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Spatially confined electrochemical conversion of metal-organic frameworks into metal-sulfides and their in situ electrocatalytic investigation via scanning electrochemical microscopy.

ABSTRACT: There is an on-going search for new earth-abundant electrocatalytic materials, suitable for replacing noble-metals as efficient accelerators of energy-conversion reactions. In this regard, over the last few years, metal-organic framework (MOF)-converted materials have demonstrated promising electrocatalytic properties. Nevertheless, the discovery of new catalytic materials requires development of methods combining high-throughput synthesis and electrochemical-activity screening. To do so, here we couple the synthetical and the analytical virtues of scanning electrochemical microscopy (SECM). Namely, we first utilized an SECM tip electrode to induce spatially confined (?m-scale) electrochemical conversion of cobalt-based ZIF-67 MOFs into patterns of cobalt sulfide with a tuned chemical composition. In turn, the same SECM setup was used to map the H2 evolution activity of the as-formed cobalt sulfide. Hence, the presented method should have great implications for future screening of new electrocatalytic materials for a variety of energy-related applications.

SUBMITTER: Liberman I

PROVIDER: S-EPMC7012070 | biostudies-literature | 2020 Jan

REPOSITORIES: biostudies-literature

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Spatially confined electrochemical conversion of metal-organic frameworks into metal-sulfides and their <i>in situ</i> electrocatalytic investigation <i>via</i> scanning electrochemical microscopy.

Liberman Itamar I He Wenhui W Shimoni Ran R Ifraemov Raya R Hod Idan I

Chemical science 20191106 1

There is an on-going search for new earth-abundant electrocatalytic materials, suitable for replacing noble-metals as efficient accelerators of energy-conversion reactions. In this regard, over the last few years, metal-organic framework (MOF)-converted materials have demonstrated promising electrocatalytic properties. Nevertheless, the discovery of new catalytic materials requires development of methods combining high-throughput synthesis and electrochemical-activity screening. To do so, here w ...[more]

PMID: 32110369

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Project description:Metal-organic frameworks (MOFs) have been an excellent platform for carbon dioxide reduction reactions (CO2RR). In this work, the feasibility of electrochemical reduction of CO2 to obtain C2-deep value-added products was investigated by the preparation of Mg-containing MOF-74 samples combined with transition metal cations (Ni2+, Co2+ and Zn2+). The prepared MOFs were used as electrocatalysts in CO2RR. Chronoamperometric analysis coupled to ATR-FTIR spectroscopy was employed to characterize the CO2 reduction products and subsequently via 1H NMR. Although an isostructural crystalline structure was observed in all synthesized MOFs, the pore diameter distribution was significantly affected due to the Mg coordination along with each transition metal nuclei with the organic ligand to form the MOF-74. Our results showed that Mg-containing MOF-74 electrocatalysts combined with Ni, Co and Zn ions successfully reduced CO2 to C2-deep products, while the monometallic Mg-MOF-74 showed only CO2 mineralization. An ester acetate, isopropyl alcohol, and formic acid were produced by Mg/Ni-MOF-74; isopropyl alcohol was provided by Mg/Co-MOF-74, and ethanol was generated by Mg/Zn-MOF-74. We observed that the change of the transition cation was a key factor in the selectivity of the obtained products, while the degree of Mg ions effectively incorporated into the MOF structure tuned the porosity and the electrocatalytic activity. Among them, Mg/Zn-MFOF-74 showed the highest Mg content loaded after synthesis and thus the most favorable electrocatalytic behavior towards CO2 reduction. Highlights • CO2-derived C2-deep reduction products were obtained by Mg-containing MOF-74 bimetallic electrocatalysts.• Mg-containing MOF-74 bimetallic electrocatalysts reduced CO2 to ester acetate, isopropanol, formic acid, and ethanol.• Mg/Zn-MOF-74 displayed the highest current density at a lower onset potential in CO2-saturated electrolyte.• The pore network could be tuned by the effective Mg content on a MOF-74 bimetallic sample.• Mg/Zn-MOF-74 showed the highest Mg content among all bimetallic electrocatalysts after the synthesis.

Dataset Information

Spatially confined electrochemical conversion of metal-organic frameworks into metal-sulfides and their in situ electrocatalytic investigation via scanning electrochemical microscopy.

Publications

Spatially confined electrochemical conversion of metal-organic frameworks into metal-sulfides and their <i>in situ</i> electrocatalytic investigation <i>via</i> scanning electrochemical microscopy.

Similar Datasets

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