Direct synthesis of hydrazine by efficient electrochemical ruthenium-catalysed ammonia oxidation

Article Chemistry, Multidisciplinary

Electrocatalytic, Homogeneous Ammonia Oxidation in Water to Nitrate and Nitrite with a Copper Complex

Han-Yu Liu et al.

Summary: In this study, a molecular catalyst has been developed for the efficient and selective ammonia oxidation reaction at room temperature and pressure.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Multidisciplinary

A Parent Iron Amido Complex in Catalysis of Ammonia Oxidation

Yongxian Li et al.

Summary: Parent amido complexes play a crucial role in ammonia-based transformations. The study introduces a well-defined ferric ammine system that efficiently catalyzes electrochemical ammonia oxidation. A formal Fe(IV)-amido species, along with its conjugated Lewis acid, is isolated and characterized for the first time. Mechanism studies reveal the formation of hydrazine through the non-innocent nature of the phenylamido ligand.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Multidisciplinary

Co/N-doped carbon nanospheres derived from an adenine-based metal organic framework enabled high-efficiency electrocatalytic nitrate reduction to ammonia

Jie Chen et al.

Summary: This study reports a novel electrocatalyst, Co@NC, with the ability to efficiently synthesize NH3 and high selectivity for NO3- reduction. Under the experimental conditions, Co@NC exhibits a high NH3 yield and excellent electrochemical stability.

CHEMICAL COMMUNICATIONS (2022)

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Article Chemistry, Multidisciplinary

Hydrazine Formation via Coupling of a Nickel(III)-NH2 Radical

Nina X. Gu et al.

Summary: The formation of Ni-III-NH2 species that undergo bimolecular coupling to generate a Ni-2(II)(N2H4) complex is discussed in this study. Further oxidation to a structurally unusual Ni-2(N2H2) species releases N-2, establishing a synthetic cycle for Ni-mediated AO using Earth-abundant, late first-row metals.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Inorganic & Nuclear

Efficient Electrochemical Water Oxidation Mediated by Pyridylpyrrole-Carboxylate Ruthenium Complexes

Guo Chen et al.

Summary: The novel ruthenium(II) complexes bearing pyridylpyrrole-carboxylate (H(2)ppc) ligands show promising water oxidation catalytic performance under neutral conditions, with the initial step involving H2O/pic exchange and ruthenium center oxidation. The kinetic studies suggest a water nucleophilic attack mechanism for the catalytic process. HPO42- in a phosphate buffer solution is involved as the proton acceptor in the water oxidation reaction.

INORGANIC CHEMISTRY (2021)

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Article Multidisciplinary Sciences

From Ru-bda to Ru-bds: a step forward to highly efficient molecular water oxidation electrocatalysts under acidic and neutral conditions

Jing Yang et al.

Summary: In this study, a ruthenium-based molecular water oxidation catalyst with negatively charged sulfonate groups was introduced, showing efficient performance under both acidic and neutral conditions. The high valent Ru intermediate Ru-V=O and seven-coordinate Ru-IV=O were found to be involved in the O-O bond formation step under acidic and neutral conditions, respectively. In both cases, the I2M pathway was dominant over the WNA pathway for O-O bond formation.

NATURE COMMUNICATIONS (2021)

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Article Chemistry, Multidisciplinary

Spontaneous N2 formation by a diruthenium complex enables electrocatalytic and aerobic oxidation of ammonia

Michael J. Trenerry et al.

Summary: The study presents a stable metal-metal complex that produces dinitrogen from ammonia at low temperatures without the need for exogenous oxidizing reagents or high potentials. It also acts as a redox mediator for the oxidation of ammonia, operating at potentials as low as -255 mV and below the potential for the oxygen reduction reaction in alkaline conditions, showing thermodynamic viability for future development of DAFCs.

NATURE CHEMISTRY (2021)

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Article Chemistry, Multidisciplinary

Enhanced Ammonia Oxidation Catalysis by a Low-Spin Iron Complex Featuring Cis Coordination Sites

Michael D. Zott et al.

Summary: This study details Fe-mediated AO electrocatalysis with a high TON and fast AO rate, highlighting the promising potential of Fe as a metal catalyst for further development in metal-mediated AO catalysis.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Inorganic & Nuclear

Synthesis, Structure, and Ammonia Oxidation Catalytic Activity of Ru-NH3 Complexes Containing Multidentate Polypyridyl Ligands

Jan Holub et al.

Summary: The study presented in this report focuses on investigating the catalytic activity of [Ru(tda-kappa-(NO)-O-3)(py)(2)] as a precursor for the ammonia oxidation reaction (AOR). Spectroscopic characterization of the newly synthesized complexes was performed, along with X-ray diffraction analysis of selected compounds. The study also examined the catalytic cycle proposed based on electrochemical and kinetic evidence, achieving promising turnover numbers under bulk electrolysis conditions in acetonitrile.

INORGANIC CHEMISTRY (2021)

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Article Chemistry, Multidisciplinary

Uncovering Redox Non-innocent Hydrogen-Bonding in Cu(I)-Diazene Complexes

Evan J. Gardner et al.

Summary: Exploring intramolecular H-bonding as a potential strategy to stabilize diazene intermediates, the study used a series of [(xHet)TpCu](2)(mu-N2H2) complexes, revealing marked changes in spectroscopy due to the presence of hydrogen bonding. DFT studies identified metal-assisted concerted dual H-atom transfer as a thermodynamically favorable pathway for N-2/N2H2 interconversion.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Multidisciplinary

Manganese-Catalyzed Ammonia Oxidation into Dinitrogen under Chemical or Electrochemical Conditions**

Hiroki Toda et al.

Summary: The study presents a manganese-catalyzed oxidative conversion of ammonia into dinitrogen, which can be conducted under chemical or electrochemical conditions. Under chemical conditions, up to 17.1 equivalents of N-2 per catalyst are generated, while under electrochemical conditions, the reaction proceeds with 96% faradaic efficiency to give up to 6.56 equivalents of N-2 per catalyst.

CHEMPLUSCHEM (2021)

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Article Chemistry, Inorganic & Nuclear

A Ru2II,III diphosphonato complex with a metal-metal bond for water oxidation

Guo Chen et al.

Summary: K-3.1, a water-soluble Ru-2(II,III) diphosphonato complex, is only involved in stoichiometric water oxidation with a maximum 67% O-2 yield under CAN/HNO3 solution. The water oxidation mechanism and intermediate products were ascertained using UV-vis, ESI-MS, and DFT calculation methods.

DALTON TRANSACTIONS (2021)

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Article Chemistry, Multidisciplinary