Revealing surface fine structure on PtAu catalysts by an<i>in situ</i>ATR-SEIRAS CO-probe method

Li, Guang; An, Z. H.; Yang, Jian; Zheng, Jinhong; Ji, Lingfei; Zhang, Junming; Ye, Jinyu; Zhang, Binwei; Jiang, Yanxia; Sun, Shi‐Gang

doi:10.1039/d3ta01668d

Cited by 9 publications

(4 citation statements)

References 61 publications

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“…By applying an electrode potential of 0.2 V to facilitate CO adsorption on the Fe site (Supplementary Fig. 10), infrared vibrational frequency data were acquired within the range of ν = 1950~2050 cm -1 , corresponding to the adsorption of monocarboxylic ligands on the Fe site 41,42 . The obtained data demonstrated that the νCO values exhibited an increase proportional to the degree of polymerization (Fig.…”

Section: Resultsmentioning

confidence: 99%

Identifying high-spin Fe3+(S=5/2) as active center for acidic oxygen reduction

Sun,

Zhao,

Wang

et al. 2023

Preprint

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The active spin state of a single Fe catalytic center in acidic oxygen reduction reaction (ORR) remains uncertain, posing a significant challenge for the precise design of Fe-based ORR catalysts. To address it, we synthesized a conjugate-bridged dual-metal iron phthalocyanine molecule that exhibits an identical Fe site and high catalytic activity comparable to real catalysts. This molecular model addresses the limitations of current model catalysts that fail to meet simultaneously both structural and activity requirements. Compared to the non-conjugate-bridged molecule, the conjugate-bridged dual-metal iron phthalocyanine molecule displayed a 76-fold increase in turnover frequency. By combining spin characterization techniques, in-situ electrochemical infrared spectroscopy, and theoretical calculations, we proposed that the conjugate bridging of two FeN4 sites induces a high-spin Fe3+(S=5/2) state. This state allows for optimal adsorption strength of hydroxyl groups, neither too strong nor too weak, resulting in high catalytic activity that approaches the peak performance. The conclusion of Fe3+(S=5/2) state as the active site was further confirmed by a linear correlation between the content of Fe3+(S=5/2) state and catalytic activity. This study deepens our comprehension of active sites and contributes to the precise design of Fe-based ORR catalysts and beyond.

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Section: Resultsmentioning

confidence: 99%

Identifying high-spin Fe3+(S=5/2) as active center for acidic oxygen reduction

Sun,

Zhao,

Wang

et al. 2023

Preprint

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“…The structure and characterization of electrochemical IR cells have been described in previous work . The plating solution was 0.03 M HAuCl 4 + 0.3 M Na 2 SO 3 + 0.1 M Na 2 S 2 O 3 5H 2 O + 0.1 M NH 4 Cl.…”

Section: Methodsmentioning

confidence: 99%

“…The structure and characterization of electrochemical IR cells have been described in previous work. 24 The plating solution was 0.03 M HAuCl 4 + 0.3 M Na 2 SO 3 + 0.1 M Na 2 S 2 O 3 5H 2 O + 0.1 M NH 4 Cl. The secondary chemical gold plating of silicon prisms/ silicon wafers is described in detail in previous reports: The prisms/silicon wafers were milled with 1, 0.3, and 0.05 μm Al 2 O 3 , and ultrasonic cleaning was done with water and acetone.…”

Section: Structural Characterizationmentioning

confidence: 99%

Revealing Adsorption Conformation and Electro-oxidation Mechanism of Urea on the Ni Film Catalyst by In Situ ATR-SEIRAS

An,

Li,

et al. 2023

J. Phys. Chem. C

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The electrochemical urea oxidation reaction (UOR) is considered as a promising alternative to the oxygen evolution reaction due to its lower thermodynamic equilibrium potential (0.37 V). Nickel (Ni)-based catalysts have been universally used for UOR due to their lower cost and higher catalytic activity. However, the lack of mechanistic clarity has limited the study of catalyst constructional relationship. Herein, electrochemical in situ attenuated total reflection-surface-enhanced infrared spectroscopy was utilized to investigate the adsorption conformation and the reaction mechanism of UOR on the Ni-based catalyst. Combining CO( 15 NH 2 ) 2 isotopic experiments and polarization spectra method, the O-terminal adsorbed structure of urea, *O� C(NH 2 ) 2 , was unveiled as a reaction precursor. Moreover, with the potential increasing, *O�C(NH 2 ) 2 was converted to the Nterminal adsorbed structure, *NHCONH 2 , which was oxidized to generate CO 2 and N 2 by undergoing dehydrogenation. The finding could promote the knowledge of the reaction mechanism of UOR on Ni-based catalysts, which is conducive to the further design of high-performance catalysts for urea oxidation.

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“…[1][2][3][4] Lithium ion batteries (LIBs) have evolved into a fundamental component of modern society, energizing a wide array of consumer electronics, including laptops, cellphones, and more. [5][6][7] Recently, the increasing demands for electric vehicles and energy storage systems have significantly elevated the cost of lithium salts. [8][9][10] Additionally, the new emerging applications usually require battery technologies characterized by low cost and high energy density.…”

Section: Introductionmentioning

confidence: 99%

Na₂S Cathodes Enabling Safety Room Temperature Sodium Sulfur Batteries

Xiong,

Nie,

Zhang

et al. 2023

Batteries & Supercaps

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Room temperature sodium‐sulfur (RT‐Na/S) battery is regarded as a promising next‐generation battery system because of their high theoretical specific capacity, and abundant availability of anodes and cathodes. Nevertheless, the direct use of sodium metal could result in the dendrite growth, causing the safety concerns. Interestingly, employing Na2S as the cathode materials can be paired with Na‐free anode to effectively avoid the problem of dendrite growth. However, the poor electronic conductivity of Na2S and the sluggish kinetic conversion to sodium polysulfides can lead to high initial charge activation barriers and rapid capacity degradation, thereby constraining their practical application. In this concept, the electrochemical mechanism of Na2S cathode is summarized to present the potential for RT‐Na/S batteries. Additionally, recent advances on Na2S cathodes have been discussed in detail with an emphasis on functionalized matrix, morphology modulation, and optimizing cell structure. Finally, the future opportunities and challenges for the development of Na2S cathode based RT‐Na/S batteries are proposed.

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Revealing surface fine structure on PtAu catalysts by anin situATR-SEIRAS CO-probe method

Abstract: The electrochemical performance of Pt-based catalysts depend on their surface structure. Nevertheless, it is still a challenge to investigate their intricate surface active sites. Here, PtAu films were utilized as...

Cited by 9 publications

References 61 publications

Identifying high-spin Fe3+(S=5/2) as active center for acidic oxygen reduction

Identifying high-spin Fe3+(S=5/2) as active center for acidic oxygen reduction

Revealing Adsorption Conformation and Electro-oxidation Mechanism of Urea on the Ni Film Catalyst by In Situ ATR-SEIRAS

Na₂S Cathodes Enabling Safety Room Temperature Sodium Sulfur Batteries

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Revealing surface fine structure on PtAu catalysts by anin situATR-SEIRAS CO-probe method

Abstract: The electrochemical performance of Pt-based catalysts depend on their surface structure. Nevertheless, it is still a challenge to investigate their intricate surface active sites. Here, PtAu films were utilized as...

Cited by 9 publications

References 61 publications

Identifying high-spin Fe3+(S=5/2) as active center for acidic oxygen reduction

Identifying high-spin Fe3+(S=5/2) as active center for acidic oxygen reduction

Revealing Adsorption Conformation and Electro-oxidation Mechanism of Urea on the Ni Film Catalyst by In Situ ATR-SEIRAS

Na2S Cathodes Enabling Safety Room Temperature Sodium Sulfur Batteries

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Product

Resources

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Na₂S Cathodes Enabling Safety Room Temperature Sodium Sulfur Batteries