Ultrafine Co Nanoparticles Encapsulated in Carbon‐Nanotubes‐Grafted Graphene Sheets as Advanced Electrocatalysts for the Hydrogen Evolution Reaction

Chen, Ziliang; Wu, Renbing; Liu, Yang; Ha, Yuan; Guo, Yanhui; Sun, Dalin; Liu, Miao; Fang, Fang

doi:10.1002/adma.201802011

Cited by 497 publications

(322 citation statements)

References 58 publications

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“…[1][2][3][4][5] So far, Pt is regarded as the most effective catalyst for hydrogen evolution reaction (HER) in acidic media, because of its appropriate adsorption of H atoms. [1][2][3][4][5] So far, Pt is regarded as the most effective catalyst for hydrogen evolution reaction (HER) in acidic media, because of its appropriate adsorption of H atoms.…”

mentioning

confidence: 99%

Ruthenium‐Based Single‐Atom Alloy with High Electrocatalytic Activity for Hydrogen Evolution

Chen

et al. 2019

Advanced Energy Materials

305

217

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performance and low price for working in alkaline solution.Ruthenium, as a member of platinumgroup metals with 1/30 price of Pt, [14] has been proved to be a promising catalyst for HER in alkaline solution due to its high efficiency on water dissociation, [15][16][17][18] however, the strong interaction between Ru and H atoms impedes the subsequent hydrogen evolution because of the well-known scaling relationship for heterogeneous catalysts. [17,[19][20][21] Many efforts had been devoted to constructing Rubased heterostructures (e.g., Ru/carbon quantum dots, [22] Ru/C 2 N, [18] RuCo/ nitrogen-doped graphene, [23] fcc-Ru/ C 3 N 4 /C, [17] Ru/nitrogen-doped carbon, [24] Ru/graphene [25] ), which show great advantages on promoting water dissociation by synergistic effect. Nevertheless, less attention was paid on the improvement of hydrogen adsorption. Recently, singleatom alloys (SAAs), which comprise separated solute atoms in metallic matrix, show great potential on circumventing scaling relationships. [23,26,27] meanwhile, the interaction between the solute atoms and matrix can modify their electronic structure, [26,28,29] leading to a suitable adsorption energy for hydrogen. Consequently, constructing Ru-based SAAs opens a new avenue toward high HER performance.Herein, we reported the synthesis of RuAu SAAs through a laser ablation in liquid (LAL) technique, which possesses strong quenching effect so as to fabricate metastable nanostructures with novel properties. [30,31] We choose Au as the alloying element on the basis of the following considerations: First, Au is known as an inert metal with weak hydrogen adsorption thus can counteract the strong hydrogen adsorption of Ru matrix. Second, the immiscibility between Au and Ru may create a unique geometric and electronic structure in RuAu SAAs. [32,33] Finally, chemically inert Au favors long-term durability during the reaction. As such, the as-prepared RuAu catalyst exhibits a low overpotential, 24 mV@10 mA cm −2 , which is much lower than Pt/C (46 mV@10 mA cm −2 ) in alkaline media. Moreover, the turnover frequency (TOF) of RuAu SAAs is three times that of the Pt/C catalyst. Density functional theory (DFT) computation reveals that the high performance originates from the relay catalysis of Ru host (for water dissociation) and Au dopant (for hydrogen evolution). To the best of our knowledge, this is the first report on the synthesis of RuAu SAAs with outstanding HER performance in alkaline media. Furthermore, the idea of the mixing immiscible metallic elements by LAL can be facilely Highly efficient and stable catalysts for the hydrogen evolution reaction, especially in alkaline conditions are crucial for the practical demands of electrochemical water splitting. Here, the synthesis of a novel RuAu single-atom alloy (SAA) by laser ablation in liquid is reported. The SAA exhibits a high stability and a low overpotential, 24 mV@10 mA cm −2 , which is much lower than that of a Pt/C catalyst (46 mV) in alkaline media. Moreover, the turnover frequency of RuAu SAA is th...

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confidence: 99%

Ruthenium‐Based Single‐Atom Alloy with High Electrocatalytic Activity for Hydrogen Evolution

Chen

et al. 2019

Advanced Energy Materials

305

217

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“…Extensive investigations have been performed to understand the synergy and underlying interaction between metal‐based catalysts and carbon substrates toward different electrocatalysis. Fang and co‐workers fabricated ultrafine Co nanoparticles encapsulated in carbon‐grafted graphene sheets as electrocatalysts for HER . Computations reveal that the combination of Co and N‐doped graphene could generate a synergistic effect, which results in charge redistributions and tunable H* adsorption and desorption of Co@C model.…”

Section: Carbon Materialsmentioning

confidence: 99%

Carbon‐Based Substrates for Highly Dispersed Nanoparticle and Even Single‐Atom Electrocatalysts

2019

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In recent decades, electrocatalysis has become an important research hotspot in energy storage and conversion technologies due to the persistently increasing energy and environmental issues. Nanostructured carbon materials with excellent electrical conductivity, competitive activity, and relatively high chemical stability are extensively studied as either electrocatalysts or substrates to support metal‐based catalysts. Especially, when used as supporting substrates for metal‐based catalysts, carbon‐based materials can not only effectively promote the dispersion of metals and even lead to single‐atom catalysts but also lead to prominent synergistic effects for enhanced activity. This review sheds light on state‐of‐the‐art carbon‐based materials employed as supporting substrates for selected electrocatalytic processes involving H2/O2/CO2/N2. By combining experimental explorations with theoretical computations, clear insight is elaborately afforded into the fundamental relationship between electrocatalytic activity and metal–substrate interaction, in order to disclose some clues for electrocatalyst design. Finally, the remaining challenges and perspectives are discussed for the future development of carbon‐supported electrocatalysts.

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“…However, formation of tightly wrapped carbon chainmail on nonprecious transitional metals particles is difficult to controlled. The most reported form of carbon materials is carbon nanotubes that precipitate from metal particles rather than tightly wrapped thin graphene layers . These deviate from ideal core‐shell structure of catalysts with effective electron penetration from inner core to its tightly contacted outer shell.…”

Section: Introductionmentioning

confidence: 99%

Nitrogen‐doped Graphene Chainmail Wrapped IrCo Alloy Particles on Nitrogen‐doped Graphene Nanosheet for Highly Active and Stable Full Water Splitting

Zhang

et al. 2019

ChemCatChem

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Electrocatalysts have been used to split water into hydrogen and oxygen for their advantages in clean energy technologies. To reduce cost and enhance stability of electrocatalysts, intensive works have been done in recent decades. Although research on noble‐metal free electrocatalysts has achieved great progress, their full water splitting performance is still incomparable to that of noble metal based catalysts. For this reason, reducing content of noble metal in catalysts is a more practical way. In this work, we report our recent progress on developing bifunctional electrocatalyst based on nitrogen‐doped graphene chainmail wrapped IrCo alloy particles on nitrogen‐doped graphene (NG@IrCo/NG). Benefited from strong interaction among iridium, cobalt and nitrogen‐doped graphene, impressively high electrocatalytic activity of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in both acid and alkaline solutions, which are comparable to commercially used Pt/C and IrO2 electrocatalysts respectively, is found. Catalyst with the structure of nitrogen doped chainmail wrapping on metal core is found to have highly stable full water splitting performance.

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Ultrafine Co Nanoparticles Encapsulated in Carbon‐Nanotubes‐Grafted Graphene Sheets as Advanced Electrocatalysts for the Hydrogen Evolution Reaction

Cited by 497 publications

References 58 publications

Ruthenium‐Based Single‐Atom Alloy with High Electrocatalytic Activity for Hydrogen Evolution

Ruthenium‐Based Single‐Atom Alloy with High Electrocatalytic Activity for Hydrogen Evolution

Carbon‐Based Substrates for Highly Dispersed Nanoparticle and Even Single‐Atom Electrocatalysts

Nitrogen‐doped Graphene Chainmail Wrapped IrCo Alloy Particles on Nitrogen‐doped Graphene Nanosheet for Highly Active and Stable Full Water Splitting

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