Data‐Driven High‐Throughput Rational Design of Double‐Atom Catalysts for Oxygen Evolution and Reduction

Wu, Lianping; Guo, Tieding; Li, Teng

doi:10.1002/adfm.202203439

Cited by 56 publications

(63 citation statements)

References 68 publications

(84 reference statements)

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“…Metal B can be then selected based on Figures a,b and so that it should have a lower decomposition energy barrier, a lower stability on the carbon surface, a lower diffusion barrier, and a synthesis temperature in step 2 lower than that in step 1. All transition metal DACs considered in this study can be stably trapped on a defective carbon surface, as shown in a recent study …”

Section: Resultssupporting

confidence: 63%

“…All transition metal DACs considered in this study can be stably trapped on a defective carbon surface, as shown in a recent study. 33 To close the design loop of the proposed DAC synthesis strategy, we demonstrate the formation process of Pt−Au DACs on a defective carbon surface, through MD simulations (see the Methods section for details), as illustrated in Figure 4. The formation of Pt SACs on a defective carbon surface has been successfully demonstrated previously in both experiments and simulations at a temperature of 1500 K (Figure 2a predicts the lowest synthesis temperature of 1375 K).…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…For example, a recent study systematically evaluates the stability and activity of 16767 DACs for OER and ORR, from which 511 types of DACs with OER activity superior to IrO 2 (110), 855 types of DACs with ORR activity superior to Pt (111), and 248 bifunctional DACs with high catalytic performance for both OER and ORR are identified. 33 For the high HER activity DAC, we can choose two immiscible metals such as Cu and Ru. Because two immiscible metals are reported to be able to improve the catalytic activity, they can be present as nonagglomerated dual SAs.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…Furthermore, the design space of DACs is vast, resulting from both a large number of combinations of transition metal species for DACs and a wide range of substrate defect structures. 33 The huge design space of DACs and the lack of mechanistic understanding of their formation and stabilization make both experimental exploration and computational studies cost-prohibitive and timeconsuming. A rational design strategy for DACs with mechanistic understanding and quantitative guidance is highly desirable.…”

Section: ■ Introductionmentioning

confidence: 99%

“…Despite recent experimental success in fabricating DACs on a carbon surface, − systematic theoretical guidance for the synthesis of DACs has not yet been established. Furthermore, the design space of DACs is vast, resulting from both a large number of combinations of transition metal species for DACs and a wide range of substrate defect structures . The huge design space of DACs and the lack of mechanistic understanding of their formation and stabilization make both experimental exploration and computational studies cost-prohibitive and time-consuming.…”

Section: Introductionmentioning

confidence: 99%

See 4 more Smart Citations

A Synthesis Strategy of Double-Atom Catalysts on a Carbon Surface

2022

J. Phys. Chem. C

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Highly active double-atom catalysts (DACs) for electrochemical reactions hold promise to enable sustainable energy conversion and storage. However, fabricating stable DACs remains challenging due to the lack of a fundamental understanding of the formation and stabilization mechanisms of DACs. Here, we present a systematic investigation of the feasibility of forming DACs on a defective carbon surface, through density functional theory calculations, from which an effective synthesis strategy of DACs is proposed. Such a synthesis strategy is validated by molecular dynamics simulations of the process of the formation of a stable array of Pt–Au DACs on a defective carbon surface. Results from this study offer a mechanistic understanding and quantitative guidance for the rational selection of transition metals and optimal synthesis conditions to fabricate DACs with desirable electrocatalyst activity in emerging energy applications.

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Section: Resultssupporting

confidence: 63%

Section: ■ Results and Discussionmentioning

confidence: 99%

Section: ■ Results and Discussionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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A Synthesis Strategy of Double-Atom Catalysts on a Carbon Surface

2022

J. Phys. Chem. C

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Next Generation Noble Metal‐Engineered Catalysts: From Structure Evolution to Structure‐Reactivity Correlation in Water Splitting

Zhang,

Yan,

et al. 2023

Adv Funct Materials

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Noble metal‐engineered catalysts (NMECs) play an important role in promoting the practical utilization of water‐splitting devices in hydrogen energy systems. While owing to the complicated catalytic centers, diverse support structures, and changing microenvironments, NMECs still face many challenges when it comes to designing and analyzing the precise catalytic sites and activity‐mechanism analyses, which are crucial for their future developments. Here, this cutting‐edge review systematically discusses recent advancements in designing NMECs for water electrolysis, including the structure evolution, microenvironment modulation, structure‐reactivity correlation, and new horizons. First, the fundamental advantages, mechanisms, and evaluation methods of NMECs for water splitting are outlined. Then, the strategies to modulate the catalytic microenvironments of NMECs are thoroughly summarized, such as crystal phase modulation, alloying effects, crystallization degrees, size effects, and substrate effects. In particular, there are valuable perspectives on bond interactions, theoretical calculations, and evaluation methods to disclose the catalytic mechanisms. Thereafter, a special emphasis is given on structure‐reactivity correlation, performances, and water‐splitting devices. Finally, a thorough discussion of the upcoming difficulties and new directions for developing next‐generation NMECs is presented. It is believed that the review will have a significant influence on creating noble metal‐based catalysts in the field of electrolytic water‐splitting.

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Data‐Driven Screening of Pivotal Subunits in Edge‐Anchored Single Atom Catalysts for Oxygen Reactions

Ye,

Yi,

Wang

et al. 2024

Adv Funct Materials

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Oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) are key reactions in diverse energy conversion devices, highlighting the importance of efficient catalysts. Edge‐anchored single atom catalysts (E‐SACs) emerge as a special class of atomic structure, but the detailed configuration and its correlation with catalytic activity remain little explored. Herein, a total of 78 E‐SACs (E‐TM‐Nx‐C) have been constructed based on 26 transition metal (TM) species with three coordination patterns. Using structural stability and ORR/OER catalytic activity as the evaluation criteria, a few catalytic structures comparable to Pt (111) for ORR and IrO2 (110) for OER are screened based on high‐throughput calculations. The screening results unveil that the E‐Rh‐N4‐C configuration exhibits most efficient bifunctional activity for both ORR and OER with an overpotential of 0.38 and 0.61 V, respectively. Electronic structure analysis confirms the distinctive edge effects on the electronic properties of TM and N species, and the feature importance derived from machine learning illustrates the efficacy of E‐TM‐Nx subunit configuration in determining the catalytic activity of E‐SACs. Finally, the trained Gradient Boosting Regression (GBR) model exhibits acceptable accuracy in predicting the OH intermediates adsorption strength for E‐SACs, thereby paving the way for expanding catalytic structures based on E‐SACs.

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Data‐Driven High‐Throughput Rational Design of Double‐Atom Catalysts for Oxygen Evolution and Reduction

Cited by 56 publications

References 68 publications

A Synthesis Strategy of Double-Atom Catalysts on a Carbon Surface

A Synthesis Strategy of Double-Atom Catalysts on a Carbon Surface

Next Generation Noble Metal‐Engineered Catalysts: From Structure Evolution to Structure‐Reactivity Correlation in Water Splitting

Data‐Driven Screening of Pivotal Subunits in Edge‐Anchored Single Atom Catalysts for Oxygen Reactions

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