Significantly enhanced electrocatalytic activity of Au25 clusters by single platinum atom doping

Lu, Yizhong; Zhang, Chun-Mei; Li, Xiaokun; Frojd, Andrew R.; Wang, Xing; Clayborne, Andre; Chen, Wei

doi:10.1016/j.nanoen.2018.05.052

Cited by 72 publications

(63 citation statements)

References 58 publications

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“…Developing efficient electrocatalyst for formic acid oxidation reaction (FAOR) is crucial for the practical applications of DFAFCs . Although platinum (Pt)‐based electrocatalysts have been investigated for FAOR, they still suffer from high cost, low catalytic activity, and poor stability . Alloying Pt with earth‐abundant metal is an effective strategy to enhance the performance of Pt‐based electrocatalysts and concurrently reduce the usage of Pt .…”

Section: Introductionmentioning

confidence: 99%

Ultrathin‐Carbon‐Layer‐Protected PtCu Nanoparticles Encapsulated in Carbon Capsules: A Structure Engineering of the Anode Electrocatalyst for Direct Formic Acid Fuel Cells

Chen²,

Zhao

et al. 2019

Part & Part Syst Charact

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Structure engineering is an effective strategy to enhance the performance of electrocatalysts for the formic acid oxidation reaction. However, it remains a challenge to prepare a highly active electrocatalyst based on a distinct understanding of its structure‐dependent performance. The design and synthesis of ultrathin‐carbon‐layer‐protected PtCu nanoparticles (NPs) encapsulated in a N‐doped carbon capsule (PtCu@NCC) is reported. This system is fabricated by using Zn‐based metal–organic frameworks as the carbon support source and metal‐containing tannic acid as the protecting shell template. It displays 9.8‐ and 9.6‐fold enhancements in mass activity and specific activity compared to commercial Pt/C. Moreover, a constructed direct formic acid fuel cell using PtCu@NCC as the anodic electrocatalyst delivers a maximum power density of 121 mW cm−2. Significantly, PtCu@NCC exhibits superior structural stability and catalytic durability in both half‐cell and full‐cell tests. A mechanism study reveals that the enhanced activity is partially attributed to facilitated electro‐oxidation kinetics of formic acid in the unique structure of PtCu@NCC, while the excellent durability stems from the “protecting effect” of the in‐situ‐formed ultrathin carbon layer on the surface of the PtCu NPs. This work opens a new avenue for the development of high‐performance electrocatalysts for fuel‐cell applications by offering essential insights into the structure–performance relationship of the materials.

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Section: Introductionmentioning

confidence: 99%

Ultrathin‐Carbon‐Layer‐Protected PtCu Nanoparticles Encapsulated in Carbon Capsules: A Structure Engineering of the Anode Electrocatalyst for Direct Formic Acid Fuel Cells

Chen²,

Zhao

et al. 2019

Part & Part Syst Charact

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“…In a follow-up study, the authors found that the HER catalytic activity of Au 24 Pt(SR) 18 can be further enhanced by incorporating a proton-relaying ligand (e.g., 3mercapto-1-propanesulfonic acid) into its protecting shell. 98 It should be noted that in many other catalytic reaction systems, including oxidation 99 and C-C coupling 100 reactions, similar doping effects of M(0) have also been recorded.…”

Section: Molecular Interactions/reactions Based On the M(0) Corementioning

confidence: 72%

Molecular reactivity of thiolate-protected noble metal nanoclusters: synthesis, self-assembly, and applications

et al. 2021

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“…Figure c shows the CVs curves for FAOR recorded with three samples, where UCS−PtZn iNPs exhibits the highest activity with lowest onset potential and highest current density. It is well known that the anodic polarization curve of FAOR on Pt‐based electrocatalysts shows two typical peaks, where the peak at relatively low potential is corresponding to the electrocatalytic oxidation of HCOOH to CO 2 through the direct pathway and the other peak at high potential is corresponding to the electrocatalytic oxidation of CO to CO 2 through the indirect pathway . In comparison with Pt/C, both UCS−PtZn iNPs and PtZn iNPs appear a stronger peak at around 0.55 V at the forward scan (as marked by stars), which is assigned to the direct oxidation of formic acid to CO 2 .…”

Section: Resultsmentioning

confidence: 98%

“…It is well known that the anodic polarization curve of FAOR on Pt-based electrocatalysts shows two typical peaks, where the peak at relatively low potential is corresponding to the electrocatalytic oxidation of HCOOH to CO 2 through the direct pathway and the other peak at high potential is corresponding to the electrocatalytic oxidation of CO to CO 2 through the indirect pathway. [37][38][39][40][41][42][43] In comparison with Pt/C, both UCSÀ PtZn iNPs and PtZn iNPs appear a stronger peak at around 0.55 V at the forward scan (as marked by stars), which is assigned to the direct oxidation of formic acid to CO 2 . As a result, it indicates that PtZn intermetallic electrocatalysts can significantly enhance the electrocatalytic performance for FAOR by facilitating direct oxidation of HCOOH to CO 2 .…”

Section: Resultsmentioning

confidence: 99%

Role of Ultrathin Carbon Shell in Enhancing the Performance of PtZn Intermetallic Nanoparticles as an Anode Electrocatalyst for Direct Formic Acid Fuel Cells

Zhao

Chen³

et al. 2019

ChemElectroChem

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Introducing a carbon shell to Pt‐based intermetallic nanoparticles (iNPs) is an effective approach to prepare structurally ordered electrocatalysts for fuel cell applications. However, it remains a huge challenge to synthesize small‐sized Pt‐based iNPs with a concisely controlled carbon shell based on fully understanding the role of the carbon shell in the electrocatalytic performance. Herein, we report the preparation of ultrathin carbon shell (UCS)‐coated, small‐sized PtZn iNPs, which are obtained by using the simple heat treatment of polypyrrole‐coated PtZn/C (PPy−PtZn/C), which can produce a carbon shell in situ and simultaneously transfer a disordered PtZn alloy into ordered intermetallic PtZn. Interestingly, the thickness of the carbon shell can be well‐controlled by tuning the polymerization time of pyrrole (Py). The obtained PtZn iNPs (an average diameter of ca. 4 nm) coated with UCS (ca. 0.5 nm thickness) shows the best electrocatalytic performance toward the formic acid oxidation reaction. Moreover, the UCS−PtZn iNPs offers remarkable long‐term stability as an anode electrocatalyst in a constructed direct formic acid fuel cell. The results demonstrate that the UCS formed in situ only acts as a physicochemical protecting shell with high permeability for the reactants, but it does not block the catalytic reaction sites of iNPs.

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Significantly enhanced electrocatalytic activity of Au25 clusters by single platinum atom doping

Cited by 72 publications

References 58 publications

Ultrathin‐Carbon‐Layer‐Protected PtCu Nanoparticles Encapsulated in Carbon Capsules: A Structure Engineering of the Anode Electrocatalyst for Direct Formic Acid Fuel Cells

Ultrathin‐Carbon‐Layer‐Protected PtCu Nanoparticles Encapsulated in Carbon Capsules: A Structure Engineering of the Anode Electrocatalyst for Direct Formic Acid Fuel Cells

Molecular reactivity of thiolate-protected noble metal nanoclusters: synthesis, self-assembly, and applications

Role of Ultrathin Carbon Shell in Enhancing the Performance of PtZn Intermetallic Nanoparticles as an Anode Electrocatalyst for Direct Formic Acid Fuel Cells

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