posted on 2024-02-13, 06:14authored byMeilan Pan, Cong Li, Xiuzhen Wei, Guanyu Liu, Edison Huixiang Ang, Bingjun Pan
The
electrocatalytic hydrodehalogenation (EHDH) process mediated
by atomic hydrogen (H*) is recognized as an efficient method for degrading
halogenated organic pollutants (HOPs). However, a significant challenge
is the excessive energy consumption resulting from the recombination
of H* to H2 production in the EHDH process. In this study,
a promising strategy was proposed to generate piezo-induced atomic
H*, without external energy input or chemical consumption, for the
degradation and dehalogenation of HOPs. Specifically, sub-5 nm Ni
nanoparticles were subtly dotted on an N-doped carbon layer coating
on BaTiO3 cube, and the resulted hybrid nanocomposite (Ni-NC@BTO)
can effectively break C-X (X = Cl and F) bonds under ultrasonic vibration
or mechanical stirring, demonstrating high piezoelectric driven dehalogenation
efficiencies toward various HOPs. Mechanistic studies revealed that
the dotted Ni nanoparticles can efficiently capture H* to form Ni–H*
(Habs) and drive the dehalogenation process to lower the
toxicity of intermediates. COMSOL simulations confirmed a “chimney
effect” on the interface of Ni nanoparticle, which facilitated
the accumulation of H+ and enhanced electron transfer for
H* formation by improving the surface charge of the piezocatalyst
and strengthening the interfacial electric field. Our work introduces
an environmentally friendly dehalogenation method for HOPs using the
piezoelectric process independent of the external energy input and
chemical consumption.