A polyoxometalate cluster-based single-atom catalyst for NH<sub>3</sub> synthesis <i>via</i> an enzymatic mechanism

Talib, Shamraiz Hussain; Yu, Xiaohu; Lu, Zhansheng; Ahmad, Kamsuriah; Yang, Tongtong; Xiao, Hai; Li, Jun

doi:10.1039/d1ta07903d

Cited by 27 publications

(21 citation statements)

References 89 publications

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“…The catalyst is considered to be the best catalyst for HER in which DGÃ H tends to its ideal value DGÃ H ffi 0 ð Þleading to the desorption of hydrogen easily from the catalyst surface either through the Tafel or the Heyrovsky step, which in turn, leaves the catalyst surface prepared for the successive adsorption of hydrogen for further reaction to proceed. 38 Here, the values of DGÃ H , as shown in the Fig. 2(d), vary from À0.2 eV to À0.79 eV which indicates that the H binds strongly with the catalyst surface that hinders the HER to proceed further.…”

Section: Resultsmentioning

confidence: 78%

Performance of the nitrogen reduction reaction on metal bound g-C₆N₆: a combined approach of machine learning and DFT

Mukherjee

Dutta

Ghosh

et al. 2022

Phys. Chem. Chem. Phys.

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Section: Resultsmentioning

confidence: 78%

Performance of the nitrogen reduction reaction on metal bound g-C₆N₆: a combined approach of machine learning and DFT

Mukherjee

Dutta

Ghosh

et al. 2022

Phys. Chem. Chem. Phys.

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“…In the chemistry of group 6 polyoxometalates, the polyoxomolybdates are significantly more labile than the polyoxotungstates, thus making researchers favor the latter in their studies of POM chemistry. However, several studies of polyoxomolybdates’ reactivity [ 39 ] and catalytic performance (electron transfer reactions) appeared [ 40 , 41 , 42 , 43 , 44 , 45 ]. One of the central complexes in this chemistry is (Bu 4 N) 4 [β-Mo 8 O 26 ] ( Scheme 1 ), which is a standard precursor of all reactions in organic media, leading to a huge number of materials with different properties [ 46 , 47 , 48 , 49 ].…”

Section: Introductionmentioning

confidence: 99%

Proton Affinity in the Chemistry of Beta-Octamolybdate: HPLC-ICP-AES, NMR and Structural Studies

et al. 2022

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The affinity of [β-Mo8O26]4− toward different proton sources has been studied in various conditions. The proposed sites for proton coordination were highlighted with single crystal X-ray diffraction (SCXRD) analysis of (Bu4N)3[β-{Ag(py-NH2)Mo8O26]}] (1) and from analysis of reported structures. Structural rearrangement of [β-Mo8O26]4− as a direct response to protonation was studied in solution with 95Mo NMR and HPLC-ICP-AES techniques. A new type of proton transfer reaction between (Bu4N)4[β-Mo8O26] and (Bu4N)4H2[V10O28] in DMSO results in both polyoxometalates transformation into [V2Mo4O19]4−, which was confirmed by the 95Mo, 51V NMR and HPLC-ICP-AES techniques. The same type of reaction with [H4SiW12O40] in DMSO leads to metal redistribution with formation of [W2Mo4O19]2−.

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“…However, selectivity analyses indicated that HER may exceed NRR on the small cluster, whereas NH 3 could have been synthesized selectively on the Ni 13 –TiO 2 (101) catalyst. Recently, Talib et al proposed that a phosphomolybdic acid (PMA) cluster, consisting of a central PO 4 tetrahedral core connected with 12 MoO 6 octahedral units can anchor TM atoms to develop suitable heterogeneous SACs for NRR. Among a series of 3d, 4d, and 5d TMs, the authors found that Mo/PMA has a superior electrocatalytic effect over others.…”

Section: Single-atom/cluster-decorated Metal-based Electrocatalystsmentioning

confidence: 99%

Recent Progress in Computational Design of Single-Atom/Cluster Catalysts for Electrochemical and Solar-Driven N₂ Fixation

et al. 2022

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Fixation of dinitrogen into ammonia is an essential biological process for the evolution of life, and at the same time ammonia is an essential component for many industrial processes, including fertilizers, plastics, and so on. NH 3 is also known as the best alternative to H 2 in fuel cells. However, due to chemical inertness, direct conversion of N 2 into NH 3 is not possible; a suitable catalyst is required. The century-old Haber−Bosch process, utilizing an Fe-based catalyst, is extremely energy-intensive and eco-unfriendly due to the consumption of fossil fuels. In recent years, huge development has taken place in the design and applications of suitable electro-and photocatalysts for artificial N 2 fixation. First-principles calculations have been considered as a powerful avenue for theoretical screening of promising catalysts through rational design and analysis of the plausible mechanisms or pathways of reactions. The present review focuses on recent theoretical developments of various unsupported nanoclusters and supported single-atom and cluster catalysts for application in electro-and photochemical N 2 reduction reactions. The support substrates include oxides, carbides, nitrides of metal-based 2D materials, porous carbonaceous materials, and metal-free 2D materials containing main-group elements like B, C, N, and P. Although some reviews have already been made, focusing on the research related to either electro-or photocatalytic N 2 fixation on different catalysts, here we give a comprehensive account of both electrochemical and photochemical nitrogen reduction reaction (NRR) activities and selectivities of various supported single-atom and polyatomic cluster catalysts. Additionally, a comparative assessment is made on the basis of free energy of adsorption, most favorable pathway, potential limiting step, and corresponding limiting potential of the NRR.

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A polyoxometalate cluster-based single-atom catalyst for NH₃ synthesis via an enzymatic mechanism

Abstract: NH3 synthesis by electrochemical N2 reduction reaction (eNRR) under mild conditions has attracted much attention. Here, by means of first principles calculations, we propose a new strategy using a transition...

Cited by 27 publications

References 89 publications

Performance of the nitrogen reduction reaction on metal bound g-C₆N₆: a combined approach of machine learning and DFT

Performance of the nitrogen reduction reaction on metal bound g-C₆N₆: a combined approach of machine learning and DFT

Proton Affinity in the Chemistry of Beta-Octamolybdate: HPLC-ICP-AES, NMR and Structural Studies

Recent Progress in Computational Design of Single-Atom/Cluster Catalysts for Electrochemical and Solar-Driven N₂ Fixation

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A polyoxometalate cluster-based single-atom catalyst for NH3 synthesis via an enzymatic mechanism

Abstract: NH3 synthesis by electrochemical N2 reduction reaction (eNRR) under mild conditions has attracted much attention. Here, by means of first principles calculations, we propose a new strategy using a transition...

Cited by 27 publications

References 89 publications

Performance of the nitrogen reduction reaction on metal bound g-C6N6: a combined approach of machine learning and DFT

Performance of the nitrogen reduction reaction on metal bound g-C6N6: a combined approach of machine learning and DFT

Proton Affinity in the Chemistry of Beta-Octamolybdate: HPLC-ICP-AES, NMR and Structural Studies

Recent Progress in Computational Design of Single-Atom/Cluster Catalysts for Electrochemical and Solar-Driven N2 Fixation

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A polyoxometalate cluster-based single-atom catalyst for NH₃ synthesis via an enzymatic mechanism

Performance of the nitrogen reduction reaction on metal bound g-C₆N₆: a combined approach of machine learning and DFT

Performance of the nitrogen reduction reaction on metal bound g-C₆N₆: a combined approach of machine learning and DFT

Recent Progress in Computational Design of Single-Atom/Cluster Catalysts for Electrochemical and Solar-Driven N₂ Fixation