Understanding the complexity in bridging thermal and electrocatalytic methanation of CO₂

Chemical Society Reviews, Год журнала: 2023, Номер 52(11), С. 3627 - 3662

Опубликована: Янв. 1, 2023

The selective methanation of CO2 is an important research area to meet the net-zero emission targets. Furthermore, it crucial develop solutions achieve carbon neutrality, hydrogen utilization, circularity, and chemical-energy storage. This conversion can be realized via thermocatalytic multistep power-to-X route or by direct electro- (or photoelectro)-catalytic technologies. Herein, we discuss need accelerate Improving these technologies requires a better understanding catalytic chemistry complexity aspects consider in bridging electrocatalytic methanation. In this tutorial review, initially analyze fundamental question competitive adsorption key reactants regulation strategies promote overall reaction. Then, approach used guide reader differences between thermocatalysis electrocatalysis. Finally, necessary include modelling designing next-generation electrocatalysts for analyzed.

Язык: Английский

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Recent Advances in Electrochemical CO₂‐to‐Multicarbon Conversion: From Fundamentals to Industrialization

Advanced Energy Materials, Год журнала: 2023, Номер 13(47)

Опубликована: Ноя. 2, 2023

Abstract The electrochemical CO 2 (eCO )‐to‐multicarbon conversion with higher value is regarded as a potential way to promote the transformation of industrial production and green balance carbon cycle. Recently, series advances have been achieved in progress eCO ‐to‐multicarbon conversion, including in‐depth exploration coupling mechanisms, up‐to‐date development characterization techniques, novel interdisciplinary design strategies catalysts electrolytic systems. Therefore, it essential systematically overview from fundamentals industrialization, compensating for limited insufficient reviews that reported. To fill aforementioned research gap, this focused on industrialization. First, possible catalytic mechanisms are accordingly summarized order reduction, small molecule‐coupled tandem conversion. Second, situ technologies assisting rationalization presented. Third, optimizing systems briefly classified advance industrialization process. Finally, challenges perspectives further reasonably proposed, aiming offer insights following work field.

Язык: Английский

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Perovskite‐Derived Bismuth with I⁻ and Cs⁺ Dual Modification for High‐Efficiency CO₂‐to‐Formate Electrosynthesis and Al‐CO₂ Batteries

Advanced Materials, Год журнала: 2023, Номер 35(36)

Опубликована: Июнь 7, 2023

Abstract Bi‐based materials are one of the most promising candidates for electrochemical CO 2 reduction reaction (CO RR) to formate; however, majority them still suffer from low current density and stability that essentially constrain their potential applications at industrial scale. Surface modification represents an effective approach modulate electrode microenvironment relative binding strength key intermediates. Herein, it is demonstrated surface comodification with halides alkali metal ions conversion halide perovskite nanocrystals a viable strategy boost RR performance Bi formate electrosynthesis. Cs 3 I 9 prepared by hot‐injection method. The as‐prepared products feature well‐defined hexagonal shape uniform size distribution. When used as precatalyst, converted + − comodified Bi. resultant catalyst exhibits high Faradaic efficiency close 100%, remarkable partial up 44 mA cm −2 in H‐cell 276 flow cell. Moreover, cathode paired Al anode Al‐CO battery simultaneous valorization power generation.

Язык: Английский

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Carbon dioxide and "methanol" economy: advances in the catalytic synthesis of methanol from CO₂

Russian Chemical Reviews, Год журнала: 2024, Номер 93(1), С. RCR5101 - RCR5101

Опубликована: Янв. 1, 2024

Development of the "methanol" economy may be a way to establish new chemistry under decarbonization conditions. Methanol here is used as raw material for production wide range chemicals, conventionally obtained from oil. The key process reduction CO₂, which, along with renewable energy, main carbon-containing resource in low-carbon industry. This review summarizes recent data on approaches methanol CO₂: catalytic hydrogenation CO₂ hydrogen heterogeneous or homogeneous catalysts; electrochemical CO2 methanol; and conversion using photocatalysis. advantages disadvantages each method, mechanisms taking into account features type catalysis, efficient catalysts are discussed.<br> bibliography includes 542 references.

Язык: Английский

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Microenvironment regulation breaks the Faradaic efficiency-current density trade-off for electrocatalytic deuteration using D2O

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Июнь 19, 2024

Abstract The high Faradaic efficiency (FE) of the electrocatalytic deuteration organics with D 2 O at a large current density is significant for deuterated electrosynthesis. However, FE and are two ends seesaw because severe evolution side reaction nearly industrial densities. Herein, we report combined scenario nanotip-enhanced electric field surfactant-modified interface microenvironment to enable arylacetonitrile in an 80% −100 mA cm −2 . increased concentration low activation energy due along tips accelerated transfer suppressed by surfactant-created deuterophobic contribute breaking trade-off between density. Furthermore, application our strategy other reactions improved efficiencies rationalizes design concept.

Язык: Английский

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Value‐Added Cascade Synthesis Mediated by Paired‐Electrolysis Using an Ultrathin Microenvironment‐Inbuilt Metalized Covalent Organic Framework Heterojunction

Advanced Energy Materials, Год журнала: 2024, Номер 14(27)

Опубликована: Апрель 25, 2024

Abstract Energy‐saving and value‐added management in advanced catalysis is highly desirable but challenged by the limitations of multifunctional catalysts catalytic modules. Herein, an azo‐linked phthalocyanine‐porphyrin covalent organic framework (COF) with ultrathin layered nanostructure grown on carbon nanotubes (NiPc‐azo‐H2Pp@CNTs) has been designed synthesized, which can serve as a active stable bifunctional heterojunction electrocatalyst for selective paired‐electrosynthesis through coupling anodic iodide oxidation reaction cathodic CO 2 conversion. Particularly, inbuilt local microenvironment conferred dihydroporphyrin moieties COF act proton reservoir to promote relay at interface during electrocatalytic process. Moreover, cascade construction dual electrocatalytic/organocatalytic modules, cathode‐generated be further converted dimethyl carbonate yield 6.21 mmol L −1 h , while anode‐produced iodine derived into iodoform hundred‐milligram scale. It worth noting that synthesis mediated paired‐electrolysis using distinctive high‐powered electrocatalysts will help advance sustainable development industrial intelligent manufacturing.

Язык: Английский

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Restructuring multi-phase interfaces from Cu-based metal–organic frameworks for selective electroreduction of CO₂ to C₂H₄

Chemical Science, Год журнала: 2024, Номер 15(24), С. 9173 - 9182

Опубликована: Янв. 1, 2024

Directional in situ reconfiguration of Ag incorporating HKUST-1 frameworks was introduced to restructure multi-phase Ag/Cu/Cu 2 O electrocatalysts for the selective electro-reduction CO C H 4 .

Язык: Английский

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Modulating Interfacial Hydrogen-Bond Environment by Electrolyte Engineering Promotes Acidic CO₂ Electrolysis

ACS Catalysis, Год журнала: 2024, Номер 14(14), С. 10529 - 10537

Опубликована: Июнь 27, 2024

Язык: Английский

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In situ reconstruction of Bi nanoparticles confined within 3D nanoporous Cu to boost CO2 electroreduction

Science China Materials, Год журнала: 2024, Номер 67(3), С. 796 - 803

Опубликована: Фев. 22, 2024

Due to the low efficiency of a single metal Bi in CO2 reduction reaction (CO2RR) formates, enhancing conductivity and yield through surface engineered composites is an alluring approach. In this study, we reconstruct nanoparticles situ growth 3D nanoporous copper structures. Benefiting from conductive network strong interaction between Cu Bi, Fermi level becomes shifted upward resulting Bi@np-Cu displays surprising CO2RR performance. demonstrates formate faradaic 97.7% at potential −0.97 V vs. reversible hydrogen electrode with remarkable current density 82 mA cm−2. Importantly, catalyst also has more than 90% for continuous 40 h. Density function theory calculations reveal that np-Cu effectively modulates electronic states optimizing intermediate adsorption energy leading increased intrinsic activity Bi. This study provides novel perspective on applications metals catalysis.

Язык: Английский

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Critical Role of Cu Nanoparticle-Loaded Cu(100) Surface Structures on Structured Copper-Based Catalysts in Boosting Ethanol Generation in CO₂ Electroreduction

ACS Applied Materials & Interfaces, Год журнала: 2024, Номер 16(27), С. 35143 - 35154

Опубликована: Июнь 29, 2024

Presently, realizing high ethanol selectivity in CO2 electroreduction remains challenging due to difficult C–C coupling and fierce product competition. In this work, we report an innovative approach for improving the efficiency of Cu-based electrocatalysts generation from electrocatalytic reduction using a crystal plane modification strategy. These novel were fabricated by electrochemically activating three-dimensional (3D) flower-like CuO micro/nanostructures grown situ on copper foils modifying with surfactants. It was demonstrated that electrocatalyst featured predominantly exposed Cu(100) surface loaded high-density Cu nanoparticles (NPs). The optimal displayed considerably improved performance, Faraday 37.9% maximum 68.0% C2+ products at −1.4 V vs RHE H-cell, accompanied current density 69.9 mA·cm–2, much better than particulate electrocatalyst. unveiled Cu(100)-rich nanoscale petals abundant under-coordinated atoms CuNPs conducive formation stabilization key *CH3CHO *OC2H5 intermediates, thereby promoting generation. This study highlighted critical role CuNP-loaded structures structured enhancing production process.

Язык: Английский

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