cs6b02871_si_001.pdf (1.58 MB)
Design of High-Performance Pd-Based Alloy Nanocatalysts for Direct Synthesis of H2O2
journal contribution
posted on 2017-02-09, 00:00 authored by Haoxiang Xu, Daojian Cheng, Yi GaoThe direct synthesis
of hydrogen peroxide (H2O2) is a promising alternative
to the commercialized indirect process.
However, it is still a big challenge for the development of Pd-based
catalysts with outstanding activity and selectivity, because the design
and optimization of the efficient catalysts cannot be effectively
achieved solely on the basis of the well-known Sabatier analysis.
In this paper, we proposed a strategy to design more efficient Pd-based
nanocatalysts combining density functional theory (DFT) calculations
and Sabatier analysis. The average valence electron of Pd-shell atoms
is identified as the intrinsic factor for the activity and selectivity
of the Pd-based nanocatalysts, which can be effectively tuned by the
dopants. By introducing dopants with suitable electronegativity, the
valence electrons of Pd-shell atoms could be adjusted to the optimal
range to enhance the activity and selectivity of the nanocluster simultaneously.
With this strategy, Pd-W, Pd-Pb, Au-Pd-W, Au-Pd-Pb, Au-Pd-Mo, and
Au-Pd-Ru are predicted as the potential candidates with catalytic
performance far exceeding the state of the art experimental systems
by a scan of the periodic table. This work not only predicts potential
Pd-based alloy nanocatalysts for direct synthesis of H2O2 for future experiments but also provides a viable way
for the design of highly efficient heterogeneous catalysts in extensive
applications.