Search

Highlights Janus quasi-solid electrolyte membranes with asymmetric porous structure were constructed, showing a high σLi+ of 1.5 × 10-4 S cm-1 and a high t + of 0.71. The solvation structures and ion transport dynamics in nanopores have been deciphered, manifesting a concentrated electrolyte-like structure and regulated transport behaviors. Quasi-solid NCM 622||Li cells have been demonstrated to stably cycle for 200 cycles at 1 C, and pouch cell has shown high tolerance for abuse.

Highlights Defect engineering for constructing Zn2+ reservoir to anchor anions. The quasi-solid electrolyte interphase as Zn2+ reservoir boosting charge and mass transfer for dendrite-free zinc battery. A Coulombic efficiency of 99.8% was achieved in Zn||Cu cell.

Abstract Electrochemical CO2 reduction reaction (CO2RR) to multi-carbon products would simultaneously reduce CO2 emission and produce high-value chemicals. Herein, we report Cu electrodes modified by metal–organic framework (MOF) exhibiting enhanced electrocatalytic performance to convert CO2 into ethylene and ethanol. The Zr-based MOF, UiO-66 would in situ transform into amorphous ZrOx nanoparticles (a-ZrOx), constructing a-ZrOx/Cu hetero-interface as a dual-site catalyst. The Faradaic efficiency of multi-carbon (C2+) products for optimal UiO-66-coated Cu (0.5-UiO/Cu) electrode reaches a high value of 74% at − 1.05 V versus RHE. The intrinsic activity for C2+ products on 0.5-UiO/Cu electrode is about two times higher than that of Cu foil. In situ surface-enhanced Raman spectra demonstrate that UiO-66-derived a-ZrOx coating can promote the stabilization of atop-bound CO* intermediates on Cu surface during CO2 electrolysis, leading to increased CO* coverage and facilitating the C–C coupling process. The present study gives new insights into tailoring the adsorption configurations of CO2RR intermediate by designing dual-site electrocatalysts with hetero-interfaces.

Abstract A robust solid-electrolyte interphase (SEI) enabled by electrolyte additive is a promising approach to stabilize Li anode and improve Li cycling efficiency. However, the self-sacrificial nature of SEI forming additives limits their capability to stabilize Li anode for long-term cycling. Herein, we demonstrate nanocapsules made from metal–organic frameworks for sustained release of LiNO3 as surface passivation additive in commercial carbonate-based electrolyte. The nanocapsules can offer over 10 times more LiNO3 than the solubility of LiNO3. Continuous supply of LiNO3 by nanocapsules forms a nitride-rich SEI layer on Li anode and persistently remedies SEI during prolonged cycling. As a result, lifespan of thin Li anode in 50 μm, which experiences drastic volume change and repeated SEI formation during cycling, has been notably improved. By pairing with an industry-level thick LiCoO2 cathode, practical Li-metal full cell demonstrates a remarkable capacity retention of 90% after 240 cycles, in contrast to fast capacity drop after 60 cycles in LiNO3 saturated electrolyte.

Abstract Transition metal oxides are promising candidates for the high-capacity anode material in lithium-ion batteries. The electrochemical performance of transition metal oxides can be improved by constructing suitable composite architectures. Herein, we demonstrate a metal–organic framework (MOF)-assisted strategy for the synthesis of a hierarchical hybrid nanostructure composed of Fe2O3 nanotubes assembled in Co3O4 host. Starting from MOF composite precursors (Fe-based MOF encapsulated in a Co-based host matrix), a complex structure of Co3O4 host and engulfed Fe2O3 nanotubes was prepared by a simple annealing treatment in air. By virtue of their structural and compositional features, these hierarchical composite particles reveal enhanced lithium storage properties when employed as anodes for lithium-ion batteries.