Abstract
Mechanistic details of catalytic reactions are critical to the development of improved catalysts. Here, we perform high quality Born-Oppenheimer molecular dynamics simulations of the reaction mechanisms associated with hydrogen-assisted CO2 reduction on Ni(110). The simulation results show direct theoretical evidence for both associative and redox mechanisms in the reaction of atomic hydrogen with CO2. Because H2 is dissociatively chemisorbed on Ni(110) with nearly unit probability, the mechanisms we find are also relevant to the reverse water-gas shift reaction (H2 with adsorbed CO2). Furthermore, we provide the first real-time demonstration of both Eley-Rideal (ER) and hot atom (HA) mechanisms when H impinges on adsorbed CO2, and we show that both occur even for low kinetic energies. The trade-off between ER or HA mechanisms is found to be strongly dependent on CO2 coverage. The results are compared with recent gas/surface measurements.
| Original language | English |
|---|---|
| Pages (from-to) | 4663-4666 |
| Number of pages | 4 |
| Journal | Journal of the American Chemical Society |
| Volume | 139 |
| Issue number | 13 |
| DOIs | |
| Publication status | Published - Apr 5 2017 |
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ASJC Scopus subject areas
- Catalysis
- Chemistry(all)
- Biochemistry
- Colloid and Surface Chemistry
Cite this
Mechanisms of Hydrogen-Assisted CO2 Reduction on Nickel. / Lin, Wei; Stocker, Kelsey M.; Schatz, George C.
In: Journal of the American Chemical Society, Vol. 139, No. 13, 05.04.2017, p. 4663-4666.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Mechanisms of Hydrogen-Assisted CO2 Reduction on Nickel
AU - Lin, Wei
AU - Stocker, Kelsey M.
AU - Schatz, George C
PY - 2017/4/5
Y1 - 2017/4/5
N2 - Mechanistic details of catalytic reactions are critical to the development of improved catalysts. Here, we perform high quality Born-Oppenheimer molecular dynamics simulations of the reaction mechanisms associated with hydrogen-assisted CO2 reduction on Ni(110). The simulation results show direct theoretical evidence for both associative and redox mechanisms in the reaction of atomic hydrogen with CO2. Because H2 is dissociatively chemisorbed on Ni(110) with nearly unit probability, the mechanisms we find are also relevant to the reverse water-gas shift reaction (H2 with adsorbed CO2). Furthermore, we provide the first real-time demonstration of both Eley-Rideal (ER) and hot atom (HA) mechanisms when H impinges on adsorbed CO2, and we show that both occur even for low kinetic energies. The trade-off between ER or HA mechanisms is found to be strongly dependent on CO2 coverage. The results are compared with recent gas/surface measurements.
AB - Mechanistic details of catalytic reactions are critical to the development of improved catalysts. Here, we perform high quality Born-Oppenheimer molecular dynamics simulations of the reaction mechanisms associated with hydrogen-assisted CO2 reduction on Ni(110). The simulation results show direct theoretical evidence for both associative and redox mechanisms in the reaction of atomic hydrogen with CO2. Because H2 is dissociatively chemisorbed on Ni(110) with nearly unit probability, the mechanisms we find are also relevant to the reverse water-gas shift reaction (H2 with adsorbed CO2). Furthermore, we provide the first real-time demonstration of both Eley-Rideal (ER) and hot atom (HA) mechanisms when H impinges on adsorbed CO2, and we show that both occur even for low kinetic energies. The trade-off between ER or HA mechanisms is found to be strongly dependent on CO2 coverage. The results are compared with recent gas/surface measurements.
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UR - http://www.scopus.com/inward/citedby.url?scp=85016985123&partnerID=8YFLogxK
U2 - 10.1021/jacs.7b01538
DO - 10.1021/jacs.7b01538
M3 - Article
AN - SCOPUS:85016985123
VL - 139
SP - 4663
EP - 4666
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 13
ER -