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Catalysis

Catalysis

The presence of a catalyst affects the rate of a chemical reaction. A catalyst is a substance that can increase the reaction rate without being consumed during the process. A basic comprehension of a catalysts’ role during chemical reactions can be understood from the concept of reaction mechanisms and energy diagrams.

Reduction of Alkenes: Asymmetric Catalytic Hydrogenation

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Catalytic hydrogenation of alkenes is a transition-metal catalyzed reduction of the double bond using molecular hydrogen to give alkanes. The mode of hydrogen addition follows syn stereochemistry.
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...

Preparation of Amines: Reduction of Amides and Nitriles

Preparation of Amines: Reduction of Amides and Nitriles

Nitriles can be reduced to primary amines using reducing agents like lithium aluminum hydride or catalytic hydrogenation. The reduction introduces an amino group with an extra carbon in the skeleton. Nitriles are formed from the reaction between alkyl halides and sodium cyanide through the SN2 mechanism. Primary alkyl halides are the preferred substrates to prepare nitriles.
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Preparation of Amines: Reduction of Oximes and Nitro Compounds

Preparation of Amines: Reduction of Oximes and Nitro Compounds

Oximes can be reduced to primary amines using catalytic hydrogenation, hydride reduction, or sodium metal reduction. The reduction of aliphatic and aromatic nitro compounds to primary amines takes place by either catalytic hydrogenation or by using active metals like Fe, Zn, and Sn in the presence of an acid.
Though catalytic hydrogenation can reduce nitrobenzenes, the reduction is nonselective in the presence of other functional groups. For instance, if nitrobenzene contains an aldehyde group,...

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A Self-Consistent Framework for Tailored Single-Atom Catalysts in Electrocatalytic Nitrogen Reduction.

Mingxin Qin¹, Lanlan Chen², Wenhua Zhang^2,3

¹Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei, Anhui 230026, China.

The Journal of Physical Chemistry Letters

|January 23, 2024

Summary

This summary is machine-generated.

Designing effective single-atom catalysts (SACs) requires considering reaction conditions. A new screening framework predicts superior nitrogen reduction reaction (NRR) activity for specific g-C3N4-supported metal catalysts.

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Area of Science:

Materials Science
Catalysis
Computational Chemistry

Background:

Single-atom catalysts (SACs) show great promise for various chemical reactions.
The performance of SACs is highly dependent on their local atomic and electronic structure, which is influenced by reaction conditions.
Designing efficient SACs necessitates a theoretical approach that accounts for these dynamic environmental factors.

Purpose of the Study:

To develop a self-consistent theoretical screening framework for designing single-atom catalysts (SACs).
To identify SACs with high activity for the nitrogen reduction reaction (NRR) using the proposed framework.
To investigate the influence of ligand configurations and reaction conditions on SAC performance.

Main Methods:

Utilized density functional theory (DFT) calculations to model SACs.
Constructed Pourbaix diagrams to determine stable configurations under various conditions.
Evaluated NRR activity by calculating the limiting potential (U_L) for different SAC configurations.
Rechecked the stability of promising configurations at their calculated U_L.

Main Results:

A novel screening framework was established for theoretical SAC design.
Identified specific configurations of g-C3N4-supported Nb and W as highly active for NRR.
Predicted superior NRR activity for AC stacking of double-layer g-C3N4-supported Nb (U_L = -0.36 V).
Predicted superior NRR activity for AA and AB stacking of double-layer g-C3N4-supported W (U_L = -0.45 V and -0.52 V, respectively).

Conclusions:

The developed screening framework accurately predicts SAC performance by considering reaction conditions.
The study highlights the potential of specific g-C3N4-supported metal SACs for efficient NRR.
The proposed methodology is broadly applicable for screening SACs in various electrocatalytic reactions.