Hydrothermal reduction of CO2 captured as NaHCO3 into formate with metal reductants and catalysts

Quintana-Gómez, Laura; Martínez‐Álvarez, Pablo; Segovia, José J.; Martín, Ángel; Bermejo, M. Dolores

doi:10.1016/j.jcou.2022.102369

Cited by 7 publications

(3 citation statements)

References 37 publications

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Section: Resultsmentioning

confidence: 55%

“…Because H 2 O is the only source of proton in this situation, produced formic acid (<2.5 ppm) and H 2 (∼1%) is comparatively limited. The production of formic acid from CO 2 in the thermal catalytic system is well established, as corroborated by the research of He et al, 12 Quintana-Goḿez et al, 13 and Andeŕez-Fernańdez et al 14 In contrast, the presence of CH 4 in the feed exerts a significant influence on the production of alcoholic products and acetic acid. Methanol and ethanol are found to reach the highest concentration when 25% CO 2 is present, with approximately 40 and 41 ppm, respectively.…”

Section: ■ Results and Discussionmentioning

confidence: 68%

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Long-Chain Hydrocarbons from Nonthermal Plasma-Driven Biogas Upcycling

Knezevic,

Zhang,

Zhou

et al. 2024

J. Am. Chem. Soc.

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The burgeoning necessity to discover new methodologies for the synthesis of long-chain hydrocarbons and oxygenates, independent of traditional reliance on high-temperature, high-pressure, and fossil fuel-based carbon, is increasingly urgent. In this context, we introduce a nonthermal plasma-based strategy for the initiation and propagation of long-chain carbon growth from biogas constituents (CO 2 and CH 4 ). Utilizing a plasma reactor operating at atmospheric room temperature, our approach facilitates hydrocarbon chain growth up to C40 in the solid state (including oxygenated products), predominantly when CH 4 exceeds CO 2 in the feedstock. This synthesis is driven by the hydrogenation of CO 2 and/or amalgamation of CH x radicals. Global plasma chemistry modeling underscores the pivotal role of electron temperature and CH x radical genesis, contingent upon varying CO 2 /CH 4 ratios in the plasma system. Concomitant with long-chain hydrocarbon production, the system also yields gaseous products, primarily syngas (H 2 and CO), as well as liquid-phase alcohols and acids. Our finding demonstrates the feasibility of atmospheric room-temperature synthesis of long-chain hydrocarbons, with the potential for tuning the chain length based on the feed gas composition.

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Section: Resultsmentioning

confidence: 55%

Section: ■ Results and Discussionmentioning

confidence: 68%

Long-Chain Hydrocarbons from Nonthermal Plasma-Driven Biogas Upcycling

Knezevic,

Zhang,

Zhou

et al. 2024

J. Am. Chem. Soc.

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“…Carbon capture, utilization, and sequestration are regarded as crucial strategies for mitigating the problems arising from an increasing CO 2 concentration in the atmosphere. Carbon utilization through photocatalysis, electrocatalysis, hydrothermal conversion, , and biological transformation is an appealing route for reducing CO 2 to produce value-added chemicals like methane, ethane, ethylene, formic acid, and large +C2 products. Electrochemical reduction of CO 2 can be performed at mild reaction conditions and can use cheap renewable electrical energy without any additional fossil-fuel-based electric power sources to obtain a wide selection of products. , Electrochemical reduction of CO 2 involves generating the anion radical (CO 2 –• ), which is formed when the CO 2 molecule gets sufficient energy and is adsorbed on the catalyst surface .…”

Section: Introductionmentioning

confidence: 99%

Copper-Doped Tin Oxides Supported on Mesoporous Carbon Xerogel for Boosting the Electrochemical Reduction of CO₂ to Formate in Bicarbonate Solution Coupled with CO₂

Kharel,

Gnanamani,

Hoque

et al. 2024

Ind. Eng. Chem. Res.

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The electrochemical reduction of CO 2 into valuable products at mild reaction conditions and using cheap renewable electrical energy are goals to sustain a low-carbon economy. Among the various CO 2 reduction reaction products, formic acid (FA) has received significant attention because of its low Gibbs free energy input requirement and the simple reduction reaction involving the transfer of 2 electrons and 2 protons. In this work, a copper-doped tin oxide catalyst supported on a mesoporous carbon xerogel was shown to enhance the electrochemical reduction of CO 2 to formate in a bicarbonate solution coupled with CO 2 . We observed that the synergistic SnCu oxides enhance the selectivity toward formate from 58.6% for Sn oxide and 28.7% for Cu oxide to over 71.2% for the SnCu oxides. The observed rate of formate production with SnCu oxide was 2.8 times higher compared to the rate of Cu oxide and about 1.5 times higher than with the Sn oxide catalyst. Our results reveal that selectivity for formate comes partly from the electrolysis of the bicarbonate solution and partly from continuous CO 2 gas purged into the solution. The contribution from the electrolysis of bicarbonate solution ranges from 15% to 40% when the concentration of bicarbonate solution ranges from 100 mM to 1 M. Chronoamperometric measurements for stability revealed that Cu oxide and Sn oxide showed stable current density for less than 30 h while under the same conditions, the stable current density was observed for more than 50 h with SnCu oxide catalyst. Additionally, the selectivity toward formate increased by 6% when the reactor pressure was increased from near ambient pressure to 4 psig. Our lab-scale electrochemical cell with SnCu oxide supported on the mesoporous carbon xerogel enhances the CO 2 solubility, minimizes the precipitation of salts that can degrade the catalytic performance, and suppresses the competitive hydrogen evolution reaction, demonstrating the feasibility of using our catalyst and system for the electrochemical conversion of CO 2 into formate with high selectivity, productivity, and stability. This could have significant implications for the mitigation of CO 2 emissions and the development of a sustainable chemical industry.

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Effect of Alkali‐ and Alkaline‐Earth‐Metal Promoters on Silica‐Supported Co−Fe Alloy for Autocatalytic CO₂ Fixation

Song,

Beyazay,

Tüysüz

2024

Angewandte Chemie

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Hydrothermal vents harbor numerous microbial communities rich in reduced carbon species such as formate, acetate, and hydrocarbons. Such essential chemicals for life are produced by H2‐dependent CO2 reduction, where serpentinization provides continuous H2 and thermal energy. Here, we show that silica‐supported bimetallic Co‐Fe alloys, naturally occurring minerals around serpentinite, can convert CO2 and H2O to key metabolic intermediates of the acetyl coenzyme A pathway such as formate (up to 72 mM), acetate, and pyruvate under mild hydrothermal vent conditions. Long‐chain hydrocarbons up to C6 including propene are also detected, just as in the Lost City hydrothermal field. The effects of promoters on structural properties and catalytic functionalities of the Co‐Fe alloy are systematically investigated by incorporating a series of alkali and alkaline earth metals including Na, Mg, K, and Ca. Alkali‐ and alkaline‐earth‐metals resulted in higher formate concentrations when dissolved in water and increased reaction pH, while alkaline earth metals also favored the formation of insoluble hydroxides and carbonates similar to the constituent minerals of the chimneys at the Lost City hydrothermal fields.

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Hydrothermal reduction of CO2 captured as NaHCO3 into formate with metal reductants and catalysts

Cited by 7 publications

References 37 publications

Long-Chain Hydrocarbons from Nonthermal Plasma-Driven Biogas Upcycling

Long-Chain Hydrocarbons from Nonthermal Plasma-Driven Biogas Upcycling

Copper-Doped Tin Oxides Supported on Mesoporous Carbon Xerogel for Boosting the Electrochemical Reduction of CO₂ to Formate in Bicarbonate Solution Coupled with CO₂

Effect of Alkali‐ and Alkaline‐Earth‐Metal Promoters on Silica‐Supported Co−Fe Alloy for Autocatalytic CO₂ Fixation

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Hydrothermal reduction of CO2 captured as NaHCO3 into formate with metal reductants and catalysts

Cited by 7 publications

References 37 publications

Long-Chain Hydrocarbons from Nonthermal Plasma-Driven Biogas Upcycling

Long-Chain Hydrocarbons from Nonthermal Plasma-Driven Biogas Upcycling

Copper-Doped Tin Oxides Supported on Mesoporous Carbon Xerogel for Boosting the Electrochemical Reduction of CO2 to Formate in Bicarbonate Solution Coupled with CO2

Effect of Alkali‐ and Alkaline‐Earth‐Metal Promoters on Silica‐Supported Co−Fe Alloy for Autocatalytic CO2 Fixation

Contact Info

Product

Resources

About

Copper-Doped Tin Oxides Supported on Mesoporous Carbon Xerogel for Boosting the Electrochemical Reduction of CO₂ to Formate in Bicarbonate Solution Coupled with CO₂

Effect of Alkali‐ and Alkaline‐Earth‐Metal Promoters on Silica‐Supported Co−Fe Alloy for Autocatalytic CO₂ Fixation