https://scholars.lib.ntu.edu.tw/handle/123456789/606873
標題: | MOF-Templated Sulfurization of Atomically Dispersed Manganese Catalysts Facilitating Electroreduction of CO2to CO | 作者: | Tan H.-Y Lin S.-C Wang J Chang C.-J Haw S.-C Lin K.-H Tsai L.D Chen H.-C Chen H.M. HAO MING CHEN |
關鍵字: | eCO2RR;metal-organic framework;operando spectroscopy;single-atom catalysts;sulfurization;XAS;Atoms;Carbon dioxide;Catalysts;Electrolytic reduction;Manganese;Metal-Organic Frameworks;Organometallics;Sulfur;Central metals;Characterization techniques;Electroreduction of CO2;Energy systems;Faradaic efficiencies;Metalorganic frameworks (MOFs);Potential materials;Spectroscopic characterization;Manganese compounds | 公開日期: | 2021 | 卷: | 13 | 期: | 44 | 起(迄)頁: | 52134-52143 | 來源出版物: | ACS Applied Materials and Interfaces | 摘要: | To reach a carbon-neutral future, electrochemical CO2 reduction reaction (eCO2RR) has proven to be a strong candidate for the next-generation energy system. Among potential materials, single-atom catalysts (SACs) serve as a model to study the mechanism behind the reduction of CO2 to CO, given their well-defined active metal centers and structural simplicity. Moreover, using metal-organic frameworks (MOFs) as supports to anchor and stabilize central metal atoms, the common concern, metal aggregation, for SACs can be addressed well. Furthermore, with their turnability and designability, MOF-derived SACs can also extend the scope of research on SACs for the eCO2RR. Herein, we synthesize sulfurized MOF-derived Mn SACs to study effects of the S dopant on the eCO2RR. Using complementary characterization techniques, the metal moiety of the sulfurized MOF-derived Mn SACs (MnSA/SNC) is identified as MnN3S1. Compared with its non-sulfur-modified counterpart (MnSA/NC), the MnSA/SNC provides uniformly superior activity to produce CO. Specifically, a nearly 30% enhancement of Faradaic efficiency (F.E.) in CO production is observed, and the highest F.E. of approximately 70% is identified at -0.45 V. Through operando spectroscopic characterization, the probing results reveal that the overall enhancement of CO production on the MnSA/SNC is possibly caused by the S atom in the local MnN3S1 moiety, as the sulfur atom may induce the formation of S-O bonding to stabilize the critical intermediate, *COOH, for CO2-to-CO. Our results provide novel design insights into the field of SACs for the eCO2RR. ? 2021 American Chemical Society. |
URI: | https://www.scopus.com/inward/record.uri?eid=2-s2.0-85111182382&doi=10.1021%2facsami.1c10059&partnerID=40&md5=8d410afef5349c6c7bd3c82998d45db6 https://scholars.lib.ntu.edu.tw/handle/123456789/606873 |
ISSN: | 19448244 | DOI: | 10.1021/acsami.1c10059 |
顯示於: | 化學系 |
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