The modulation of electron density is an effective option for efficient alternative electrocatalysts. Here, p‐n junctions are constructed in 3D free‐standing FeNi‐LDH/CoP/carbon cloth (CC) electrode (LDH=layered double hydroxide). The positively charged FeNi‐LDH in the space‐charge region can significantly boost oxygen evolution reaction. Therefore, the j at 1.485 V (vs. RHE) of FeNi‐LDH/CoP/CC achieves ca. 10‐fold and ca. 100‐fold increases compared to those of FeNi‐LDH/CC and CoP/CC, respectively. Density functional theory calculation reveals OH− has a stronger trend to adsorb on the surface of FeNi‐LDH side in the p‐n junction compared to individual FeNi‐LDH further verifying the synergistic effect in the p‐n junction. Additionally, it represents excellent activity toward water splitting. The utilization of heterojunctions would open up an entirely new possibility to purposefully regulate the electronic structure of active sites and promote their catalytic activities.

Silicon is a low price and high capacity anode material for lithium-ion batteries. The yolk-shell structure can effectively accommodate Si expansion to improve stability. However, the limited rate performance of Si anodes can’t meet people’s growing demand for high power density. Herein, the phosphorus-doped yolk-shell Si@C materials (P-doped Si@C) were prepared through carbon coating on P-doped Si/SiOx matrix to obtain high power and stable devices. Therefore, the as-prepared P-doped Si@C electrodes delivered a rapid increase in Coulombic efficiency from 74.4% to 99.6% after only 6 cycles, high capacity retention of ∼ 95% over 800 cycles at 4 A·g−1, and great rate capability (510 mAh·g−1 at 35 A·g−1). As a result, P-doped Si@C anodes paired with commercial activated carbon and LiFePO4 cathode to assemble lithium-ion capacitor (high power density of ∼ 61,080 W·kg−1 at 20 A·g−1) and lithium-ion full cell (good rate performance with 68.3 mAh·g−1 at 5 C), respectively. This work can provide an effective way to further improve power density and stability for energy storage devices.

No abstract

Huge volume changes of Si during lithiation/delithiation lead to regeneration of solid-electrolyte interphase (SEI) and consume electrolyte. In this article, γ-glycidoxypropyl trimethoxysilane (GOPS) was incorporated in Si/PEDOT:PSS electrodes to construct a flexible and conductive artificial SEI, effectively suppressing the consumption of electrolyte. The optimized electrode can maintain 1000 mAh g−1 for nearly 800 cycles under limited electrolyte compared with 40 cycles of the electrodes without GOPS. Also, the optimized electrode exhibits excellent rate capability. The use of GOPS greatly improves the interface compatibility between Si and PEDOT:PSS. XPS Ar+ etching depth analysis proved that the addition of GOPS is conducive to forming a more stable SEI. A full battery assembled with NCM 523 cathode delivers a high energy density of 520 Wh kg−1, offering good stability.

PEDOT:PSS has been studied as a silicon-based binder due to its inherent superior electricity and electrochemical stability. However, it cannot effectively alleviate the huge volume changes of silicon during lithiation/delithiation due to its linear structure, resulting in poor cycling stability. Ion-cross-linking is a usual method to cross-link linear polymers into 3D structures. In this paper, multivalent cations of the 5th period and Group 2 cross-linked PEDOT:PSS were applied as silicon anode binders and studied systematically. It was found that the variation trend of viscosity and conductivity of PEDOT:PSS after cross-linking was consistent with that of ionic potential and softness parameters of multivalent cations. The mesostructure of a binder after cross-linking is influenced by the solubility product constant of sulfites or hydroxides of cations and the growth characteristics of crystals. An Sn4+-cross-linked binder displayed increased viscosity and electrical conductivity and higher reduced modulus and hardness due to its positive softness parameter and higher ion potential. The Si electrode with the Sn4+-cross-linked binder showed improved cycling stability (1876.4 mAh g–1 compared with 1068.4 mAh g–1 of the electrode with the pure PEDOT:PSS binder after 100 cycles) and superior rate capability (∼800 mAh g–1 at an ultrahigh current density of 8.0 A g–1).