Microwave-assisted synthesis of sulfur-doped graphene supported PdW nanoparticles as a high performance electrocatalyst for the oxygen reduction reaction

Li, Yongliang; Li, Wanhui; Ke, Tenggui; Zhang, Peixin; Ren, Xiangzhong; Deng, Libo

doi:10.1016/j.elecom.2016.06.006

Cited by 18 publications

(5 citation statements)

References 21 publications

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“…The charge localization around the dopant S atom unveils that the C–S bond could act as an important catalytic active site for attractive functional materials in energy conversion/storage and adsorption as metal-free, electrocatalysts for fuel cells, anode materials in Li-ion batteries, , and so on. It was addressed that the introduction of the dopant S atom could improve the selectivity of the oxygen reduction reaction (ORR). − Theoretical calculations predicted that S-doping would induce more strain and defect sites in the graphene panel due to the larger atom radius and the change of spin density, contributing to the enhanced ORR activity of S-doped graphene. In experiments, some S-doped-graphene-based systems, e.g., S-doped graphene “ Idli” , edge activated S-doped Fe-N-graphene, and Pt nanowires on S-doped graphene, have been demonstrated to exhibit excellent catalytic activity, and some of them even outperform commercial Pt/C in terms of durability and selectivity (in addition to the considerably lower materials cost), indicating that S-doped graphene templates hold great potential in replacing conventional Pt/C catalysts in alkaline media .…”

Section: Results and Discussionmentioning

confidence: 99%

Theoretical Designs of Photoresponsive Energy-Storage Materials Based on Attachment of π-Conjugated Molecules onto Sulfur-Doped Graphene

Zhao

2016

J. Phys. Chem. C

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Introducing heteroatom active sites and functional units is essential for achieving high-performance graphene in potential applications of optoelectronic devices and sustainable solar-heat energy conversion/storage. Density functional theory calculations with long-range van der Waals effects (vdW-DF2) were performed to study the electronic structures and energy storage/release of graphene through sulfur (S)-doping and physisorption of π-conjugated photoresponsive molecules, trans/cis-azobenzene (AB) derivatives with an electron-donating substituent group and trans/cisstilbene (ST), respectively. With the increase of the S-doping concentration from 0.4 to 0.8 atom/nm 2 , the band gap of graphene exhibits the enhanced metallic characteristics with a direct-to-indirect transition. Although AB and ST molecules have different unsaturated bridge bonds, −NN− versus −CH CH−, physisorption of these two photoresponsive molecules onto the graphene can both broaden the band gap to about 0.02 eV, as a result of the π−π interfacial interactions. Under the exposure to the solar light, the facile trans-to-cis isomerization of the AB (ST) molecule adsorbed onto graphene renders the energy storage of about 1.04 eV (0.49 eV) in each molecule. The noncovalent physisorption of trans/cis-AB molecules onto graphene is unexpectedly more favorable to energy storage than that of covalent binding. In addition, a multifunctional graphene model, with the combination of both S-doping and physisorption of photoresponsive moelcules, could not only open a band gap of about 0.27 eV but also induce energy storage of 0.84 eV per molecule via the conformational change from transto cis-AB isomer. Strong charge localization at the S dopant may become the active sites for catalysis and energy storage, and meanwhile, photoactive adsorbates could further promote the energy conservation and release.

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Section: Results and Discussionmentioning

confidence: 99%

Theoretical Designs of Photoresponsive Energy-Storage Materials Based on Attachment of π-Conjugated Molecules onto Sulfur-Doped Graphene

Zhao

2016

J. Phys. Chem. C

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“…Bimetal-based N and S doped catalysts have also been reported. Li et al synthesized PdW alloy nanoparticles decorated S-doped graphene via a microwave irradiation method [26]. S-doping contributed to the formation of small particles and the uniform distribution of alloy particles.…”

Section: M-n-s-based Active Sitesmentioning

confidence: 99%

The Role of Sulfur-Related Species in Oxygen Reduction Reactions

Xu¹,

Wu²

2019

Chalcogen Chemistry

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Heteroatom (metal and nonmetal) doping is essential to achieve excellent oxygen reduction reaction (ORR) activity of carbon materials. Among the heteroatoms that have been studied to date, sulfur (S) doping, including metal sulfides and sulfur atoms, has attracted tremendous attention. Since S-doping can modify spin density distributions around the metal centers as well as the synergistic effect between S and other doped heteroatoms, the S-C bond and metal sulfides can function as important ORR active sites. Furthermore, the S-doped hybrid sample shows a small charge-transfer resistance. Therefore, S-doping contributes to the superior ORR performance. This chapter describes the recent advancements of S-doped carbon materials, and their development in the area of ORR with regard to components, structures, and their ORR activities of S-related species.

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“…In alkaline solutions, the oxygen can be reduced through a four-electron pathway or a two-electron pathway [35]. A lot of novel Pd-based electrocatalysts for ORR exist, including carbon or metal supported Pd alloys [36][37][38], nitrogen and sulfur co-doped carbon supported PdNi catalyst (PdNi-NS/C) [39], Pd supported on TiO 2 with oxygen vacancy (Pd/TiO 2 -Vo) [40], PdW nanoparticles supported on sulfur-doped graphene (PdW/SG) [41], PdNiCu/PdNiCo supported on nitrogen dope graphene [42], PdSnCo/nitrogen-doped-graphene [43], electrochemically reduced graphene-oxide supported Pd-Mn 2 O 3 nanoparticles [44], AuPd@PdAu alloy nanocrystals [45], three-dimensional nitrogen-doped graphene supports for palladium nanoparticles (Pd-N/3D-GNS) [46], and so on. Most of the research above on Pd-based electrocatalysts for ORR in alkaline media is supported on graphene specially treated (doping, modifying, and so on).…”

Section: Introductionmentioning

confidence: 99%

Electrocatalytic Performance of Carbon Supported WO3-Containing Pd–W Nanoalloys for Oxygen Reduction Reaction in Alkaline Media

Cui

Guo

et al. 2018

Catalysts

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In this paper, we report that WO x containing nanoalloys exhibit stable electrocatalytic performance in alkaline media, though bulk WO 3 is easy to dissolve in NaOH solution. Carbon supported oxide-rich Pd-W alloy nanoparticles (PdW/C) with different Pd:W atom ratios were prepared by the reduction-oxidation method. Among the catalysts, the oxide-rich Pd 0.8 W 0.2 /C (Pd/W = 8:2, atom ratio) exhibits the highest catalytic activity for the oxygen reduction reaction. The X-ray photoelectron spectroscopy data shows that~40% of Pd atoms and~60% of the W atoms are in their oxide form. The Pd 3d 5/2 binding energy of the oxide-rich Pd-W nanoalloys is higher than that of Pd/C, indicating the electronic structure of Pd is affected by the strong interaction between Pd and W/WO 3. Compare to Pd/C, the onset potential of the oxygen reduction reaction at the oxide-rich Pd 0.8 W 0.2 /C shifts to a higher potential. The current density (mA•mg Pd −1) at the oxide-rich Pd 0.8 W 0.2 /C is~1.6 times of that at Pd/C. The oxide-rich Pd 0.8 W 0.2 /C also exhibits higher catalytic stability than Pd/C, which demonstrates that it is a prospective candidate for the cathode of fuel cells operating with alkaline electrolyte.

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Microwave-assisted synthesis of sulfur-doped graphene supported PdW nanoparticles as a high performance electrocatalyst for the oxygen reduction reaction

Cited by 18 publications

References 21 publications

Theoretical Designs of Photoresponsive Energy-Storage Materials Based on Attachment of π-Conjugated Molecules onto Sulfur-Doped Graphene

Theoretical Designs of Photoresponsive Energy-Storage Materials Based on Attachment of π-Conjugated Molecules onto Sulfur-Doped Graphene

The Role of Sulfur-Related Species in Oxygen Reduction Reactions

Electrocatalytic Performance of Carbon Supported WO3-Containing Pd–W Nanoalloys for Oxygen Reduction Reaction in Alkaline Media

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