Menny Shalom

Ben-Gurion University of the Negev

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Michael Volokh

Ben-Gurion University of the Negev

Jesús Barrio

Imperial College London

Markus Antonietti

Max Planck Institute of Colloids and Interfaces

Neeta Karjule

Ben-Gurion University of the Negev

Jonathan Tzadikov

Ben-Gurion University of the Negev

Jingsan Xu

Queensland University of Technology

Arie Zaban

Bar-Ilan University

Guiming Peng

University of Chicago

Adi Azoulay

Ben-Gurion University of the Negev

Idan Hod

Ben-Gurion University of the Negev

Cooperative Institutions

Ben-Gurion University of the Negev

Max Planck Institute of Colloids and Interfaces

Bar-Ilan University

Chinese Academy of Sciences

Wuhan University of Technology

Max Planck Society

Fuzhou University

The Technological College of Beer Sheva

Nanjing University of Science and Technology

Institut Català d'Investigació Química

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Controlled Nucleation and Growth of Carbon Nitride Films on CNT Fiber Fabric for Photoelectrochemical Applications

Advanced Sustainable Systems (2021)

Neeta Karjule Moumita Rana Menny Shalom Jesús Barrio Juan J. Vilatela

The controlled growth of carbon nitride (CN) films with tailored electronic properties and surface area is quite challenging due to the solid-state reaction and the lack of efficient interaction between C-N monomers and substrates. Herein, controlled growth of CN films over robust carbon nanotubes (CNT) fiber fabric is reported, which is obtained by either direct calcination of melamine on their surface, that yields a bulk material, or by its chemical vapor deposition resulting in hybrid films. These materials are effective electrodes consisting of high surface-area CN containing CNT fiber fabrics acting as a scaffold and a highly conducting built-in current collector. The results confirm that CNTs act as nucleation centers for the formation of CN films, forming close contact at the CN/CNT interphase, and resulting in efficient charge transfer upon illumination and enhanced electrochemical surface area.

Carbon nitride

10.1002/adsu.202000265

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Citations (2)

Ultralong Nanostructured Carbon Nitride Wires and Self-Standing C-Rich Filters from Supramolecular Microspheres

ACS Applied Materials & Interfaces (2018)

Jesús Barrio Menny Shalom

The rational design of ultralong carbon nitride nanostructures is highly attractive due to their high aspect ratio alongside their high surface-to-bulk ratio, which make them suitable candidates for various applications such as photocatalysts, water treatment, and sensors. However, the synthesis of ultralong, continuous carbon nitride wires is highly challenging. Here we report the synthesis of 4 cm long and large lateral size carbon nitride wires by utilizing unique supramolecular spheres composed of graphitic carbon nitride (g-CN) monomers as the reactants. In situ scanning electron microscopy studies reveal that upon calcination the g-CN wires spontaneously start to grow from the spheres, while the remaining assembly which acts as a substrate creates self-standing carbon-rich g-CN porous films. The different morphology, chemical composition, and electronic properties of the wires and carbon-rich g-CN allow their utilization as both photocatalyst and water cleaning materials. The g-CN wires exhibit excellent photoactivity for hydrogen production whereas the porous carbon-rich g-CN porous film can be efficiently used for water cleaning applications. The reported work opens opportunities for tailored design of g-CN nanostructures and their use as multifunctional materials for photocatalysis, sensing, and other energy-related applications.

Carbon nitride

Carbon fibers

Graphitic carbon nitride

10.1021/acsami.8b13873

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Citations (37)

Covalent Functionalization of Carbon Nitride Frameworks through Cross‐Coupling Reactions

Chemistry - A European Journal (2018)

Jing‐Wen Sun Ravindra S. Phatake Adi Azoulay Guiming Peng Chenhui Han

A new and simple synthetic route is introduced to covalently functionalize the carbon nitride (CN) framework by the implementation of halogenated phenyl groups (Cl, Br and I), which serve as a chemically reactive center, within the CN framework. The covalent modification is demonstrated here by substituting phenyl and tert-butyl propionate onto the modified-CN framework through Suzuki and reductive-Heck cross-coupling reactions, respectively. The effective functionalization leads to a facile exfoliation of the CN framework into thinner layers and greatly enhances the dispersibility in many solvents as well as the photocatalytic activity compared to the unmodified CN. The general covalent modification opens the possibility for tailor-made design of dispersible CN materials, including their photophysical and chemical properties, toward their exploitation in many fields, such as photocatalysis, bio-imaging, sensing, and heterogeneous catalysis.

Surface Modification

Exfoliation joint

Carbon nitride

Coupling reaction

Graphitic carbon nitride

Carbon fibers

Covalent organic framework

Chemical modification

10.1002/chem.201803201

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Citations (42)

Design and synthesis of TiO₂/C nanosheets with a directional cascade carrier transfer

Chemical Science (2022)

Si‐Ming Wu Yitian Wang Shi‐Tian Xiao Yanxiang Zhang Ge Tian

Directional charge transfer in TiO 2 nanosheets is achieved by design of TiO 2 lattice-Ti vacancy-interlayered sp 2 carbon at the interface.

10.1039/d2sc01872a

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Citations (13)

Unraveling the Mechanisms of Electrocatalytic Oxygenation and Dehydrogenation of Organic Molecules to Value‐Added Chemicals Over a Ni–Fe Oxide Catalyst

Advanced Energy Materials (2021)

Biswajit Mondal Neeta Karjule Chanderpratap Singh Ran Shimoni Michael Volokh

Abstract Electrocatalytic oxidative upgrading of organic molecules is a promising alternative process to water oxidation for clean hydrogen production. Yet, its underlying mechanism is still not fully understood, and suitable low‐cost electrocatalysts with good product selectivity and activity are still sought after. Here, an active NiFeO x ‐based catalyst is reported on as a general platform for the electro‐oxidative upgrading of organic molecules through oxygenation and dehydrogenation, with hydrogen coproduction. Detailed mechanistic studies unveil that C–H bond oxidation (with a bond dissociation energy BDE C–H of ≈88–96 kcal mol −1 ) is involved in the rate‐limiting step, which differs significantly from the oxygen evolution reaction mechanism. These findings show that the oxidation efficacy is linearly correlated with the BDE C–H of the molecule. Thus, the catalyst can be used as a general platform for large‐scale electro‐oxidation of various substrates through oxygenation and dehydrogenation at high current density (25 mA cm −2 ), with a good Faradaic yield. The platform's generality is further demonstrated by the selective oxidation of 5‐(hydroxymethyl)furfural into 2,5‐furandicarboxylic acid with good efficiency.

10.1002/aenm.202101858

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Citations (83)

Carbon Nitrides from Supramolecular Crystals: From Single Atoms to Heterojunctions and Advanced Photoelectrodes

Chemistry - A European Journal (2023)

Jesús Barrio Junyi Li Menny Shalom

Abstract Carbon nitride materials (CN) have become one of the most studied photocatalysts within the last 15 years. While CN absorbs visible light, its low porosity and fast electron‐hole recombination hinder its photoelectric performance and have motivated the research in the modification of its physical and chemical properties (such as energy band structure, porosity, or chemical composition) by different means. In this Concept we review the utilization of supramolecular crystals as CN precursors to tailor its properties. We elaborate on the features needed in a supramolecular crystal to serve as CN precursor, we delve on the influence of metal‐free crystals in the morphology and porosity of the resulting materials and then discuss the formation of single atoms and heterojunctions when employing a metal‐organic crystal. We finally discuss the performance of CN photoanodes derived from crystals and highlight the current standing challenges in the field.

Photoelectric effect

Carbon nitride

Crystal (programming language)

Carbon fibers

10.1002/chem.202302377

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Citations (4)

Formation of H2O2 in Near‐Neutral Zn‐air Batteries Enables Efficient Oxygen Evolution Reaction

Angewandte Chemie International Edition (2024)

Roman R. Kapaev Nicole Leifer Alagar Raja Kottaichamy Amit Ohayon Langyuan Wu

Rechargeable Zn‐air batteries (ZABs) with near‐neutral electrolytes hold promise as cheap, safe and sustainable devices, but they suffer from slow charge kinetics and remain poorly studied. Here we reveal a charge storage mechanism of near‐neutral Zn‐air batteries that is mediated by formation of dissolved hydrogen peroxide upon cell discharge and its oxidation upon charge. This H2O2‐mediated pathway facilitates oxygen evolution reaction (OER) at ~1.5 V vs. Zn2+/Zn, reducing charge overpotentials by ~0.2–0.5 V and mitigating carbon corrosion — a common issue in ZABs. The manifestation of this mechanism strongly depends on the electrolyte composition and positive electrode material, contributing up to ~60% of the capacity with ZnSO4 solutions and carbon nanotubes. Enhancing the H2O2‐mediated pathway offers a route to higher energy efficiency and durability in near‐neutral ZABs, advancing practical, sustainable energy storage.

Oxygen evolution

Carbon fibers

10.1002/anie.202418792

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Citations (0)

Fluorescent Carbon Nitride Macrostructures Derived from Triazine‐Based Cocrystals

Advanced Optical Materials (2021)

Jesús Barrio S. Barzilai Neeta Karjule Pilar Amo‐Ochoa Félix Zamora

Abstract Carbon nitride (CN) based materials have emerged as efficient photo‐ and electrocatalysts for various reactions. However, despite their intriguing optical properties (i.e., fluorescence), their utilization as solid‐state sensing platforms remains in its infancy, owing to the formation of defect states during the materials synthesis, leading to low emission for the CN powder. Here, a bottom‐up synthesis of CN macrostructures with good photoluminescence properties in both liquid and solid state is introduced, from designed triazine‐based cocrystals with ordered morphology and tailored chemical composition. Upon calcination at 500 °C, the starting morphology and chemical composition are retained, resulting in the alteration of the HOMO‐LUMO distribution of the CN materials, as further supported by density functional theory (DFT) calculations. The good photoluminescence properties of the new CN materials enable their exploitation as environmentally friendly, robust, and cheap sensing material for latent fingerprints labeling and metal‐ion detection in water.

Triazine

Graphitic carbon nitride

Carbon nitride

Carbon fibers

Characterization

10.1002/adom.202100683

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Citations (10)

Local CO2 reservoir layer promotes rapid and selective electrochemical CO2 reduction

Nature Communications (2024)

Subhabrata Mukhopadhyay Muhammad Saad Naeem G. Shiva Shanker Arnab Ghatak Alagar Raja Kottaichamy

Abstract Electrochemical CO 2 reduction reaction in aqueous electrolytes is a promising route to produce added-value chemicals and decrease carbon emissions. However, even in Gas-Diffusion Electrode devices, low aqueous CO 2 solubility limits catalysis rate and selectivity. Here, we demonstrate that when assembled over a heterogeneous electrocatalyst, a film of nitrile-modified Metal-Organic Framework (MOF) acts as a remarkable CO 2 -solvation layer that increases its local concentration by ~27-fold compared to bulk electrolyte, reaching 0.82 M. When mounted on a Bi catalyst in a Gas Diffusion Electrode, the MOF drastically improves CO 2 -to-HCOOH conversion, reaching above 90% selectivity and partial HCOOH currents of 166 mA/cm 2 (at −0.9 V vs RHE). The MOF also facilitates catalysis through stabilization of reaction intermediates, as identified by operando infrared spectroscopy and Density Functional Theory. Hence, the presented strategy provides new molecular means to enhance heterogeneous electrochemical CO 2 reduction reaction, leading it closer to the requirements for practical implementation.

10.1038/s41467-024-47498-9

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Citations (25)

Highly Porous Materials as Tunable Electrocatalysts for the Hydrogen and Oxygen Evolution Reaction

Advanced Functional Materials (2014)

Marc Ledendecker Guylhaine Clavel Markus Antonietti Menny Shalom

The facile preparation of highly porous, manganese doped, sponge‐like nickel materials by salt melt synthesis embedded into nitrogen doped carbon for electrocatalytic applications is shown. The incorporation of manganese into the porous structure enhances the nickel catalyst's activity for the hydrogen evolution reaction in alkaline solution. The best catalyst demonstrates low onset overpotential (0.15 V) for the hydrogen evolution reaction along with high current densities at higher potentials. In addition, the possibility to alter the electrocatalytic properties of the materials from the hydrogen to oxygen evolution reaction by simple surface oxidation is shown. The surface area increases up to 1200 m 2 g −1 after mild oxidation accompanied by the formation of nickel oxide on the surface. A detailed analysis shows a synergetic effect of the oxide formation and the material's surface area on the catalytic performance in the oxygen evolution reaction. In addition, the synthesis of cobalt doped sponge‐like nickel materials is also delineated, demonstrating the generality of the synthesis. The facile salt melt synthesis of such highly porous metal based materials opens new possibilities for the fabrication of diverse electrode nanostructures for electrochemical applications.

Overpotential

Oxygen evolution

Cobalt oxide

10.1002/adfm.201402078

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Citations (175)