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.

In this study, we selected 10 Co-based double-atom catalysts (DACs) catalysts, namely CoMN6-gra(OH) (M ​= ​Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn), and investigated their oxygen reduction reactions (ORR) catalytic performances with/without considering the magnetic coupling by means of density functional theory (DFT) calculations. It was found that CoNiN6-gra(OH), CoCuN6-gra(OH), and CoZnN6-gra(OH) exhibit good catalytic activity of ORR (with low overpotentials of 0.33, 0.34 and 0.23 ​V, respectively) when the magnetic coupling is considered. In particular, magnetic changes in CoMN6-gra(OH) candidates play a vital role in their ORR catalytic activity. Interestingly, the d-band center can be utilized to well rationalize the ORR catalytic activity. This work highlights the importance of considering the magnetic coupling to well predict the activity of ORR catalysts, and discloses that the manipulation of the magnetic coupling between transition metal atoms is an emerging and powerful approach for the development of high-performance electrocatalysts for ORR and other related reactions. 

Revisiting catalytic performance of supported metal dimers for oxygen reduction reaction via magnetic coupling from first principles

In the present work the authors show that anodic TiO2 nanotubes (NT) show excellent harvesting properties for Pt single atoms (Pt SAs) from highly dilute Pt solutions. The tube walls of anodic nanotubes, after adequate annealing to anatase, provide ample of suitable trapping sites-that is, surface Ti3+ -Ov (Ov : oxygen vacancy) defects that are highly effective to extract and accumulate Pt in the form of SAs. A saturated (maximized) SA density can be achieved by an overnight immersion of a TiO2 NT layer to a H2 PtCl6 solution with a concentration that is as low as 0.01 mm Pt. Such TiO2 NTs with surface trapped Pt SAs provide a maximized high activity for photocatalytic H2 generation (reaching a turnover frequency (TOF) of 1.24 × 106 h-1 at a density of 1.4 × 105 Pt atoms µm-2 )-a higher loading with Pt nanoparticles does not further increase the photocatalytic activity. Overall, these findings show that anodic TiO2 nanotubes provide a remarkable substrate for Pt extraction and recovery from very dilute solutions that directly results in a highly efficient photocatalyst, fabricated by a simple immersion technique.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/smll.202104892

Optimized Pt Single Atom Harvesting on TiO2 Nanotubes-Towards a Most Efficient Photocatalyst.

The development of highly efficient bifunctional electrocatalysts to boost oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is highly desirable for energy conversion and storage devices. Herein, by means of comprehensive first-principles computations, we systematically explored the catalytic activities of a series of single transition metal atoms anchored on two-dimensional VS2 monolayers (TM@VS2) for ORR/OER. Our results revealed that Ni@VS2 exhibits low overpotentials for both ORR (0.45 V) and OER (0.31 V), suggesting its great potential as a bifunctional catalyst, which is mainly induced by its moderate interaction with oxygenated intermediates according to the established scaling relationship and volcano plot. Interestingly, the substituted doping of nitrogen heteroatoms into the VS2 substrate can further effectively improve the ORR/OER activity of the active metal atom to achieve more eligible ORR/OER bifunctional catalysts. Our results not only propose a new class of potential bifunctional oxygen catalysts but also offer a feasible strategy for further tuning their catalytic activity.

Computational screening of single-atom catalysts supported by VS2 monolayers for electrocatalytic oxygen reduction/evolution reactions.

Room-temperature sodium–sulfur (RT Na–S) batteries have recently captured intensive research attention from the community and are regarded as one of promising next-generation energy storage devices since they not only integrate the advantages in high abundance and low commercial cost of elemental Na/S but also exhibit exceptionally high theoretical capacity and energy density. Whereas, the notorious shuttle effect of soluble intermediates and sluggish kinetics remain two main obstacles for RT Na–S batteries to step into new developmental stage. Recently, impressive advancements of metal-based electrocatalysts have offered a viable solution to stabilize S cathodes and unlocked new opportunities for RT Na–S batteries. Here, we underline the recent progress on metal-based electrocatalysts for RT Na–S batteries for the first time by shedding light on this emerging but promising field. The involved metal-based electrocatalysts include metals, metal oxides, metal sulfides, metal carbides, and other metal-based catalytic species. Our emphasis is focused on the discussion of design, fabrication, and properties of these electrocatalysts as well as interactions between electrocatalysts and sodium polysulfides. Otherwise, some potential electrocatalysts for RT Na–S batteries are pointed out as well. At last, perspectives for the future development of RT Na–S batteries with S cathode electrocatalysts are offered.

Metal-based electrocatalysts for room-temperature Na-S batteries.

Supported single-atom catalysts (SACs) have received a lot of attention due to their super-high atom utilization and outstanding catalytic performance. However, the instability of the supported transition-metal (TM) atoms hampers their widespread applications. Exploration of an appropriate substrate to stabilize the supported single atom is crucial for the future implementation of SACs. In recent years, two-dimensional materials have been proposed as possible substrates due to their large specific surface areas, but their chemically inert surfaces are difficult to stabilize TM atoms without defecting or doping. Herein, by means of systematic first-principles calculations, we demonstrate that the defect-free MoS2 monolayer in the unconventional phase (1T') can effectively immobilize single TM atoms owing to its unique electrophilic property as compared to the conventional 2H phase. As a prototype probe, we investigated oxygen reduction reaction (ORR) catalyzed by a total of 21 single TM atoms stabilized on 1T'-MoS2 and successfully screened out two candidates, Cu and Pd@1T'-MoS2, which have a low overpotential of 0.41 and 0.32 V respectively, outperforming most of the previously reported ORR catalysts. Furthermore, we reveal that the adsorption energy of the ORR intermediate, *OH, provides an excellent descriptor to assess the ORR activity, which is further determined by the d-band center of the supported TM adatoms, thus being a great advantage for future design of stable and high-performance SACs.

Single Transition Metal Atom Bound to the Unconventional Phase of the MoS2 Monolayer for Catalytic Oxygen Reduction Reaction: A First-Principles Study.

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Single Transition Metal Atom Bound to the Unconventional Phase of the MoS2 Monolayer for Catalytic Oxygen Reduction Reaction: A First-Principles Study.