Unveiling the Excellent Electrocatalytic Activity of Grain-Boundary Enriched Anisotropic Pure Gold Nanostructures toward Hydrogen Evolution Reaction: A Combined Approach of Experiment and Theory

Mondal, Subrata; De, Sandip Kumar; Jana, Rajkumar; Roy, Abhijit Sinha; Mukherjee, M.; Datta, Ayan; Satpati, Biswarup; Senapati, Dulal

doi:10.1021/acsaem.0c02527

Cited by 10 publications

(8 citation statements)

References 83 publications

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“…In any case, we note that in contrast to acidic and alkaline conditions, [49][50][51] variations in HER performance due to Pt deposition only become apparent in neutral electrolytes after several hundred cycles, [52] i.e., timescales much longer than those over which the LSVs were conducted (typically 3 min), and leads to improvements in HER that are far lower than those observed in the present work with the SRBW forcing.…”

Section: Resultscontrasting

confidence: 63%

“…[ 48 ] Besides the absence of any evidence of Pt deposition on the Au working electrode, as confirmed from the X‐ray photoelectron spectroscopy (XPS) measurements on the electrode in Figure S6 (Supporting Information), similar performance enhancements were noted with the SRBW excitation when the Pt counter electrode was replaced with Au foil (Figure S7, Supporting Information). In any case, we note that in contrast to acidic and alkaline conditions, [ 49–51 ] variations in HER performance due to Pt deposition only become apparent in neutral electrolytes after several hundred cycles, [ 52 ] i.e., timescales much longer than those over which the LSVs were conducted (typically 3 min), and leads to improvements in HER that are far lower than those observed in the present work with the SRBW forcing.…”

Section: Resultsmentioning

confidence: 52%

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Acoustically‐Induced Water Frustration for Enhanced Hydrogen Evolution Reaction in Neutral Electrolytes

Ehrnst

Sherrell

Rezk

et al. 2022

Advanced Energy Materials

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Despite its appeal of green H 2 production using energy from renewable sources, water electrolysis currently only accounts for a small percentage of global H 2 production due to the need for expensive electrocatalysts to compensate for Ohmic losses associated with the kinetic overpotential of the system. [4][5][6] At present, H 2 production via electrolysis is predominantly carried out in strong acidic/alkaline electrolytes using state-of-the-art platinum group metal (PGM) electrocatalysts, which enables hydrogen evolution reactions (HER) to be conducted at the lowest onset potential, albeit at practically insurmountable industrial costs due to the metal's scarcity. [7,8] To attain industrially-relevant current densities (200-500 mA cm −2 ), an overpotential between 1.8 and 2.5 V is typically required. [9] At these levels though, acidic electrolytes-while providing an abundant source of protons (H + ) and hydronium (H 3 O + ) ions-produce acid fog under high temperatures that can corrode the electrolyzer and contaminate the product. [10] Alkaline electrolysis, on the other hand, is commonly plagued by unstable electrocatalysts and the need for expensive pH-tolerant membranes. [11][12][13] It is therefore desirable to carry out electrolysis in neutral or near-neutral electrolytes (pH 5-9) with non-PGM electrocatalysts. [14] The HER rate under these conditions is, nevertheless, significantly lower than those for electrolytes with extreme pH levels. In addition to diffusion limitations, this is due to the rapid consumption of H 3 O + , which creates a bottleneck that limits the extent of reaction until higher overpotentials are able to drive H 2 O reduction. [10,[15][16][17] Even with the best electrodes (i.e., PGMs), H 2 production is several orders of magnitude lower under neutral conditions, [7] such that the overpotential required to reach a current density of −4 mA cm −2 exceeds 0.25 V in a 0.1 M KClO 4 electrolyte compared to as little as 30 mV in 0.5 M H 2 SO 4 . [18,19] Similarly poor performance is obtained with the use of nickel-based electrocatalysts, which are generally favored for alkaline conditions, given their affinity for OH − adsorption. [20] To circumvent these limitations, novel electrocatalysts have been designed, in which the electrode is doped to tailor its catalytic sites for both H* and OH* adsorption to complement the electrolytic conditions, [21][22][23] or through the introduction of complex architectures that facilitate more favorable local pH environments, [24] although these strategies A novel strategy utilizing high-frequency (10 MHz) hybrid sound waves to dramatically enhance hydrogen evolution reactions (HER) in notoriously difficult neutral electrolytes by modifying their network coordination state is presented. Herein, the practical limitations associated with existing electrolyzer technology is addressed, including the need for highly corrosive electrolytes and expensive electrocatalysts, by redefining conceptually-poor hydrogen electrocatalysts in neutral electrolytes. The impro...

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Section: Resultscontrasting

confidence: 63%

Section: Resultsmentioning

confidence: 52%

Acoustically‐Induced Water Frustration for Enhanced Hydrogen Evolution Reaction in Neutral Electrolytes

Ehrnst

Sherrell

Rezk

et al. 2022

Advanced Energy Materials

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“…The 22%- YO configuration having the most localized O arrangements among all configurations exhibits a medium Ga–O interaction with an IpCOHP value of −2.44 eV. Importantly, the hydrogen adsorption free energies of 17%- Y , 17%- L , 17%- O , and 22%- YO are almost thermoneutral with Δ G H values of 0.13, 0.05, 0.02, and 0.06 eV, respectively, which are close or even superior to the performance of Pt (Δ G H = −0.09 eV), Pt/Co 3 O 4 (Δ G H = 0.07 eV), and grain-boundary-enriched Au (Δ G H = −0.03 eV), suiting to promote both hydrogen adsorption and desorption.…”

Section: Resultsmentioning

confidence: 99%

“…However, when more O atoms are available, it is reasonable to expect that more configurations with O arranged at adjacent positions (O-Ga-O) would be available. Controlling such more localized O arrangements of GaSe 1−x O x can fine-tune its ΔG H value, which Pt/Co 3 O 4 (ΔG H = 0.07 eV), 65 and grain-boundary-enriched Au (ΔG H = −0.03 eV), 66 suiting to promote both hydrogen adsorption and desorption. Bandgap Engineering.…”

Section: 33mentioning

confidence: 99%

Structure–Property Relationship of Oxygen-Doped Two-Dimensional Gallium Selenide for Hydrogen Evolution Reaction Revealed from Density Functional Theory

Demissie

Tang

Siu

2022

ACS Appl. Energy Mater.

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Two-dimensional (2D) gallium selenide (GaSe) is known for its inert surface and wide bandgap, limiting its application as a photocatalytic material for the hydrogen evolution reaction (HER). Partial substitution of Se with O atoms can improve its catalytic efficiency. This work discovered that the surface activity of the substitutional O-doped single-layer GaSe surfaces (GaSe1–x O x , for x ≤ 22%) and their bandgap sizes are dependent on the detailed atomic configuration of the dopants, as revealed from density functional theory. For GaSe1–x O x at low O contents, where all O atoms are favorably separated by at least one -Ga-Se-Ga- unit, the surface activity for the HER is insignificantly improved by increasing dopant concentration. By contrast, when more O dopants are available and arranged in adjacent positions (O-Ga-O), the hydrogen adsorption efficiency of GaSe1–x O x increases and their bandgaps are reduced with increasing dopant concentration. These important features are attributed to weakening of the Ga–O covalent interaction in these more localized dopant arrangements, which in turn strengthens the O–H bonds. This weakened Ga–O covalent bond also descends the conduction band minimum toward the Fermi level, resulting in bandgap reduction and thus favoring visible-light absorption. Optimal atomic configurations (all having localized O-dopant arrangements) have been identified, and they exhibit almost thermoneutral hydrogen adsorption free energy ΔG H and small bandgaps (2.09–2.21 eV), making them promising materials to perform an efficient HER. Fine-tuning the Ga–O interaction by applying tensile strength T S parallel to the 2D surface of up to 1% further reduces their bandgaps to 1.95–2.05 eV. Our theoretical predictions suggest that controlling the atomic configuration of dopants provides opportunities for engineering single-layered GaSe1–x O x materials with surface reactivity and bandgaps that suit photocatalytic water splitting.

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“…In this regard, great efforts have been devoted to developing single-atom Pt catalysts, which can not only maximize the metal utilization efficiencies but also potentially deliver high catalytic activities [17][18][19][20][21][22]. It is noted that HER in acidic media takes place with the initial adsorption of hydrogen ions (H + ) on the active sites, followed by the formation of H* intermediates and then the generation of H 2 [23][24][25][26]. However, the strong interactions between H + and the oxygen atoms of water molecules usually induce undesirable formation of hydronium ions with H + surrounded by water molecules, which would decrease the concentration of H + and thereby result in excessive overpotentials for acidic HER [27][28][29][30][31].…”

Section: Introductionmentioning

confidence: 99%

Atomically dispersed platinum supported onto nanoneedle-shaped protonated polyaniline for efficient hydrogen production in acidic water electrolysis

Bai

Lai

et al. 2023

Sci. China Mater.

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Developing high-performance single-atom platinum (Pt) catalysts for acidic hydrogen evolution reaction (HER) is of significance. However, their HER kinetics are limited due to the low concentration of hydrogen ions (H + ) near the Pt sites in acidic electrolytes, where hydronium ions are undesirably formed with H + surrounded by water molecules. Here, we seek to improve the HER kinetics by anchoring single-atom Pt catalyst on nanoneedle-shaped protonated polyaniline supports, which can not only capture H + from the hydronium ions but also facilitate the electroreduction of H + by promoting the electron accumulation. As a result, the turnover frequency of single-atom Pt supported on the nanoneedle-shaped protonated polyaniline is appreciably enhanced, compared with that of the single-atom Pt supported on the flat-shaped protonated polyaniline. By combining the X-ray photoelectron spectroscopy, finite-element simulation and electrochemical studies, we find that the enhanced HER activity of single-atom Pt on nanoneedle-shaped protonated polyaniline support may arise from a hydrogen spillover pathway induced by the increased local concentration of H + near the Pt sites.

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Unveiling the Excellent Electrocatalytic Activity of Grain-Boundary Enriched Anisotropic Pure Gold Nanostructures toward Hydrogen Evolution Reaction: A Combined Approach of Experiment and Theory

Cited by 10 publications

References 83 publications

Acoustically‐Induced Water Frustration for Enhanced Hydrogen Evolution Reaction in Neutral Electrolytes

Acoustically‐Induced Water Frustration for Enhanced Hydrogen Evolution Reaction in Neutral Electrolytes

Structure–Property Relationship of Oxygen-Doped Two-Dimensional Gallium Selenide for Hydrogen Evolution Reaction Revealed from Density Functional Theory

Atomically dispersed platinum supported onto nanoneedle-shaped protonated polyaniline for efficient hydrogen production in acidic water electrolysis

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