Correction to “Dinitrogen Fixation and Reduction by Ta3N3H0,1– Cluster Anions at Room Temperature: Hydrogen-Assisted Enhancement of Reactivity”

Zhao, Yue; Cui, Jia-Tong; Wang, Ming; Valdivielso, David Yubero; Fielicke, André; Hu, Lianrui; Cheng, Xin; Liu, Qingyu; Li, Ziyu; He, Sheng‐Gui; Ma, Jia-Bi

doi:10.1021/jacs.9b08813

Cited by 4 publications

(3 citation statements)

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“…Recently, we have reported Ta single-atom catalysts for the NRR process, where the Ta−N center affords higher selectivity as compared to Ta−O. 29 In fact, recent gas-phase studies 30,31 have revealed that the M−N (M = V, 32 Nb, 33 Ta 34,35 ) containing structures are promising in dinitrogen activation. For example, the nitrogen ligand weakens the electrondonating inclination of Ta through induced electron rearrangement.…”

Section: ■ Introductionmentioning

confidence: 99%

Theory-Guided Construction of the Unsaturated V–N₂ Site with Carbon Defects for Highly Selective Electrocatalytic Nitrogen Reduction

Wang

Qian

Zhou

2023

ACS Appl. Mater. Interfaces

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Renewable energy-driven, electrocatalytic nitrogen reduction reaction (NRR) is a promising strategy for ammonia synthesis. However, improving catalyst activity and selectivity under ambient conditions has long been challenging. In this work, we obtained the potential active V–N center through theoretical prediction and successfully constructed the associated V–N2/N3 structure on N-doped carbon materials. Surprisingly, such a catalyst exhibits excellent electrocatalytic NRR performance. The V–N2 catalyst affords a remarkably high faradaic efficiency of 76.53% and an NH3 yield rate of 31.41 μgNH3 h–1 mgCat. –1 at −0.3 V vs RHE. The structural characterization and density functional theory (DFT) calculations verified that the high performance of the catalyst originates from the tuned d-band upon coordination with nitrogen, in line with the original design intention as derived theoretically. Indeed, the V–N2 center with carbon defects enhances dinitrogen adsorption and charge transfer, thereby lowering the energy barriers to form the *NNH intermediates. Such a strategy as a rational designcontrollable synthesistheoretical verification may prove effective as well for other chemical processes.

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Section: ■ Introductionmentioning

confidence: 99%

Theory-Guided Construction of the Unsaturated V–N₂ Site with Carbon Defects for Highly Selective Electrocatalytic Nitrogen Reduction

Wang

Qian

Zhou

2023

ACS Appl. Mater. Interfaces

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“…The study of reactions between the gas-phase metalcontaining species and small molecules under isolated conditions provides an ideal arena for revealing mechanisms of chemical reactions, such as N 2 fixation and reduction, at a strictly molecular level. It is worth noting that in the gas-phase studies of N 2 reduction reactions, NN triple bonds can be cleaved mediated by metal species, such as Sc 2 , 18 Ta 2 + , 19 Ta 2 C 4 − , 20 Ta 4 + , 21 V 3 C 4 − , 22 V 5 N 5 − , 23 Ta 3 N 3 H 0,1 − , 24 NbH 2 − , 25 NbB 3 O 2 − , 26 Sc 3 N + , 27 FeV 2 C 2 − , 28 FeTaC 2 − , 29 and AuNb-BO − , 30 and all of these investigations are focused on roles of transition-metal atoms in reactions with N 2 . In contrast, the function of alkali metal, such as lithium, has not been reported.…”

Section: Introductionmentioning

confidence: 99%

Lithium-Assisted Dinitrogen Reduction Mediated by Nb₂LiNO_1–4^– Cluster Anions: Electron Donors or Structural Units

Ding

Chen

et al. 2022

J. Phys. Chem. A

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Alkali atoms are usually used as promoters to significantly increase the catalytic activity of transition-metal catalysts in a wide range of reactions such as dinitrogen conversion reactions. However, the role of alkali metal atoms remains controversial. Herein, a series of quaternary cluster anions containing lithium atoms Nb 2 LiNO 1−4 − have been synthesized and reacted with N 2 at room temperature. The detailed experimental and theoretical investigations indicate that Nb 2 LiNO − is capable to cleave the NN bond and the Li atoms in Nb 2 LiNO 1,2 − act as electron donors in the N 2 reduction reaction. With the increase in the number of oxygen atoms, the reactivity toward N 2 is reduced from adsorption via a side-on end-on mode in Nb 2 LiNO 2 − to the inertness of Nb 2 LiNO 4 − . In Nb 2 LiNO 3,4 − anions, the Li atoms are bonded with oxygen atoms, acting as structural units to stabilize structures. Therefore, the roles of alkali atoms are able to change with different chemical environments of active sites. For the first time, we reveal how the number of ligands (oxygen atoms herein) can be used to finely regulate the reactivity toward N 2 .

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“…It has an extremely high bond dissociation energy of 9.92 eV, which is even slightly higher than that of dinitrogen (9.75 eV) . As an isoelectronic molecule of acetylene, the NN triple bond of N 2 can be effectively activated and completely cleaved by metal dimers in forming ring and cage nitrides. − …”

Section: Introductionmentioning

confidence: 99%

Iridium Dimer Anion-Mediated C≡C Triple Bond Cleavage and Successive Dehydrogenation of Acetylene in the Gas Phase

Liu

et al. 2022

J. Phys. Chem. A

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The reactions of the iridium dimer anion [Ir 2 ] − with acetylene have been studied by mass spectrometry in the gas phase, which indicate that the [Ir 2 ] − anion can consecutively react with C 2 H 2 molecules to form the [Ir 2 C 2x ] − (x = 1, 2) and [Ir 2 C 2y H 2 ] − (y = 3−5) anions as major products with the successive release of H 2 molecules at room temperature. The reactions are confirmed by the reactions of the mass-selected product [Ir 2 C 2 ] − anion with C 2 H 2 to produce [Ir 2 C 4 ] − and [Ir 2 C 2y H 2 ] − (y = 3−5). Photoelectron spectra and quantum chemistry calculations confirm that the [Ir 2 C 2x ] − (x = 1, 2) product anions possess cyclic [Ir(μ-C) 2 Ir] − and [Ir(μ-C)(μ-C 3 )Ir] − structures, implying that the robust CC triple bond of acetylene can be completely cleaved by the [Ir 2 ] − anion.

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Correction to “Dinitrogen Fixation and Reduction by Ta₃N₃H_0,1^– Cluster Anions at Room Temperature: Hydrogen-Assisted Enhancement of Reactivity”

Cited by 4 publications

References 0 publications

Theory-Guided Construction of the Unsaturated V–N₂ Site with Carbon Defects for Highly Selective Electrocatalytic Nitrogen Reduction

Theory-Guided Construction of the Unsaturated V–N₂ Site with Carbon Defects for Highly Selective Electrocatalytic Nitrogen Reduction

Lithium-Assisted Dinitrogen Reduction Mediated by Nb₂LiNO_1–4^– Cluster Anions: Electron Donors or Structural Units

Iridium Dimer Anion-Mediated C≡C Triple Bond Cleavage and Successive Dehydrogenation of Acetylene in the Gas Phase

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Correction to “Dinitrogen Fixation and Reduction by Ta3N3H0,1– Cluster Anions at Room Temperature: Hydrogen-Assisted Enhancement of Reactivity”

Cited by 4 publications

References 0 publications

Theory-Guided Construction of the Unsaturated V–N2 Site with Carbon Defects for Highly Selective Electrocatalytic Nitrogen Reduction

Theory-Guided Construction of the Unsaturated V–N2 Site with Carbon Defects for Highly Selective Electrocatalytic Nitrogen Reduction

Lithium-Assisted Dinitrogen Reduction Mediated by Nb2LiNO1–4– Cluster Anions: Electron Donors or Structural Units

Iridium Dimer Anion-Mediated C≡C Triple Bond Cleavage and Successive Dehydrogenation of Acetylene in the Gas Phase

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Product

Resources

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Correction to “Dinitrogen Fixation and Reduction by Ta₃N₃H_0,1^– Cluster Anions at Room Temperature: Hydrogen-Assisted Enhancement of Reactivity”

Theory-Guided Construction of the Unsaturated V–N₂ Site with Carbon Defects for Highly Selective Electrocatalytic Nitrogen Reduction

Theory-Guided Construction of the Unsaturated V–N₂ Site with Carbon Defects for Highly Selective Electrocatalytic Nitrogen Reduction

Lithium-Assisted Dinitrogen Reduction Mediated by Nb₂LiNO_1–4^– Cluster Anions: Electron Donors or Structural Units