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Formation of Complex Ions03:45

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A type of Lewis acid-base chemistry involves the formation of a complex ion (or a coordination complex) comprising a central atom, typically a transition metal cation, surrounded by ions or molecules called ligands. These ligands can be neutral molecules like H2O or NH3, or ions such as CN− or OH−. Often, the ligands act as Lewis bases, donating a pair of electrons to the central atom. These types of Lewis acid-base reactions are examples of a broad subdiscipline called coordination...
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Mechanistic Insight and Local Structure Evolution of NiPS3 upon Electrochemical Lithiation.

Christopher Choi1, David Ashby1,2, You Rao3

  • 1Department of Materials Science and Engineering, University of California, Los Angeles, Los Angeles, California 90095, United States.

ACS Applied Materials & Interfaces
|January 11, 2022
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Summary

Researchers studied lithium-ion storage in nickel phosphorus trisulfide (NiPS3) materials. They discovered a sequential intercalation and conversion reaction mechanism, offering insights into these promising energy storage systems.

Keywords:
2D materialsLi-ion insertion mechanismconversion reactionsintercalation reactionsmetal phosphorus trichalcogenides

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Transition metal phosphorus trisulfide materials have shown potential for energy conversion and storage since the late 20th century.
  • Understanding the fundamental mechanisms of lithium-ion (Li-ion) storage in these compounds is crucial for optimizing their performance.
  • Current knowledge regarding Li-ion storage mechanisms in these materials remains limited.

Purpose of the Study:

  • To investigate the detailed lithiation process and Li-ion storage mechanisms in nickel phosphorus trisulfide (NiPS3).
  • To elucidate the complex ion insertion and storage dynamics within the layered polyanionic structure of NiPS3.
  • To provide a foundational understanding for developing advanced phosphorus trisulfide-based energy storage systems.

Main Methods:

  • Utilized in situ pair-distribution function analysis to observe structural changes during lithiation.
  • Employed Monte Carlo molecular dynamics calculations to simulate ion behavior and storage mechanisms.
  • Conducted a series of ex situ characterizations to complement in situ observations.

Main Results:

  • The lithiation of NiPS3 involves a complex interplay of ion insertion and storage.
  • A sequential mechanism involving both intercalation and conversion reactions was identified.
  • Detailed insights into the dynamic structural and chemical transformations during Li-ion storage were obtained.

Conclusions:

  • The study clarifies the Li-ion storage mechanism in NiPS3, characterized by sequential intercalation and conversion reactions.
  • This work provides a model for understanding Li-ion storage in transition metal phosphorus sulfide materials.
  • Identified challenges in achieving reliable, high-energy phosphorus trisulfide systems are highlighted, guiding future research efforts.