10.1021/acscatal.6b02871.s001
Haoxiang Xu
Haoxiang
Xu
Daojian Cheng
Daojian
Cheng
Yi Gao
Yi
Gao
Design of High-Performance Pd-Based Alloy Nanocatalysts
for Direct Synthesis of H<sub>2</sub>O<sub>2</sub>
American Chemical Society
2017
Sabatier analysis
selectivity
strategy
Pd-shell atoms
DFT
synthesis
Pd-based nanocatalysts
Pd-based alloy nanocatalysts
dopant
valence
electron
H 2 O 2
High-Performance Pd-Based Alloy Nanocatalysts
2017-02-09 00:00:00
Journal contribution
https://acs.figshare.com/articles/journal_contribution/Design_of_High-Performance_Pd-Based_Alloy_Nanocatalysts_for_Direct_Synthesis_of_H_sub_2_sub_O_sub_2_sub_/4668790
The direct synthesis
of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) 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 H<sub>2</sub>O<sub>2</sub> for future experiments but also provides a viable way
for the design of highly efficient heterogeneous catalysts in extensive
applications.