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Journal ArticleDOI

Acid-Resistant Catalysis without Use of Noble Metals: Carbon Nitride with Underlying Nickel

TLDR
In this paper, a nanocomposite able to function as a hydrogenation catalyst under strongly acidic conditions without the presence of noble metals is synthesized and thoroughly studied, which possesses a unique structure composed of carbon nitride (CN) with underlying nickel, in which the nickel endows the CN with new active sites for hydrogen adsorption and activation while it itself is physically isolated from the reactive environment.
Abstract
A nanocomposite able to function as a hydrogenation catalyst under strongly acidic conditions without the presence of noble metals is synthesized and thoroughly studied. This specially designed catalyst possesses a unique structure composed of carbon nitride (CN) with underlying nickel, in which the nickel endows the CN with new active sites for hydrogen adsorption and activation while it itself is physically isolated from the reactive environment and protected from poisoning or loss. The CN is inert for hydrogenation without the help of nickel. The catalyst shows good performance for hydrogenation of nitro compounds under strong acidic conditions, including the one-step hydrogenation of nitrobenzene in 1.5 M H2SO4 to produce p-amoniophenol, for which the acid in the reaction system has restricted the catalyst only to noble metals in previous studies. Further characterization has demonstrated that the nickel in the catalyst is in an electron-deficient state because some of its electron has been donated to...

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Citations
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Journal ArticleDOI

Catalysis with two-dimensional materials and their heterostructures

TL;DR: Recent advances in the use of graphene and other 2D materials in catalytic applications are reviewed, focusing in particular on the catalytic activity of heterogeneous systems such as van der Waals heterostructures (stacks of several 2D crystals).
Journal ArticleDOI

Enhanced Electron Penetration through an Ultrathin Graphene Layer for Highly Efficient Catalysis of the Hydrogen Evolution Reaction

TL;DR: Density functional theory (DFT) calculations indicate that the ultrathin graphene shells strongly promote electron penetration from the CoNi nanoalloy to the graphene surface, which results in superior HER activity on the graphene shells.
Journal ArticleDOI

Selective Hydrogenation over Supported Metal Catalysts: From Nanoparticles to Single Atoms

TL;DR: The key factors affecting the catalytic activity/selectivity, in particular, the geometric and electronic structure of the active sites, are discussed with the aim to extract fundamental principles for the development of efficient and selective catalysts in hydrogenation as well as other transformations.
Journal ArticleDOI

Single layer graphene encapsulating non-precious metals as high-performance electrocatalysts for water oxidation

TL;DR: In this paper, a universal strategy was proposed to directly synthesize single layer graphene encapsulating uniform earth-abundant 3D transition-metal nanoparticles such as Fe, Co, Ni and their alloys in a confined channel of mesoporous silica.
Journal ArticleDOI

Nitroarene reduction: a trusted model reaction to test nanoparticle catalysts

TL;DR: The reaction kinetics is discussed considering its elegance and importance enlightening the long known Langmuir-Hinshelwood mechanism and Eley-Rideal mechanism at length, along with a few other mechanisms recently reported.
References
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Journal ArticleDOI

A metal-free polymeric photocatalyst for hydrogen production from water under visible light

TL;DR: It is shown that an abundant material, polymeric carbon nitride, can produce hydrogen from water under visible-light irradiation in the presence of a sacrificial donor.
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Polymeric Graphitic Carbon Nitride as a Heterogeneous Organocatalyst: From Photochemistry to Multipurpose Catalysis to Sustainable Chemistry

TL;DR: The "polymer chemistry" of g-C(3)N(4) is described, how band positions and bandgap can be varied by doping and copolymerization, and how the organic solid can be textured to make it an effective heterogenous catalyst.
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Prediction of new low compressibility solids.

TL;DR: The empirical model indicates that hypothetical covalent solids formed between carbon and nitrogen are good candidates for extreme hardness and first principles pseudopotential total energy calculation on the system shows that materials like the prototype can have bulk moduli comparable to or greater than diamond.
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New interpretations of XPS spectra of nickel metal and oxides

TL;DR: In this paper, a scheme for fitting the Ni 2p spectra using multiplet envelopes is proposed, based on charge transfer assignments of the main peak at 854.6 eV and the broad satellite centred at around 861 eV to the cd 9 L and the unscreened cd 8 final state configurations, respectively.
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Polymer semiconductors for artificial photosynthesis: hydrogen evolution by mesoporous graphitic carbon nitride with visible light.

TL;DR: It is shown that the efficiency of hydrogen production by photochemical water reduction can be improved by approximately 1 order of magnitude by introducing the right type of mesoporosity into polymeric C(3)N(4).
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