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Publication date: Aug 06, 2024
In the pursuit of selective conversion of methane directly to methanol in the liquid phase, a common challenge is the concurrent formation of undesirable liquid oxygenates or combustion byproducts. However, we demonstrate that monometallic Pd-CeO2 catalysts, modified by carbon, created by a simple mechanochemical synthesis method exhibit 100% selectivity towards methanol at 75°C, using hydrogen peroxide as oxidizing agent. The solvent-free synthesis yields a distinctive Pd-iC-CeO2 interface, where interfacial carbon (iC) modulates metal-oxide interactions and facilitates tandem methane activation and peroxide decomposition, thus resulting in an exclusive methanol selectivity of 100% with a rate of 117 µmol/gcat at 75°C. Notably, solvent interactions of H2O2 (aq) were found to be critical for methanol selectivity through a DFT-simulated Eley-Rideal-like mechanism. This mechanism uniquely enables the direct conversion of methane into methanol via a solid-liquid-gas process.
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File name | Size | Description |
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references.zip
MD5md5:a4d3b68b3d8fd790c1e10abc2a1b2ce4
|
6.1 MiB | This file includes the DFT calculations for two catalysts, Pd.CeO2 and PdiC.CeO2, as well as the molecules CH4, H2O2, and CH3OH in the gas phase. |
CH4_activation.zip
MD5md5:83f66b825abb8454938d7a25257afb59
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54.9 MiB | Contains the adsorbed molecular state of CH4 and the dissociated state of CH3+H on each catalyst |
H2O2_activation.zip
MD5md5:f8afeaf5fc418bc9ef8cbebc24c883ff
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43.3 MiB | Includes the adsorbed molecular state of H2O2 and the dissociated state of OOH+H on each catalyst |
Langmuir-Hinshelwood_mechanism.zip
MD5md5:cc80cccc71c96bc73f35841b2e180f57
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222.8 MiB | Features the stable states considered through the Langmuir-Hinshelwood mechanism on each catalyst, corresponding to the two mechanisms shown in Figure 8. There are six states for PdiC.CeO2 with folders named A to F, and nine states for Pd.CeO2 with folders named a to i. |
Eley-Rideal_mechanism.zip
MD5md5:90dadc7c978402096dbfbdfdc34b6ad4
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196.5 MiB | Contains the stable states considered through the Langmuir-Hinshelwood mechanism for each catalyst, corresponding to the two mechanisms in Figure 9. There are three states, a, b, and c for PdiC.CeO2, and A, B, and C for Pd.CeO2. |
README.txt
MD5md5:b226dd0785c5267c8dcb48b48d0f0b59
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1.8 KiB | Readme file, includes tge description of the uploaded data |
2024.117 (version v1) [This version] | Aug 06, 2024 | DOI10.24435/materialscloud:dz-zz |