Mono‐Atomic Fe Centers in Nitrogen/Carbon Monolayers for Liquid‐Phase Selective Oxidation Reaction

Abstract

Two-dimensional catalyst supports with mono-atomic transition metals stabilized in special surface pockets conceptually promise excellent catalytic activity. Similar heterogenized monoatomic metal-based catalysts usually suffer from poor stability in liquid-phase reaction system, whilst highly ligand-stabilized metal-centers are less accessible for reactions. We report a twodimensional mono-atomic Fe/N/C layered nanostructure (2D-FeNC), generated through the direct polycondensation of C,N-containing molecules and Fe salts. With a 2D structure similar to graphene, the ultrathin CN support act as a solid ligand, leaving the z-direction open at molecular scale. This approach significantly promotes reactivity and the mass transfer to the Fe centers, here exemplified by the selective oxidation of alcohols using molecular oxygen. The catalysts show also high mechanical and chemical stability for good to excellent reusability.

In Situ Preparation of Ru@N-Doped Carbon Catalyst for the Hydrogenolysis of Lignin To Produce Aromatic Monomers

“…Recently, N-doped carbon-supported metal catalysts have received widespread attention since N dopants can enhance the electronic interaction between metal and carbon support, − alter the acid–base properties of the support surface, and therefore, increase the catalytic activity. − Li et al prepared a N-functionalized mesoporous carbon-supported Pd catalyst by postsynthesis treatment with NH 3 or melamine. When this catalyst was used in the hydrogenation of phenol, a ∼80% conversion of phenol and a ∼100% selectivity to cyclohexanone were obtained.…”

Efficient Conversion of Benzyl Alcohol on a Mesoporous Co3O4

“…Benzyl alcohol as a vital raw material is a kind of extremely popular chemical reactant in many catalytic reactions, which can be converted into various products, such as aldehydes, esters, amines . In fact, it has been demonstrated that benzaldehyde could be obtained by selectively oxidizing benzyl alcohol with some oxidants such as H 2 O 2 , KMnO 4 , CrO 3 , and O 2 . ,,− Among them, O 2 is an optimal choice due to environmental and energy crisis, which is a cheap and environmentally friendly oxidant . However, there are still many challenges since high-efficiency, stable, and cheap catalysts are urgently needed …”

“…To date, some metal-based materials played a more and more important role in heterogeneous catalysis, such as Fe-based, Co-based, and Ni-based catalysts. It has been demonstrated that mesoporous metal-based materials possess widely applications owing to the large superficial area and porosity, which were widely used as microwave absorbers, electrode materials, , sensors, , and catalysts, − etc.…”

“…1,6,9−13 Among them, O 2 is an optimal choice due to environmental and energy crisis, which is a cheap and environmentally friendly oxidant. 14 However, there are still many challenges since high-efficiency, stable, and cheap catalysts are urgently needed. 15 To date, some metal-based materials played a more and more important role in heterogeneous catalysis, such as Febased, 14 Co-based, 7 and Ni-based 8 catalysts.…”

Selective Catalytic Oxidation of Benzyl Alcohol to Benzaldehyde by Nitrates

“…In the former method, the chlorinated by-products and corresponding toxic acidic would be generated, which brought troubles to the industrial application (Mal et al, 2018;Lu et al, 2019), while the vapor/liquid oxidation of toluene was also limited because of the harsh reaction conditions and low selectivity (Miao et al, 2016). Recently, BzH production with benzyl alcohol oxidation was widely adopted in industry, based on its advantages of easy-control condition and high yield (Lv et al, 2018;Thao et al, 2018). In this method, potassium permanganate (KMnO 4 ) (Mahmood et al, 1999) and dichromate (K 2 Cr 2 O 7 ) (Thottathil et al, 1986) with a strong oxidizing property are chosen as oxidants.…”