Single-Atom Catalysts: A Perspective toward Application in Electrochemical Energy Conversion

Speck, Florian; Kim, Jae Hyung; Bae, Geunsu; Joo, Sang Hoon; Mayrhofer, Karl Johann Jakob; Choi, Chang Hyuck; Cherevko, Serhiy

doi:10.1021/jacsau.1c00121

Cited by 58 publications

(59 citation statements)

References 125 publications

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“… 82 Under the OER or ORR conditions, the carbon atoms in widely investigated Fe–N–C catalysts can be oxidized to CO or CO 2 . 12 Thus, according to the working conditions, criteria related to possible side reactions are expected to be provided to comprehensively evaluate the stability of SACs during the theoretical design of new SACs.…”

Section: Design Criteriamentioning

confidence: 99%

Understanding Single-Atom Catalysis in View of Theory

Zhang

Luo

et al. 2021

JACS Au

118

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In the past decade, isolated single atoms have been successfully dispersed on various substrates, with their potential applications being intensively investigated in different reactions. While the essential target of research in single-atom catalysis is the precise synthesis of stable single-atom catalysts (SACs) with clear configurations and impressive catalytic performance, theoretical investigations have also played important roles in identifying active sites, revealing catalytic mechanisms, and establishing structure–activity relationships. Nevertheless, special attention should still be paid in theoretical works to the particularity of SACs. In this Perspective, we will summarize the theoretical progress made on the understanding of the rich phenomena in single-atom catalysis. We focus on the determination of local structures of SACs via comparison between experiments and simulations, the discovery of distinctive catalytic mechanisms induced by multiadsorption, synergetic effects, and dynamic evolutions, to name a few, the proposal of criteria for theoretically designing SACs, and the extension of original concepts of single-atom catalysis. We hope that this Perspective will inspire more in-depth thinking on future theoretical studies of SACs.

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Section: Design Criteriamentioning

confidence: 99%

Understanding Single-Atom Catalysis in View of Theory

Zhang

Luo

et al. 2021

JACS Au

118

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“…These properties, along with the increased number of under-coordinated metal atoms, i.e., the increased amount of active catalytic sites, make nanocluster catalysts highly active towards a wide range of chemical reactions, such as CO 2 RR and HER [22][23][24][25]. The ideal case, corresponding to the minimum size and the maximum metal-utilization of the nanocluster is represented by the metal single atom: at this size, individual metal atoms become accessible, and therefore active for catalysis [26]. More generally, in order to guarantee high dispersion and to avoid agglomeration, nanoparticle catalysts are typically dispersed on a support surface.…”

Section: Introductionmentioning

confidence: 99%

Single-Atom Catalysts for the Electro-Reduction of CO2 to Syngas with a Tunable CO/H2 Ratio: A Review

Scarpa

Sarno

2022

Catalysts

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Nowadays, transition towards green chemistry is becoming imperative. In this scenario, an attractive perspective consists in the generation of CO through the electrochemical reduction of CO2 under ambient conditions. This approach allows storage of the electrical energy from intermittent renewable sources in the form of chemical bonds, and simultaneously reduces greenhouse gas emissions, giving carbon a second chance of life. However, most catalysts adopted for this process, i.e., noble metal-based nanoparticles, still have several issues (high costs, low current densities, high overpotentials), and in the view of generating syngas through co-electrolysis of H2O and CO2, do not enable a widely tunable CO/H2 ratio. Single-atom catalysts with N-doped carbon supports have been recently introduced to face these challenges. The following review aims to answer the demand for an extended and exhaustive analysis of the metal single-atom catalysts thus far explored for the electro-reduction of CO2 in aqueous electrolyte solution. Moreover, focus will be placed on the objective of generating a syngas with a tunable CO/H2 ratio. Eventually, the advantages of single-atom catalysts over their noble metal-based nano-sized counterparts will be identified along with future perspectives, also in the view of a rapid and feasible scaling-up.

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“…[3][4][5] Among all identified PGM-free candidates, iron-nitrogen-doped carbon (Fe-N-C) is the most promising to catalyse the sluggish ORR. 6,7 Recent studies have theoretically and experimentally demonstrated that Fe-N-C catalysts are more active and stable in alkaline than in acidic media. [8][9][10] This indicates the unique possibility to use Fe-N-C as a relatively efficient, earth abundant and cheap cathode catalyst material in alternative anion exchange membrane fuel cell (AEMFCs) technology.…”

Section: Introductionmentioning

confidence: 99%

“…In particular, understanding of Fe x+ leaching and consequent implementation of mitigation strategies to its suppression are considered main challenges. 6,8,15,16 So far, four key Fe-N-C degradation mechanisms have been suggested to occur in parallel or series in acidic media, 7 providing clues also to studies in alkaline electrolytes:…”

Section: Introductionmentioning

confidence: 99%

Oxygen Reduction Reaction Causes Iron Leaching from Fe-N-C Electrocatalysts

Ehelebe

Bierling

et al. 2021

Preprint

Self Cite

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The electrochemical activity of modern Fe-N-C electrocatalysts in alkaline media is on par with that of platinum. For successful application in fuel cells, however, also high durability and longevity must be demonstrated. Currently, design and synthesis of simultaneously active and stable platinum group metal-free electrocatalysts is hindered by a limited understanding of Fe-N-C degradation, especially under operando conditions. In this work, using a gas diffusion electrode half-cell coupled with inductively coupled plasma mass spectrometry setup, Fe dissolution is studied under more realistic conditions, i.e. real catalyst layer and current densities up to 125 mA·cm-2. Varying the rate of oxygen reduction reaction, we show a remarkable correlation between Faradaic electrode charge and Fe dissolution. This finding is rationalized assuming that oxygen reduction and Fe dissolution reactions are interlinked, likely through a common intermediate formed during the Fe3+/Fe2+ redox transitions in coordinated Fe cations. Moreover, such linear correlation allows an introduction and use of a simple metric (stability number). Hence, in the current work, a powerful tool for a more applied stability screening of different electrocatalysts is introduced, which allows on the one hand fast performance investigations under more realistic conditions, and on the other hand more advanced mechanistic understanding of Fe-N-C degradation in catalyst layers.

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Single-Atom Catalysts: A Perspective toward Application in Electrochemical Energy Conversion

Cited by 58 publications

References 125 publications

Understanding Single-Atom Catalysis in View of Theory

Understanding Single-Atom Catalysis in View of Theory

Single-Atom Catalysts for the Electro-Reduction of CO2 to Syngas with a Tunable CO/H2 Ratio: A Review

Oxygen Reduction Reaction Causes Iron Leaching from Fe-N-C Electrocatalysts

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