Capacitive deionization (CDI), a m ethod with notable
advantages
of relatively low energy consumption and environmental friendliness,
has been widely used in desalination of saltwater. However, due to
the weak electrical double-layer electrosorption of ions from water,
CDI has suffered from low throughput capacity that may limit its commercial
applications. Thus, it is of importance to develop a high-efficiency
and engineering-feasible CDI process. Manganese and cobalt and their
oxides, being faradic materials, have a relatively high pseudocapacitance,
which can cause an increase of positive and negative charges on opposing
electrodes. However, their low conductivity properties limit their
electrochemical applications. Pseudocapacitive Mn3O4 nanoparticles encapsulated within a conducting carbon shell
(Mn3O4@C) were prepared to enhance charge transfer
and capacitance for CDI. Desalination performances of the Mn3O4@C (5–15 wt %) core–shell nanoparticles
on activated carbon (AC) (Mn3O4@C/AC) serving
as CDI electrodes have thus been investigated. The pseudocapacitive
Mn3O4@C/AC electrodes with relatively low diffusion
resistances have much greater capacitance (240–1300 F/g) than
the pristine AC electrode (120 F/g). In situ synchrotron
X-ray absorption near-edge structure spectra of the Mn3O4@C/AC electrodes during CDI (under 1.2 and −1.2
V for electrosorption and regeneration, respectively) demonstrate
that reversible faradic redox reactions cause more negative charges
on the negative electrode and more positive charges on the positive
electrode. Consequently, the pseudocapacitive electrodes for CDI of
saltwater ([NaCl] = 1000 ppm) show much better desalination performances
with a high optimized salt removal (600 mg/g·day), electrosorption
efficiency (48%), and electrosorption capacity (EC) (25 mg/g) than
the AC electrodes (288 mg/g·day, 23%, and 12 mg/g, respectively).
The Mn3O4@C/AC electrode has a maximum EC of
29 mg/g for CDI under +1.2 V. Also, the Mn3O4@C/AC electrodes have much higher pseudocapacitive electrosorption
rate constants (0.0049–0.0087 h–1) than the
AC electrode (0.0016 h–1). This work demonstrates
the feasibility of high-efficiency CDI of saltwater for water recycling
and reuse using the low-cost and easily fabricated pseudocapacitive
Mn3O4@C/AC electrodes.