Atomic interface effect of a single atom copper catalyst for enhanced oxygen reduction reactions

Jiang, Zhuoli; Sun, Wenming; Shang, Huishan; Chen, Wenxing; Sun, Tingting; Li, Haijing; Dong, Juncai; Zhou, Jing; Li, Zhi; Wang, Yu; Cao, Rui; Sarangi, Ritimukta; Yang, Zhengkun; Wang, Dingsheng; Zhang, Jiatao; Li, Yadong

doi:10.1039/c9ee02974e

Cited by 293 publications

(220 citation statements)

References 51 publications

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“…1(c)) and Fe-Cl1N4 coordination could also be distinguished separately by comparing the EXAFS spectra and corresponding fitting curves in R spaces as reported by Wang et al [40,55]. This strategy could also be applied to predict the highershell coordination of Cu-N4-C8S2, as reported by Zhang et al [38]. Further investigation on higher-shell coordination requires more precise characterization and a deeper theoretical basis.…”

Section: Characterization Of Coordination Environmentmentioning

confidence: 88%

“…For example, Zhang et al reported the synthesis of low valence Cu + -N4-C8S2 SACs, which was investigated by EXAFS together with DFT calculation (Figs. 9(f)-9(h)) [38]. Compared to S free Cu-N4/CN SACs, the Cu + -N4-C8S2 SACs exhibited improved ORR performance in alkaline media.…”

Section: The Second-and Higher-coordination Shellmentioning

confidence: 98%

“…Metal atoms coordinated by different atoms from the support will exhibit different binding energies characterized by XPS and XANES. The coordination atoms and valence states of central metal atoms could be concluded by the fitting of the spectra and concerning the XPS database [38]. In Wang's study, the difference of Fe-S, Co-S and Ni-S coordination could be determined based on the different binding energies of S 2p detected by high-resolution XPS (as illustrated in Fig.…”

Section: Characterization Of Coordination Environmentmentioning

confidence: 99%

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Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance

et al. 2020

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The local coordination environment of catalysts has been investigated for an extended period to obtain enhanced catalytic performance. Especially with the advancement of single-atom catalysts (SACs), research on the coordination environment has been advanced to the atomic level. The surrounding coordination atoms of central metal atoms play important roles in their catalytic activity, selectivity and stability. In recent years, remarkable improvements of the catalytic performance of SACs have been achieved by the tailoring of coordination atoms, coordination numbers and second-or higher-coordination shells, which provided new opportunities for the further development of SACs. In this review, the characterization of coordination environment, tailoring of the local coordination environment, and their related adjustable catalytic performance will be discussed. We hope this review will provide new insights on further research of SACs.

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Section: Characterization Of Coordination Environmentmentioning

confidence: 88%

Section: The Second-and Higher-coordination Shellmentioning

confidence: 98%

Section: Characterization Of Coordination Environmentmentioning

confidence: 99%

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Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance

et al. 2020

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“…They also found that sulfuration of Fe-N-C embedded with Fe x C/Fe species could generate the Fe-S bonds at the interface, which could remarkably enhanced the ORR performance in acidic media with a half-wave potential of 0.821 V and without deactivation after 10000 CV cycles [171]. Jiang et al reported that sulfur dopant in the carbon matrix could also enhance the ORR activity of Cu-based SAECs (Cu-SA/SNC) [164]. As shown in Figure 11(d), XAS analysis together with DFT calculations confirms that the excellent ORR activity stems from the strong synergistic interaction at the atomic interface between Cu atoms and the N and S codoped carbon supports, leading to the reduction of the reaction-free energy for the intermediate adsorption.…”

Section: Saecs With Binary Ligandsmentioning

confidence: 97%

“…Zhang et al synthesized a series of porous N and S codoped carbon framework-supported SAECs (M-SAs/NSC, M=Fe, Co, Ni) [172]. Although M-SAs/NSC were prepared through the same synthetic method, Fe-SAs/NSC contains a FeN 4 S 2 Reproduced from [164]. (e) ORR-free energy diagram on as-prepared catalysts.…”

Section: Saecs With Binary Ligandsmentioning

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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Characterization of Supported Metal Single‐Atom Catalysts

Zhang¹,

Doyle‐Davis

Sun

2022

Supported Metal Single Atom Catalysis

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Atomic interface effect of a single atom copper catalyst for enhanced oxygen reduction reactions

Abstract: By the in situ X-ray absorption results, the gradually decrease of Cu oxidation state under applied potential implied that low-valence Cu (+1) species in the atomic interface of Cu–N4–C8S2 may work as the catalytic sites during an ORR process.

Cited by 293 publications

References 51 publications

Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance

Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance

Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction

Characterization of Supported Metal Single‐Atom Catalysts

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