Journal
ACS APPLIED ENERGY MATERIALS
Volume 4, Issue 5, Pages 4302-4307Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.1c00434
Keywords
active site; hydrogen evolution reaction; noble-metal-less electrocatalyst; Pd-Pd bonding; negatively charged Pd
Funding
- National Natural Science Foundation of China [51922105, 51772322, 51722205]
- National Key Research and Development Program of China [2018YFE0202601, 2017YFA0304700, 2016YFA0300600]
- Frontier Sciences of the Chinese Academy of Sciences [QYZDJ-SSW-SLH013]
- Canada Foundation for Innovation (CFI)
- Natural Sciences and Engineering Research Council (NSERC)
- National Research Council (NRC)
- Canadian Institutes of Health Research (CIHR)
- Government of Saskatchewan
- University of Saskatchewan
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The catalytic activity in LnPdAsO (Ln = La, Ce, Pr) was reported, showing improved overpotentials toward HER by elongating the distance of Pd-Pd in the PdAs- layer. LaPdAsO demonstrated superior Tafel slope and long-term stability compared to optimized Pd and Pd/C. Density functional theory calculations revealed that the active sites lie at the center of Pd's net, providing a low free energy barrier for H-H reaction.
We report the catalytic activity in LnPdAsO (Ln = La, Ce, Pr). In this PdAs- layer (II), by elongating the distance of Pd-Pd, the overpotentials toward HER are 110.0, 89.5, and 62.0 mV at 10 mA/cm(2) for PrPdAsO, CePdAsO, and LaPdAsO, respectively. Furthermore, the Tafel slope and robust long-term stability in LaPdAsO even surpasses the capability of optimized Pd and Pd/C. Density functional theory calculations reveal that the active sites lie at the center of Pd-'s net with a free energy barrier of 0.09 eV for H-H reaction. The present engineering two-dimensional Pd provides a route for exploring superior electrocatalyst on the basis of known noble metals.
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