From Methane to Methanol: Pd-iC-CeO2 Catalysts Engineered for High Selectivity via Mechano-Chemical Synthesis
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{
"id": "2281",
"updated": "2024-08-06T07:49:28.554634+00:00",
"metadata": {
"version": 1,
"contributors": [
{
"givennames": "Juan D.",
"affiliations": [
"Chemistry Division, Brookhaven National Laboratory, Upton, NY, 11973, USA"
],
"familyname": "Jim\u00e9nez"
},
{
"givennames": "Pablo G.",
"affiliations": [
"Institute of Catalysis and Petrochemistry, ICP, Spanish National Research Council, CSIC, 28049 Madrid, Spain"
],
"email": "p.lustemberg@csic.es",
"familyname": "Lustemberg"
},
{
"givennames": "Maila",
"affiliations": [
"Polytechnic Department, University of Udine and INSTM, Via del Cotonificio 108, 33100 Udine"
],
"familyname": "Danielis"
},
{
"givennames": "Estefan\u00eda",
"affiliations": [
"Institute of Catalysis and Petrochemistry, ICP, Spanish National Research Council, CSIC, 28049 Madrid, Spain",
"Universitat Polit\u00e8cnica de Val\u00e8ncia, Cam\u00ed de Vera s/n, 46022, Val\u00e8ncia, Spain"
],
"familyname": "Fern\u00e1ndez-Villanueva"
},
{
"givennames": "Sooyeon",
"affiliations": [
"Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, 11973, USA"
],
"familyname": "Hwang"
},
{
"givennames": "Iradwikanari",
"affiliations": [
"National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, New York 11973, USA"
],
"familyname": "Waluyo"
},
{
"givennames": "Adrian",
"affiliations": [
"National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, New York 11973, USA"
],
"familyname": "Hunt"
},
{
"givennames": "Dominik",
"affiliations": [
"National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, New York 11973, USA"
],
"familyname": "Wierzbicki"
},
{
"givennames": "Jie",
"affiliations": [
"Ames National Laboratory, Iowa State University, Ames, Iowa, 50011, USA"
],
"familyname": "Zhang"
},
{
"givennames": "Long",
"affiliations": [
"Ames National Laboratory, Iowa State University, Ames, Iowa, 50011, USA"
],
"familyname": "Qi"
},
{
"givennames": "Alessandro",
"affiliations": [
"Polytechnic Department, University of Udine and INSTM, Via del Cotonificio 108, 33100 Udine"
],
"familyname": "Trovarelli"
},
{
"givennames": "Jose A.",
"affiliations": [
"Chemistry Division, Brookhaven National Laboratory, Upton, NY, 11973, USA",
"Department of Chemistry, State University of New York Stony Brook, Stony Brook, NY 11794, USA"
],
"familyname": "Rodriguez"
},
{
"givennames": "Sara",
"affiliations": [
"Polytechnic Department, University of Udine and INSTM, Via del Cotonificio 108, 33100 Udine"
],
"familyname": "Colussi"
},
{
"givennames": "M. Ver\u00f3nica",
"affiliations": [
"Institute of Catalysis and Petrochemistry, ICP, Spanish National Research Council, CSIC, 28049 Madrid, Spain"
],
"familyname": "Ganduglia-Pirovano"
},
{
"givennames": "Sanjaya D.",
"affiliations": [
"Chemistry Division, Brookhaven National Laboratory, Upton, NY, 11973, USA"
],
"familyname": "Senanayake"
}
],
"title": "From Methane to Methanol: Pd-iC-CeO2 Catalysts Engineered for High Selectivity via Mechano-Chemical Synthesis",
"_oai": {
"id": "oai:materialscloud.org:2281"
},
"keywords": [
"Pd.CeO2",
"PdC.CeO2",
"CH4",
"CH3OH",
"H2O2",
"Eley-Rideal mechanism"
],
"publication_date": "Aug 06, 2024, 09:49:28",
"_files": [
{
"key": "references.zip",
"description": "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.",
"checksum": "md5:a4d3b68b3d8fd790c1e10abc2a1b2ce4",
"size": 6429030
},
{
"key": "CH4_activation.zip",
"description": "Contains the adsorbed molecular state of CH4 and the dissociated state of CH3+H on each catalyst",
"checksum": "md5:83f66b825abb8454938d7a25257afb59",
"size": 57538912
},
{
"key": "H2O2_activation.zip",
"description": "Includes the adsorbed molecular state of H2O2 and the dissociated state of OOH+H on each catalyst",
"checksum": "md5:f8afeaf5fc418bc9ef8cbebc24c883ff",
"size": 45390441
},
{
"key": "Langmuir-Hinshelwood_mechanism.zip",
"description": "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.",
"checksum": "md5:cc80cccc71c96bc73f35841b2e180f57",
"size": 233610454
},
{
"key": "Eley-Rideal_mechanism.zip",
"description": "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.",
"checksum": "md5:90dadc7c978402096dbfbdfdc34b6ad4",
"size": 205999985
},
{
"key": "README.txt",
"description": "Readme file, includes tge description of the uploaded data",
"checksum": "md5:b226dd0785c5267c8dcb48b48d0f0b59",
"size": 1853
}
],
"references": [
{
"citation": "J. D. Jim\u00e9nez, P. G. Lustemberg, M. Danielis, E. Fern\u00e1ndez-Villanueva, S. Hwang, I. Waluyo, A. Hunt, D. Wierzbicki, J. Zhang, L. Qi, A. Trovarelli, J. A. Rodriguez, S. Colussi, M. V. Ganduglia-Pirovano, S. D. Senanayake, J. Am. Chem. Soc, XX, XXX-XXX (2024)",
"type": "Journal reference"
}
],
"description": "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\u00b0C, 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 \u00b5mol/gcat at 75\u00b0C. 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.",
"status": "published",
"license": "Creative Commons Attribution 4.0 International",
"conceptrecid": "2280",
"is_last": true,
"mcid": "2024.117",
"edited_by": 98,
"id": "2281",
"owner": 64,
"license_addendum": null,
"doi": "10.24435/materialscloud:dz-zz"
},
"revision": 5,
"created": "2024-08-02T14:48:36.448477+00:00"
}