Nano-geometric deformation and synergistic Co nanoparticles—Co-N<sub>4</sub> composite sites for proton exchange membrane fuel cells

Cheng, Xinjian; Yang, Jian; Yan, Wei; Han, Yu; Qu, Xi‐Ming; Yin, Shuhu; Chen, Chi; Ji, Ruiyi; Li, Yanrong; Li, Guang; Li, Gen; Jiang, Yanxia; Sun, Shi‐Gang

doi:10.1039/d1ee01715b

Cited by 112 publications

(89 citation statements)

References 35 publications

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“…Several of the above‐mentioned electrocatalysts are identified to be active in oxygen electrocatalysis. For example, Sun and co‐workers prepared an electrocatalyst with CoN 4 and Co NP ‐CoN 4 sites, [ 116 ] where the SiO 2 coating layer generated localized stress on the internal ZnCo‐ZIF framework, deforming the isolated Co‐N 4 sites in geometry structure. A metalorganic gaseous doping approach was utilized to deposit Co nanoparticles onto the surface of deformed Co SA ‐N‐C (d‐Co SA ‐N‐C).…”

Section: Integrating Single Atoms With Nanoparticlesmentioning

confidence: 99%

“…Several of the above-mentioned electrocatalysts are identified to be active in oxygen electrocatalysis. For example, Sun and co-workers prepared an electrocatalyst with CoN 4 and Co NP -CoN 4 sites, [116] where the SiO 2 coating layer generated localized stress on the internal ZnCo-ZIF framework, deforming the isolated Co-N 4 sites F I G U R E 11 (A) Schematic of the in situ electrochemical deposition process of Mo 2 TiC 2 T x -Pt SA . Reproduced with permission.…”

Section: Electrocatalysis Involving Omentioning

confidence: 99%

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Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Zhang

Zhu

et al. 2022

Interdisciplinary Materials

143

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Single‐atom catalysts, featuring some of the most unique activities, selectivity, and high metal utilization, have been extensively studied over the past decade. Given their high activity, selectivity, especially towards small molecules or key intermediate conversions, they can be synergized together with other active species (typically other single atoms, atomic clusters, or nanoparticles) in either tandem or parallel or both, leading to much better performance in complex catalytic processes. Although there have been reports on effectively combining the multiple components into one single catalytic entity, the combination and synergy between single atoms and other active species have not been reviewed and examined in a systematic manner. Herein, in this overview, the key synergistic interactions, binary complementary effects, and the bifunctional functions of single atoms with other active species are defined and discussed in detail. The integration functions of their marriages are investigated with particular emphasis on the homogeneous and heterogeneous combinations, spatial distribution, synthetic strategies, and the thus‐derived outstanding catalytic performance, together with new light shined on the catalytic mechanisms by zooming in several case studies. The dynamic nature of each of the active species and in particular their interactions in such new catalytic entities in the heterogeneous electrocatalytic processes are visited, on the basis of the in situ/operando evidence. Last, we feature the current challenges and future perspectives of these integrated catalytic entities that can offer guidance for advanced catalyst design by the rational combination and synergy of binary or multiple active species.

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Section: Integrating Single Atoms With Nanoparticlesmentioning

confidence: 99%

Section: Electrocatalysis Involving Omentioning

confidence: 99%

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Zhang

Zhu

et al. 2022

Interdisciplinary Materials

143

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“…Moreover, the surface of NC@FeÀ NÀ C appears as a rough and curved graphitic layer with plentiful defects to a certain extent, leading to more localization of FeÀ N x active sites, [40,41] and the possible formation of deformed geometries of the FeÀ N x species at the external surface of the catalyst for facilitating the ORR process. [42] On one hand, the surface depression changes the distortion degree of FeÀ N x site. The OÀ O bond length increases, and the O 2 dissociation barrier is decreased.…”

Section: Resultsmentioning

confidence: 99%

Space‐Confined Anchoring of Fe−N_x on Concave N‐Doped Carbon Cubes for Catalyzing Oxygen Reduction

et al. 2022

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Carbon-based electrocatalysts with atomically dispersed FeÀ NÀ C display promising performance for oxygen reduction reaction (ORR) amongst non-precious electrocatalysts. Nonetheless, increasing the number and utilization of FeÀ NÀ C active sites is challenging. Designing morphologies and adjusting the pore structure of carbon-based electrocatalysts would boost the mass transfer, enhance the utilization of the active sites, and increase the overall ORR performance. In this work, a concave N-doped carbon cubes structure adorned with highly external FeÀ N x was designed and produced by the space-confined induced strategy. The optimal electrocatalyst revealed excellent ORR activity in both alkaline and acidic electrolytes, with halfwave potentials of 0.86 and 0.75 V, respectively. The superior performance arose from its unique concave structure, possessing more accessible active sites with improved intrinsic activity, which holds promising potential for preparing advanced ORR electrocatalysts.

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“…The energy increasing of bonding energy suggested the reduced binding effect of the central iron atom to O species during ORR. Subsequently, DOS analysis for each ORR step was calculated (Figure 5c,d;Figure S16,Supporting Information). The overlap between Fe d xy + d yz , d z 2 and O 2p also positively shifted in RDS.…”

Section: Theoretical Calculation and Analysismentioning

confidence: 99%

Facet Strain Strategy of Atomically Dispersed FeNC Catalyst for Efficient Oxygen Electrocatalysis

Yang

Zhang

Yang

et al. 2022

Adv Funct Materials

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Increasing the portion of highly active metal centers in atomically dispersed MNC catalysts is significant for the overall oxygen reduction reaction (ORR) performance. A "facet strain strategy" is designed by using a translayer compressive strain of the {110} facet of FeCo nanoparticles encapsulated in graphitic FeNC layers to further activate the primitive FeN 4 catalytic centers on the graphitic sub-layer that are omitted in commonly direct access activation strategies. Using X-ray absorption near-edge spectroscopy and extended X-ray absorption fine structure, the highly active FeN 4 type is detected with compressed FeN bonds. Density functional theory calculation discloses that, in virtue of lattice mismatch, FeCo {110} facets transmit a trans-layer compressive strain to reconstruct the FeN 4 sites on surrounding graphitic sublayers to optimize the Fe-OH* adsorption energy in the rate-determining step. The redesigned catalyst exhibits enhanced ORR activity, outperforming the primitive FeNC and commercial Pt/C benchmarks. This study will enrich insights toward developing MN 4 and nanoparticle composite electrocatalysts.

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Nano-geometric deformation and synergistic Co nanoparticles—Co-N₄ composite sites for proton exchange membrane fuel cells

Abstract: Co single-atom (CoSA) catalysts of the CoN4 moiety usually show an unsatisfactory oxygen reduction reaction (ORR) activity due to poor O2 activation. Herein, we open up a novel strategy to...

Cited by 112 publications

References 35 publications

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Space‐Confined Anchoring of Fe−N_x on Concave N‐Doped Carbon Cubes for Catalyzing Oxygen Reduction

Facet Strain Strategy of Atomically Dispersed FeNC Catalyst for Efficient Oxygen Electrocatalysis

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Nano-geometric deformation and synergistic Co nanoparticles—Co-N4 composite sites for proton exchange membrane fuel cells

Abstract: Co single-atom (CoSA) catalysts of the CoN4 moiety usually show an unsatisfactory oxygen reduction reaction (ORR) activity due to poor O2 activation. Herein, we open up a novel strategy to...

Cited by 112 publications

References 35 publications

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Space‐Confined Anchoring of Fe−Nx on Concave N‐Doped Carbon Cubes for Catalyzing Oxygen Reduction

Facet Strain Strategy of Atomically Dispersed FeNC Catalyst for Efficient Oxygen Electrocatalysis

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Product

Resources

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Nano-geometric deformation and synergistic Co nanoparticles—Co-N₄ composite sites for proton exchange membrane fuel cells

Space‐Confined Anchoring of Fe−N_x on Concave N‐Doped Carbon Cubes for Catalyzing Oxygen Reduction