A microkinetic study of CO 2 hydrogenation to methanol on Pd 1 -Cu(111) and Pd 1 -Ag(111) catalysts: a DFT analysis.

التفاصيل البيبلوغرافية
العنوان:	A microkinetic study of CO 2 hydrogenation to methanol on Pd 1 -Cu(111) and Pd 1 -Ag(111) catalysts: a DFT analysis.
المؤلفون:	Ibrahim AO; Department of Chemical Engineering, University of Malaya, Kuala Lumpur, Malaysia. ashri@um.edu.my.; Sustainable Process Engineering Centre (SPEC), University of Malaya, Kuala Lumpur, Malaysia.; Department of Chemical Engineering, Ahmadu Bello University, Zaria 810222, Nigeria. ibrahimabdulrauf@abu.edu.ng., Wan Daud WMA; Department of Chemical Engineering, University of Malaya, Kuala Lumpur, Malaysia. ashri@um.edu.my.; Sustainable Process Engineering Centre (SPEC), University of Malaya, Kuala Lumpur, Malaysia., Abdul Patah MF; Department of Chemical Engineering, University of Malaya, Kuala Lumpur, Malaysia. ashri@um.edu.my.; Sustainable Process Engineering Centre (SPEC), University of Malaya, Kuala Lumpur, Malaysia., Halilu A; Department of Chemical Engineering, University of Malaya, Kuala Lumpur, Malaysia. ashri@um.edu.my.; Sustainable Process Engineering Centre (SPEC), University of Malaya, Kuala Lumpur, Malaysia., Juan JC; Nanotechnology & Catalysis Research Centre, Institute for Advanced Studies, University of Malaya, Kuala Lumpur, Malaysia., Tanimu G; Center for Refining & Advanced Chemicals, King Fahd University of Petroleum & Minerals, Dhahran 31261, Saudi Arabia.
المصدر:	Physical chemistry chemical physics : PCCP [Phys Chem Chem Phys] 2024 Apr 03; Vol. 26 (14), pp. 10622-10632. Date of Electronic Publication: 2024 Apr 03.
نوع المنشور:	Journal Article
اللغة:	English
بيانات الدورية:	Publisher: Royal Society of Chemistry Country of Publication: England NLM ID: 100888160 Publication Model: Electronic Cited Medium: Internet ISSN: 1463-9084 (Electronic) Linking ISSN: 14639076 NLM ISO Abbreviation: Phys Chem Chem Phys Subsets: PubMed not MEDLINE; MEDLINE
أسماء مطبوعة:	Original Publication: Cambridge [England] : Royal Society of Chemistry, c1999-
مستخلص:	The thermochemical conversion of CO 2 into methanol, a process known for its selectivity, often encounters a significant obstacle: the reverse water gas reaction. This problem emerges due to the demanding high temperatures and pressures, causing instability in catalytic performance. Recent endeavours have focused on innovatively designing catalysts capable of withstanding such conditions. Given the costliness of experimental approaches, a theoretical framework has emerged as a promising avenue for addressing the challenges in methanol production. It has been reported that transition metals, especially Pd, provide ideal binding sites for CO 2 molecules and hydrogen atoms, facilitating their interactions and subsequent conversion to methanol. In the geometric single-atom form, their surface enables precise control over the reaction pathways and enhances the selectivity towards methanol. In our study, we employed density functional theory (DFT) to explore the conversion of CO 2 to CH 3 OH on Pd 1 -Cu(111) and Pd 1 -Ag(111) single-atom alloy (SAA) catalysts. Our investigation involved mapping out the complex reaction pathways of CO 2 hydrogenation to CH 3 OH using microkinetic reaction modelling and mechanisms. We examined three distinct pathways: the COOH* formation pathway, the HCOO* formation pathway, and the dissociation of CO 2 * to CO* pathway. This comprehensive analysis encompassed the determination of adsorption energies for all reactants, transition states, and resultant products. Additionally, we investigated the thermodynamic and kinetic profiles of individual reaction steps. Our findings emphasised the essential role of the Pd single atom in enhancing the activation of CO 2 , highlighting the key mechanism underlying this catalytic process. The favoured route for methanol generation on the Pd 1 -Ag(111) single-atom alloy (SAA) surface unfolds as follows: CO 2 * progresses through a series of transformations, transitioning successively into HCOO, HCOOH, H 2 COOH, CH 2 O, and CH 2 OH, terminating in the formation of CH 3 OH, due to lower activation energies and higher rate constants.
تواريخ الأحداث:	Date Created: 20240320 Latest Revision: 20240409
رمز التحديث:	20240409
DOI:	10.1039/d4cp00070f
PMID:	38506646
قاعدة البيانات:	MEDLINE

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