The renaissance of the Sabatier reaction and its applications on Earth and in space

Vogt, Charlotte; Monai, Matteo; Kramer, Gert Jan; Weckhuysen, Bert M.

doi:10.1038/s41929-019-0244-4

Cited by 475 publications

(315 citation statements)

References 76 publications

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“…The CO 2 stream produced from the decarbonation cell may also have value in applications that up-cycle captured CO 2 . CO 2 is already used to enhance oil recovery (EOR) (63,64) and to make chemicals such as urea, salicylic acid, methanol, carbonates (65), synthetic fuel (via the Fischer-Tropsch process) (66), and synthetic natural gas (via the Sabatier reaction) (67). There is growing interest in finding ways to react CO 2 electrochemically or photochemically to create chemicals and fuels from captured CO 2 using renewable electricity (68).…”

Section: Discussionmentioning

confidence: 99%

Toward electrochemical synthesis of cement—An electrolyzer-based process for decarbonating CaCO ₃ while producing useful gas streams

Ellis

Badel

Chiang

et al. 2019

Proc. Natl. Acad. Sci. U.S.A.

177

107

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Cement production is currently the largest single industrial emitter of CO2, accounting for ∼8% (2.8 Gtons/y) of global CO2emissions. Deep decarbonization of cement manufacturing will require remediation of both the CO2emissions due to the decomposition of CaCO3to CaO and that due to combustion of fossil fuels (primarily coal) in calcining (∼900 °C) and sintering (∼1,450 °C). Here, we demonstrate an electrochemical process that uses neutral water electrolysis to produce a pH gradient in which CaCO3is decarbonated at low pH and Ca(OH)2is precipitated at high pH, concurrently producing a high-purity O2/CO2gas mixture (1:2 molar ratio at stoichiometric operation) at the anode and H2at the cathode. We show that the solid Ca(OH)2product readily decomposes and reacts with SiO2to form alite, the majority cementitious phase in Portland cement. Electrochemical calcination produces concentrated gas streams from which CO2may be readily separated and sequestered, H2and/or O2may be used to generate electric power via fuel cells or combustors, O2may be used as a component of oxyfuel in the cement kiln to improve efficiency and lower CO2emissions, or the output gases may be used for other value-added processes such as liquid fuel production. Analysis shows that if the hydrogen produced by the reactor were combusted to heat the high-temperature kiln, the electrochemical cement process could be powered solely by renewable electricity.

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Section: Discussionmentioning

confidence: 99%

Toward electrochemical synthesis of cement—An electrolyzer-based process for decarbonating CaCO ₃ while producing useful gas streams

Ellis

Badel

Chiang

et al. 2019

Proc. Natl. Acad. Sci. U.S.A.

177

107

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“…The hydrogen gas liberated at the cathode could then be stored, and eventually combined with oxygen in a fuel cell, providing an entirely renewable and clean energy supply with water as the only reaction product. Hydrogen produced via this method could also be utilized for the reduction of anthropogenic CO 2 to produce chemical feedstocks and hydrocarbon fuels which are easier to transport than H 2 3,4 .…”

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confidence: 99%

Universal scaling relations for the rational design of molecular water oxidation catalysts with near-zero overpotential

et al. 2019

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A major roadblock in realizing large-scale production of hydrogen via electrochemical water splitting is the cost and inefficiency of current catalysts for the oxygen evolution reaction (OER). Computational research has driven important developments in understanding and designing heterogeneous OER catalysts using linear scaling relationships derived from computed binding energies. Herein, we interrogate 17 of the most active molecular OER catalysts, based on different transition metals (Ru, Mn, Fe, Co, Ni, and Cu), and show they obey similar scaling relations to those established for heterogeneous systems. However, we find that the conventional OER descriptor underestimates the activity for very active OER complexes as the standard approach neglects a crucial one-electron oxidation that many molecular catalysts undergo prior to O-O bond formation. Importantly, this additional step allows certain molecular catalysts to circumvent the "overpotential wall", leading to enhanced performance. With this knowledge, we establish fundamental principles for the design of ideal molecular OER catalysts.

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“…The utilization of carbon dioxide (CO 2 ), an important greenhouse gas , as a C 1 source has been the subject of intensive research over the past several decades. The use of CO 2 as a chemical feedstock could be a means of reducing atmospheric CO 2 concentrations, and CO 2 is also abundant, nontoxic and readily available . There is thus significant interest in the catalytic transformation of CO 2 via hydrogenation to produce chemicals, especially methanol (MeOH), because this is an important commodity chemical that serves as a versatile C 1 building block in chemical synthesis .…”

Section: Figurementioning

confidence: 99%

Catalytic Methylation of Aromatic Hydrocarbons using CO₂/H₂ over Re/TiO₂ and H‐MOR Catalysts

et al. 2020

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A combined catalyst comprising TiO 2 -supported Re (Re(1)/TiO 2 ; Re = 1 wt%) and H-MOR (SiO 2 /Al 2 O 3 = 90) was found to promote the methylation of benzene using CO 2 and H 2 . This catalytic system exhibited high performance with regard to the synthesis of methylated benzenes and gave high yields of total methylated products (up to 52 % benzene-based yield and 42 % CO 2based yield) under the reaction conditions employed in this study (p CO2 = 1 MPa; p H2 = 5 MPa; T = 250°C; t = 20 h) in a batch reactor. Catalyst screening demonstrated that a combination of Re(1)/TiO 2 and H-MOR (SiO 2 /Al 2 O 3 = 90) exhibited superior performance compared to other combinations of supported metal catalysts and zeolites in terms of both yield and selectivity for methylated benzenes.

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The renaissance of the Sabatier reaction and its applications on Earth and in space

Cited by 475 publications

References 76 publications

Toward electrochemical synthesis of cement—An electrolyzer-based process for decarbonating CaCO ₃ while producing useful gas streams

Toward electrochemical synthesis of cement—An electrolyzer-based process for decarbonating CaCO ₃ while producing useful gas streams

Universal scaling relations for the rational design of molecular water oxidation catalysts with near-zero overpotential

Catalytic Methylation of Aromatic Hydrocarbons using CO₂/H₂ over Re/TiO₂ and H‐MOR Catalysts

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The renaissance of the Sabatier reaction and its applications on Earth and in space

Cited by 475 publications

References 76 publications

Toward electrochemical synthesis of cement—An electrolyzer-based process for decarbonating CaCO 3 while producing useful gas streams

Toward electrochemical synthesis of cement—An electrolyzer-based process for decarbonating CaCO 3 while producing useful gas streams

Universal scaling relations for the rational design of molecular water oxidation catalysts with near-zero overpotential

Catalytic Methylation of Aromatic Hydrocarbons using CO2/H2 over Re/TiO2 and H‐MOR Catalysts

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Toward electrochemical synthesis of cement—An electrolyzer-based process for decarbonating CaCO ₃ while producing useful gas streams

Toward electrochemical synthesis of cement—An electrolyzer-based process for decarbonating CaCO ₃ while producing useful gas streams

Catalytic Methylation of Aromatic Hydrocarbons using CO₂/H₂ over Re/TiO₂ and H‐MOR Catalysts