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Preparation of Amines: Reduction of Oximes and Nitro Compounds01:29

Preparation of Amines: Reduction of Oximes and Nitro Compounds

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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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Nitriles to Amines: LiAlH4 Reduction00:55

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Nitriles are reduced to amines in the presence of strong reducing agents like lithium aluminum hydride through a typical nucleophilic acyl substitution. The reaction requires two equivalents of the reducing agent. The reducing agent acts as a source of hydride ions.
As shown below, the mechanism involves three steps. Firstly, the hydride ion acting as a nucleophile attacks the nitrile carbon to form an anion. In the second step, a second equivalent of the hydride ion attacks the anion to...
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Reduction of Alkenes: Asymmetric Catalytic Hydrogenation02:17

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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 Alkynes to cis-Alkenes: Catalytic Hydrogenation02:24

Reduction of Alkynes to cis-Alkenes: Catalytic Hydrogenation

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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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Reduction of Alkenes: Catalytic Hydrogenation02:13

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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.
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Preparation of Amines: Reduction of Amides and Nitriles01:13

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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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A simple descriptor for the nitrogen reduction reaction over single atom catalysts.

Zhanzhao Fu1, Mingliang Wu1, Qiang Li1

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|January 4, 2023
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A new descriptor, the effective d electron number (Φ), quantifies metal-support interactions for nitrogen reduction reaction (NRR) catalysts. This method rapidly screens high-performance catalysts like Mo@WTe2, Mo@V2CO2, and Re@NbS2 without complex calculations.

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Area of Science:

  • Heterogeneous Catalysis
  • Materials Science
  • Electrochemistry

Background:

  • Metal-support interactions are crucial for supported catalyst performance.
  • Quantifying structure-activity relationships in supported catalysts is challenging.
  • Nitrogen reduction reaction (NRR) is vital for ammonia synthesis and nitrogen fixation.

Purpose of the Study:

  • To develop a simple descriptor for quantifying metal-support interactions in supported catalysts.
  • To establish a structure-activity relationship for the nitrogen reduction reaction (NRR).
  • To enable rapid screening of efficient NRR catalysts.

Main Methods:

  • Construction of the effective d electron number (Φ) descriptor based on intrinsic catalyst properties.
  • Utilizing the descriptor to predict the limiting potential (U_L) for NRR.
  • Applying the descriptor to various metal dichalcogenide and MXene-supported single atom catalysts (SACs).

Main Results:

  • The effective d electron number (Φ) descriptor accurately predicts NRR limiting potential (U_L) without DFT calculations.
  • The descriptor shows broad applicability across different material systems, including MoS2, WS2, MoSe2, WSe2, WTe2, NbS2, V2CO2, Ti2CO2, and Nb2CO2.
  • Three promising NRR catalysts (Mo@WTe2, Mo@V2CO2, Re@NbS2) were identified with low U_L values of -0.32, -0.24, and -0.31 V, respectively.

Conclusions:

  • The effective d electron number (Φ) descriptor provides a facile and accurate method for evaluating NRR activity.
  • This approach facilitates the rapid discovery and design of high-performance NRR catalysts.
  • The developed design principle is expected to be widely applicable to other catalytic systems.