Synergistic Effects for Enhanced Catalysis in a Dual Single-Atom Catalyst

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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confidence: 99%

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

Santiago

Kong

et al. 2021

Small

115

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“…The synergetic effects between adjacent active sites on heterogeneous catalysis have drawn increasing attention in experimental work. 5,[22][23][24][25][26] In parallel, the computational approach plays an indispensable role in dissecting mechanisms and structure-property relationships associated with SACs. 27 Previously, we have conducted a first-principle study on cooperative communications between two neighboring active centers, and impacts of active site density on oxygen reduction reaction (ORR) and nitrogen reduction reaction (NRR) respectively.…”

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confidence: 99%

Cooperative Single-Atom Active Centers for Attenuating the Linear Scaling Effect in the Nitrogen Reduction Reaction

Yao

et al. 2021

J. Phys. Chem. Lett.

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Cooperative effects of adjacent active centers are critical for single-atom catalysts (SACs) as active site density matters. Yet how it affects scaling relationships in many important reactions like nitrogen reduction reaction (NRR) is underexplored. Herein we elucidate how the cooperation of two active centers can attenuate the linear scaling effect in NRR, through the first-principle study on 39 SACs comprised of two adjacent (~4 Å apart) four N-coordinated metal centers (MN4 duo) embedded in graphene. Bridge-on adsorption of dinitrogen-containing species appreciably tilts the balance of adsorption of N2H and NH2 towards N2H and thus substantially loosens the restraint of scaling relations in NRR, achieving low onset potential (V) and direct N≡N cleavage (Mo, Re) at room temperature, respectively. The potential of MN4 duo in NRR casts new insight into circumventing limitations of scaling relations in heterogeneous catalysis.

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“…Therefore, developing simple methods suitable for large‐scale production is currently the major direction in the synthesis of SACs with high metal loading. Moreover, dual SACs 159 and single‐atom alloy catalysts 160,161 have recently become new popular research thrusts in the field of SACs. The electrochemical properties of these catalysts have been tailored via alloy bonding.…”

Section: Discussionmentioning

confidence: 99%

Recent advances in high‐loading catalysts for low‐temperature fuel cells: From nanoparticle to single atom

Shen

et al. 2021

SusMat

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Low‐temperature fuel cells (LTFCs) are considered to be one of the most promising power sources for widespread application in sustainable and renewable energy conversion technologies. Although remarkable advances have been made in the mass activity of catalysts, mass transport impedance needs to be urgently addressed at a well‐designed membrane electrode assembly (MEA) scale. Increasing the loading of electrocatalysts is conducive to prepare thinner and more efficient MEAs owing to the resulting enhanced reactant permeability, better proton diffusion, and lower electrical resistance. Herein, recent progress in high‐loading (≥40 wt.%) Pt nanoparticle catalysts (NPCs) and high‐loading (≥2 wt.%) single‐atom catalysts (SACs) for LTFC applications are reviewed. A summary of various synthetic approaches and support materials for high‐loading Pt NPCs and SACs is systematically presented. The influences of high surface area and appropriate surface functionalization for Pt NPCs, as well as coordination environment, spatial confinement effect, and strong metal‐support interactions (SMSI) for SACs are highlighted. Additionally, this review presents some ideas regarding challenges and future opportunities of high‐loading catalysts in the application of LTFCs.

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Synergistic Effects for Enhanced Catalysis in a Dual Single-Atom Catalyst

Cited by 213 publications

References 57 publications

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

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

Cooperative Single-Atom Active Centers for Attenuating the Linear Scaling Effect in the Nitrogen Reduction Reaction

Recent advances in high‐loading catalysts for low‐temperature fuel cells: From nanoparticle to single atom

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