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Heterogeneous Catalysis01:22

Heterogeneous Catalysis

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Heterogeneous catalysis involves a catalyst in a different phase from the reactants. It is a process where the catalyst and the reactants are in distinct phases, typically solid and gas or liquid.Most heterogeneous catalysts are metals, metal oxides, or acids. The list includes transition metals like iron (Fe), cobalt (Co), nickel (Ni), palladium (Pd), platinum (Pt), chromium (Cr), manganese (Mn), tungsten (W), silver (Ag), and copper (Cu). These metals possess partially vacant d orbitals that...
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Reduction of Alkenes: Asymmetric Catalytic Hydrogenation02:17

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...
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Reduction of Alkenes: Catalytic Hydrogenation02:13

Reduction of Alkenes: Catalytic Hydrogenation

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Alkenes undergo reduction by the addition of molecular hydrogen to give alkanes. Because the process generally occurs in the presence of a transition-metal catalyst, the reaction is called catalytic hydrogenation.
Metals like palladium, platinum, and nickel are commonly used in their solid forms — fine powder on an inert surface. As these catalysts remain insoluble in the reaction mixture, they are referred to as heterogeneous catalysts.
The hydrogenation process takes place on the...
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Catalysis02:50

Catalysis

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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.
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Thermal and Photochemical Electrocyclic Reactions: Overview01:26

Thermal and Photochemical Electrocyclic Reactions: Overview

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Electrocyclic reactions are reversible reactions. They involve an intramolecular cyclization or ring-opening of a conjugated polyene. Shown below are two examples of electrocyclic reactions. In the first reaction, the formation of the cyclic product is favored. In contrast, in the second reaction, ring-opening is favored due to the high ring strain associated with cyclobutene formation.
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Reduction of Alkynes to cis-Alkenes: Catalytic Hydrogenation02:24

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Introduction
Like alkenes, alkynes can be reduced to alkanes in the presence of transition metal catalysts such as Pt, Pd, or Ni. The reaction involves two sequential syn additions of hydrogen via a cis-alkene intermediate.
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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction

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Single-atom catalysts for CO2 electroreduction with significant activity and selectivity improvements.

Seoin Back1, Juhyung Lim1, Na-Young Kim2

  • 1Graduate School of EEWS , Korea Advanced Institute of Science and Technology (KAIST) , 291 Daehakro , Daejeon 34141 , Korea .

Chemical Science
|April 29, 2017
PubMed
Summary

Single-atom catalysts (SACs) show high selectivity for CO2 electroreduction, offering a promising pathway for sustainable chemical production. DFT calculations reveal specific SACs, like Pt@dv-Gr, significantly reduce energy barriers for methanol synthesis.

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Area of Science:

  • Computational materials science
  • Catalysis
  • Electrochemistry

Background:

  • Single-atom catalysts (SACs) exhibit unique electronic structures and high activity in various reactions, but their performance origins remain unclear.
  • SACs offer potential for reduced noble metal usage in applications like CO oxidation and fuel cells.
  • Understanding SACs for CO2 electroreduction is crucial for developing efficient catalysts.

Purpose of the Study:

  • To investigate the potential of single transition metal atoms anchored on defective graphene (M@sv-Gr or M@dv-Gr) as CO2 electroreduction catalysts.
  • To identify promising SACs for specific CO2 reduction products like methanol and methane.
  • To elucidate the fundamental origins of enhanced activity in SACs.

Main Methods:

  • Density functional theory (DFT) calculations were employed to study CO2 electroreduction on various single-atom catalysts.
  • Free energy profiles were calculated to assess catalytic activity and selectivity.
  • The electronic structures and binding energies of adsorbates on SACs were analyzed.

Main Results:

  • Several SACs demonstrated high selectivity for CO2 reduction over hydrogen evolution due to favorable adsorption of *COOH or *OCHO intermediates.
  • Ni@dv-Gr and Pt@dv-Gr were identified as promising catalysts for CH3OH production (U_L = -0.41 V and -0.27 V, respectively).
  • Os@dv-Gr and Ru@dv-Gr showed potential for CH4 production (U_L = -0.52 V).
  • The Pt@dv-Gr catalyst exhibited a significantly reduced limiting potential for methanol production compared to existing catalysts.
  • The enhanced activity of SACs was attributed to the lack of atomic ensembles, unique electronic structures, and orbital interactions, deviating from conventional scaling relations.

Conclusions:

  • Single-atom catalysts anchored on defective graphene show great potential for efficient and selective CO2 electroreduction.
  • Specific SACs, particularly Pt@dv-Gr, offer remarkable performance improvements for valuable chemical production.
  • The study provides insights into the electronic origins of SAC activity, guiding future catalyst design.