Atomically Dispersed Reduced Graphene Aerogel-Supported Iridium Catalyst with an Iridium Loading of 14.8 wt %

Babucci, Melike; Oztuna, F. Eylul Sarac; Debefve, Louise M.; Boubnov, Alexey; Bare, Simon R.; Gates, Bruce C.; Ünal, Uğur; Uzun, Alper

doi:10.1021/acscatal.9b02231

Cited by 60 publications

(79 citation statements)

References 33 publications

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“…The rGA substrate provides highly effective bonding sites for metal anchoring superior to those of metal oxides, due to the merits of uniformity and high density. This approach could prepare a single-atom Ir catalyst with remarkably high Ir loading up to 14.8 wt% [ 109 ]. With carbon cloth- (CC-) supported NiO (NiO/CC) as the support, Wang et al prepared a single-atom Ir catalysts with the Ir loading as high as 18 wt% [ 105 ].…”

Section: Synthetic Methods For Saecsmentioning

confidence: 99%

Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction

2020

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Oxygen reduction reaction (ORR) plays significant roles in electrochemical energy storage and conversion systems as well as clean synthesis of fine chemicals. However, the ORR process shows sluggish kinetics and requires platinum-group noble metal catalysts to accelerate the reaction. The high cost, rare reservation, and unsatisfied durability significantly impede large-scale commercialization of platinum-based catalysts. Single-atom electrocatalysts (SAECs) featuring with well-defined structure, high intrinsic activity, and maximum atom efficiency have emerged as a novel field in electrocatalytic science since it is promising to substitute expensive platinum-group noble metal catalysts. However, finely fabricating SAECs with uniform and highly dense active sites, fully maximizing the utilization efficiency of active sites, and maintaining the atomically isolated sites as single-atom centers under harsh electrocatalytic conditions remain urgent challenges. In this review, we summarized recent advances of SAECs in synthesis, characterization, oxygen reduction reaction (ORR) performance, and applications in ORR-related H2O2 production, metal-air batteries, and low-temperature fuel cells. Relevant progress on tailoring the coordination structure of isolated metal centers by doping other metals or ligands, enriching the concentration of single-atom sites by increasing metal loadings, and engineering the porosity and electronic structure of the support by optimizing the mass and electron transport are also reviewed. Moreover, general strategies to synthesize SAECs with high metal loadings on practical scale are highlighted, the deep learning algorithm for rational design of SAECs is introduced, and theoretical understanding of active-site structures of SAECs is discussed as well. Perspectives on future directions and remaining challenges of SAECs are presented.

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Section: Synthetic Methods For Saecsmentioning

confidence: 99%

Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction

2020

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“…Iridium SAs with surface oxygen atoms as the binding sites achieved a high loading of 14.8 wt%. [ 46 ] O has a role in tuning the d‐electron density of Mn atoms through the synergistic effect of electronic connection similar to N (Figure 9b). [ 103 ] The presence of O/N dopants also help promote the polarity of carbon.…”

Section: Design Principles For Sasmentioning

confidence: 99%

“…For example, some iridium atoms migrated to form clusters under the influence of the electron beam. [ 46 ] Another challenge of HAADF‐STEM is to provide only local information. Therefore, scientists apply X‐ray absorption spectroscopy (XAS), which not only provides better statistical information from samples than HAADF‐STEM, but also offers more information on local electronic structure.…”

Section: Introductionmentioning

confidence: 99%

Design Principles of Single Atoms on Carbons for Lithium–Sulfur Batteries

et al. 2020

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is a senior scientist at the X-ray Science Division in Argonne National Laboratory. He has developed in situ X-ray techniques to understand the fundamental chemistry of complex disordered solid and solution systems, such as energy storage materials, catalysts, soot, heavy petroleum, oil shale, and carbons. Chemistry is combined with characterization techniques, including mass spectrometry, IR, NMR, and X-ray scattering and spectroscopy. IR and MS are used simultaneously with X-ray techniques. In 2009, he was elected to the inaugural class of the ACS Fellows and was the chair of the 2018 International Conference on Small Angle Scattering.

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“…Furthermore, metal atoms can be stably fixed in the surface of the carbon support in isolation. [ 31 ] In this case, it is widely used that heteroatoms such as N, S, P, and O and defect sites are introduced in carbon support for futher stabilizing SACs structure, [ 32 ] such as M‐N x C y V z (M = metal atoms, C = carbon atoms, V = vacancies in support). The favorable coordination environment of metal atoms in the surface not only prevents their aggregation but also changes the electronic and geometric structure of the metal active sites.…”

Section: Support and Structure Of Active Sitesmentioning

confidence: 99%

Recent Advances in Strategies for Improving the Performance of CO₂ Reduction Reaction on Single Atom Catalysts

et al. 2020

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Excessive consumption of fossil fuels gives rise to the increasing emission of carbon dioxide (CO2) in the atmosphere and furthers the ecocrisis. Electrochemical CO2 reduction (ECR) has both functions of dwindling greenhouse gas concentration and converting it into valuable products. Due to the intrinsic chemical inertness of CO2 molecules, the study on efficient and low‐cost catalysts has attracted much attention. Recently isolated atoms, dispersed in stable support, play an important role in decreasing energy barriers of intermediate steps and obtaining target products with high activity and selectivity for ECR. The effective regulation of central atoms or coordination environment is significant to realize the desired performances of ECR with a high efficiency and selectivity. Hence, a comprehensive summary about strategies for improving the performance of ECR on single atom catalysts (SACs) is necessary. Herein, the SACs on various supports are introduced, the methods to design stable SACs are discussed, and the strategies for tuning the performance of ECR on SACs are summarized. The localized environment manipulation is widely used for high‐performance SACs design, including regulating central atoms and coordination environment. Finally, the perspectives are discussed to shed light on the rational design of intriguing SACs for ECR.

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Atomically Dispersed Reduced Graphene Aerogel-Supported Iridium Catalyst with an Iridium Loading of 14.8 wt %

Cited by 60 publications

References 33 publications

Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction

Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction

Design Principles of Single Atoms on Carbons for Lithium–Sulfur Batteries

Recent Advances in Strategies for Improving the Performance of CO₂ Reduction Reaction on Single Atom Catalysts

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Atomically Dispersed Reduced Graphene Aerogel-Supported Iridium Catalyst with an Iridium Loading of 14.8 wt %

Cited by 60 publications

References 33 publications

Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction

Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction

Design Principles of Single Atoms on Carbons for Lithium–Sulfur Batteries

Recent Advances in Strategies for Improving the Performance of CO2 Reduction Reaction on Single Atom Catalysts

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Product

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Recent Advances in Strategies for Improving the Performance of CO₂ Reduction Reaction on Single Atom Catalysts