Does the Oxygen Evolution Reaction follow the classical OH*, O*, OOH* path on single atom catalysts?

Barlocco, Ilaria; Cipriano, Luis A.; Liberto, Giovanni Di; Pacchioni, Gianfranco

doi:10.1016/j.jcat.2022.12.014

Cited by 51 publications

(57 citation statements)

References 72 publications

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“…68 We observe that the binding energies of the TM atoms are larger, in absolute value, than those of the same species on N-doped graphene or carbon nitride. 14,46 For instance, Co has a binding energy to COF of À9.27 eV, while it binds to N-Gr and C 3 N 4 by À7.79 eV and À3.34 eV, respectively. Similarly, the binding energy of Pt is À10.58 eV in COF, to be compared with À7.99 eV (N-Gr) and À2.79 eV (C 3 N 4 ).…”

Section: Resultsmentioning

confidence: 99%

“…The formation of such unconventional intermediate has been previously predicted on other SACs supported on carbon-based materials. 14 The role of unconventional intermediates for the OER on SACs has been emphasized only recently, and their formation opens interestingly new routes for the catalyst optimization. Furthermore, they are indicative of how complex is the chemistry of SACs.…”

Section: Oxygen Evolutionmentioning

confidence: 99%

“…Furthermore, they are indicative of how complex is the chemistry of SACs. 13,14 In general, once OH* adsorbs to the catalyst,…”

Section: Oxygen Evolutionmentioning

confidence: 99%

“…7,8,12 This hallmark of SACs has intriguing potential implications in catalysis, since the reactivity can be substantially different from that of conventional catalysts based on extended metal surfaces. 13,14 Typical supports of SACs are 2D materials such as graphene, nitrogen-doped graphene, carbon nitride, MoS 2 and MXenes. 2,[15][16][17][18][19][20][21][22][23][24][25] A relatively novel family of supports is that of Covalent Organic Frameworks (COF), porous crystalline polymers.…”

Section: Introductionmentioning

confidence: 99%

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Hydrogen and oxygen evolution reactions on single atom catalysts stabilized by a covalent organic framework

2023

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Section: Resultsmentioning

confidence: 99%

Section: Oxygen Evolutionmentioning

confidence: 99%

“…Furthermore, they are indicative of how complex is the chemistry of SACs. 13,14 In general, once OH* adsorbs to the catalyst,…”

Section: Oxygen Evolutionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Hydrogen and oxygen evolution reactions on single atom catalysts stabilized by a covalent organic framework

2023

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“…In the four steps of OER, each step can release one electron, which determines the overpotential of reaction. Recently, a new OER mechanism over SACs has been well studied by Pacchioni's group based on their theoretical calculations, and they found that OER over SACs followed the new reaction path involving OH*OH*, O*OH* and O*O* species, [ 37 ] not the classical OER path mentioned above. This new OER path was based on carbon‐supported SACs, and the actual OER path over non‐carbon supported SACs would need the in situ experimental verification, on top of the theoretical calculations.…”

Section: Sacs For Oxygen Evolution Reactionmentioning

confidence: 99%

SACs on Non‐Carbon Substrates: Can They Outperform for Water Splitting?

Sun

Zang

Sun

et al. 2023

Adv Funct Materials

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Non‐carbon‐supported single‐atom electrocatalysts (SACs) have attracted tremendous research interest for water splitting, owning to their remarkable differences in bond and coordination, and better and tunable catalytic performance, compared with those carbon‐supported SACs and commercial catalysts. The electrocatalytic performance of these non‐carbon‐supported SACs is intimately related to the structure, surficial chemical groups, and vacancy defects of non‐carbon host materials, as well as the physico‐chemical properties and population of single atoms. The much widened range of host materials and types of single atoms create virtually limitless opportunities in the design of SACs with tunable structures and electrocatalysis behaviors. In this review, the recent progress of non‐carbon‐supported SACs for both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is visited, where the unique local structures, electrocatalytic performance, catalytic centers and key preparation processes are presented. The characterizations down to atomic scales that can reveal the key local structures and catalytic mechanism are also investigated. New insights into the correlations between the structural evolution of these SACs during electrocatalytic reactions and their catalytic performance are examined. Finally, the major challenges faced by these new SACs are summarized, together with future perspectives on the rational design of superior non‐carbon‐supported SACs.

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Complimentary Computational Cues for Water Electrocatalysis: A DFT and ML Perspective

Badreldin,

Bouhali,

Abdel‐Wahab

2023

Adv Funct Materials

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Heterogenous electrocatalysis continues to witness propagating interest in a plethora of non‐limiting electrochemical fields. Of which, water electrolysis has moved from lab‐scale systems to commercial electrolyzers albeit high dependence on historic benchmark noble‐metal based catalysts is still the status quo. Notwithstanding, advances in material groups such as single‐atom catalysts, perovskites, high‐entropy alloys, among others continue to see an increased interest toward utilization in next‐generation electrolyzers. To that end, progress in electrocatalyst discovery techniques is revolutionized through synergistically combining density functional theory (DFT) and machine learning (ML) techniques. The success of ML herein depends on numerous interlinked factors such as the algorithm employed, data availability and accuracy, with descriptors being critical to encapsulate physicochemical perspectives. Historic utilization of ML frameworks in areas other than materials discovery has left a lack of standardization toward appropriating suitable methods of high‐throughput DFT, ML approaches, and feature engineering that bridge the gap between activity‐structure‐electronic relationships. This review outlines needed considerations toward DFT calculations, important criteria during filtering out screened surfaces, and synergistic approaches toward utilizing theoretical and/or experimental datasets for formulating effective ML frameworks. Persisting challenges, perspectives, and recommendations thereof are highlighted to expedite and generalize future work pertaining to high‐volume water electrocatalysis discovery.

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Does the Oxygen Evolution Reaction follow the classical OH, O, OOH* path on single atom catalysts?

Cited by 51 publications

References 72 publications

Hydrogen and oxygen evolution reactions on single atom catalysts stabilized by a covalent organic framework

Hydrogen and oxygen evolution reactions on single atom catalysts stabilized by a covalent organic framework

SACs on Non‐Carbon Substrates: Can They Outperform for Water Splitting?

Complimentary Computational Cues for Water Electrocatalysis: A DFT and ML Perspective

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