For
the first time, few-layer Ti3C2T
x
(FL-Ti3C2T
x
) supporting highly dispersed nano-Ni particles with
an interconnected and interlaced structure was elaborated through
a self-assembly reduction process. FL-Ti3C2T
x
not only acts as a supporting material but
also self-assembles with Ni2+ ions through the electrostatic
interaction, assisting in the reduction of nano-Ni. After ball milling
with MgH2, Ni30/FL-Ti3C2T
x
(few-layer Ti3C2T
x
supported 30 wt % nano-Ni via self-assembly
reduction) shows superior catalytic activity for MgH2.
For example, MgH2-5 wt % Ni30/FL-Ti3C2T
x
can release approximately
5.83 wt % hydrogen within 1800 s at 250 °C and absorb 5 wt %
hydrogen within 1700 s at 100 °C. The combined effects of finely
dispersed nano-Ni in situ-grown on FL-Ti3C2T
x
, large specific area of FL-Ti3C2T
x
, multiple-valence Ti
(Ti4+, Ti3+, Ti2+, and Ti0) derived from FL-Ti3C2T
x
, and the electronic interaction between Ni and FL-Ti3C2T
x
can explain the superb
hydrogen storage performance. Our results will attract more attention
to the elaboration of the metal/FL-Ti3C2T
x
composite via self-assembly reduction and
provide a guideline to design high-efficiency composite catalysts
with MXene in hydrogen storage fields.