capacity retention of 83% after 5000 cycles. This study demonstrates the great promise of 1T‐MoS2/d‐Ti3C2Tx heterostructures as anode for high‐performance LICs. [ABSTRACT FROM AUTHOR]