Search for chemisorbed HCO: The interaction of formaldehyde, glyoxal, and atomic hydrogen + CO with Rh

Yates, John T.

doi:10.1016/0021-9517(82)90013-6

Cited by 52 publications

(14 citation statements)

References 32 publications

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“…After anchoring Au clusters, the intensities of absorption bands assigned to HCO 3 − , CO 2 − , and COOH* have decreased. There is a new band appearing at 1043 cm −1 , which is assigned to HCO* 42,43 . This indicates that part of the formed COOH* is converted to HCO*.…”

Section: Resultsmentioning

confidence: 99%

Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction

et al. 2021

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The surface electron density significantly affects the photocatalytic efficiency, especially the photocatalytic CO2 reduction reaction, which involves multi-electron participation in the conversion process. Herein, we propose a conceptually different mechanism for surface electron density modulation based on the model of Au anchored CdS. We firstly manipulate the direction of electron transfer by regulating the vacancy types of CdS. When electrons accumulate on vacancies instead of single Au atoms, the adsorption types of CO2 change from physical adsorption to chemical adsorption. More importantly, the surface electron density is manipulated by controlling the size of Au nanostructures. When Au nanoclusters downsize to single Au atoms, the strong hybridization of Au 5d and S 2p orbits accelerates the photo-electrons transfer onto the surface, resulting in more electrons available for CO2 reduction. As a result, the product generation rate of AuSA/Cd1−xS manifests a remarkable at least 113-fold enhancement compared with pristine Cd1−xS.

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Section: Resultsmentioning

confidence: 99%

Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction

et al. 2021

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“…This shift confirms the assignment of the 2015−2040 cm -1 band shown in Figure to linear CO instead of adsorbed CHO species. Yates and Cavanagh have shown that the wavenumber of the adsorbed CHO does not vary with its intensity . The shift in adsorbed CO wavenumber can be attributed to a dipole−dipole interaction between the linear CO on the surface of Rh. , If the supported Rh is highly dispersed, however, then adsorbed CO species would not interact with one another and thus would not give rise to a wavenumber shift.…”

Section: Resultsmentioning

confidence: 99%

“…The shift in the wavenumber of adsorbed CO with its intensity from 2038 to 2019 cm -1 , indicative of dipole−dipole interactions, is consistent with the observations depicted in Figure . Although the wavenumber of Rh−CHO species (Rh carbonyl hydride) falls in the same range as that of linear CO, the invariance of the Rh−CHO wavenumber with its intensity as well as the downward shift of the 2038−2019 cm -1 bands with their intensities ruled out the assignment of the 2038−2019 cm -1 band to a Rh−CHO species.…”

Section: Resultsmentioning

confidence: 99%

In Situ IR Study of Transient CO₂ Reforming of CH₄ over Rh/Al₂O₃

Stevens

Chuang

2003

J. Phys. Chem. B

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The CO2−CH4 reaction on Rh/Al2O3 was studied by in situ infrared spectroscopy coupled with pulse and step transient techniques. Steady-state isotopic 13CO transient studies at 773 K and 0.1 MPa show that the formation of gaseous 13CO2 closely follows that of linear 13CO, indicating that linear CO is an active adsorbate. Pulsing CH4 into CO2 flow and step switching from He to CO2/CH4 flow showed that the formation of H2 led that of CO, revealing that the first step of the reaction sequence is the decomposition of CH4 into *CH x species and hydrogen. Hydrogen activated adsorbed CO2 to produce linear CO. The linear CO was found to be the major species on Rh/Al2O3 during the reaction by in situ infrared spectroscopy. The accumulation of the linear CO on Rh0 sites revealed that the surface of Rh crystallites on Al2O3 remained in a reduced state throughout the study. The O2 pulse into CO2/CH4 resulted in (i) a total oxidation of CH4 to CO2 and H2O and then (ii) a net increase in the formation of the desired products, CO/H2, at a ratio of 1:1, revealing the promotion of the CO2−CH4 reaction. These are the first reported results on the enhancement of the CO and H2 formation rate via the pulse addition of oxygen into the CO2−CH4 reaction. The difference in product formation can be explained by two different types of adsorbed oxygen: one responsible for total oxidation and the other responsible for partial oxidation. The net increase in CO and H2 formation from the O2 pulse further suggests that combining mixed reforming of CH4 with CO2/O2 and selective poisoning of the total oxidation sites would enhance the selectivity and rate of CO/H2 formation.

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“…*COOH is widely accepted as a critical intermediate for CO 2 -to-CH 4 reduction, formed through a proton-coupled electron transfer process (CO 2 + e – + H + → *COOH). , Another two absorption bands at 1042 and 1166 cm –1 were the feature bands of *CH 3 O, while the absorption band at 1089 cm –1 was the characteristic band of *CHO. Both *CH 3 O and *CHO are the important intermediate products of CO 2 -to-CH 4 reduction. ,, A shoulder peak next to *COOH at 1683 cm –1 was the asymmetric stretching of *HCO 3 . Based on the in situ FTIR analysis, the selective CO 2 reduction to CH 4 was likely to proceed via the following steps It is still ambiguous why CH 3 OH was not the primary product despite its low reduction potential.…”

Section: Resultsmentioning

confidence: 99%

“…Both *CH 3 O and *CHO are the important intermediate products of CO 2 -to-CH 4 reduction. 13,37,38 A shoulder peak next to *COOH at 1683 cm −1 was the asymmetric stretching of *HCO 3 . 35 Based on the in situ FTIR analysis, the selective CO 2 reduction to CH 4 was likely to proceed via the following steps The data in the decaying curve could be correctly fitted by a doubleexponential function of I(t) = A 1 exp(-t/τ 1 ) + A 2 (-t/τ 2 ).…”

Section: Resultsmentioning

confidence: 99%

Highly Selective Photocatalytic CO₂ Reduction to CH₄ by Ball-Milled Cubic Silicon Carbide Nanoparticles under Visible-Light Irradiation

Sun

2021

ACS Appl. Mater. Interfaces

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The ultimate goal of photocatalytic CO2 reduction is to achieve high selectivity for a single product with high efficiency. One of the most significant challenges is that expensive catalysts prepared through complex processes are usually used. Herein, gram-scale cubic silicon carbide (3C-SiC) nanoparticles are prepared through a top-down ball-milling approach from low-priced 3C-SiC powders. This facile mechanical milling strategy ensures large-scale production of 3C-SiC nanoparticles with an amorphous silicon oxide (SiO x ) shell and simultaneously induces abundant surface states. The surface states are demonstrated to trap the photogenerated carriers, thus remarkably enhancing the charge separation, while the thin SiO x shell prevents 3C-SiC from corrosion under visible light. The unique electronic structure of 3C-SiC tackles the challenge associated with low selectivity of photocatalytic CO2 reduction to C1 compounds. In conjugation with efficient water oxidation, 3C-SiC nanoparticles can reduce CO2 into CH4 with selectivity over 90%.

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Search for chemisorbed HCO: The interaction of formaldehyde, glyoxal, and atomic hydrogen + CO with Rh

Cited by 52 publications

References 32 publications

Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction

Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction

In Situ IR Study of Transient CO₂ Reforming of CH₄ over Rh/Al₂O₃

Highly Selective Photocatalytic CO₂ Reduction to CH₄ by Ball-Milled Cubic Silicon Carbide Nanoparticles under Visible-Light Irradiation

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Search for chemisorbed HCO: The interaction of formaldehyde, glyoxal, and atomic hydrogen + CO with Rh

Cited by 52 publications

References 32 publications

Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction

Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction

In Situ IR Study of Transient CO2 Reforming of CH4 over Rh/Al2O3

Highly Selective Photocatalytic CO2 Reduction to CH4 by Ball-Milled Cubic Silicon Carbide Nanoparticles under Visible-Light Irradiation

Contact Info

Product

Resources

About

In Situ IR Study of Transient CO₂ Reforming of CH₄ over Rh/Al₂O₃

Highly Selective Photocatalytic CO₂ Reduction to CH₄ by Ball-Milled Cubic Silicon Carbide Nanoparticles under Visible-Light Irradiation