Molecular-level insights into CO2 activation on Ni(111) from in situ infrared spectroscopy
Source abstract
Abstract
The activation of CO 2 on nickel surfaces is the first step of various CO 2 conversion processes. Consequently, understanding the surface intermediates formed during this step and their adsorption sites is crucial for elucidating reaction mechanisms. In this study, we employ in situ infrared spectroscopy to investigate the interaction of 1 mbar CO 2 with a model Ni(111) catalyst between 25°C and 300°C. Under these conditions, CO 2 is activated via a direct dissociation into CO and atomic oxygen, while the oxidation state of the Ni(111) surface is primarily determined by residual H 2 and O 2 . The high surface coverage of CO and oxygen at ambient CO 2 pressure induces a competitive adsorption mechanism on the energetically favored hollow sites. This mechanism leads to a temperature-dependent distribution of CO between top and hollow sites, potentially explaining the effect of reaction conditions on the adsorption site of CO intermediates in CO 2 conversion reactions.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Catalytic Processes in Materials Science · CO2 Reduction Techniques and Catalysts · Catalysts for Methane Reforming
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (62)
Show source-provided references
1. CO2 hydrogenation to high-value products via heterogeneous catalysis10.1038/s41467-019-13638-9 ↗
2. Heterogeneous Catalysts toward CO2 Hydrogenation for Sustainable Carbon Cycle10.1021/accountsmr.2c00006 ↗
3. CO2 utilization: Developments in conversion processes10.1016/j.petlm.2016.11.003 ↗
4. Recent Advances in Electrochemical CO2-to-CO Conversion on Heterogeneous Catalysts10.1002/adma.201802066 ↗
5. Catalytic Dry Reforming of Methane: Insights from Model Systems10.1002/cctc.201902142 ↗
6. Catalyst design for dry reforming of methane: Analysis review10.1016/j.rser.2017.09.076 ↗
7. A review on catalyst development for dry reforming of methane to syngas: Recent advances10.1016/j.rser.2019.03.054 ↗
8. Heterogeneous catalytic CO2 conversion to value-added hydrocarbons10.1039/c001514h ↗
9. Recent Advances in Carbon Dioxide Hydrogenation to Methanol via Heterogeneous Catalysis10.1021/acs.chemrev.9b00723 ↗
10. State of the art and perspectives in heterogeneous catalysis of CO2 hydrogenation to methanol10.1039/C9CS00614A ↗
11. Methanation of CO2 and reverse water gas shift reactions on Ni/SiO2 catalysts: the influence of particle size on selectivity and reaction pathway10.1039/C5CY00667H ↗
12. Structure Sensitivity in Steam and Dry Methane Reforming over Nickel: Activity and Carbon Formation10.1021/acscatal.9b04193 ↗
13. Recent scientific progress on developing supported Ni catalysts for dry (CO2) reforming of methane10.3390/catal8030110 ↗
14. The renaissance of the Sabatier reaction and its applications on Earth and in space10.1038/s41929-019-0244-4 ↗
15. Unravelling structure sensitivity in CO2 hydrogenation over nickel10.1038/s41929-017-0016-y ↗
16. Tuning Selectivity of CO2 Hydrogenation Reactions at the Metal/Oxide Interface10.1021/jacs.7b05362 ↗
17. Chemisorption of CO2 on nickel surfaces10.1021/jp052355g ↗
18. CO2 Activation over Catalytic Surfaces10.1002/cphc.201700782 ↗
19. Surface chemistry of CO2 - Adsorption of carbon dioxide on clean surfaces at ultrahigh vacuum10.1016/j.progsurf.2014.03.002 ↗
20. Investigating CO2 Methanation on Ni and Ru: DFT Assisted Microkinetic Analysis10.1002/cctc.202100073 ↗
21. Reaction Kinetics of CO and CO2 Methanation over Nickel10.1021/acs.iecr.1c00389 ↗
22. Mechanistic and multiscale aspects of thermo-catalytic CO2 conversion to C1 products10.1039/D1CY00922B ↗
23. Structure Sensitivity of CO2 Conversion over Nickel Metal Nanoparticles Explained by Micro-Kinetics Simulations10.1021/jacsau.2c00430 ↗
24. Effect of the structure of Ni/TiO2 catalyst on CO2 methanation10.1016/j.ijhydene.2016.08.093 ↗
25. Multiscale Study of the Mechanism of Catalytic CO2 Hydrogenation: Role of the Ni(111) Facets10.1021/acscatal.0c01599 ↗
26. A comparative study of CO chemisorption on flat and stepped Ni surfaces using density functional theory10.1016/S0039-6028(03)00616-2 ↗
27. Optimizing Active Sites for High CO Selectivity during CO2 Hydrogenation over Supported Nickel Catalysts10.1021/jacs.0c12689 ↗
28. Dynamic Oxygen on Surface: Catalytic Intermediate and Coking Barrier in the Modeled CO2 Reforming of CH4 on Ni (111)10.1021/acscatal.6b00357 ↗
29. Recycling of CO2: Probing the Chemical State of the Ni(111) Surface during the Methanation Reaction with Ambient-Pressure X-Ray Photoelectron Spectroscopy10.1021/jacs.6b06939 ↗
30. CO2 Activation on Ni(111) and Ni(100) Surfaces in the Presence of H2O: An Ambient-Pressure X-ray Photoelectron Spectroscopy Study10.1021/acs.jpcc.8b11698 ↗
31. Beam-Induced Effects in Ambient Pressure Experiments with X-rays10.1021/bk-2021-1396.ch010 ↗
32. Contamination Issues in Ambient Pressure Experiments10.1021/bk-2021-1396.ch011 ↗
33. Site interconversion in chemisorbed CO on Ni(111): IRAS and work function studies10.1016/0039-6028(88)90594-8 ↗
34. IRAS study of the adsorption of CO on Ni(111): Interrelation between various bonding modes of chemisorbed CO10.1016/0039-6028(88)90593-6 ↗
35. Vibrational phase relaxation at surfaces: CO on Ni(111)10.1103/PhysRevLett.54.2119 ↗
36. The structure of CO on Ni(111)10.1063/1.442674 ↗
37. Extraction of kinetic parameters in temperature programmed desorption: A comparison of methods10.1063/1.453409 ↗
38. Displacement reaction of CO by NO on the Ni(111) surface10.1016/j.susc.2013.03.001 ↗
39. Determination of adsorption sites of pure and coadsorbed CO on Ni(111) by high resolution X-ray photoelectron spectroscopy10.1016/S0039-6028(98)80020-4 ↗
40. XPS/HREELS study of NiO films grown on Ni(111)10.1103/PhysRevB.60.2900 ↗
41. Insights into the mechanisms of CO2 methanation on Ni(111) surfaces by density functional theory10.1016/j.apsusc.2015.05.173 ↗
42. DFT study of the water-gas shift reaction and coke formation on Ni(111) and Ni(211) surfaces10.1021/jp302488f ↗
43. Insight into the mechanism of methane synthesis from syngas on a Ni(111) surface: a theoretical study10.1039/C4RA17096B ↗
44. DFT Investigation on the Competition of the Water-Gas Shift Reaction Versus Methanation on Clean and Potassium-Modified Nickel(111) Surfaces10.1002/cctc.201500547 ↗
45. Computational Investigation of Thermochemistry and Kinetics of Steam Methane Reforming on Ni(111) under Realistic Conditions10.1021/jp806527q ↗
46. Carbon monoxide interaction with oxygenated nickel single-crystal surfaces studied by vibrational spectroscopy10.1016/j.vibspec.2010.12.010 ↗
47. Vibrational investigation of catalyst surfaces: Change of the adsorption site of CO molecules upon coadsorption10.1021/jp202212a ↗
48. The surface geometry of carbon monoxide and oxygen co-adsorbed on Ni{11110.1524/zpch.218.8.915.35977 ↗
49. Co-adsorption of oxygen and carbon monoxide on Ni(111)10.1016/S0039-6028(03)00573-9 ↗
50. Interactions between chemisorbed CO and oxygen on Ni(111)10.1016/0039-6028(93)90329-I ↗
51. Adsorption of CO and NO on NiO (111)/Ni(111) surface studied by infrared-visible sum frequency generation spectroscopy10.1016/S0039-6028(97)00366-X ↗
52. Adsorption of CO and NO on NiO and CoO: A comparison10.1016/0039-6028(95)00997-3 ↗
53. Self-limited oxide formation in Ni(111) oxidation10.1103/PhysRevB.84.115441 ↗
54. Phase diagram of oxygen chemisorbed on nickel (111)10.1103/PhysRevB.23.6340 ↗
55. Ambient pressure photoelectron spectroscopy: Practical considerations and experimental frontiers10.1088/1361-648X/29/5/053002 ↗
56. Kinetics of reduction of nickel oxide with CO10.1002/aic.690180308 ↗
57. Surface oxidation of supported Ni particles and its impact on the catalytic performance during dynamically operated methanation of CO210.3390/catal7090279 ↗
58. The Electron Stimulated Interaction of H2O with a Nickel Surface
59. Mind the gap! Spectroscopy of catalytically active phases10.1016/S1748-0132(07)70114-7 ↗
60. Surface chemistry and catalysis of oxide model catalysts from single crystals to nanocrystals10.1016/j.surfrep.2019.100471 ↗
61. Effect of Surface Orientation on Methanol Adsorption and Thermally Induced Structural Transformations on Copper Surfaces10.1021/acs.jpcc.0c10278 ↗
62. Identification of Adsorbed Species and Surface Chemical State on Ag(111) in the Presence of Ethylene and Oxygen Studied with Infrared and X-ray Spectroscopies