Regulating and identifying the structures of PdAu alloys with splendid oxygen reduction activity for rechargeable zinc–air batteries

Qiao, Sicong; Shou, Hongwei; Xu, Wenjie; Cao, Yuyang; Zhou, Yuzhu; Wang, Zhouxin; Wu, Xiaojun; He, Qun; Song, Li

doi:10.1039/d3ee02719h

Cited by 17 publications

(10 citation statements)

References 49 publications

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“…The band O 2 – also appears in the Ni–N–C system. In addition, the band *OOH (1130 cm –1 ) appears at −0.2 V in both Fe–N–C and Ni–N–C systems, while the vibration of *OOH is more intense in the Ni–N–C, which indicates that the absorbed *OOH on the surface of Ni–N–C SACs is easily deprotonated to generate O 2 ·– combined with previous ECL and EPR data analysis. Cu–N–C SACs with moderate oxygen affinity can appropriately adsorb and desorb oxygen-containing intermediate species, generating ROS such as ·OH and O 2 ·– in the system and providing dual-potential ECL output.…”

Section: Resultsmentioning

confidence: 78%

Regulating Reactive Oxygen Species over M–N–C Single-Atom Catalysts for Potential-Resolved Electrochemiluminescence

Zhou,

Wu,

Luo

et al. 2024

J. Am. Chem. Soc.

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The development of potential-resolved electrochemiluminescence (ECL) systems with dual emitting signals holds great promise for accurate and reliable determination in complex samples. However, the practical application of such systems is hindered by the inevitable mutual interaction and mismatch between different luminophores or coreactants. In this work, for the first time, by precisely tuning the oxygen reduction performance of M−N−C single-atom catalysts (SACs), we present a dual potential-resolved luminol ECL system employing endogenous dissolved O 2 as a coreactant. Using advanced in situ monitoring and theoretical calculations, we elucidate the intricate mechanism involving the selective and efficient activation of dissolved O 2 through central metal species modulation. This modulation leads to the controlled generation of hydroxyl radical (•OH) and superoxide radical (O 2 •− ), which subsequently trigger cathodic and anodic luminol ECL emission, respectively. The well-designed Cu−N−C SACs, with their moderate oxophilicity, enable the simultaneous generation of •OH and O 2 •− , thereby facilitating dual potential-resolved ECL. As a proof of concept, we employed the principal component analysis statistical method to differentiate antibiotics based on the output of the dual-potential ECL signals. This work establishes a new avenue for constructing a potentialresolved ECL platform based on a single luminophore and coreactant through precise regulation of active intermediates.

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Section: Resultsmentioning

confidence: 78%

Regulating Reactive Oxygen Species over M–N–C Single-Atom Catalysts for Potential-Resolved Electrochemiluminescence

Zhou,

Wu,

Luo

et al. 2024

J. Am. Chem. Soc.

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“…The adsorbed oxygen can be electrochemically removed before the happening of CO 2 RR, thus, the TM-PPc system should be an appropriate research platform for this study. 29 Notably, the presence of TM-C scattering paths is observed, further demonstrating the long-range ordering of TM-PPc. 3 The fitting of TM-C paths is not done due to the high inaccuracy caused by the uneven structure.…”

mentioning

confidence: 86%

“…Furthermore, Fourier transform extended X-ray absorption fine structure (FT-EXAFS) fitting results exhibited that the coordination numbers of TM sites in all TM-PPc are between 4.7 and 5.4, which further indicates that the TM-N 4 sites in the samples were adsorbed with oxygen (Figure g,h and Table S2). The adsorbed oxygen can be electrochemically removed before the happening of CO 2 RR, thus, the TM-PPc system should be an appropriate research platform for this study . Notably, the presence of TM-C scattering paths is observed, further demonstrating the long-range ordering of TM-PPc .…”

mentioning

confidence: 93%

Identification of Synergies in Fe, Co-Coordinated Polyphthalocyanines Scaffolds for Electrochemical CO₂ Reduction Reaction

Wang,

Qian,

Cao

et al. 2024

Nano Lett.

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The synergistic interaction between the isolated metal sites promoted the electrocatalytic activity of the catalysts. However, the structural heterogeneity of the isolated sites makes it challenging to evaluate this effect accurately. In this work, metal-coordinated polyphthalocyanine molecules (Fe-PPc, Co-PPc, FeCo-PPc) with long-range ordered and precise coordination structures are used as a platform to study the synergies of different isolated metal sites in the electrochemical CO 2 reduction reaction. The combination means of experimental and theoretical calculation clearly reveal that the coexistence of Fe and Co sites in PPc significantly enhances the conjugation effect of the macrocycle. This enhancement subsequently causes the metal sites to lose more electrons, thereby improving their adsorption of CO 2 and facilitating the formation of intermediate *COOH on them. As a result, FeCo-PPc achieves a CO partial current density of about 57.4 mA/cm 2 with a high turnover frequency of over 49000 site −1 h −1 at −0.9 V (vs RHE).

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“…Recently, palladium (Pd), with its relatively abundant global reserves and catalytic performance comparable to that of Pt, has received extensive attention. − Nevertheless, the O adsorption over Pd is still too strong for realizing optimized ORR performance . Alloying Pd with late transition metals, such as Fe, , Co, Ni, Cu, and Au offers an effective strategy to reduce O adsorption and thus improve the ORR activity. Very few investigations have been carried out on alloying Pd with early transition metals (ETMs), partially because ETMs themselves are not favored as active ORR catalysts.…”

Section: Introductionmentioning

confidence: 99%

Enhancing Oxygen Reduction Activity via Tailoring Microstrain in PdMo Nanoalloy through Repetitive Hydrogen Absorption–Release

Chen,

Sun,

et al. 2024

ACS Catal.

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The catalytic activities of noble-metal electrocatalysts are heavily correlated to their defective surface structures. However, controllably constructing surface defects on noble-metal nanocrystals remains a great challenge. In this work, an electrochemical method is developed to tailor the surface structure of the PdMo nanoalloy electrocatalyst, involving H absorption followed by its subsequent release near the surface of Pd. The optimized PdMo nanoalloy electrocatalyst exhibits an oxygen reduction reaction (ORR) half-wave potential (E 1/2 ) of 0.929 V (vs reversible hydrogen electrode, RHE) with a specific activity (SA) as high as 5.09 mA/cm 2 at 0.9 V (vs RHE) in an alkaline electrolyte, ∼10.6 times that of the state-of-the-art Pt/C electrocatalyst. Density functional theory calculations together with ex situ and in situ electrochemical and structural characterizations unravel that the microstrain generated at the PdMo nanoalloy surface by electrochemically induced H absorption−release can downshift the d-band center of Pd (the ORR active site) in PdMo to decrease oxygen binding and promote *OOH to *O transformation as well as *OH desorption for fast ORR. This work provides a surface defect engineering strategy to develop highperformance noble-metal electrocatalysts for energy applications.

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Regulating and identifying the structures of PdAu alloys with splendid oxygen reduction activity for rechargeable zinc–air batteries

Abstract: Alloying improves catalytic performance, but control is challenging due to element contributions. Here, we study the structural differences in PdxAuy alloys to understand their impact on oxygen reduction reaction activity....

Cited by 17 publications

References 49 publications

Regulating Reactive Oxygen Species over M–N–C Single-Atom Catalysts for Potential-Resolved Electrochemiluminescence

Regulating Reactive Oxygen Species over M–N–C Single-Atom Catalysts for Potential-Resolved Electrochemiluminescence

Identification of Synergies in Fe, Co-Coordinated Polyphthalocyanines Scaffolds for Electrochemical CO₂ Reduction Reaction

Enhancing Oxygen Reduction Activity via Tailoring Microstrain in PdMo Nanoalloy through Repetitive Hydrogen Absorption–Release

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Regulating and identifying the structures of PdAu alloys with splendid oxygen reduction activity for rechargeable zinc–air batteries

Abstract: Alloying improves catalytic performance, but control is challenging due to element contributions. Here, we study the structural differences in PdxAuy alloys to understand their impact on oxygen reduction reaction activity....

Cited by 17 publications

References 49 publications

Regulating Reactive Oxygen Species over M–N–C Single-Atom Catalysts for Potential-Resolved Electrochemiluminescence

Regulating Reactive Oxygen Species over M–N–C Single-Atom Catalysts for Potential-Resolved Electrochemiluminescence

Identification of Synergies in Fe, Co-Coordinated Polyphthalocyanines Scaffolds for Electrochemical CO2 Reduction Reaction

Enhancing Oxygen Reduction Activity via Tailoring Microstrain in PdMo Nanoalloy through Repetitive Hydrogen Absorption–Release

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Identification of Synergies in Fe, Co-Coordinated Polyphthalocyanines Scaffolds for Electrochemical CO₂ Reduction Reaction