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Electrochemically coupled CH₄ and CO₂ consumption driven by microbial processes.

ABSTRACT: The chemical transformations of methane (CH₄) and carbon dioxide (CO₂) greenhouse gases typically have high energy barriers. Here we present an approach of strategic coupling of CH₄ oxidation and CO₂ reduction in a switched microbial process governed by redox cycling of iron minerals under temperate conditions. The presence of iron minerals leads to an obvious enhancement of carbon fixation, with the minerals acting as the electron acceptor for CH₄ oxidation and the electron donor for CO₂ reduction, facilitated by changes in the mineral structure. The electron flow between the two functionally active microbial consortia is tracked through electrochemistry, and the energy metabolism in these consortia is predicted at the genetic level. This study offers a promising strategy for the removal of CH₄ and CO₂ in the natural environment and proposes an engineering technique for the utilization of major greenhouse gases.

SUBMITTER: Zheng Y

PROVIDER: S-EPMC11006836 | biostudies-literature | 2024 Apr

REPOSITORIES: biostudies-literature

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Electrochemically coupled CH4 and CO2 consumption driven by microbial processes.

Zheng Yue Y Wang Huan H Liu Yan Y Liu Peiyu P Zhu Baoli B Zheng Yanning Y Li Jinhua J Chistoserdova Ludmila L Ren Zhiyong Jason ZJ Zhao Feng F

Nature communications 20240410 1

The chemical transformations of methane (CH4) and carbon dioxide (CO2) greenhouse gases typically have high energy barriers. Here we present an approach of strategic coupling of CH4 oxidation and CO2 reduction in a switched microbial process governed by redox cycling of iron minerals under temperate conditions. The presence of iron minerals leads to an obvious enhancement of carbon fixation, with the minerals acting as the electron acceptor for CH ...[more]

PMID: 38600111

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Project description:Solar-light driven reduction of CO2 to CH4 is a complex process involving multiple electron and proton transfer processes with various intermediates. Therefore, achieving high CH4 activity and selectivity remains a significant challenge. Covalent organic frameworks (COFs) represent an emerging class of photoactive semiconductors with molecular level structural tunability, modular band gaps, and high charge carrier generation and transport within the network. Here, we developed a new heterocyclic triazole ring containing COF, TFPB-TRZ, through the condensation reaction between 1,3,5-tris(4-formylphenyl)benzene (TFPB) and 3,5-diamino-1,2,4-triazole (TRZ). The TFPB-TRZ COF with multiple heteroatoms shows suitable visible light absorption, high CO2 uptake capability and an appropriate band diagram for CO2 photoreduction. Photocatalysis results reveal a maximum CO2 to CH4 conversion of 2.34 mmol g-1 with a rate of 128 μmol g-1 h-1 and high selectivity (∼99%) using 1-benzyl-1,4-dihydronicotinamide (BNAH) and triethylamine (TEA) as sacrificial agents. Under similar reaction conditions in the presence of direct sunlight, the TFPB-TRZ COF displays a maximum CH4 yield of 493 μmol g-1 with a rate of 61.62 μmol g-1 h-1, suggesting the robustness and light-harvesting ability of the COF photocatalyst. A femtosecond transient absorption (TA) spectroscopy study shows fast decay of excited state absorption (ESA) in the COF compared to the TFPB building unit due to efficient electron transfer to the catalytic site in the framework. The mechanism of CO2 reduction to CH4 is studied by DFT-based theoretical calculation, which is further supported by an in situ diffuse reflectance infrared Fourier transform spectroscopic (DRIFTS) study. The DFT results reveal that the lone pair of electrons on nitrogen heteroatoms present in the triazole ring of the TRZ moiety help in the stabilization of the CO intermediate during CO2 to CH4 conversion. Overall, this work demonstrates the use of a metal-free, recyclable COF-based photocatalytic system for solar energy storage by CO2 reduction.

Dataset Information

Electrochemically coupled CH₄ and CO₂ consumption driven by microbial processes.

Publications

Electrochemically coupled CH<sub>4</sub> and CO<sub>2</sub> consumption driven by microbial processes.

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