Incorporating Catalytic Units into Nanomaterials: Rational Design of Multipurpose Catalysts for CO₂ Valorization

Accounts of Chemical Research, Journal Year: 2023, Volume and Issue: 56(16), P. 2225 - 2240

Published: Aug. 3, 2023

ConspectusCO2 conversion to valuable chemicals is effective at reducing CO2 emissions. We previously proposed valorization strategies and developed efficient catalysts address thermodynamic stability kinetic inertness issues related conversion. Earlier, we molecular capture reagents integrate conversion, i.e., in situ transformation. Based on the mechanistic understanding of capture, activation, transformation a level, set out develop heterogeneous by incorporating catalytic units into nanomaterials via immobilization active onto designing with intrinsic sites.In thermocatalytic carbonaceous metal-organic framework (MOF)-based were for nonreductive reductive Novel Cu- Zn-based MOFs carbon-supported Cu prepared successfully applied cycloaddition, carboxylation, carboxylative cyclization reactions CO2, generating cyclic carbonates, carboxyl acids, oxazolidinones as respective target products. Reductive especially functionalization promising strategy produce chemicals, alleviating chemical production that relies petrochemistry. explored hierarchical using organocatalysts regulate reduction triggering catalyst investigation. Introducing multiple sites opens possibilities novel strategies. realized an N-doped Zn complex MOF materials adsorbents catalysts. These nanomaterial-based feature high excellent efficiency act shape-selective some cases due their unique pore structure.Nanomaterial-based are also appealing candidates photocatalytic (PCO2RR) electrocatalytic (ECO2RR), so series hybrid photo-/electrocatalysts metal complexes different matrixes such porous organic polymers (POPs), layers (MOLs), micelles, conducting polymers. By introducing Re-bipyridine Fe-porphyrin POPs regulating structure polymer chain, increased PCO2RR. PCO2RR aqueous solution was Re-bipyridine-containing amphiphilic form micelles nanoreactors. MOLs two metallic centers, Ni-bipyridine site Ni-O node, improve synergistic effect these centers. Sulfylphenoxy-decorated cobalt phthalocyanine (CoPc) cross-linked polypyrrole used cathode, achieving diluted benefiting from adsorption capability polypyrrole. fabricated immobilized 4-(t-butyl)-phenoxy Bi-MOF cathodes promote paired electrolysis 5-hydroxymethylfurfural (HMF) obtained products 2,5-furandicarboxylic acid (FDCA) efficiently.

Language: Английский

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Recent progress in CO₂ conversion into organic chemicals by molecular catalysis

Green Chemistry, Journal Year: 2023, Volume and Issue: 25(17), P. 6538 - 6560

Published: Jan. 1, 2023

An activation toolbox for the effective catalytic conversion of CO 2 to chemicals is proposed along with challenges and prospects related future development this exciting technology.

Language: Английский

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Recent Advances in Reactions Involving Carbon Dioxide Radical Anion

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(24), P. 15991 - 16011

Published: Nov. 28, 2023

Carbon dioxide radical anion (CO2•–) is a highly reactive nucleophilic species that has recently emerged in organic chemistry as strong single electron donor (reductant) and reactant for the synthesis of carboxylic acids. In general, CO2•– can be generated by either direct reduction CO2 or HAT formate salts. Achievements reactions involving have been witnessed recent years. This Review summarizes advances highlighting some challenges identifying potential areas improvement, which may offer inspiration future studies.

Language: Английский

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Photocatalytic Reduction of Carbon Dioxide to Methanol: Carbonaceous Materials, Kinetics, Industrial Feasibility, and Future Directions

Energy & Fuels, Journal Year: 2023, Volume and Issue: 37(11), P. 7577 - 7602

Published: May 16, 2023

Photocatalytic carbon dioxide reduction (PCCR) for methanol synthesis (CH3OH) targeting renewable energy resources is an attractive way to create a sustainable environment and also balance the carbon-neutral series. The application of PCCR enables generation solar while reducing CO2, killing two birds with one stone in terms environment. In recent years, research on CO2 utilization has focused hydrogenation due global warming. This article mainly focuses selective carbonaceous materials such as graphene, mesoporous carbon, nanotubes (CNTs) catalysts heterogeneous photocatalytic methanol. addition, special emphasis will be placed state art this type great benefit further development field. main features reaction kinetics, techno-economic study, current technological developments are covered detail.

Language: Английский

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CO2 capture and in-situ conversion to organic molecules

Journal of CO2 Utilization, Journal Year: 2024, Volume and Issue: 82, P. 102753 - 102753

Published: March 30, 2024

To address the CO2 accumulation in atmosphere, various initiatives have been proposed, among which capture and utilization (CCU) is regarded as an appealing strategy to reconcile carbon emission resource utilization. Especially, integrated (ICCU), i.e. performing in-situ conversion can circumvent energy-intensive desorption step thus facilitate establishing step- energy-efficient process, rendering at mild conditions particularly low pressure due substantial activation upon uptake. However, not simple add-up of these two processes. Its successful implementation relies on harmonization reagents, substrates corresponding catalysts. By far, tremendous efforts made this field a plethora reagents including inorganic bases, organic ionic liquids carbonaceous materials utilized protocols such hydrogenation, cycloaddition, carboxylative cyclization etc. explored for captured CO2. As result, valuable products containing methanol, methane, carbonates, carbamates, oxazolidinones, ureas, quinazolinone obtained from more importantly, chemistry theory also enriched via investigating structure reactivity reactions. In review, we summarize progress based reaction types absorbents. It's hoped that review shed light design inspire further development field.

Language: Английский

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Recent Progress on Photocatalytic CO₂ Conversion Reactions over Plasmonic Metal-based Catalysts

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(15), P. 10177 - 10204

Published: July 20, 2023

The massive consumption of fossil energy leads to excessive emissions CO2, which has caused global warming. Solar-driven CO2 conversion is a promising avenue that could solve the crisis and environmental pollution issues simultaneously. For photocatalytic reactions, several photocatalysts have been developed such as semiconductors plasmonic metal-based catalysts. Among them, catalysts attracted extensive attention due their strong light harvesting capacities low electron–hole pair recombination rates, are beneficial for conversion. This review summarizes progress in reduction with H2, CH4, H2O, organic chemicals generalizes mechanism reactions.

Language: Английский

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Efficient Solar‐Driven CO₂ Methanation and Hydrogen Storage Over Nickel Catalyst Derived from Metal–Organic Frameworks with Rich Oxygen Vacancies

Advanced Science, Journal Year: 2023, Volume and Issue: 10(34)

Published: Oct. 22, 2023

Solar-driven photothermal conversion of carbon dioxide (CO2 ) to methane (CH4 is a promising approach remedy energy shortage and climate changes, where highly efficient catalysts for CO2 methanation urgently need be designed. Herein, nickel-based (Ni/ZrO2 derived from metal-organic frameworks (MOFs) are fabricated studied methanation. The optimized catalyst 50Ni/ZrO2 achieves stable CH4 production rate 583.3 mmol g-1 h-1 in continuous stability test, which almost tenfold higher than that 50Ni/C-ZrO2 synthesized via commercial ZrO2 . Physicochemical properties indicate generates more tetragonal possesses oxygen vacancies (OVs) as well enhanced nickel-ZrO2 interaction. As result, exhibits the strong abilities light absorption light-to-heat conversion, superior adsorption capacities reactants (H2 , ), an intermediate product (CO), finally boosts formation. This work provides strategy design photothermocatalyst through utilizing MOFs-derived support.

Language: Английский

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Adaptive mechanism of the marine bacterium Pseudomonas sihuiensis-BFB-6S towards pCO2 variation: Insights into synthesis of extracellular polymeric substances and physiochemical modulation

International Journal of Biological Macromolecules, Journal Year: 2024, Volume and Issue: 261, P. 129860 - 129860

Published: Feb. 1, 2024

Language: Английский

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Nickel-Catalyzed Lactamization Reaction of 2-Arylanilines with CO₂

Organic Letters, Journal Year: 2024, Volume and Issue: 26(18), P. 3940 - 3944

Published: April 30, 2024

Transition-metal-catalyzed lactamization and lactonization of C–H bonds with CO2 assisted by the chelation amino or hydroxyl groups have been developed but limited to use precious metal catalysts such as palladium rhodium. In this work, we report nonprecious nickel-catalyzed reaction 2-arylanilines under redox-neutral conditions via bond activation. The displayed excellent functional group tolerance, providing various phenanthridinones moderate high yields.

Language: Английский

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Improved CO selectivity during CO2 hydrogenation by bimetallic copper-cobalt supported SBA-15

Journal of CO2 Utilization, Journal Year: 2025, Volume and Issue: 92, P. 103032 - 103032

Published: Jan. 30, 2025

Language: Английский

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