High-density dispersion of single platinum atoms on graphene by plasma sputtering in N<sub>2</sub> atmosphere

Yamazaki, Kenji; Maehara, Yosuke; Kitajima, Ryo; Fukami, Yuta; Gohara, Kazutoshi

doi:10.7567/apex.11.095101

Cited by 10 publications

(28 citation statements)

References 26 publications

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“…Apart from the heteroatoms, the introduction of vacancies on graphene would also be a novel approach for improving the stability of single atoms . Generally, high energy atom/ion bombardment or plasma sputtering is the common strategy to reconstruct the surface structure for generating vacancies or defects on graphene . For instance, the controllable formation of mono or divacancies on graphene was achieved by manipulating a focused electron beam at 80 kV .…”

Section: Fabrication Strategies and Characteristic Methods Of Sagmentioning

confidence: 99%

Single Atoms on Graphene for Energy Storage and Conversion

et al. 2019

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Single atoms are attracting much attention in the field of energy conversion and storage due to their maximal atomic utilization, high efficiency, and good selectivity. Moreover, their unique electronic structure could improve the intrinsic activity of the active sites. However, the high surface free energy of single atoms inevitably results in their serious aggregation, leading to degraded catalytic activity and poor cycling life. To solve these issues, supports with high surface areas have to be developed to reduce loading density of single atoms and further decrease the surface free energy. Furthermore, engineering the active sites of these substrates can also regulate chemical coordination of single atoms, enhancing their catalytic performance. Owing to high surface area, excellent conductivity and adjustable surface properties, graphene is widely utilized to load atomic metal catalysts. In this review, the fabrication strategies and characterization methods of single atoms on graphene (SAG) are summarized first. Subsequently, the electrochemical applications of SAG on the oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, carbon dioxide reduction, and methane oxidation are discussed in detail. Finally, the future developments and prospects in fabrication and application of SAG are also discussed.

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Section: Fabrication Strategies and Characteristic Methods Of Sagmentioning

confidence: 99%

Single Atoms on Graphene for Energy Storage and Conversion

et al. 2019

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“…In addition to the methods described above, other approaches such as mass selected soft‐landing method, high‐temperature atom trapping, plasma sputtering, and etc. have also been developed for the synthesis of SACs.…”

Section: Synthesis Strategies For Sacsmentioning

confidence: 99%

Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis

et al. 2019

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metal atoms are highly desirable for supported noble-metal (NM) catalysts. [2] Single-atom catalyst (SAC), defined as a catalyst composing only isolated singleatom active sites on supports, was first introduced by Zhang and co-workers in 2011. [3] Owing to the single-atom feature of active sites, SACs provide great advantages in minimizing the usage of precious metal with a 100% atom-utilization efficiency, which thus result in an improved catalytic reactivity, and have aroused extensive attention in the field of catalysis over the past few years. [4] Meanwhile, since the electronic properties of active sites greatly depend on the size and shape of metal particles, which then governs the performance of a catalyst, [5] downsizing metal nanoparticles (NPs) to single atom with the decreased low coordination and the quantized orbital of active sites, is recognized as the other important factor in tuning the catalytic performance of SACs. [5,6] However, due to the tendency of aggregation of single atoms during preactivation and under reaction procedures, utilization of metal/support interactions to immobilize single atom on supports plays a crucial role on the stability of SACs, and the development of effective synthesis strategies is indispensable to realize the distribution and chemical bonding of active sites on supports for the further applications of SACs.In particular, high density of active sites with well-defined local coordination structure to give appreciable catalytic activity/ selectivity and long-term stability are the ultimate goals in catalysis. [7] Thus, long-standing interest exists in fabricating heterogeneous catalysts that feature atomically dispersed metal atoms as active sites for catalytic processes. Even though, considerable efforts have been devoted to, and many advances have been achieved in supported NM-SACs for various heterogeneous catalytic applications, inclusive of CO oxidation, selective hydrogenation, water-gas shift, CO 2 reduction, electrocatalysis, and etc. [2b,7b,8] The achievements from recent studies have greatly contributed to the fast development of single-atom catalysis and paves the way for the rational design of efficient SACs in much broader catalytic systems.In this review, we will focus on this new kind of material, with great attention on the geometric and electronic structure of the single atom active sites, as well as its stability on supports. The recently developed strategies for synthesizing SACs with high metal loading and precise structure are also Single-atom catalysts (SACs), with atomically distributed active metal sites on supports, serve as a newly advanced material in catalysis, and open broad prospects for a wide variety of catalytic processes owing to their unique catalytic behaviors. To construct SACs with precise structures and high density of accessible single-atom sites, while preventing aggregation to large nanoparticles, various strategies for their chemical synthesis have been recently developed by improving the distribution and chemical bondi...

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“…There are a variety of ways to construct metal single sites on solid supports to generate active catalysts, as discussed in several excellent reviews. [52,53] Many physical approaches typically rely on thermal/laser evaporation, [35,54] sputtering, [55] and in some cases, aided by mass selection process. [56] Chemical approaches include atomic layer deposition [57] chemical/photochemical reduction and deposition, [22,58] or through chelating metal complexes directly on support surface.…”

Section: Materials Chemistrymentioning

confidence: 99%

Toward Efficient Carbon and Water Cycles: Emerging Opportunities with Single‐Site Catalysts Made of 3d Transition Metals

2019

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Advances in the chemical and electrochemical transformation of carbon and water are vital for delivering affordable and environmentally friendly energy sources and chemicals. Central to this challenge is the performance of materials. Traditionally, noble metal particles or metal-complexes have been used as catalysts for many reactions. Recently, 3d transition-metal single-site catalysts (3dTM-SSCs) have emerged as potentially transformational candidates for the next generation highperformance noble-metal-free catalysts. Designing catalysts at the molecular level can lead to a more efficient utilization of metal atoms and at the same time enhance catalytic performance under harsh reaction conditions. Despite these promises, several fundamental issues remain, in particular the structural evolution of 3dTM-SSCs during the synthesis, the molecular-level insights into the structure of the active sites, catalytic mechanisms, and the long-term cycling stability. In this progress report, the material chemistries that facilitate the 3dTM-SSCs generation through the controlled synthesis are discussed, and the underlying performance descriptors that can tune the catalytic properties in various critical reactions in carbon and water cycles are elucidated. The current challenges and possible solutions for improving these novel catalytic materials are also highlighted. Received: ((will be filled in by the editorial staff)) Revised: ((will be filled in by the editorial staff)) Published online: ((will be filled in by the editorial staff))

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High-density dispersion of single platinum atoms on graphene by plasma sputtering in N₂ atmosphere

Cited by 10 publications

References 26 publications

Single Atoms on Graphene for Energy Storage and Conversion

Single Atoms on Graphene for Energy Storage and Conversion

Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis

Toward Efficient Carbon and Water Cycles: Emerging Opportunities with Single‐Site Catalysts Made of 3d Transition Metals

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High-density dispersion of single platinum atoms on graphene by plasma sputtering in N2 atmosphere

Cited by 10 publications

References 26 publications

Single Atoms on Graphene for Energy Storage and Conversion

Single Atoms on Graphene for Energy Storage and Conversion

Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis

Toward Efficient Carbon and Water Cycles: Emerging Opportunities with Single‐Site Catalysts Made of 3d Transition Metals

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High-density dispersion of single platinum atoms on graphene by plasma sputtering in N₂ atmosphere