Theoretical insights into the performance of single and double transition metal atoms doped on N-graphenes for N2 electroreduction

Qu, Mengnan; Qin, Gangqiang; Fan, Jianxi; Du, Aijun; Sun, Qiao

doi:10.1016/j.apsusc.2020.148012

Cited by 32 publications

(22 citation statements)

References 78 publications

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“…The calculated WBIs (≈0.0001) and charge transfer confirm the N2 physisorption on Mn3Cu3@C24N24. Regardless of all possible bi-metal distributions into the porphyrin C24N24 cavities, the three TixCuz@C24N24, TizMny@C24N24, and MnyCuz@C24N24 (x, z, y = 0-6) complexes with Although the Mn 3 Cu 3 @C 24 N 24 complex adsorbs N 2 molecule with lower E ads , due to its lower catalytic activity toward gas adsorption, this value is still higher than that on Mn-Fe bi-metal atoms anchored pyridinic nitrogen-doped graphene (E ads = −0.53 eV) [63]. The calculated WBIs (≈0.0001) and charge transfer confirm the N 2 physisorption on Mn 3 Cu 3 @C 24 N 24 .…”

Section: Adsorption Of N2 and No2mentioning

confidence: 99%

“…Although the Mn 3 Cu 3 @C 24 N 24 complex adsorbs N 2 molecule with lower E ads , due to its lower catalytic activity toward gas adsorption, this value is still higher than that on Mn-Fe bi-metal atoms anchored pyridinic nitrogen-doped graphene (E ads = −0.53 eV) [ 63 ]. The calculated WBIs (≈0.0001) and charge transfer confirm the N 2 physisorption on Mn 3 Cu 3 @C 24 N 24 .…”

Section: Catalytic Behavior Of Bi-metal Complexes Toward Adsorption Of Gas Speciesmentioning

confidence: 99%

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Linking Bi-Metal Distribution Patterns in Porous Carbon Nitride Fullerene to Its Catalytic Activity toward Gas Adsorption

Nematollahi

Neyts

2021

Nanomaterials

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Immobilization of two single transition metal (TM) atoms on a substrate host opens numerous possibilities for catalyst design. If the substrate contains more than one vacancy site, the combination of TMs along with their distribution patterns becomes a design parameter potentially complementary to the substrate itself and the bi-metal composition. By means of DFT calculations, we modeled three dissimilar bi-metal atoms (Ti, Mn, and Cu) doped into the six porphyrin-like cavities of porous C24N24 fullerene, considering different bi-metal distribution patterns for each binary complex, viz. TixCuz@C24N24, TixMny@C24N24, and MnyCuz@C24N24 (with x, y, z = 0–6). We elucidate whether controlling the distribution of bi-metal atoms into the C24N24 cavities can alter their catalytic activity toward CO2, NO2, H2, and N2 gas capture. Interestingly, Ti2Mn4@C24N24 and Ti2Cu4@C24N24 complexes showed the highest activity and selectively toward gas capture. Our findings provide useful information for further design of novel few-atom carbon-nitride-based catalysts.

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Section: Adsorption Of N2 and No2mentioning

confidence: 99%

Section: Catalytic Behavior Of Bi-metal Complexes Toward Adsorption Of Gas Speciesmentioning

confidence: 99%

Linking Bi-Metal Distribution Patterns in Porous Carbon Nitride Fullerene to Its Catalytic Activity toward Gas Adsorption

Nematollahi

Neyts

2021

Nanomaterials

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“…Owing to the excellent catalytic performance, HDACs are widely investigated for NRR. [67][68][69][70][71] Similar to NRR, CO 2 activation and reduction is also very difficult due to the seriously restricted scaling relations. Ouyang et al [72] designed heteronuclear transition-metal dimers supported on monolayer C 2 N as effective dual-atom catalysts to break the scaling relations during CO 2 RR.…”

Section: Low-dimensional Networkmentioning

confidence: 99%

Atomically Dispersed Heteronuclear Dual‐Atom Catalysts: A New Rising Star in Atomic Catalysis

Santiago

Kong

et al. 2021

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115

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carbon dioxide reduction, which can also be driven by clean and renewable energies such as wind, solar and hydropower resources, represent crucial steps of these renewable energy devices. However, the performances of these chemical reactions strongly rely on the energy storage and conversion efficiencies of the catalytic materials deposited on the electrodes. [6][7][8][9][10] Therefore, the development of robust and earth-abundant catalysts with both high catalytic activity and selectivity play a critical role in the real application of these devices.Current catalysts for energy-related chemical reactions are heavily dependent on noble metals, which impedes their large potential commercialization. [11][12][13] Further, the catalytic process mostly occurred on the metal surfaces, leading to the very low utilization efficiency of the catalysts. To minimize the waste of the non-accessible atoms in the bulk metals, researchers developed several strategies to modify metal structures in order to expose as many metal atoms as possible. [10,[14][15][16][17][18] One of the most popular methods is to downsize the solid metal catalysts to the atomic level (Figure 1). More interestingly, the catalytic behaviors of the metal catalysts with different sizes have significantly Atomic catalysts (AC) are gaining extensive research interest as the most active new frontier in heterogeneous catalysis due to their unique electronic structures and maximum atom-utilization efficiencies. Among all the atom catalysts, atomically dispersed heteronuclear dual-atom catalysts (HDACs), which are featured with asymmetric active sites, have recently opened new pathways in the field of advancing atomic catalysis. In this review, the up-todate investigations on heteronuclear dual-atom catalysts together with the last advances on their theoretical predictions and experimental constructions are summarized. Furthermore, the current experimental synthetic strategies and accessible characterization techniques for these kinds of atomic catalysts, are also discussed. Finally, the crucial challenges in both theoretical and experimental aspects, as well as the future prospects of HDACs for energy-related applications are provided. It is believed that this review will inspire the rational design and synthesis of the new generation of highly effective HDACs.

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“…In the literature, low-valence elements have been employed as potential active sites or co-catalysts for NRR, − which deserve more investigation, such as the relationship between catalysis performance and oxidation state. Compared with single-atom catalysts − and defects, , M + (M = Na, K, Li, etc.) can be abundant and obtained readily from the solution, without resulting in any issue of stabilities.…”

Section: Results and Discussionmentioning

confidence: 99%

Insight into the Reactivity of Carbon Structures for Nitrogen Reduction Reaction

Qiu

Yan

et al. 2021

Langmuir

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Graphene-based structures have been widely reported as promising metal-free catalysts for nitrogen reduction reaction. To explain the reactivity origin, various structures have been proposed and debated, including defects, functional groups, and doped heteroatoms. This computational work demonstrates that these structures may evolve from one to another under electrochemical conditions, generating weakly coordinated carbons, which have been identified as the active sites for N 2 adsorption and activation.

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Theoretical insights into the performance of single and double transition metal atoms doped on N-graphenes for N2 electroreduction

Cited by 32 publications

References 78 publications

Linking Bi-Metal Distribution Patterns in Porous Carbon Nitride Fullerene to Its Catalytic Activity toward Gas Adsorption

Linking Bi-Metal Distribution Patterns in Porous Carbon Nitride Fullerene to Its Catalytic Activity toward Gas Adsorption

Atomically Dispersed Heteronuclear Dual‐Atom Catalysts: A New Rising Star in Atomic Catalysis

Insight into the Reactivity of Carbon Structures for Nitrogen Reduction Reaction

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