Single‐Atom Cr−N<sub>4</sub> Sites Designed for Durable Oxygen Reduction Catalysis in Acid Media

Luo, Ergui; Zhang, Hao; Wang, Xian; Gao, Liqin; Gong, Liyuan; Zhao, Tiebiao; Zhao, Jianmin; Ge, Junjie; Jiang, Zheng; Liu, Changpeng; Wang, Xing

doi:10.1002/ange.201906289

Cited by 46 publications

(29 citation statements)

References 60 publications

(16 reference statements)

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“…Heteroatom coordinated M-N-C SACs (M = Fe, Co, Mn, Cu, etc.) are promising alternatives to Pt-based ORR catalysts (65,(80)(81)(82)(83)(84)(85)(86). The intrinsic activity and ORR reaction pathway catalyzed by M-N-C SACs highly depend on the geometrical and electronic environment of the single-atom metal centers.…”

Section: Oxygen Reduction Reactionmentioning

confidence: 99%

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

et al. 2020

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Single-atom catalysts (SACs) have become the most attractive frontier research field in heterogeneous catalysis. Since the atomically dispersed metal atoms are commonly stabilized by ionic/covalent interactions with neighboring atoms, the geometric and electronic structures of SACs depend greatly on their microenvironment, which, in turn, determine the performances in catalytic processes. In this review, we will focus on the recently developed strategies of SAC synthesis, with attention on the microenvironment modulation of single-atom active sites of SACs. Furthermore, experimental and computational advances in understanding such microenvironment in association to the catalytic activity and mechanisms are summarized and exemplified in the electrochemical applications, including the water electrolysis and O2/CO2/N2 reduction reactions. Last, by highlighting the prospects and challenges for microenvironment engineering of SACs, we wish to shed some light on the further development of SACs for electrochemical energy conversion.

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Section: Oxygen Reduction Reactionmentioning

confidence: 99%

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

et al. 2020

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“…As a result, Pt-and Fe-free high-performance catalysts are highly desirable to improve the ORR performance in acidic media. For example, the unexpected Fenton reaction could be substantially reduced on single-atom CrN 4 sites [152]. The ORR activity of the single-atom M-N-C catalysts follows the order of Fe > Co > Mn > Cu > Ni in acid electrolytes.…”

Section: Oxygen Reductionmentioning

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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“…[7][8][9] Therefore, increasingly more studies have focused on the development of cost-effective nonnoble metal catalysts for the replacement of the platinum-based catalysts. [10][11][12] In recent years, transition-metal (TM) single-atom catalysts (SACs) have been found to be effective in ORR, including Cr-N 4 , 13 Fe-N 4 , 14 Fe-N 5 , 15 Co-N 4 , 16 Ni-N 4 , 17 Cu-N 3 , 18 and Zn-N 4 19 sites. These TM SACs have been regarded as the most promising alternatives to commercial Pt/C catalysts.…”

Section: Introductionmentioning

confidence: 99%

Precise regulation of pyrrole‐type single‐atom Mn‐N₄ sites for superior pH‐universal oxygen reduction

Yan

Xie

et al. 2021

Carbon Energy

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The study of atomically dispersed metal-nitrogen electrocatalysts is still limited in terms of understanding their catalytic mechanism because of the inability to precisely regulate the coordination number and type of N in combination with the metal elements. Inspired by the high catalytic activity and selectivity of natural enzymes, herein, we have designed and fabricated ultrathin carbon nanosheet-supported Mn single-atom catalysts (SACs) with a precise pyrrole-type Mn-N 4 (PT-MnN 4 ) configuration using a bio-mimicking strategy. The PT-MnN 4 SACs display outstanding oxygen reduction reaction (ORR) activity, with a half-wave potential (E 1/2 ) of 0.88 V (vs. revisible hydrogen electrode [RHE]) and extremely high stability in alkaline media. Moreover, superior ORR activities are also obtained, E 1/2 of 0.73 V and 0.63 V in acid and neutral electrolytes, respectively, indicating the efficient pHuniversal ORR performances. The assembled zinc-air battery using the PT-MnN 4 SACs as air cathodes exhibits a high peak power density (175 mW cm −2 ) and long-term stability up to 150 h, implying its promising application in metal-air batteries. This study has paved the way toward the rational design and precise regulation of single-atom electrocatalysts.

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Single‐Atom Cr−N₄ Sites Designed for Durable Oxygen Reduction Catalysis in Acid Media

Cited by 46 publications

References 60 publications

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction

Precise regulation of pyrrole‐type single‐atom Mn‐N₄ sites for superior pH‐universal oxygen reduction

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Single‐Atom Cr−N4 Sites Designed for Durable Oxygen Reduction Catalysis in Acid Media

Cited by 46 publications

References 60 publications

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction

Precise regulation of pyrrole‐type single‐atom Mn‐N4 sites for superior pH‐universal oxygen reduction

Contact Info

Product

Resources

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Single‐Atom Cr−N₄ Sites Designed for Durable Oxygen Reduction Catalysis in Acid Media

Precise regulation of pyrrole‐type single‐atom Mn‐N₄ sites for superior pH‐universal oxygen reduction