Monolithic catalysts have irreplaceable advantages in
hydrogen
(H2) production through catalytic dehydrogenation from
liquid-phase hydrogen storage materials. However, monolithic catalysts
suffer from an inevitable reduction in accessible active sites due
to the reduced specific surface area and hindered mass transfer. Therefore,
a rational three-dimensional (3D) structure of monolithic catalysts
is needed to adjust the structural factors for maximizing performance.
Herein, a series of efficient and low-cost 3D catalysts with designed
periodic structures were successfully fabricated. Due to the optimized
specific surface area and bubble transport of the elaborate 3D structure,
compared to the disordered foam structure, the new series of monolithic
catalysts showed 2.3- and 1.6-fold improvement in overall catalytic
performance at 298 and 318 K without any change in physiochemical
characteristics, with hydrogen generation rates of 2548 and 3885 mL
gcat
–1 min–1, respectively.
In addition, a three-period structural design philosophy for 3D catalysts
was summarized, and the concept of surface activity was introduced
to provide quantifiable criteria for guidance of structural optimization.
The outcomes in this paper may open up new insights for building high-efficiency
monolithic catalysts.