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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.

Thermal Electrocyclic Reactions: Stereochemistry

Thermal Electrocyclic Reactions: Stereochemistry

The stereochemistry of electrocyclic reactions is strongly influenced by the orbital symmetry of the polyene HOMO. Under thermal conditions, the reaction proceeds via the ground-state HOMO.
Selection Rules: Thermal Activation
Conjugated systems containing an even number of π-electron pairs undergo a conrotatory ring closure. For example, thermal electrocyclization of (2E,4E)-2,4-hexadiene, a conjugated diene containing two π-electron pairs, gives trans-3,4-dimethylcyclobutene.

Pericyclic Reactions: Introduction

Pericyclic Reactions: Introduction

Pericyclic reactions are organic reactions that occur via a concerted mechanism without generating any intermediates. The reactions proceed through the movement of electrons in a closed loop to form a cyclic transition state, where rearrangement of the σ and π bonds yields specific products.
Pericyclic reactions can be classified into three categories: electrocyclic reactions, cycloaddition reactions, and sigmatropic rearrangements. Electrocyclic reactions and sigmatropic...

Thermal and Photochemical Electrocyclic Reactions: Overview

Thermal and Photochemical Electrocyclic Reactions: Overview

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.

Photochemical Electrocyclic Reactions: Stereochemistry

Photochemical Electrocyclic Reactions: Stereochemistry

The absorption of UV–visible light by conjugated systems causes the promotion of an electron from the ground state to the excited state. Consequently, photochemical electrocyclic reactions proceed via the excited-state HOMO rather than the ground-state HOMO. Since the ground- and excited-state HOMOs have different symmetries, the stereochemical outcome of electrocyclic reactions depends on the mode of activation; i.e., thermal or photochemical.
Selection Rules: Photochemical Activation

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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction

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Decoding Surface Electron Density-Reactivity Relationship in Ni-Porous Organic Polymer Catalyst for Cyclohexene

Dhruba Jyoti Deka^1,2, Priyanka Kalita³, Ratul Paul⁴

¹Organic & Medicinal Chemistry Division, CSIR-Indian Institute of Chemical Biology, 4-Raja S. C. Mullick Road, Jadavpur, Kolkata 700032, India.

Inorganic Chemistry

|December 5, 2025

Summary

We developed a novel nickel-metalated porous polymer (Ni@CAB) for green oxidation chemistry. This sustainable catalyst shows high efficiency and recyclability in aerobic allylic oxidation under ambient conditions.

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Area of Science:

Materials Science
Catalysis
Green Chemistry

Background:

Efficient and sustainable heterogeneous catalysts are crucial for advancing green oxidation chemistry.
Metalated porous organic polymers offer tunable properties for catalytic applications.

Purpose of the Study:

To synthesize and characterize a novel Ni-salphen-derived metalated porous organic polymer (Ni@CAB).
To evaluate the catalytic performance of Ni@CAB in aerobic oxidation reactions.
To establish surface electron density as an activity descriptor for oxidation catalysts.

Main Methods:

Friedel-Crafts alkylation for polymer synthesis.
2D solid-state NMR, XPS, synchrotron-based XAS, and electron microscopy for characterization.
Density Functional Theory (DFT) calculations for mechanistic insights.

Main Results:

Ni@CAB possesses an amorphous porous architecture with uniformly dispersed Ni-N2O2 active sites.
The catalyst exhibits enhanced Lewis acidity due to reduced surface electron density at Ni sites.
Exceptional performance in aerobic allylic oxidation of cyclohexene: complete conversion, high selectivity, and excellent recyclability without Ni leaching.

Conclusions:

Ni@CAB is a highly effective and sustainable heterogeneous catalyst for green oxidation chemistry.
Surface electron density is a key descriptor for predicting and enhancing catalytic activity.
Rationally engineered metalated porous polymers hold significant promise for sustainable catalysis.