期刊
APPLIED SURFACE SCIENCE
卷 606, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apsusc.2022.154944
关键词
Formic acid oxidation; Pd-Ni cluster; Graphene; Electrocatalysts; First-principles calculation
类别
资金
- Ministry of Science and Technology (MOST) , Taiwan
- Chung Yuan Christian University (CYCU)
- National Center for High-Performance Computing, Taiwan
- [MOST 111-2113-M-033-013]
- [MOST 110-2113-M-033-009]
- [MOST 109-2113-M-033-001]
The electrocatalytic formic acid oxidation (FAO) on graphene supported Pd-Ni catalysts was investigated using periodic density functional theory calculations. The role of Ni content in different Pd-Ni atomic ratio and the hydrogen coverage effect were elucidated.
By means of periodic density functional theory calculations, we have investigated the electrocatalytic formic acid oxidation (FAO) on graphene supported Pd-Ni catalysts and elucidate the detail about the role of Ni content in different Pd-Ni atomic ratio and the hydrogen coverage effect. The FAO reaction often onsets at low oxidation potential range, where deposition of hydrogen is alive and affect the catalytic performance of Pd-Ni clusters, accordingly, the FAO reaction on varied H* ratio Pd-Ni clusters accompanying with enhanced external potential is also considered. In our calculation, the H* saturated situation would suppress the formation of COOH* much more than that of HCOO*, even controlling the reaction energy of HCOO* from HCOOH become moderate in FAO reaction. In addition, the potential requirements to proceed the FAO reaction on Pd10-gra and Pd8Ni2- graphene are similar but Ni content could also suppress formation of COOH* and enhance the interaction be-tween Pd8Ni2-graphene and HCOO* species. Pd6Ni4-grahene model is another choice for FAO reaction, in which the HCOO* species on clean Pd6Ni4-graphene model has lowest onset potential of 0.18 V for HCOO* deproto-nation to CO2 in all of our models. However, excess Ni content would cause Ni exposed on Pd2Ni8-grahene, where the HCOO* is downhill in energy with a larger onset potential of 0.59 V for the deprotonation of HCOO*, but the hydride formation of 8H* and 9H* Pd2Ni8-graphene could overcome the question.
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