Understanding the structure-performance relationship of active sites at atomic scale

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

Selective conversion of specific functional groups to desired products is highly important but still challenging in industrial catalytic processes. The adsorption state of surface species is the key factor in modulating the conversion of functional groups, which is correspondingly determined by the uniformity of active sites. However, the non‐identical number of metal atoms, geometric shape, and morphology of conventional nanometer‐sized metal particles/clusters normally lead to the non‐uniform active sites with diverse geometric configurations and local coordination environments, which causes the distinct adsorption states of surface species. Hence, it is highly desired to modulate the homogeneity of the active sites so that the catalytic transformations can be better confined to the desired direction. In this review, the construction strategies and characterization techniques of the uniform active sites that are atomically dispersed on various supports are examined. In particular, their unique behavior in boosting the catalytic performance in various chemical transformations is discussed, including selective hydrogenation, selective oxidation, Suzuki coupling, and other catalytic reactions. In addition, the dynamic evolution of the active sites under reaction conditions and the industrial utilization of the single‐atom catalysts are highlighted. Finally, the current challenges and frontiers are identified, and the perspectives on this flourishing field is provided.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202201520

Homogeneity of Supported Single‐Atom Active Sites Boosting the Selective Catalytic Transformations

Single-atom catalysts (SACs) hold the promise of utilizing 100% of the participating atoms in a reaction as active catalytic sites, achieving a remarkable boost in catalytic efficiency. Thus, they present great potential for noble metal-based electrochemical application systems, such as water electrolyzers and fuel cells. However, their practical applications are severely hindered by intrinsic complications, namely atom agglomeration and relocation, originating from the uncontrollably high surface energy of isolated single-atoms (SAs) during postsynthetic treatment processes or catalytic reactions. Extensive efforts have been made to develop new methodologies for strengthening the interactions between SAs and supports, which could ensure the desired stability of the active catalytic sites and their full utilization by SACs. This review covers the recent progress in SACs development while emphasizing the association between the regulation of coordination environments (e.g., coordination atoms, numbers, sites, structures) and the electrocatalytic performance of the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). The crucial role of coordination chemistry in modifying the intrinsic properties of SACs and manipulating their metal-loading, stability, and catalytic properties is elucidated. Finally, the future challenges of SACS development and the industrial outlook of this field are discussed.

Modulating the Local Coordination Environment of Single-Atom Catalysts for Enhanced Catalytic Performance in Hydrogen/Oxygen Evolution Reaction.

Achieving high-temperature stability/duration without compromising the activity remains an arduous task in catalyst design, particularly for MoS 2 materials. Herein, a robust catalyst with Mo doped Co 9 S 8 nanoparticles anchored on Al 2 O 3 matrix is fabricated, which could selectively convert lignin to arenes with high hydrodeoxygenation activity, selectivity and particularly excellent stability. In the hydrodeoxygenation of diphenyl ether, this catalyst afforded 99.8% conversion and 91.0% yield of benzene at 265 °C for at least 10 reaction runs. The resultant Mo-Co 9 S 8 structure with chemical connection by covalent bonds of Mo-S-Co type on the Co 9 S 8 surface demonstrates strong ability in the adsorption and activation of oxygen-containing substrates, which enables the effective C-O cleavage whilst avoids undesirable hydrogenation of benzene ring. The superior stability and water-resistance at elevated temperature was attributed to the anchoring effect of Al 2 O 3 matrix and “protection” of surface-rich Co 9 S 8 species to the active Mo-Co 9 S 8 center. This strategy provides new sights for the rational design of efficient and stable sulfide catalysts towards the applications in demanding high-temperature reactions. A facile strategy for fabricating high-temperature stable Mo-Co 9 S 8 /Al 2 O 3 catalyst was demonstrated, which could selectively convert lignin to arenes at 265 °C for at least 10 reaction runs, featuring high activity, selectivity and particularly excellent stability. • High temperature stable and efficient Mo-Co 9 S 8 /Al 2 O 3 catalyst was fabricated. • Novel Mo-Co 9 S 8 structure with covalent bonds of Mo-S-Co type was formed on the Co 9 S 8 surface. • The catalyst could selectively convert lignin to arenes at 265 °C for at least 10 reaction runs. • The superior activity and stability were attributed to the formation of Mo-Co 9 S 8 center. 

Fabricating high temperature stable Mo-Co9S8/Al2O3 catalyst for selective hydrodeoxygenation of lignin to arenes

Metal-support interactions are of great importance in determining the support-activity in heterogeneous catalysis. Here we report a low-temperature synthetic strategy to create atomically dispersed palladium atoms anchored on defective hexagonal boron nitride (h-BN) nanosheet. Density functional theory (DFT) calculations suggest that the nitrogen-containing B vacancy can provide stable anchoring sites for palladium atoms. The presence of single palladium atoms was confirmed by spherical aberration correction electron microscopy and extended X-ray absorption fine structure measurement. This catalyst showed exceptional efficiency in chemoselective hydrogenation of cinnamaldehyde, along with excellent recyclability, sintering-resistant ability, and scalability. We anticipate this synthetic approach for the synthesis of high-quality SACs based on h-BN support is amenable to large-scale production of bench-stable catalysts with maximum atom efficiency for industrial applications.

Low-Temperature Synthesis of Single Palladium Atoms Supported on Defective Hexagonal Boron Nitride Nanosheet for Chemoselective Hydrogenation of Cinnamaldehyde

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Low-Temperature Synthesis of Single Palladium Atoms Supported on Defective Hexagonal Boron Nitride Nanosheet for Chemoselective Hydrogenation of Cinnamaldehyde