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Engineered assembly of water-dispersible nanocatalysts enables low-cost and green CO₂ capture.

ABSTRACT: Catalytic solvent regeneration has attracted broad interest owing to its potential to reduce energy consumption in CO₂ separation, enabling industry to achieve emission reduction targets of the Paris Climate Accord. Despite recent advances, the development of engineered acidic nanocatalysts with unique characteristics remains a challenge. Herein, we establish a strategy to tailor the physicochemical properties of metal-organic frameworks (MOFs) for the synthesis of water-dispersible core-shell nanocatalysts with ease of use. We demonstrate that functionalized nanoclusters (Fe₃O₄-COOH) effectively induce missing-linker deficiencies and fabricate mesoporosity during the self-assembly of MOFs. Superacid sites are created by introducing chelating sulfates on the uncoordinated metal clusters, providing high proton donation capability. The obtained nanomaterials drastically reduce the energy consumption of CO₂ capture by 44.7% using only 0.1 wt.% nanocatalyst, which is a ∽10-fold improvement in efficiency compared to heterogeneous catalysts. This research represents a new avenue for the next generation of advanced nanomaterials in catalytic solvent regeneration.

SUBMITTER: Alivand MS

PROVIDER: S-EPMC8913730 | biostudies-literature | 2022 Mar

REPOSITORIES: biostudies-literature

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Engineered assembly of water-dispersible nanocatalysts enables low-cost and green CO<sub>2</sub> capture.

Alivand Masood S MS Mazaheri Omid O Wu Yue Y Zavabeti Ali A Christofferson Andrew J AJ Meftahi Nastaran N Russo Salvy P SP Stevens Geoffrey W GW Scholes Colin A CA Mumford Kathryn A KA

Nature communications 20220310 1

Catalytic solvent regeneration has attracted broad interest owing to its potential to reduce energy consumption in CO<sub>2</sub> separation, enabling industry to achieve emission reduction targets of the Paris Climate Accord. Despite recent advances, the development of engineered acidic nanocatalysts with unique characteristics remains a challenge. Herein, we establish a strategy to tailor the physicochemical properties of metal-organic frameworks (MOFs) for the synthesis of water-dispersible c ...[more]

PMID: 35273166

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Project description:Supported by increasingly available reserves, natural gas is achieving greater adoption as a cleaner-burning alternative to coal in the power sector. As a result, carbon capture and sequestration from natural gas-fired power plants is an attractive strategy to mitigate global anthropogenic CO2 emissions. However, the separation of CO2 from other components in the flue streams of gas-fired power plants is particularly challenging due to the low CO2 partial pressure (∼40 mbar), which necessitates that candidate separation materials bind CO2 strongly at low partial pressures (≤4 mbar) to capture ≥90% of the emitted CO2. High partial pressures of O2 (120 mbar) and water (80 mbar) in these flue streams have also presented significant barriers to the deployment of new technologies for CO2 capture from gas-fired power plants. Here, we demonstrate that functionalization of the metal-organic framework Mg2(dobpdc) (dobpdc4- = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) with the cyclic diamine 2-(aminomethyl)piperidine (2-ampd) produces an adsorbent that is capable of ≥90% CO2 capture from a humid natural gas flue emission stream, as confirmed by breakthrough measurements. This material captures CO2 by a cooperative mechanism that enables access to a large CO2 cycling capacity with a small temperature swing (2.4 mmol CO2/g with ΔT = 100 °C). Significantly, multicomponent adsorption experiments, infrared spectroscopy, magic angle spinning solid-state NMR spectroscopy, and van der Waals-corrected density functional theory studies suggest that water enhances CO2 capture in 2-ampd-Mg2(dobpdc) through hydrogen-bonding interactions with the carbamate groups of the ammonium carbamate chains formed upon CO2 adsorption, thereby increasing the thermodynamic driving force for CO2 binding. In light of the exceptional thermal and oxidative stability of 2-ampd-Mg2(dobpdc), its high CO2 adsorption capacity, and its high CO2 capture rate from a simulated natural gas flue emission stream, this material is one of the most promising adsorbents to date for this important separation.

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Engineered assembly of water-dispersible nanocatalysts enables low-cost and green CO₂ capture.

Publications

Engineered assembly of water-dispersible nanocatalysts enables low-cost and green CO<sub>2</sub> capture.

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Engineered assembly of water-dispersible nanocatalysts enables low-cost and green CO2 capture.

Publications

Engineered assembly of water-dispersible nanocatalysts enables low-cost and green CO<sub>2</sub> capture.

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OmicsDI is part of the ELIXIR infrastructure

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Engineered assembly of water-dispersible nanocatalysts enables low-cost and green CO₂ capture.