A novel phosphotungstic acid-supported single metal atom catalyst with high activity and selectivity for the synthesis of NH<sub>3</sub> from electrochemical N<sub>2</sub> reduction: a DFT prediction

Gao, Liye; Wang, Feiteng; Ming-an, YU; Wei, Fenfei; Qi, Jiamin; Lin, Sen; Xie, Daiqian

doi:10.1039/c9ta06470b

Cited by 73 publications

(37 citation statements)

References 47 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The stability of Mn on graphene is evaluated by the binding energy; the binding energy of Mn on MnN 3 -SV and MnN 3 -DV was −4.352 and −7.414 eV, respectively, which were significantly smaller than the cohesive energy of bulk Mn (−4.12 eV). 41 To study the interaction between Mn and the surrounding atoms, we analyzed the partial density of states (PDOS) of MnN 3 -SV and MnN 3 -DV ( Figure 1 ). We found that there is an obvious hybridization between the d orbitals of Mn atom and the p orbitals of C or N atoms and significant charge transfer between atoms, which is consistent with the electron density environment shown by the deformation density of MnN 3 -SV and MnN 3 -DV ( Figure 2 a1,b1).…”

Section: Resultsmentioning

confidence: 99%

Theoretical Calculation of Different Reaction Mechanisms for CO Oxidation on MnN₃-Doped Graphene

et al. 2020

View full text Add to dashboard Cite

In recent decades, great expectation has always been placed on catalysts that can convert toxic CO into CO 2 under mild conditions. The catalytic mechanism of CO oxidation by Mn-coordinated N-doped graphene with a single vacancy (MnN 3 -SV) and a double vacancy (MnN 3 -DV) was studied by density functional theory (DFT) calculations. Molecular dynamics simulations showed that CO 2 on MnN 3 -SV could not be desorbed from the substrate and MnN 3 -SV was not suitable for use as a CO oxidation catalyst. MnN 3 -DV was more suitable for CO oxidation (COOR) and from the electronic structure it was found that the Mn atom was the main active site, which was the reaction site for CO oxidation. At temperatures of 0 and 298.15 K, CO oxidation on MnN 3 -DV via the Langmuir–Hinshelwood (LH) mechanism was the best reaction pathway. The rate-determining step using MnN 3 -DV as the catalyst for CO oxidation through the LH mechanism was O 2 + CO → OOCO, and the energy barrier was 0.861 eV at 298.15 K. MnN 3 -DV was suitable as a catalyst for CO oxidation in terms of both thermodynamics and kinetics. This study provides a comprehensive understanding of the various reaction mechanisms of CO oxidation on MnN 3 -DV, which is conducive to guiding the development and design of efficient catalysts for CO oxidation.

show abstract

Section: Resultsmentioning

confidence: 99%

Theoretical Calculation of Different Reaction Mechanisms for CO Oxidation on MnN₃-Doped Graphene

et al. 2020

View full text Add to dashboard Cite

show abstract

“…Moreover, the overpotential of NRR on Mo/BP surface is close to that on the previously reported Re (111) surface (0.50 V), [62] which still comparable to other reported Fe-Bx [56] and Mo SACs. [34,37,64] Therefore, the designed Mo-embedded BP monolayer is expected to be a high-performance single TM electrocatalyst for the nitrogen fixation reaction.…”

Section: Resultsmentioning

confidence: 99%

“…), [15][16][17][18][19][20][21] metal-free-based materials (B, S, C, P, N, etc. ), [3,[22][23][24][25][26][27] single-atom catalysts, [4,[28][29][30][31][32][33][34] dual-atom catalysts, [35,36,38] and their hybrids. Among them, the transition metal-based materials are considered to be promising catalysts due to their availability of d-orbital electrons for the antibonding orbitals of N 2 , which may solve the kinetic problem of strong N≡N triple bond activation.…”

mentioning

confidence: 99%

Computational Design of Single Mo Atom Anchored Defective Boron Phosphide Monolayer as a High‐performance Electrocatalyst for the Nitrogen Reduction Reaction

Liu

Huang

Chang

et al. 2020

Energy & Environ Materials

View full text Add to dashboard Cite

show abstract

“…In contrast, for POM-SACs, the molecular structure of the POM-support is typically well known from single-crystal XRD studies, so that suitable structural POM-SAC models can be provided for advanced calculations. Several groups have used this metal-functionalized POM-SAC model system (where the SAC is located in the 4-H site) for computational studies on reduction/oxidation reactions including alkene epoxidation, [61] N 2 reduction, [62,63] NO x (NO and N 2 O) reduction, [64][65][66] and CO oxidation. [67][68][69][70] In 2019, Sautet, Yan and co-workers investigated how metalsupport interactions affect stability and hydrogenation activity of Class I POM-SACs.…”

Section: Noble-metal-functionalized Pom-sacsmentioning

confidence: 99%

Polyoxometalate‐Single Atom Catalysts (POM‐SACs) in Energy Research and Catalysis

Liu

Streb

2021

Advanced Energy Materials

View full text Add to dashboard Cite

have only been explored since the early 21st century, mainly because their identification and characterization has been virtually impossible before, due to a lack of high-resolution instrumentation (such as electron or scanning probe microscopies). [1,4] Beyond classical heterogeneous SACs, much research has recently focused on developing molecular SAC model systems. Here, polyoxometalate-single atom catalysts (POM-SACs) are of enormous interest as these molecular metal oxides could form the link between molecularly well-defined prototypes and technologically relevant solid-state SACs. In this Review, we will provide a brief introduction into the current status in SACs chemistry. We then discuss pioneering studies as well as current research challenges in POM-SACs chemistry with an emphasis on sustainable energy research. Finally, we will identify future areas in POM-SAC research and highlight the bottlenecks which need to be overcome to further develop this field. Classical Single Atom Catalysts Common Anchoring Strategies and Applications of SACsSACs offer the ultimate atomic reactivity, as each single atom is interacting with its environment and can act as catalytic site. [7][8][9] The key to the successful preparation of SACs is to stabilize catalytic metal centers as individual atoms by utilizing hosts/supports featuring strong binding motifs (Figure 1). Early model systems included high specific surface area carbons, [10,11] metal oxides, [12,13] as well as materials with uniform pores and regular structures, such as zeolites, [14] metal organic frameworks (MOFs) [5,[14][15][16][17][18][19] and covalent organic frameworks (COFs). [20,21] Stabilization of single-atoms on supports requires a support-surface with specific anchoring sites, such as coordinatively unsaturated surface atoms (e.g., O 2− , OH − ), surface vacancies or heteroatom dopants (e.g., N, P, S, and halogens). The SACs can be stabilized on the support surface by covalent or ionic interactions, or by geometric enclosure in small pores. Each anchoring mode offers several benefits and challenges. For instance, the coordination of a single metal atom to surface oxo ligands makes the single-atom accessible from the outside, e.g., for binding of a substrate. However, it also leads to high surface-energy and destabilization of the single-atom, so that leaching, or agglomeration are possible. In contrast, Single atom catalysts-SACs-have received intense interest in sustainable energy research due to their enormous application potential and broad catalytic scope. In particular, SACs anchored on molecular metal oxides-polyoxometalates (POMs)-offer unrivalled possibilities as models to understand the function of these complex systems on the atomic level. Research questions which are difficult to address for classical heterogeneous SACs can be addressed by experiment and theory using POM-SACs as prototype catalysts. This review reviews the emerging field of POM-SAC research with a focus on fundamental properties and their application in energy conversion...

show abstract

A novel phosphotungstic acid-supported single metal atom catalyst with high activity and selectivity for the synthesis of NH₃ from electrochemical N₂ reduction: a DFT prediction

Abstract: A phosphotungstic acid-supported single metal atom is a potential electrocatalyst for the nitrogen reduction reaction with high activity and high selectivity.

Cited by 73 publications

References 47 publications

Theoretical Calculation of Different Reaction Mechanisms for CO Oxidation on MnN₃-Doped Graphene

Theoretical Calculation of Different Reaction Mechanisms for CO Oxidation on MnN₃-Doped Graphene

Computational Design of Single Mo Atom Anchored Defective Boron Phosphide Monolayer as a High‐performance Electrocatalyst for the Nitrogen Reduction Reaction

Polyoxometalate‐Single Atom Catalysts (POM‐SACs) in Energy Research and Catalysis

Contact Info

Product

Resources

About

A novel phosphotungstic acid-supported single metal atom catalyst with high activity and selectivity for the synthesis of NH3 from electrochemical N2 reduction: a DFT prediction

Abstract: A phosphotungstic acid-supported single metal atom is a potential electrocatalyst for the nitrogen reduction reaction with high activity and high selectivity.

Cited by 73 publications

References 47 publications

Theoretical Calculation of Different Reaction Mechanisms for CO Oxidation on MnN3-Doped Graphene

Theoretical Calculation of Different Reaction Mechanisms for CO Oxidation on MnN3-Doped Graphene

Computational Design of Single Mo Atom Anchored Defective Boron Phosphide Monolayer as a High‐performance Electrocatalyst for the Nitrogen Reduction Reaction

Polyoxometalate‐Single Atom Catalysts (POM‐SACs) in Energy Research and Catalysis

Contact Info

Product

Resources

About

A novel phosphotungstic acid-supported single metal atom catalyst with high activity and selectivity for the synthesis of NH₃ from electrochemical N₂ reduction: a DFT prediction

Theoretical Calculation of Different Reaction Mechanisms for CO Oxidation on MnN₃-Doped Graphene

Theoretical Calculation of Different Reaction Mechanisms for CO Oxidation on MnN₃-Doped Graphene