Artificial spherical chromatophore nanomicelles for selective CO2 reduction in water

Nature Catalysis, Год журнала: 2023, Номер 6(6), С. 464 - 475

Опубликована: Май 18, 2023

Язык: Английский

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Efficient Photocatalytic CO₂ Reduction in Ellagic Acid–Based Covalent Organic Frameworks

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(23), С. 16229 - 16236

Опубликована: Май 30, 2024

Employing covalent organic frameworks (COFs) for the photocatalytic CO2 reduction reaction (CDRR) to generate high-value chemical fuels and mitigate greenhouse gas emissions represents a sustainable catalytic conversion approach. However, achieving superior CDRR performance is hindered by challenges of low charge separation efficiency, poor stability, high preparation costs associated with COFs. Herein, in this work, we utilized perfluorinated metallophthalocyanine (MPcF16) biomolecule compound ellagic acid (EA) as building blocks actualize functional named EPM-COF (M = Co, Ni, Cu). The designed EPCo-COF, featuring cobalt metal active sites, demonstrated an impressive CO production rate selectivity (CDRR). Moreover, following alkaline treatment (EPCo-COF-AT), COF exposed carboxylic anion (COO–) hydroxyl group (OH), thereby enhancing electron-donating capability EA. This modification achieved heightened 17.7 mmol g–1 h–1 outstanding 97.8% efficient CDRR. Theoretical calculations further illustrated that EPCo-COF-AT functionalized COO– OH can effectively alleviate energy barriers involved process, which facilitates proton-coupled electron transfer processes enhances on sites within EPCo-COF-AT.

Язык: Английский

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Ligand-Bound CO₂ as a Nonclassical Route toward Efficient Photocatalytic CO₂ Reduction with a Ni N-Confused Porphyrin

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(15), С. 10550 - 10558

Опубликована: Апрель 8, 2024

Implementing the synergistic effects between metal and ligand has successfully streamlined energetics for CO2 activation gained high catalytic activities, establishing important breakthroughs in photocatalytic reduction. Herein, we describe a Ni(II) N-confused porphyrin complex (NiNCP) featuring an acidic N–H group. It is readily deprotonated exists anion form during catalysis. Owing to this functional site, NiNCP gave rise outstanding turnover number (TON) as 217,000 with 98% selectivity reduction CO, while parent (NiTPP) was found be nearly inactive. Our mechanistic analysis revealed nonclassical reaction pattern where effectively activated via attack of Lewis-basic ligand. The resulting ligand-bound adduct could further reduced produce CO. This new metal–ligand effect anticipated inspire design highly active catalysts small molecule activations.

Язык: Английский

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Identifying a highly efficient molecular photocatalytic CO2 reduction system via descriptor-based high-throughput screening

Nature Catalysis, Год журнала: 2025, Номер unknown

Опубликована: Фев. 7, 2025

Язык: Английский

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Bioinspired N4-metallomacrocycles for electrocatalytic oxygen reduction reaction

Coordination Chemistry Reviews, Год журнала: 2021, Номер 442, С. 213996 - 213996

Опубликована: Май 13, 2021

Язык: Английский

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