Conspectus
Liquid metals,
defined as metals or alloys with melting points
below or near room temperature, can be regarded as an amorphous solid
without any crystallinity in the molten state, exhibiting fundamentally
different fluidities and metallicities from solid metals and other
liquids. In the past decade, gallium as a typical representative liquid
metal with a melting point of ∼29.8 °C, virtually nonexistent
vapor pressure, and negligible toxicity has been proposed as a base
material for the construction of gallium (Ga)-based liquid metals
(LMs). This class of extraordinary materials with unique physicochemical
properties, such as superb thermal and electrical conductivity, fluidity,
shape transformability, self-healing capability and biocompatibility,
biodegradability, catalytic properties, plasmonic effect, and facile
functionalization accessibility, has attracted considerable attention
in widespread applications. Generally, under the action of ambient
oxygen and water, the ultrathin oxide layers will be formed at the
LM–ambient environment interface, which may provide a physical,
chemical, and electrical barrier to prevent the LMs from further oxidation.
The introduction of excitations, such as electrical, chemical, electrochemical,
mechanical, and ultrasonic, and the alteration of reaction conditions
including ingredients, temperature, and time will promote oxide formation.
However, the existence of oxides is a double-edged sword, sometimes
considered as a nuisance because of the deterioration of performance
and stability; for example, the oxides will adhere to the system,
which brings problems for fluidic applications (such as heat-transfer
media, pump media, and microfluidity). Conversely, in some cases,
oxides are considered essential to improve functionality, such as
shape transformation, substrate adhesion, intracellular uptake, etc.
For this reason, the main aim of oxidation regulation is to alter
the fundamental physicochemical properties or even endow distinct
and fascinating properties for the LMs, thereby expanding the scope
of applications. Although technological advances have shown dramatic
progress and great potential of the LMs, their oxidation regulation
remains in its infancy, thus deserving further attention. In this
Account, we present a relatively elaborate summary of the oxidation
regulation of LMs. First, the fundamental properties of LM oxides
and their performance impact on LMs are reviewed. Then, the visions
expanding to precise oxidation regulation in terms of vital structural
statuses of LMs. After that, representative applications focusing
on our own contributions to this field in recent years are described.
Finally, brief perspectives and challenges are also presented here.
Overall, this Account not only sheds light on the valuable balance
between pristine LMs and oxides but also proposes prospective principles
for the design and synthesis of advanced LM materials with tunable
or even unprecedented properties.