Chemical Structure of Nitrogen-Doped Graphene with Single Platinum Atoms and Atomic Clusters as a Platform for the PEMFC Electrode

Stambula, Samantha; Gauquelin, Nicolas; Bugnet, Matthieu; Gorantla, Sandeep; Turner, Stuart; Sun, Shuhui; Liu, Jian; Zhang, Gaixia; Sun, Xueliang; Botton, Gianluigi A.

doi:10.1021/jp408979h

Cited by 126 publications

(117 citation statements)

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“…[12][13] Botton et al, also reported the formation of a mixture of Pt atoms and clusters on the N-doped graphene support using Pt ALD. 14 Selective hydrogenation of 1,3-butadiene in an excess of alkenes is an important industrial process to purify the alkenes streams from petroleum cracking. 15 The critical requirements in this process are: (i) to achieve high selectivity to butenes, especially to 1-butene (the most desirable product) at high conversions; (ii) to minimize hydrogenation of the alkenes streams at high conversions; (iii) to achieve long durability against deactivation via carbonaceous deposits formation.…”

Section: Supporting Informationmentioning

confidence: 99%

Single-Atom Pd₁/Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene

et al. 2015

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We reported that atomically dispersed Pd on graphene can be fabricated using the atomic layer deposition technique. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy both confirmed that isolated Pd single atoms dominantly existed on the graphene support. In selective hydrogenation of 1,3-butadiene, the single-atom Pd1/graphene catalyst showed about 100% butenes selectivity at 95% conversion at a mild reaction condition of about 50 °C, which is likely due to the changes of 1,3-butadiene adsorption mode and enhanced steric effect on the isolated Pd atoms. More importantly, excellent durability against deactivation via either aggregation of metal atoms or carbonaceous deposits during a total 100 h of reaction time on stream was achieved. Therefore, the single-atom catalysts may open up more opportunities to optimize the activity, selectivity, and durability in selective hydrogenation reactions.

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Section: Supporting Informationmentioning

confidence: 99%

Single-Atom Pd₁/Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene

et al. 2015

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“…[31][32][33][34] Although the ALD methodh as been employedi n variouse nergy-storage applications, such as LIBs, fuel cells, and lithium-sulfur batteries, coating of metal oxides on SIB cathodesw ith ALD has not yet been explored. [33,[35][36][37][38] Han et al reported the ALD of an Al 2 O 3 thin film on an Sn nanostructured anode for SIBs, along with improved cycling performance. [39] However,t he use of ALD metal-oxide coatings for SIB cathodes has not yet been reported.…”

Section: Introductionmentioning

confidence: 99%

Highly Stable Na_2/3(Mn_0.54Ni_0.13Co_0.13)O₂ Cathode Modified by Atomic Layer Deposition for Sodium‐Ion Batteries

et al. 2015

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For the first time, atomic layer deposition (ALD) of Al2 O3 was adopted to enhance the cyclic stability of layered P2-type Na2/3 (Mn0.54 Ni0.13 Co0.13 )O2 (MNC) cathodes for use in sodium-ion batteries (SIBs). Discharge capacities of approximately 120, 123, 113, and 105 mA h g(-1) were obtained for the pristine electrode and electrodes coated with 2, 5, and 10 ALD cycles, respectively. All electrodes were cycled at the 1C discharge current rate for voltages between 2 and 4.5 V in 1 M NaClO4 electrolyte. Among the electrodes tested, the Al2 O3 coating from 2 ALD cycles (MNC-2) exhibited the best electrochemical stability and rate capability, whereas the electrode coated by 10 ALD cycles (MNC-10) displayed the highest columbic efficiency (CE), which exceeded 97 % after 100 cycles. The enhanced electrochemical stability observed for ALD-coated electrodes could be a result of the protection effects and high band-gap energy (Eg =9.00 eV) of the Al2 O3 coating layer. Additionally, the metal-oxide coating provides structural stability against mechanical stresses occurring during the cycling process. The capacity, cyclic stability, and rate performance achieved for the MNC electrode coated with 2 ALD cycles of Al2 O3 reveal the best results for SIBs. This study provides a promising route toward increasing the stability and CE of electrode materials for SIB application.

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“…Thus, we need to discover an effective means to synthesize this ideal single-atom catalyst. In this paper, the atomic layer deposition (ALD) technique was utilized, as it has been proven to be a powerful tool for large-scale synthesis of stable single-atom and cluster catalysts1924. ALD has the ability to precisely control the size and distribution of particles on a substrate by using sequential and self-limiting surface reactions252627.…”

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Platinum single-atom and cluster catalysis of the hydrogen evolution reaction

et al. 2016

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Platinum-based catalysts have been considered the most effective electrocatalysts for the hydrogen evolution reaction in water splitting. However, platinum utilization in these electrocatalysts is extremely low, as the active sites are only located on the surface of the catalyst particles. Downsizing catalyst nanoparticles to single atoms is highly desirable to maximize their efficiency by utilizing nearly all platinum atoms. Here we report on a practical synthesis method to produce isolated single platinum atoms and clusters using the atomic layer deposition technique. The single platinum atom catalysts are investigated for the hydrogen evolution reaction, where they exhibit significantly enhanced catalytic activity (up to 37 times) and high stability in comparison with the state-of-the-art commercial platinum/carbon catalysts. The X-ray absorption fine structure and density functional theory analyses indicate that the partially unoccupied density of states of the platinum atoms' 5d orbitals on the nitrogen-doped graphene are responsible for the excellent performance. S ecuring renewable and reliable sources of clean energy is one of the world's foremost challenges. Addressing this challenge is not only critical for the global economy but will also aid in the mitigation of environmental and health hazards caused by fossil fuels 1 . Hydrogen is the cleanest fuel available and is believed to be one of the most promising energy sources of the twenty-first century 2,3 . However, the majority of the hydrogen produced today is derived from steam-reformed methane, which is sourced from fossil reserves and produces a substantial amount of CO 2 (ref. 4). The production of hydrogen from water electrolysis is a promising alternative to the current CO 2 -emitting fossil fuel-based energy systems 5,6 .Platinum (Pt)-based catalysts are generally considered to be the most effective electrocatalysts for the hydrogen evolution reaction (HER) 5,7 . Unfortunately, Pt is expensive and scarce, limiting the commercial potential for such catalysts. The development of active, stable and inexpensive electrocatalysts for water splitting is a key step in the realization of a hydrogen economy, which is based on the use of molecular hydrogen for energy storage.Significant effort has been devoted to the search of non-preciousmetal-based HER catalysts, including sulfide-based materials 8-11 , and C 3 N 4 (refs 12-14). Although these candidate materials show promising activities for the HER, the activities of these catalysts in their present form are insufficient for industrial applications 15 .To overcome the challenges associated with the Pt HER catalysts and to drive the cost of H 2 production from water electrolysis down, it is very important to markedly decrease the Pt loading and increase the Pt utilization efficiency. Currently, supported Pt nanoparticles (NPs) are typically used to promote Pt activity towards the HER. Unfortunately, the geometry of the NPs limit the majority of the Pt atoms to the particle core, deeming them ineffect...

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Chemical Structure of Nitrogen-Doped Graphene with Single Platinum Atoms and Atomic Clusters as a Platform for the PEMFC Electrode

Cited by 126 publications

References 56 publications

Single-Atom Pd₁/Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene

Single-Atom Pd₁/Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene

Highly Stable Na_2/3(Mn_0.54Ni_0.13Co_0.13)O₂ Cathode Modified by Atomic Layer Deposition for Sodium‐Ion Batteries

Platinum single-atom and cluster catalysis of the hydrogen evolution reaction

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Chemical Structure of Nitrogen-Doped Graphene with Single Platinum Atoms and Atomic Clusters as a Platform for the PEMFC Electrode

Cited by 126 publications

References 56 publications

Single-Atom Pd1/Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene

Single-Atom Pd1/Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene

Highly Stable Na2/3(Mn0.54Ni0.13Co0.13)O2 Cathode Modified by Atomic Layer Deposition for Sodium‐Ion Batteries

Platinum single-atom and cluster catalysis of the hydrogen evolution reaction

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Product

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Single-Atom Pd₁/Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene

Single-Atom Pd₁/Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene

Highly Stable Na_2/3(Mn_0.54Ni_0.13Co_0.13)O₂ Cathode Modified by Atomic Layer Deposition for Sodium‐Ion Batteries