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Metal-free dehydrogenation of formic acid to H2 and CO2 using boron-based catalysts.

ABSTRACT: Formic acid is at the crossroads of novel sustainable energy strategies because it is an efficient H2 carrier. Yet, to date, its decomposition to H2 relies on metal-based catalysts. Herein, we describe the first metal-free catalysts able to promote the dehydrogenation of formic acid. Using dialkylborane derivatives, HCOOH is decomposed to H2 and CO2 in the presence of a base with high selectivity. Experimental and computational results point to the involvement of bis(formyloxy)borates as key intermediates in the C-H bond activation of a formate ligand.

SUBMITTER: Chauvier C

PROVIDER: S-EPMC5655896 | biostudies-other | 2015 May

REPOSITORIES: biostudies-other

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Metal-free dehydrogenation of formic acid to H2 and CO2 using boron-based catalysts.

Chauvier Clément C Tlili Anis A Das Neves Gomes Christophe C Thuéry Pierre P Cantat Thibault T

Chemical science 20150306 5

Formic acid is at the crossroads of novel sustainable energy strategies because it is an efficient H2 carrier. Yet, to date, its decomposition to H2 relies on metal-based catalysts. Herein, we describe the first metal-free catalysts able to promote the dehydrogenation of formic acid. Using dialkylborane derivatives, HCOOH is decomposed to H2 and CO2 in the presence of a base with high selectivity. Experimental and computational results point to the inv ...[more]

PMID: 29308170

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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

Metal-free dehydrogenation of formic acid to H2 and CO2 using boron-based catalysts.

Publications

Metal-free dehydrogenation of formic acid to H<sub>2</sub> and CO<sub>2</sub> using boron-based catalysts.

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