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Metal–Nitrogen–Carbon Catalysts by Dynamic Template Removal for Highly Efficient and Selective Electroreduction of CO 2

التفاصيل البيبلوغرافية
العنوان: Metal–Nitrogen–Carbon Catalysts by Dynamic Template Removal for Highly Efficient and Selective Electroreduction of CO 2
المؤلفون: Laurent Delafontaine (12866574), Alessio Cosenza (14317462), Eamonn Murphy (12574436), Yuanchao Liu (706751), Jiazhe Chen (14317465), Baiyu Sun (573321), Plamen Atanassov (522652)
سنة النشر: 2023
مصطلحات موضوعية: Biochemistry, Evolutionary Biology, Ecology, Infectious Diseases, Environmental Sciences not elsewhere classified, Chemical Sciences not elsewhere classified, substantial industrial limitations, require harsh acid, reducing greenhouse gase, prime cathode candidates, low overpotential (<, common pyrolytic precursors, based precursors via, ammonia atmosphere yield, 85 %) even, sacrificial poymer approach, 9 ± 0, nonabundant metal macrocycles, dynamic template removal, nonprecious metal catalysts, co , 2 , highly selective catalyst, e <, − 0, situ removal, postpyrolytic removal, highly efficient, highly desired, metal center
الوصف: The renewable electroreduction of CO 2 to CO is a key component of future clean energy scenarios. These scenarios allow for the recycling of carbon emissions into value-added chemicals which achieves the joint goal of reducing greenhouse gase(s) while producing valuable chemical product(s). A catalyst which has a high activity and selectivity for the electroreduction of CO 2 to CO is highly desired for these applications. Nonprecious metal catalysts (non-PGM) and specifically metal–nitrogen–carbon (M–N–C) catalysts are prime cathode candidates as they are selective for CO and H 2 formation with only trace amounts of other products such as CH 4 . The traditional method of production of atomically dispersed M–N–C proceeds either through a sacrificial poymer approach or through hard-templating the catalyst with silica. The other is through the direct pyrolysis of nonabundant metal macrocycles such as MOF-based precursors via a soft-templating approach. These syntheses have substantial industrial limitations as they require harsh acid or basic solvents for postpyrolytic removal of the support or they require rare chemical precursors. The method herein uses mechanochemical mixing of a fluorine-containing polymer with common pyrolytic precursors for the in situ removal of the template during the first pyrolysis. Further ball-milling and post-treatment in ammonia atmosphere yield a highly selective catalyst for CO 2 reduction. The role of the metal center in these M–N–C catalysts in promoting CO 2 reduction is explored (M = Fe, Ni, Co, Mn) vs the performance of metal-free N–C. A mechanistic pathway for CO 2 reduction on the various M–N–C catalysts is suggested. The champion catalyst in terms of overall selectivity/activity (Ni–N–C) boasts a 98.9 ± 0.2% faradaic efficiency for CO formation (FE co ) at −1.1 V vs RHE and an unmatched selectivity for CO 2 reduction (FE co > 85%) even at low overpotential ( E = −0.3 V vs RHE) compared to traditional Ni–N–C. The catalysts synthesized here present a promising class of ...
نوع الوثيقة: article in journal/newspaper
اللغة: unknown
Relation: https://figshare.com/articles/journal_contribution/Metal_Nitrogen_Carbon_Catalysts_by_Dynamic_Template_Removal_for_Highly_Efficient_and_Selective_Electroreduction_of_CO_sub_2_sub_/21804166
DOI: 10.1021/acsaem.2c02811.s001
الاتاحة: https://doi.org/10.1021/acsaem.2c02811.s001
Rights: CC BY-NC 4.0
رقم الانضمام: edsbas.DAB9540F
قاعدة البيانات: BASE
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