N,P co-coordinated Fe species embedded in carbon hollow spheres for oxygen electrocatalysis

Zhu, Xiaofeng; Tan, Xin; Wu, Kuang‐Hsu; Chiang, Chao–Lung; Lin, Yiping; Lin, Yan‐Gu; Wang, Da‐Wei; Smith, Sean C.; Lu, Xunyu; Amal, Rose

doi:10.1039/c9ta03011e

Cited by 88 publications

(50 citation statements)

References 64 publications

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“…As shown by the relationship between

U^{normalo normaln normals normale normalt}

and

{Δ G}_{{O H}^{^{*}}}

in Figure 5a, the closer the point is to the top of the volcano, the higher the catalytic activity is. The positions of FeNPC, MnNPC, CoNPC and NiNPC with the same quasi‐octahedral site structure on the volcano are shown in Figure 5b, and their theoretical ORR activity is in agreement with the experimental results [25] . However,

{Δ G}_{{normalO normalH}^{^{*}}}

is not a structural feature of the active site.…”

Section: Theoretical Advancessupporting

confidence: 73%

“…Due to the large size, P atoms also attach onto the surface of graphene as a ligand. As shown in Figure 2d, Fe−N 4 is located in the carbon plane with an additional ligand of (HO) 3 P−O outside the plane [25] …”

Section: Theoretical Advancesmentioning

confidence: 97%

“…With the addition of nitrogen, M−N x P y sites have more configurations than M−P x sites. The configurations of M−N x P y can be classified into three groups based on the relative positions of N and P: (1) both N and P in the basal plane of graphene; [15,26] (2) both N and P at the edge position; [24] and (3) N in the graphene plane while P as an additional ligand as shown in Figure 2 [25] . All the three groups of M−N x P y sites are thermodynamically stable.…”

Section: Theoretical Advancesmentioning

confidence: 99%

“…The four‐electron ORR could have the dissociative and associative pathways. In acidic media, ORR at M−P x and M−N x P y sites usually follow the associative pathway [12,15,19,24–26] . O 2 is first adsorbed on the active site, then protonated to form OOH*, and the reaction continues with the cleavage of the O−O bond to form O* and H 2 O. H 2 O is desorbed and O* undergoes protonation to form another H 2 O.…”

Section: Theoretical Advancesmentioning

confidence: 99%

“…In the past few years, theoretical and experimental studies have been carried out on the phosphorus coordination active sites, including phosphorus‐coordinated metal (M−P x ) [10–12,19–22] and nitrogen‐phosphorus dual‐coordinated metal (M−N x P y ) [15,23–26] . These catalysts have shown superiority in activity in comparison with N‐coordinated ones.…”

Section: Introductionmentioning

confidence: 99%

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Recent Advances in Phosphorus‐Coordinated Transition Metal Single‐Atom Catalysts for Oxygen Reduction Reaction

et al. 2020

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Carbon‐supported heteroatom‐coordinated metal single‐atom catalysts (SACs) are promising electrocatalysts for oxygen reduction reaction (ORR) due to their low cost and tunable catalytic activity. Adjusting the electronic structure of the active center is an effective way to improve the activity of SACs. Compared with the intensively studied nitrogen‐coordinated transition metal atoms (e. g. Fe, Co and Mn), phosphorus‐coordinated and nitrogen‐phosphorus dual‐coordinated ones exhibit different electronic structures, which changes the reaction energy barrier and enhances the catalytic activity. This review summarizes recent advances in phosphorus coordination SACs for ORR in terms of theoretical study, site structure determination, synthesis method and catalytic activity. Further research is called for to explore the precise synthesis of phosphorus coordination SACs in a controllable manner and check the SACs under actual working conditions.

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“…As shown by the relationship between

U^{normalo normaln normals normale normalt}

and

{Δ G}_{{O H}^{^{*}}}

{Δ G}_{{normalO normalH}^{^{*}}}

is not a structural feature of the active site.…”

Section: Theoretical Advancessupporting

confidence: 73%

Section: Theoretical Advancesmentioning

confidence: 97%

Section: Theoretical Advancesmentioning

confidence: 99%

Section: Theoretical Advancesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Recent Advances in Phosphorus‐Coordinated Transition Metal Single‐Atom Catalysts for Oxygen Reduction Reaction

et al. 2020

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Preparation of Supported Metal Single‐Atom Catalysts on Carbon Supports

Rivera‐Cárcamo

2022

Supported Metal Single Atom Catalysis

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Recent Developments of Microenvironment Engineering of Single‐Atom Catalysts for Oxygen Reduction toward Desired Activity and Selectivity

Huang

Tang

et al. 2021

Adv Funct Materials

108

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Oxygen reduction reaction (ORR) is an essential process for sustainable energy supply and sufficient chemical production in modern society. Singleatom catalysts (SACs) exhibit great potential on maximum atomic efficiency, high ORR activity, and stability, making them attractive candidates for pursuing next-generation catalysts. Despite substantial efforts being made on building diversiform single-atom active sites (SAASs), the performance of the obtained catalysts is still unsatisfactory. Fortunately, microenvironment regulation of SACs provides opportunities to improve activity and selectivity for ORR. In this review, first, ORR mechanism pathways on N-coordinated SAAS, electrochemical evaluation, and characterization of SAAS are displayed. In addition, recent developments in tuning microenvironment of SACs are systematically summarized, especially, strategies for microenvironment modulation are introduced in detail for boosting the intrinsic 4e − /2e − ORR activity and selectivity. Theoretical calculations and cutting-edge characterization techniques are united and discussed for fundamental understanding of the synthesis-construction-performance correlations. Furthermore, the techniques for building SAAS and tuning their microenvironment are comprehensively overviewed to acquire outstanding SACs. Lastly, by proposing perspectives for the remaining challenges of SACs and infant microenvironment engineering, the future directions of ORR SACs and other analogous procedures are pointed out.

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N,P co-coordinated Fe species embedded in carbon hollow spheres for oxygen electrocatalysis

Abstract: Carbon hollow spheres (FeNPC) with single-atomic and octahedral FeNxPy active sites are fabricated for oxygen electrocatalysis.

Cited by 88 publications

References 64 publications

Recent Advances in Phosphorus‐Coordinated Transition Metal Single‐Atom Catalysts for Oxygen Reduction Reaction

Recent Advances in Phosphorus‐Coordinated Transition Metal Single‐Atom Catalysts for Oxygen Reduction Reaction

Preparation of Supported Metal Single‐Atom Catalysts on Carbon Supports

Recent Developments of Microenvironment Engineering of Single‐Atom Catalysts for Oxygen Reduction toward Desired Activity and Selectivity

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