Fe–N–C Catalyst Graphitic Layer Structure and Fuel Cell Performance

Workman, Michael J.; Serov, Alexey; Tsui, Lok‐kun; Atanassov, Plamen; Artyushkova, Kateryna

doi:10.1021/acsenergylett.7b00391

Cited by 107 publications

(64 citation statements)

References 24 publications

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“…In a work with FeN x sites supported on graphite, a negative correlation between the number of graphitic layers and fuel cell performance was observed, implying that FeN x sites within the graphitic plane also highly contributes to the catalytic activity. [66] Similar to the configurations at the edges, Pt atoms anchored on highly curved supports exhibited excellent HER activity. [51] The high curvature of the support could lead to the accumulation of electrons around the Pt regions, which induces a local electric field for proton (H + ) enrichment, thus accelerating the catalytic kinetics ( Figure 2b).…”

Section: Local Environments Of Single-atom Sitesmentioning

confidence: 90%

“…In addition, the SACs on edges are more easily accessible to reactants, which is beneficial for mass transfer. In a work with FeN x sites supported on graphite, a negative correlation between the number of graphitic layers and fuel cell performance was observed, implying that FeN x sites within the graphitic plane also highly contributes to the catalytic activity . Similar to the configurations at the edges, Pt atoms anchored on highly curved supports exhibited excellent HER activity .…”

Section: Engineering Sacs On Carbon‐based Substratesmentioning

confidence: 98%

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Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Zhu

Sokolowski

Song

et al. 2019

Advanced Energy Materials

267

230

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Carbon‐based heteroatom‐coordinated single‐atom catalysts (SACs) are promising candidates for energy‐related electrocatalysts because of their low‐cost, tunable catalytic activity/selectivity, and relatively homogeneous morphologies. Unique interactions between single metal sites and their surrounding coordination environments play a significant role in modulating the electronic structure of the metal centers, leading to unusual scaling relationships, new reaction mechanisms, and improved catalytic performance. This review summarizes recent advancements in engineering of the local coordination environment of SACs for improved electrocatalytic performance for several crucial energy‐convention electrochemical reactions: oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, CO2 reduction reaction, and nitrogen reduction reaction. Various engineering strategies including heteroatom‐doping, changing the location of SACs on their support, introducing external ligands, and constructing dual metal sites are comprehensively discussed. The controllable synthetic methods and the activity enhancement mechanism of state‐of‐the‐art SACs are also highlighted. Recent achievements in the electronic modification of SACs will provide an understanding of the structure–activity relationship for the rational design of advanced electrocatalysts.

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Section: Local Environments Of Single-atom Sitesmentioning

confidence: 90%

Section: Engineering Sacs On Carbon‐based Substratesmentioning

confidence: 98%

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Zhu

Sokolowski

Song

et al. 2019

Advanced Energy Materials

267

230

View full text Add to dashboard Cite

show abstract

“…As plenty of studies have focused on the distinction of real active sites for ORR electrocatalysis, M-N x -C moieties were regarded as catalytic centers [125]. For the center metal atoms, despite the debate of iron direct participation in ORR process, the metal-based M-N x -C exhibits much higher performance of non-metal electrocatalysts.…”

Section: Atomic Coordination Configurationmentioning

confidence: 99%

Local structure engineering for active sites in fuel cell electrocatalysts

et al. 2020

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In this review, we surveyed the significance of local structure engineering on electrocatalysts and electrodes for the performance of oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). Both on precious metal catalysts (PMC) and non-precious metal catalysts (NPMC), the main methods to modulate local structure of active sites have been summarized. By change of atomic coordination, modulation of bonding distortion and synergy effect from hierarchical structure, local structure engineering has influence on the intrinsic activity and stability of electrocatalysts. Moreover, we emphasized the intimate correlation between lyophobicity of electrocatalysts and membrane electrodes by local structure engineering. Our review aimed to inspire the exploration of advanced electrocatalysts and mechanism study for PEMFCs based on local structure engineering. local structure engineering, proton exchange membrane fuel cells, oxygen reduction reaction, active sites

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“…Being one of the most potential cost‐effective non‐noble‐metal catalysts, Fe‐based catalysts are likely to play a pivotal role in the transition to a sustainable society. One of the key aspects for Fe‐based catalysts is to ensure a high conductivity by improving charge‐carrier concentrations . This can be achieved by the doping of carbon by Fe atoms to obtain optimal electronic and geometric structures, and strategies for this are summarized below.…”

Section: Iron‐based Electrocatalystsmentioning

confidence: 99%

Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis

Sharifi

Gracia‐Espino

Chen

et al. 2019

Advanced Energy Materials

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The oxygen reduction reaction (ORR) is of great importance in energy‐converting processes such as fuel cells and in metal–air batteries and is vital to facilitate the transition toward a nonfossil dependent society. The ORR has been associated with expensive noble metal catalysts that facilitate the O2 adsorption, dissociation, and subsequent electron transfer. Single‐ or few‐atom motifs based on earth‐abundant transition metals, such as Fe, Co, and Mo, combined with nonmetallic elements, such as P, S, and N, embedded in a carbon‐based matrix represent one of the most promising alternatives. Often these are referred to as single atom catalysts; however, the coordination number of the metal atom as well as the type and nearest neighbor configuration has a strong influence on the function of the active sites, and a more adequate term to describe them is metal‐coordinated motifs. Despite intense research, their function and catalytic mechanism still puzzle researchers. They are not molecular systems with discrete energy states; neither can they fully be described by theories that are adapted for heterogeneous bulk catalysts. Here, recent results on single‐ and few‐atom electrocatalyst motifs are reviewed with an emphasis on reports discussing the function and the mechanism of the active sites.

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Fe–N–C Catalyst Graphitic Layer Structure and Fuel Cell Performance

Cited by 107 publications

References 24 publications

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Local structure engineering for active sites in fuel cell electrocatalysts

Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis

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