Over
the past two decades, the solid–electrolyte interphase
(SEI) layer that forms on an electrode’s surface has been believed
to be pivotal for stabilizing the electrode’s performance in
lithium-ion batteries (LIBs). However, more and more researchers currently
are realizing that the metal-ion solvation structure (e.g., Li+) in electrolytes and the derived interfacial model (i.e.,
the desolvation process) can affect the electrode’s performance
significantly. Thus, herein we summarize recent research focused on
how to discover the importance of an electrolyte’s solvation
structure, develop a quantitative model to describe the solvation
structure, construct an interfacial model to understand the electrode’s
performance, and apply these theories to the design of electrolytes.
We provide a timely review on the scientific relationship between
the molecular interactions of metal ions, anions, and solvents in
the interfacial model and the electrode’s performance, of which
the viewpoint differs from the SEI interpretations before. These discoveries
may herald a new, post-SEI era due to their significance for guiding
the design of LIBs and their performance improvement, as well as developing
other metal-ion batteries and beyond.
Transition
metal doped semiconductor nanocrystals (d-dots) possess
fundamentally different emission properties upon photo- or electroexcitation,
which render them as unique emitters for special applications. However,
in comparison with intrinsic semiconductor nanocrystals, the potential
of d-dots has been barely realized, because many of their unique emission
properties mostly rely on precise control of their photoluminescence
(PL) decay dynamics. Results in this work revealed that it would be
possible to obtain bright d-dots with nearly single-exponential PL
decay dynamics. By tuning the number of Mn2+ ions per dot
from ∼500 to 20 in Mn2+ doped ZnSe nanocrystals
(Mn:ZnSe d-dots), the single-exponential PL decay lifetime was continuously
tuned from ∼50 to 1000 μs. A synthetic scheme was further
developed for uniform and epitaxial growth of thick ZnS shell, ∼7
monolayers. The resulting Mn:ZnSe/ZnS core/shell d-dots were found
to be essential for necessary environmental durability of the PL properties,
both steady-state and transient ones, for the d-dot emitters. These
characteristics combined with intense absorption and high PL quantum
yields (70 ± 5%) enabled greatly simplified schemes for various
applications of PL lifetime multiplexing using Mn:ZnSe/ZnS core/shell
d-dots.
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