Proton selective adsorption on Pt–Ni nano-thorn array electrodes for superior hydrogen evolution activity

Nairan, Adeela; Liang, Caiwu; Chiang, Sum Wai; Wu, Yi; Zou, Peichao; Khan, Usman; Li, Wendong; Kang, Feiyu; Guo, Shaojun; Wu, Jianbo; Yang, Cheng

doi:10.1039/d1ee00106j

Cited by 82 publications

(66 citation statements)

References 25 publications

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“…The electric fields around the tips obviously increase as the cones sharpen from 4.5 to 1.5 nm ( Fig. 1D ), which is caused by the migration of free electrons to the tips of the charged Pd electrode due to the electrostatic repulsion ( 27 ). The impact of the enhanced local electric field on the distribution of ions around the surface is then estimated by the Gouy-Chapman-Stern model, which provides the mapping of the surface K + and OH − concentrations in the Helmholtz layer of the electrical double layer close to the surface of the Pd electrode.…”

Section: Resultsmentioning

confidence: 99%

“…In particular, sulfur modification has been proved to be an efficient route to improve the intrinsic activity and stability of Pd toward electrochemical HER and thermocatalytic organic hydrogenation reactions ( 22 – 24 ). In addition, high-curvature structures exhibit a high local electric field that increases the concentration of reactants or electrolytes around the tips, hence enhancing electrochemical CO 2 RR and HER performances ( 25 – 27 ). For example, Liu et al .…”

Section: Introductionmentioning

confidence: 99%

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Field-induced reagent concentration and sulfur adsorption enable efficient electrocatalytic semihydrogenation of alkynes

et al. 2022

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Efficient electrocatalytic alkyne semihydrogenation with potential/time-independent selectivity and Faradaic efficiency (FE) is vital for industrial alkene productions. Here, sulfur-tuned effects and field-induced reagent concentration are proposed to promote electrocatalytic alkyne semihydrogenation. Density functional theory calculations reveal that bulk sulfur anions intrinsically weaken alkene adsorption, and surface thiolates lower the activation energy of water and the Gibbs free energy for H* formation. The finite element method shows high-curvature structured catalyst concentrates K + by enhancing electric field at the tips, accelerating more H* formation from water electrolysis via sulfur anion–hydrated cation networks, and promoting alkyne transformations. So, self-supported Pd nanotips with sulfur modifiers are developed for electrochemical alkyne semihydrogenation with up to 97% conversion yield, 96% selectivity, 75% FE, and a reaction rate of 465.6 mmol m −2 hour −1 . Wide potential window and time irrelevance for high alkene selectivity, good universality, and easy access to deuterated alkenes highlight the promising potential.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Field-induced reagent concentration and sulfur adsorption enable efficient electrocatalytic semihydrogenation of alkynes

et al. 2022

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“…[ 46 ] The performance of CNT‐O@Pt is also higher than that of Pt‐based catalysts reported recently (Figure 5d and Table S6, Supporting Information). [ 47–62 ] The Tafel slope of CNT‐O@Pt was calculated to be 49 mV dec −1 , which is smaller than that of CNT@Pt (68 mV dec −1 ), indicating a faster kinetic property (Figure S27, Supporting Information). Furthermore, the active site utilization of CNT‐O@Pt and controlled samples were quantitatively characterized by an CV method (Figure 5e).…”

Section: Resultsmentioning

confidence: 99%

Flame‐Assisted Synthesis of O‐Coordinated Single‐Atom Catalysts for Efficient Electrocatalytic Oxygen Reduction and Hydrogen Evolution Reaction

Xie

et al. 2021

Small Methods

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Single‐atom catalysts (SACs) exhibit intriguing performance in electrocatalysis owing to their maximized atom utilizations and unique electronic structures, but effective anchoring metal atoms with defined coordination structure on hierarchical integrated electrode remain a challenge. Herein, a fast and facial flame‐assisted strategy is developed to construct oxygen‐coordinated SACs on integrated carbon nanotube (CNT) arrays with promising applications in electrocatalysis. Density functional theory calculations show that oxygen in carbon substrate imparts homogeneous sites for the efficient anchoring of metal atoms, thereby enabling SACs to disperse uniformly and firmly and thus bringing optimized activities. Moreover, the integrated CNT array with abundant oxygen‐containing groups is constructed and has been used as an efficient matrix for anchoring metal atoms (CNT‐O@M) via a flame‐assisted method. The as‐prepared CNT‐O@M (M = Co and Pt as typical examples) shows excellent activities in electrocatalytic oxygen reduction reaction and hydrogen evolution reaction with utilization of active site as high as 75.7%, which is superior to the reported SACs. Particularly, the performance of CNT‐O@M can maintain stably under various harsh conditions, showing a promising prospect in the long‐time applications. The methodology and concept proposed in this work could be extended to the synthesis of a variety of integrated SACs for efficient electrocatalysis.

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“…For the first time, Adeela Nairan et al reported a unique self-limiting magneticfield-driven growth technology to prepare PtNi nanospine arrays with high curvature. [45] By affecting a concentrated local electric field, PtNi nanostructure with high curvature promotes the selective accumulation of H + around the cathode surface, realizing a "pseudo-acid" local environment. In electrocatalytic HER test, a very low overpotential of 71 mV was achieved at a current density of 200 mA cm À 2 .…”

Section: Materials With Curled Surfacementioning

confidence: 99%

The Role of Surface Curvature in Electrocatalysts

Wang

Bao

Shi

et al. 2021

Chemistry A European J

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Excessive consumption of fossil fuels has caused unavoidable environmental problems. The development of renewable and clean alternatives is essential for the sustainable and green development of human society. Electrocatalysts are most important parts in these energy-related devices. Recently, scientists found that the surface curvature of electrocatalysts could play an important role for the improvement of catalytic performance and the optimization of intrinsic catalytic activity during electrocatalytic process. The role of surface curvature in electrocatalysts is still under investigating. In this minireview, we summarized the latest progress of electrocatalysts with different surface curvatures and their applications in energy-related applications. This review mainly involves the strategies for preparation of electrocatalysts with different surface curvatures, three typical electrocatalysts with different surface curvatures (curled surface, onion-like structure, and spiral structure), and the potential mechanisms that surface curvature in electrocatalysts affects activities.

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Proton selective adsorption on Pt–Ni nano-thorn array electrodes for superior hydrogen evolution activity

Abstract: Conventional acidic water electrolysis for large-scale hydrogen production needs to involve noble metal catalyst for anode to resist electrochemical oxidation; while alkaline electrolysis can provide better anode protection, but hydrogen...

Cited by 82 publications

References 25 publications

Field-induced reagent concentration and sulfur adsorption enable efficient electrocatalytic semihydrogenation of alkynes

Field-induced reagent concentration and sulfur adsorption enable efficient electrocatalytic semihydrogenation of alkynes

Flame‐Assisted Synthesis of O‐Coordinated Single‐Atom Catalysts for Efficient Electrocatalytic Oxygen Reduction and Hydrogen Evolution Reaction

The Role of Surface Curvature in Electrocatalysts

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