Polynary transition-metal atom catalysts are promising to supersede platinum (Pt)-based catalysts for oxygen reduction reaction (ORR). Regulating the local configuration of atomic catalysts is the key to catalyst performance enhancement. Different from the previously reported single-atom or dual-atom configurations, a new type of ternary-atom catalyst, which consists of atomically dispersed, nitrogen-coordinated Co-Co dimers, and Fe single sites (i.e., Co2 -N6 and Fe-N4 structures) that are coanchored on highly graphitized carbon supports is developed. This unique atomic ORR catalyst outperforms the catalysts with only Co2 -N6 or Fe-N4 sites in both alkaline and acid conditions. Density functional theory calculations clearly unravels the synergistic effect of the Co2 -N6 and Fe-N4 sites, which can induce higher filling degree of Fe-d orbitals and favors the binding capability to *OH intermediates (the rate determining step). This ternary-atom catalyst may be a promising alternative to Pt to drive the cathodic ORR in zinc-air batteries.

Atomically Dispersed Co2 -N6 and Fe-N4 Costructures Boost Oxygen Reduction Reaction in Both Alkaline and Acidic Media.

Imaging Hydrogen Bonds The decoration of atomic force microscope tips with terminal CO molecules has afforded much higher resolution of the bonding of adsorbed molecules. Zhang et al. (p. 611, published online 26 September) show that this method, in combination with density function theory calculations, can image and characterize hydrogen-bonding contacts formed between 8-hydroxyquinoline molecules adsorbed on the (111) surface of copper under cryogenic conditions. At room temperature, a different bonding configuration was revealed that was the result of the molecules dehydrogenating on the copper surface and coordinating with surface copper atoms. An atomic force microscope tip bearing a single carbon monoxide molecule was used to resolve hydrogen-bonding contacts between molecules. We report a real-space visualization of the formation of hydrogen bonding in 8-hydroxyquinoline (8-hq) molecular assemblies on a Cu(111) substrate, using noncontact atomic force microscopy (NC-AFM). The atomically resolved molecular structures enable a precise determination of the characteristics of hydrogen bonding networks, including the bonding sites, orientations, and lengths. The observation of bond contrast was interpreted by ab initio density functional calculations, which indicated the electron density contribution from the hybridized electronic state of the hydrogen bond. Intermolecular coordination between the dehydrogenated 8-hq and Cu adatoms was also revealed by the submolecular resolution AFM characterization. The direct identification of local bonding configurations by NC-AFM would facilitate detailed investigations of intermolecular interactions in complex molecules with multiple active sites.

/pdf/real-space-identification-of-intermolecular-bonding-with-1dozqwwpb1.pdf

Real-space identification of intermolecular bonding with atomic force microscopy

The in-depth understanding of local atomic environment-property relationships of p-block metal single-atom catalysts toward the 2 e- oxygen reduction reaction (ORR) has rarely been reported. Here, guided by first-principles calculations, we develop a heteroatom-modified In-based metal-organic framework-assisted approach to accurately synthesize an optimal catalyst, in which single In atoms are anchored by combined N,S-dual first coordination and B second coordination supported by the hollow carbon rods (In SAs/NSBC). The In SAs/NSBC catalyst exhibits a high H2 O2 selectivity of above 95 % in a wide range of pH. Furthermore, the In SAs/NSBC-modified natural air diffusion electrode exhibits an unprecedented production rate of 6.49 mol peroxide gcatalyst-1 h-1 in 0.1 M KOH electrolyte and 6.71 mol peroxide gcatalyst-1 h-1 in 0.1 M PBS electrolyte. This strategy enables the design of next-generation high-performance single-atom materials, and provides practical guidance for H2 O2 electrosynthesis. 

Engineering the Local Atomic Environments of Indium Single‐Atom Catalysts for Efficient Electrochemical Production of Hydrogen Peroxide

Understanding the Synergistic Effects of Cobalt Single Atoms and Small Nanoparticles: Enhancing Oxygen Reduction Reaction Catalytic Activity and Stability for Zinc-Air Batteries

The construction of single-atom catalysts (SACs) with high single atom densities, favorable electronic structures and fast mass transfer is highly desired. We have utilized metal-triazolate (MET) frameworks, a subclass of metal-organic frameworks (MOFs) with high N content, as precursors since they can enhance the density and regulate the electronic structure of single-atom sites, as well as generate abundant mesopores simultaneously. Fe single atoms dispersed in a hierarchically porous N-doped carbon matrix with high metal content (2.78 wt %) and a FeN4 Cl1 configuration (FeN4 Cl1 /NC), as well as mesopores with a pore:volume ratio of 0.92, were obtained via the pyrolysis of a Zn/Fe-bimetallic MET modified with 4,5-dichloroimidazole. FeN4 Cl1 /NC exhibits excellent oxygen reduction reaction (ORR) activity in both alkaline and acidic electrolytes. Density functional theory calculations confirm that Cl can optimize the adsorption free energy of Fe sites to *OH, thereby promoting the ORR process. The catalyst demonstrates great potential in zinc-air batteries. This strategy selects, designs, and adjusts MOFs as precursors for high-performance SACs.

Metal-Triazolate-Framework-Derived FeN 4 Cl 1 Single-Atom Catalysts with Hierarchical Porosity for the Oxygen Reduction Reaction.

Single-atom electrocatalysts (SAECs) have recently attracted tremendous research interest due to their often remarkable catalytic responses, unmatched by conventional catalysts. The electrocatalytic performance of SAECs is closely related to the specific metal species and their local atomic environments, including their coordination number, the determined structure of the coordination sites, and the chemical identity of nearest and second nearest neighboring atoms. The wide range of distinct chemical bonding configurations of a single-metal atom with its surrounding host atoms creates virtually limitless opportunities for the rational design and synthesis of SAECs with tunable local atomic environment for high-performance electrocatalysis. In this review, the authors first identify fundamental hurdles in electrochemical conversions and highlight the relevance of SAECs. They then critically examine the role of the local atomic structures, encompassing the first and second coordination spheres of the isolated metal atoms, on the design of high-performance SAECs. The relevance of single-atom dopants for host activation is also discussed. Insights into the correlation between local structures of SAECs and their catalytic response are analyzed and discussed. Finally, the authors summarize major challenges to be addressed in the field of SAECs and provide some perspectives in the rational construction of superior SAECs for a wide range of electrochemical conversions.

Design of Local Atomic Environments in Single-Atom Electrocatalysts for Renewable Energy Conversions.

Intermolecular strain has long been used to steer and promote chemical reactions towards desired products in wet chemical synthesis. However, similar protocols have not been adopted for the on-surface synthesis on solid substrates due to the complexity of reaction processes. Recent advances in the sub-molecular resolution with scanning probe microscopy allow us to capture on-surface reaction pathways and to gain substantial insights into the role of strain in chemical reactions. The primary focus of this review is to highlight the recent findings on strain-induced on-surface reactions. Such substrate-induced processes can be applied to alter the chemical reactivity and to drive on-surface chemical reactions in different manners, which provides a promising alternative approach for on-surface synthesis. This review aims to shed light on the utilization of substrate-induced strain for on-surface transformation and synthesis of atomically-precise novel functional nanomaterials.

Substrate induced strain for on-surface transformation and synthesis

Recent advances in bond-resolved scanning tunneling microscopy (BRSTM) have demonstrated the tremendous potential of this characterization technique to attain an ultra-high spatial resolution at th...

Recent advances in bond-resolved scanning tunneling microscopy

Organic radicals consisting of light elements exhibit a low spin–orbit coupling and weak hyperfine interactions with a long spin coherence length, which are crucial for future applications in molec

Real-space imaging of a single-molecule monoradical reaction

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Design of Local Atomic Environments in Single-Atom Electrocatalysts for Renewable Energy Conversions.

Substrate induced strain for on-surface transformation and synthesis

Recent advances in bond-resolved scanning tunneling microscopy

Real-space imaging of a single-molecule monoradical reaction