Strong negative nanocatalysis: oxygen reduction and hydrogen evolution at very small (2 nm) gold nanoparticles

Wang, Ying; Laborda, Eduardo; Tschulik, Kristina; Damm, Christine; Molina, Á.; Compton, Richard G.

doi:10.1039/c4nr03850a

Cited by 32 publications

(58 citation statements)

References 45 publications

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“…Given their generally high stability and amenability to widespread use, such surfaces have been able to produce large amounts of H 2 at rates rivalling those of enzymatic systems and many new examples have recently emerged. 106,107 New developments in this field are instead focused on increasing catalytic selectivity for H 2 evolution over O 2 reduction in order to maximise efficiency. 12,104,105 Their use includes a few disadvantages however, as they have generally low 'per atom activity' and ascertaining the exact nature of the catalytically active site and mechanism can be difficult.…”

Section: Oxygen-tolerant Catalytic Surfacesmentioning

confidence: 99%

Oxygen-tolerant proton reduction catalysis: much O₂ about nothing?

Wakerley

Reisner

2015

Energy Environ. Sci.

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Section: Oxygen-tolerant Catalytic Surfacesmentioning

confidence: 99%

Oxygen-tolerant proton reduction catalysis: much O₂ about nothing?

Wakerley

Reisner

2015

Energy Environ. Sci.

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“…Bulk gold metal shows moderate ORR activity and its activity depends on the size in nanoparticles. For example Crompton and coworkers 36 showed that ultra small (1.5-2nm) citrate capped gold nanoparticles acts as negative catalyst for ORR in compare to Au macro-electrode. It is also reported by them 37 that the 17-40 nm AuNPs showed comparable ORR properties with Au electrode and H 2 O 2 was the final product due to two electron reduction of oxygen.…”

Section: Introductionmentioning

confidence: 99%

Gold aerogel supported on graphitic carbon nitride: an efficient electrocatalyst for oxygen reduction reaction and hydrogen evolution reaction

2015

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Fabrication of high surface area interconnected porous network of metallic nanomaterials is important for their applications in various fields such as catalysis, sensors, and electrochemistry. Here we report a facile bottom up synthesis of high surface area and porous, gold aerogel supported on carbon nitride sheets (CNx). The reduction of HAuCl4 in presence of carbon nitride nanosheets using sodium brohydride and ultrasonic treatment produces gold aerogel supported on carbon nitride (Au-aerogel-CNx). When the reduction of HAuCl4 in presence CNx nano sheets was done only with ultrasonication, highly dispersed ultra small ( ~2 nm) gold nanoparticles on CNx sheets (AuNPs-CNx) were formed. The Au aerogel supported on CNx sheets was well characterized by powder X-ray diffraction, tunneling electron microscopy, selected area electron diffraction, energy dispersive X-ray spectroscopy, scanning electron microscopy, UV-Visible and Xray photo electron spectroscopic methods. The Au-aerogel-CNx and AuNPs-CNx composites exhibited superior electro catalytic activity towards oxygen reduction reaction (ORR) in alkaline and acidic media. The Au-aerogel-CNx composite show ORR onset potentials at 0.92 V and 0.43 V (Vs RHE) in 0.5 M KOH and H2SO4 solution. The four electron oxygen reduction proceess occurs at these supported catalysts in both alkaline and acidic media. In alkaline (KOH) medium the onset potential at Au-aerogel-CNx is more positive ( ~ 30 mV) than that of commercial Pt/C catalyst. The composites display excellent methanol tolerance and comparable durability with commercial Pt/C. Furthermore, the Au-aerogel-CNx composites exhibited high catalytic activity for hydrogen reduction reaction (HER) with small onset potential of -30 mV and a Tafel slope of 53 mV dec -1 in acidic medium. At a small Au loading of 0.130 mg cm -2 , this catlyst also exhibit a current density of 10 mA cm -2 at a low overpotential of -185 mV with an excellent stability. The ORR and HER performaneces on porous, Au-aerogel-CNx composites is better than that of AuNPs-CNx catalyst and commercial flat gold electrode. The superior ORR and HER activity at Au-aerogel-CNx composite are originated from the unique synergistic effects between porous Au network and carbon nitride (CNx) support. Please do not adjust margins Please do not adjust margins approaches are available in literature for synthesis of different non metal aerogel such as carbon aerogel 11 , silica aerogel 12 , organic-inorganic hybrid 13 , metal oxide 14 , and metal chalcogenides 15 . But only few methods are available for the production of metal aerogel 8,16,17,18 . For example, Eychmüller and coworkers 8,16 have reported synthesis for monometallic, bi-metallic and composite aerogels based on controlled aggregation of metal nanoparticles using controllable destabilization and spontaneous gelation methods. Leventis and his co-workers 17,18 developed methods for synthesis of different metallic (Fe, cu, Ni, Co) aerogels by nanosmelting (sol-gel method) of hybrid polymer-metal oxide composit...

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“…To sustainably consider the globally rapid increasing demand of energy, tremendous efforts are being devoted to advance the technologies for clean and renewable energy conversion [1][2][3][4][5][6][7][8][9][10][11]. Among these green energy approaches, the hydrogen evolution reaction (HER) is attracting significant attention due to its role in electrochemical water splitting and the subsequent use of the generated hydrogen in fuel cells [9,[11][12][13].…”

Section: Introductionmentioning

confidence: 99%

“…(2)) or the Heyrovsky step (Eq. (3)) depending on the nature of the electrode material [1,2,6,[8][9][10]14,15]. …”

Section: Introductionmentioning

confidence: 99%

Activation Effect of Electrochemical Cycling on Gold Nanoparticles towards the Hydrogen Evolution Reaction in Sulfuric Acid

Wang

Sun

Liao

et al. 2016

Electrochimica Acta

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A B S T R A C TThis article reports a study of electrochemical cycling effects on hydrogen evolution catalytic activity of gold nanoparticles in sulfuric acid. We found that after cycling within the double layer regime, up to 0.64 V vs RHE, there is a dramatic effect on the HER activity of gold nanoparticles: 128 mV drop of the overpotential, a decrease of 23 mV/dec for the Tafel slope as well as a nearly twenty times increase of the turn-over frequency (TOF). This enhanced activity is tentatively assigned to the formation of stepped like structures by the consecutive electrochemical cycling in the double layer region.

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Strong negative nanocatalysis: oxygen reduction and hydrogen evolution at very small (2 nm) gold nanoparticles

Cited by 32 publications

References 45 publications

Oxygen-tolerant proton reduction catalysis: much O₂ about nothing?

Oxygen-tolerant proton reduction catalysis: much O₂ about nothing?

Gold aerogel supported on graphitic carbon nitride: an efficient electrocatalyst for oxygen reduction reaction and hydrogen evolution reaction

Activation Effect of Electrochemical Cycling on Gold Nanoparticles towards the Hydrogen Evolution Reaction in Sulfuric Acid

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Strong negative nanocatalysis: oxygen reduction and hydrogen evolution at very small (2 nm) gold nanoparticles

Cited by 32 publications

References 45 publications

Oxygen-tolerant proton reduction catalysis: much O2 about nothing?

Oxygen-tolerant proton reduction catalysis: much O2 about nothing?

Gold aerogel supported on graphitic carbon nitride: an efficient electrocatalyst for oxygen reduction reaction and hydrogen evolution reaction

Activation Effect of Electrochemical Cycling on Gold Nanoparticles towards the Hydrogen Evolution Reaction in Sulfuric Acid

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Oxygen-tolerant proton reduction catalysis: much O₂ about nothing?

Oxygen-tolerant proton reduction catalysis: much O₂ about nothing?