In recent years, dual-atom catalysts (DACs) have attracted extensive attention, as an extension of single-atom catalysts (SACs). Compared with SACs, DACs have higher metal loading and more complex and flexible active sites, thus achieving better catalytic performance and providing more opportunities for electrocatalysis. This review introduces the research progress in recent years on how to design new DACs to enhance the performance of electrocatalysis. Firstly, the advantages of DACs in increasing metal loading are introduced. Then, the role of DACs in changing the adsorption condition of reactant molecules on metal atoms is discussed. Moreover, the ways in which DACs can reduce the reaction energy barrier of key steps and change the reaction path are explored. Catalytic applications in different electrocatalytic reactions, including the carbon dioxide reduction reaction, oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, and nitrogen reduction reaction are followed. Finally, a brief summary is made and the key challenges and prospects of DACs are introduced. 

Superiority of Dual‐Atom Catalysts in Electrocatalysis: One Step Further Than Single‐Atom Catalysts

https://doi.org/10.1038/s41467-022-28987-1

Oxo dicopper anchored on carbon nitride for selective oxidation of methane

Hydrogenation of CO2 into valuable chemicals is of great significance but very challenging due to its chemical inertness and selectivity controlling. Here, we report that CeO2 supported Pd dimers can efficiently convert CO2 to ethanol with significantly higher activity and selectivity compared to those in literatures, which gives a selectivity of 99.2 % to ethanol with a space-time yield of 45.6 gethanol gPd−1 h−1. The Pd dimers possessing unique Pd2O4 configuration and high homogeneity enables to directly dissociate CO2 to CO, trigger C C coupling but appropriately inhibit further C2+ coupling, which benefits to selectively form ethanol. The Pd2O4 configuration can strongly bind CO on Pd2/CeO2, which prevents CO desorption and promotes the coupling between CO and CH3 intermediates to form the precursor of ethanol. The strategy of constructing atom-precision active sites reported in this work opens new avenues to develop highly selective catalysts for CO2/CO hydrogenation reactions.

CeO2 supported Pd dimers boosting CO2 hydrogenation to ethanol

Development of effective and stable catalysts for CO2 hydrogenation into ethanol remains a challenge. Herein, we report that Rh1/CeTiOx single-atom catalyst constructed by embedding monoatomic Rh onto Ti-doped CeO2 support has shown a super high ethanol selectivity (~99.1%), record-breaking turnover frequency (493.1 h-1), and outstanding stability. Synergistic effects of Ti-doption and monoatomic Rh contribute to this excellent catalytic performance by firstly facilitating oxygen vacancies formation to generate oxygen-vacancy-Rh Lewis-acid-base pairs, which favor CO2 adsorption and activation, cleavage of C-O bonds in CHxOH* and COOH* into CHx* and CO* species, subsequent C-C coupling and hydrogenation into ethanol, and secondly generating strong Rh-O bond by Ti-doping-induced crystal reconstruction, which contributes to striking stability. This work stresses the importance of support elaborating regulation for single-atom catalyst design to improve the catalytic performance.

Ti-doped CeO2 Stabilized Single-Atom Rhodium Catalyst for Selective and Stable CO2 Hydrogenation to Ethanol.

Platinum (Pt)-based catalysts often failed to possess high CO2 conversion and high CO selectivity at the same time (especially at high reaction temperature) in reverse water gas shift (RWGS) reaction. Herein, we found that atomically dispersed Pt species was the crucial factor in improving the selectivity of CO and inhibiting the formation of CH4. Three Pt/CeO2 catalysts, including atomically dispersed Pt species, and Pt clusters or particles with different sizes, were synthesized. It was found that the atomically dispersed Pt/CeO2 catalyst led to an outstanding CO selectivity (>98 %) in the temperature range of 200∼450 °C, while the CO selectivities over Pt nanoparticles decreased conspicuously as the reaction temperature increased. CO-TPD and in situ FTIR experiments demonstrated that CH4 was produced by the further hydrogenation of CO. And the atomically dispersed Pt species had the relatively weak adsorption strength toward CO, which prevented excessive hydrogenation and promoted CO selectivity in RWGS reaction. Our investigation provides a new thinking for designing the RWGS reaction catalyst with an outstanding CO selectivity and emphasize the significance of atomically dispersed catalysts in catalytic reactions again.

Atomically dispersed Pt/CeO2 catalyst with superior CO selectivity in reverse water gas shift reaction

Catalytically converting CH4 to chemicals and fuels is of paramount importance but remains a major challenge to simultaneously obtain high activity and selectivity. Here, we report Cu1/ZSM-5 single atom catalyst is highly active (C1 oxygenates productivity of 4800 μmol⋅gcat−1 at 50 °C and 12,000 μmol⋅gcat-1 at 70 °C within 30 min) and selective (C1 oxygenates selectivity of 99 % at 50 °C) for direct CH4 oxidation, comparable to most of those state-of-the-art noble metal catalysts. The combined DFT calculation, electronic microscope, X-ray absorption and electron paramagnetic resonance results confirm that each isolated Cu atom stabilized by four O moieties on the ZSM-5 support possesses uniform Cu1-O4 entity as active site and preferentially activates CH4 instead of CH3OH that is advantageous for highly selective C1 oxygenates production, especially for methanol. Our molecular-level finding on the atomic structure of Cu active site paves the way to design better catalysts for methane conversion.

Direct oxidation of methane to oxygenates on supported single Cu atom catalyst

Selective activation of carbon‐oxygen bonds (like C−O and C=O) represents an essential part of the biomass conversion, but it is difficult to selectively activating the inert carbon‐oxygen bonds. We report 2D MoS2 edges confined single Pt atoms efficiently catalyze biomass‐derived crotonaldehyde to crotyl alcohol with selectivity from 90 to 100 %. The Pt1/MoS2 single‐atom catalysts have a unique HO−Mo−S−Pt1−S−Mo−OH configuration, reminiscent of an enzyme pocket‐like active site, which restricts the adsorption configuration of crotonaldehyde by a steric hindrance effect. The Pt1 atoms possess unique electronic structures due to the Pt1‐S4 configuration, which easily dissociates H2 to H species and boosts the activity. The activated H species spillover and react with O atoms on edges, forming OH and creating the HO−Mo−S−Pt1−S−Mo−OH configuration, which restricts the adsorption configuration of crotonaldehyde and yields high selectivity. The tactics of fabricating pocket‐like active sites with metal single atoms and 2D nanosheet edges shed a light on developing highly selective catalysts for biomass conversion reactions.

Edge-Confined Pt1/MoS2 Single-Atom Catalyst Promoting the Selective Activation of Carbon-Oxygen Bond

The invention discloses a supported metal diatomic catalyst, a preparation method and applications thereof. The preparation method comprises the following steps: dissolving chlorides or nitrates of platinum group metals in water or an alcohol solvent to obtain a metal precursor solution, and controlling the temperature of the precursor solution to be 20-40 DEG C and the isoelectric point of the solution to be 1-8, so that the platinum group metals in the metal precursor solution form a binary coordination structure; dispersing an oxide carrier in water or an alcohol solvent to prepare a carrier solution, wherein the oxide carrier comprises CeO2, Ga2O3, In2O3 and ZnO; adding the metal precursor solution into the carrier solution, so that the metal precursor is uniformly dispersed on the surface of the oxide carrier; and filtering, drying, and roasting in air or oxygen to obtain the supported metal diatomic catalyst. The supported metal diatomic catalyst provided by the invention has high activity and high selectivity on ethanol generated by CO2 catalytic hydrogenation.

Supported metal diatomic catalyst as well as preparation method and application thereof

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CeO2 supported Pd dimers boosting CO2 hydrogenation to ethanol

Direct oxidation of methane to oxygenates on supported single Cu atom catalyst

Edge-Confined Pt1/MoS2 Single-Atom Catalyst Promoting the Selective Activation of Carbon-Oxygen Bond

Supported metal diatomic catalyst as well as preparation method and application thereof