Tuning the electronic structure of PtRu bimetallic nanoparticles for promoting the hydrogen oxidation reaction in alkaline media

Long, Chang; Wang, Kun; Shi, Yanan; Yang, Zihao; Zhang, Xiaofei; Zhang, Yin; Han, Jianyu; Bao, Yi-Ni; Chang, Lin; Liu, Shaoqin; Tang, Zhiyong

doi:10.1039/c9qi00942f

Cited by 49 publications

(39 citation statements)

References 37 publications

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“…ydrogen fuel cell is considered as one of the most promising energy conversion devices due to its high energy efficiency and pollution-free feature [1][2][3][4][5] . Over the past decades, great efforts have been devoted to developing catalysts for hydrogen oxidation reaction (HOR) for enhancing the energy conversion efficiency of the hydrogen fuel cell 6,7 .…”

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confidence: 99%

Subnanometer high-entropy alloy nanowires enable remarkable hydrogen oxidation catalysis

et al. 2021

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High-entropy alloys (HEAs) with unique physicochemical properties have attracted tremendous attention in many fields, yet the precise control on dimension and morphology at atomic level remains formidable challenges. Herein, we synthesize unique PtRuNiCoFeMo HEA subnanometer nanowires (SNWs) for alkaline hydrogen oxidation reaction (HOR). The mass and specific activities of HEA SNWs/C reach 6.75 A mgPt+Ru−1 and 8.96 mA cm−2, respectively, which are 2.8/2.6, 4.1/2.4, and 19.8/18.7 times higher than those of HEA NPs/C, commercial PtRu/C and Pt/C, respectively. It can even display enhanced resistance to CO poisoning during HOR in the presence of 1000 ppm CO. Density functional theory calculations reveal that the strong interactions between different metal sites in HEA SNWs can greatly regulate the binding strength of proton and hydroxyl, and therefore enhances the HOR activity. This work not only provides a viable synthetic route for the fabrication of Pt-based HEA subnano/nano materials, but also promotes the fundamental researches on catalysis and beyond.

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confidence: 99%

Subnanometer high-entropy alloy nanowires enable remarkable hydrogen oxidation catalysis

et al. 2021

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“…The Tafel curves derived from the polarization curves are shown in Fig. 7c, f ) indicated that FeP@PGL exhibited a faster kinetics in alkaline media [51][52][53].…”

Section: Orr Activities Of Catalysts In Acidic and Alkaline Mediamentioning

confidence: 93%

Encapsulated FeP nanoparticles with in-situ formed P-doped graphene layers: Boosting activity in oxygen reduction reaction

Chen

et al. 2020

Sci. China Mater.

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Nonprecious metal-based oxygen reduction reaction (ORR) electrocatalysts with high efficiency in both alkaline and acidic media are being intensively studied for the purpose of replacing expensive Pt-based catalysts; however, it is still a challenge to achieve superior ORR performances, especially in acidic media. Herein, by pyrolysis of mixed precursors of diammonium phosphate, melamine and hemin, we prepared a nanocomposite catalyst (denoted as FeP@PGL) composed of nitrogen-doped carbon nanosheets with embedded FeP nanoparticles (NPs), which were encapsulated by in-situ formed phosphorus-doped graphene layers. It is found that phosphorous was preferentially doped in the coating layers on FeP NPs, instead of in the carbon nanosheets. The FeP@PGL catalyst exhibited excellent ORR performance, with the onset and half-wave potential up to 1.01 and 0.90 V vs. the reversible hydrogen electrode (RHE) in alkaline media, and 0.95 and 0.81 V vs. RHE in acidic media, respectively. By thorough microscopy and spectroscopy characterizations, the interfacial charge transfer between the encapsulated FeP NPs and P-doped graphene layers was identified, and the local work function of the catalyst surface was also reduced by the interfacial interaction. The interfacial synergy between the encapsulated FeP and phosphorus-doped graphene layers was essential to enhance the ORR performance. This study not only demonstrates the promising ORR properties of the encapsulated-FeP-based nanocomposite catalyst, but also provides direct evidence of the interfacial charge transfer effect and its role in ORR process.

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“…The binding energy of H ad on the Pt surface is relatively high, so the Volmer step usually restricts the HOR kinetics of most the Pt‐based nanocatalysts in the alkaline medium. [ 38 ] However, the evolution of the Tafel slope from the Pt/PC to Ru‐increased nanocatalyst suggests that the Ru‐increased nanostructure changes the rate‐determining step (RDS) of the Pt sites, possibly shifting from the Volmer to Tafel or Heyrovsky step. [ 17,39 ] The Ru‐based catalysts in the literature also have similar lower Tafel slope values (such as 43 mV dec –1 of Ru‐doped Pt/C [ 17 ] and ≈30 mV dec –1 of Ru x Pt y , [ 40 ] Table S1, Supporting Information).…”

Section: Resultsmentioning

confidence: 99%

Engineering the Near‐Surface of PtRu₃ Nanoparticles to Improve Hydrogen Oxidation Activity in Alkaline Electrolyte

Zhang

Shen

et al. 2021

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Tailoring the near‐surface composition of Pt‐based alloy can optimize the surface chemical properties of a nanocatalyst and further improve the sluggish H2 electrooxidation performance in an alkaline electrolyte. However, the construction of alloy nanomaterials with a precise near‐surface composition and smaller particle size still needs to overcome huge obstacles. Herein, ultra‐small PtRu3 binary nanoparticles (<2 nm) evenly distributed on porous carbon (PtRu3/PC), with different near‐surface atomic compositions (Pt‐increased and Ru‐increased), are successfully synthesized. XPS characterizations and electrochemical test confirm the transformation of a near‐surface atomic composition after annealing PtRu3/PC‐300 alloy; when annealing in CO atmosphere, forming the Pt‐increased near‐surface structure (500 °C), while the Ru‐increased near‐surface structure appears in an Ar heat treatment process (700 °C). Furthermore, three PtRu3/PC nanocatalysts all weaken the hydrogen binding strength relative to the Pt/PC. Remarkably, the Ru‐increased nanocatalyst exhibits up to 38.8‐fold and 9.2‐fold HOR improvement in mass activity and exchange current density, compared with the Pt/PC counterpart, respectively. CO‐stripping voltammetry tests demonstrate the anti‐CO poisoning ability of nanocatalysts, in the sequence of Ru‐increased ≥ PtRu3/PC‐300 > Pt‐increased > Pt/PC. From the perspective of engineering a near‐surface structure, this study may open up a new route for the development of high‐efficiency electrocatalysts with a strong electronic effect and oxophilic effect.

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Tuning the electronic structure of PtRu bimetallic nanoparticles for promoting the hydrogen oxidation reaction in alkaline media

Abstract: Alloying degree of PtRu bimetallic nanoparticles can be controlled to finely tune electronic effect for enhanced Hydrogen oxidation reaction in alkaline.

Cited by 49 publications

References 37 publications

Subnanometer high-entropy alloy nanowires enable remarkable hydrogen oxidation catalysis

Subnanometer high-entropy alloy nanowires enable remarkable hydrogen oxidation catalysis

Encapsulated FeP nanoparticles with in-situ formed P-doped graphene layers: Boosting activity in oxygen reduction reaction

Engineering the Near‐Surface of PtRu₃ Nanoparticles to Improve Hydrogen Oxidation Activity in Alkaline Electrolyte

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Tuning the electronic structure of PtRu bimetallic nanoparticles for promoting the hydrogen oxidation reaction in alkaline media

Abstract: Alloying degree of PtRu bimetallic nanoparticles can be controlled to finely tune electronic effect for enhanced Hydrogen oxidation reaction in alkaline.

Cited by 49 publications

References 37 publications

Subnanometer high-entropy alloy nanowires enable remarkable hydrogen oxidation catalysis

Subnanometer high-entropy alloy nanowires enable remarkable hydrogen oxidation catalysis

Encapsulated FeP nanoparticles with in-situ formed P-doped graphene layers: Boosting activity in oxygen reduction reaction

Engineering the Near‐Surface of PtRu3 Nanoparticles to Improve Hydrogen Oxidation Activity in Alkaline Electrolyte

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Engineering the Near‐Surface of PtRu₃ Nanoparticles to Improve Hydrogen Oxidation Activity in Alkaline Electrolyte