Superior methanol electrooxidation performance of (110)-faceted nickel polyhedral nanocrystals

Li, Junshan; Zuo, Yong; Liu, Junfeng; Wang, Xiang; Yu, Xiaoting; Du, Ruifeng; Zhang, Ting; Infante‐Carrió, Maria F.; Tang, Pengyi; Arbiol, Jordi; Llorca, Jordi; Luo, Zhishan; Cabot, Andreu

doi:10.1039/c9ta07066d

Cited by 47 publications

(32 citation statements)

References 43 publications

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“…This proves that these two catalysts have the ability to catalyze the oxidation of ethanol. [31,32] Apparently, the NiO@C/CC has a very superior electrocatalytic activity compared to the Ni@C/CC, whether in 1.0 or 2.0 m ethanol ( Figure S6, Supporting Information). Furthermore, Figure 3c and Table S1, Supporting Information display an EOR peak current density of NiO@C/CC (119.1 mA cm −2 ) normalized to the mass of NiO (1985.0 mA mg −1 ) in 1.0 m KOH + 1.0 m ethanol, which is nearly 1.3 times higher than that of the Ni@C/CC (94.1 mA cm −2 ).…”

Section: Resultsmentioning

confidence: 99%

Air‐Assisted Transient Synthesis of Metastable Nickel Oxide Boosting Alkaline Fuel Oxidation Reaction

Liu

Zhou

Zhang

et al. 2020

Advanced Energy Materials

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Low molecular weight alcohols, such as ethanol, are clean, economical and sustainable energy sources which can be easily obtained, stored, and transported. [1] At present, the platinum-based noble metal catalysts are considered as highly efficient electrocatalysts for alkaline alcohols oxidation reactions. [4-6] Nevertheless, vulnerable CO poisoning effect, sluggish kinetics of anodic oxidation as well as high price of noble metal catalysts seriously hampered their development. Therefore, the research interests in developing high efficiency and low cost anodic electrocatalysts are activated to facilitate the largescale commercialization of fuel cell in the future. Non-noble metal materials which have made great progress to date are regarded as suitable and promising alternative electrocatalysts for alcohols electrooxidation. [7-9] Among them, nickel-based materials have been introduced as a kind of active electrocatalysts in the oxidation of methanol and other alcohols. [10-13] Despite considerable progress, the high onset potential and the inferior catalytic activity for alcohols electrooxidation severely hinder the further applications of nickelbased materials. In this case, it is necessary to design catalysts Construction of active and durable non-noble-metals based electrocatalysts is one of important requirements for the practical application and development of fuel cells, which are presently inhibited by relative sluggish charge transport and reaction kinetics. Herein, highly dispersed ultrathin carbon-coated nickel oxide nanoparticles settled on carbon cloth (NiO@C/CC) as efficient catalysts for alkaline fuels oxidation are synthesized via an air-assisted transient thermal shock strategy. This NiO@C/CC catalyst induces an outstanding catalytic activity (up to 119.1 mA cm −2) and durability (a little current decay during tests) in electrooxidation for ethanol, even for methanol and ethylene glycol, which outperforms most of the reported non-noble metal catalysts. The excellent catalytic performance of NiO@C/CC is essentially attributed to the oxygen vacancies, high concentration, high-valence-state Ni, and carbon layers of NiO@C NPs, which contribute to regulate the surface properties and electronic structure, enhance charge transfer, and provide abundant active sites, promoting adsorption capacity of reactant molecules on its surface. The facile and promising air-assisted transient thermal shock strategy can be extended to guide rational design and rapid synthesis of transition metal compounds as advanced catalysts for alkaline direct alcohol fuel cells.

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Section: Resultsmentioning

confidence: 99%

Air‐Assisted Transient Synthesis of Metastable Nickel Oxide Boosting Alkaline Fuel Oxidation Reaction

Liu

Zhou

Zhang

et al. 2020

Advanced Energy Materials

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“…Considering that the proton diffusion governs the Ni 2+ ↔Ni 3+ redox reaction process, its diffusion coefficient ( D ) was determined by the Randles‐Sevcik equation (see Figures S6ef and S7b and calculations) [34] . The proton diffusion coefficients obtained in Ni 3 C, up to 5.99×10 −9 cm 2 s −1 in 1.0 m KOH (Figure 2 c), were well above to the values measured for pure Ni NPs [14] . This value indicated the N 3 C structure to facilitate the Ni 2+ /Ni 3+ redox process at the basis of the high electrocatalytic activity of Ni‐based catalysts.…”

Section: Figurementioning

confidence: 51%

“…[34] The proton diffusion coefficients obtained in Ni 3 C, up to 5.99 10 À9 cm 2 s À1 in 1.0 m KOH (Figure 2 c), were well above to the values measured for pure Ni NPs. [14] This value indicated the N 3 C structure to facilitate the Ni 2+ /Ni 3+ redox process at the basis of the high electrocatalytic activity of Ni-based catalysts. The larger D value was ascribed to the lower onset potential, leaving larger potential window (the same applied potential below OER region) for MOR in 1.0 m KOH (Figure 2 a).…”

Section: Angewandte Chemiementioning

confidence: 94%

“…These changes occurred during the electrocatalytic process in critical alkaline media at high potential. [14,[38][39][40] Additionally, CP measurements showed that an additional potential of just 0.03 V, above the initial 0.55 V, were required to maintain a current density of 120 mA cm À2 for 50 000 s (Figure 3 d).…”

Section: Angewandte Chemiementioning

confidence: 99%

“…Among the several alternative materials proposed to replace noble metals as MOR catalysts, Ni offers the highest cost-effectiveness. A plethora of Ni [12][13][14] and Ni-based catalysts, including oxides/ hydroxides, [15][16][17] metal alloys, [18][19][20][21][22][23] phosphides, [24] chalcogenides, [25] and nitrides, [26] have been developed and tested toward MOR. Surprisingly, the nickel carbide, which a priori offers suitable properties as electrocatalysts, for example, stability, electrical conductivity and element abundance, has not been tested toward MOR.…”

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confidence: 99%

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Selective Methanol‐to‐Formate Electrocatalytic Conversion on Branched Nickel Carbide

Wei

Wang

et al. 2020

Angewandte Chemie

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A methanol economy will be favored by the availability of low‐cost catalysts able to selectively oxidize methanol to formate. This selective oxidation would allow extraction of the largest part of the fuel energy while concurrently producing a chemical with even higher commercial value than the fuel itself. Herein, we present a highly active methanol electrooxidation catalyst based on abundant elements and with an optimized structure to simultaneously maximize interaction with the electrolyte and mobility of charge carriers. In situ infrared spectroscopy combined with nuclear magnetic resonance spectroscopy showed that branched nickel carbide particles are the first catalyst determined to have nearly 100 % electrochemical conversion of methanol to formate without generating detectable CO2 as a byproduct. Electrochemical kinetics analysis revealed the optimized reaction conditions and the electrode delivered excellent activities. This work provides a straightforward and cost‐efficient way for the conversion of organic small molecules and the first direct evidence of a selective formate reaction pathway.

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Porous Pd‐PdO Nanotubes for Methanol Electrooxidation

Wang

Huang

et al. 2020

Adv Funct Materials

170

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Palladium (Pd) nanostructures are highly active non-platinum anodic electrocatalysts in alkaline direct methanol fuel cells (ADMFCs) and their electrocatalytic performance relies highly on their morphology and composition. Herein, a facile high-temperature pyrolysis method to synthesize high-quality Pd-palladium oxide (PdO) porous nanotubes (PNTs) by using Pd(II)-dimethylglyoxime complex (Pd(II)-DMG) nanorods as a selftemplate is reported. The chemical component of pyrolysis products highly correlates with pyrolysis temperature. The electrochemical measurements and density functional theory calculations show the existence of PdO enhances the electroactivity of metallic Pd for both methanol oxidation reaction (MOR) and carbon monoxide oxidation reaction in alkaline media. Benefiting from its one-dimensionally porous architecture and evident synergistic effect between PdO and Pd (e.g., electronic effect and bifunctional mechanism), Pd-PdO PNTs achieve a 3.7-fold mass activity enhancement and improved durability for MOR compared to commercial Pd nanocrystals. Considering the simple synthesis, excellent activity, and long-term stability, Pd-PdO PNTs may be highly promising anodic electrocatalysts in ADMFCs.optimal chemical component and structural advantage, Pd-PdO PNTs with optimal component revealed eminent electrocatalytic activity and durability for MOR in alkaline medium.

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Superior methanol electrooxidation performance of (110)-faceted nickel polyhedral nanocrystals

Abstract: Colloidal (110)-faceted nickel polyhedral nanocrystals present superior methanol electrooxidation performance in alkaline media.

Cited by 47 publications

References 43 publications

Air‐Assisted Transient Synthesis of Metastable Nickel Oxide Boosting Alkaline Fuel Oxidation Reaction

Air‐Assisted Transient Synthesis of Metastable Nickel Oxide Boosting Alkaline Fuel Oxidation Reaction

Selective Methanol‐to‐Formate Electrocatalytic Conversion on Branched Nickel Carbide

Porous Pd‐PdO Nanotubes for Methanol Electrooxidation

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