Boosting alkaline hydrogen evolution: the dominating role of interior modification in surface electrocatalysis

Li, Zhao; Niu, Wenhan; Yang, Zhenzhong; Kara, Abdelkader; Wang, Qi; Wang, Maoyu; Gu, Meng; Feng, Zhenxing; Du, Yingge; Yang, Yang

doi:10.1039/d0ee01750g

Cited by 94 publications

(58 citation statements)

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“…Thus, such a significant HER activity improvement of Pt 2 Ir 1 /CoP (Supplementary Fig. 12 ) might be explained by three possible pathways: 22 , 59 – 61 (a) Pt 2 Ir 1 itself delivers the dominant HER contributions owing to the alloying effects; (b) CoP itself exhibits the main HER contributions owing to the electronic metal-support interaction; (c) hydrogen spillover shows the leading HER contributions owing to the integration of the beneficial proton adsorption on the alloyed PtIr and the easy hydrogen desorption on CoP.…”

Section: Resultsmentioning

confidence: 99%

A fundamental viewpoint on the hydrogen spillover phenomenon of electrocatalytic hydrogen evolution

et al. 2021

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Hydrogen spillover phenomenon of metal-supported electrocatalysts can significantly impact their activity in hydrogen evolution reaction (HER). However, design of active electrocatalysts faces grand challenges due to the insufficient understandings on how to overcome this thermodynamically and kinetically adverse process. Here we theoretically profile that the interfacial charge accumulation induces by the large work function difference between metal and support (∆Φ) and sequentially strong interfacial proton adsorption construct a high energy barrier for hydrogen transfer. Theoretical simulations and control experiments rationalize that small ∆Φ induces interfacial charge dilution and relocation, thereby weakening interfacial proton adsorption and enabling efficient hydrogen spillover for HER. Experimentally, a series of Pt alloys-CoP catalysts with tailorable ∆Φ show a strong ∆Φ-dependent HER activity, in which PtIr/CoP with the smallest ∆Φ = 0.02 eV delivers the best HER performance. These findings have conclusively identified ∆Φ as the criterion in guiding the design of hydrogen spillover-based binary HER electrocatalysts.

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Section: Resultsmentioning

confidence: 99%

A fundamental viewpoint on the hydrogen spillover phenomenon of electrocatalytic hydrogen evolution

et al. 2021

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“…Yet, despite substantial progress in the alkaline media, it remains challenging to achieve a viable activity in acid, as compared to Pt/C. The other is to reduce the amount of Pt used and hence to diminish the catalyst cost but without compromising the electrocatalytic performance [ 10 – 14 ]. One intuitive strategy is to reduce the size of Pt NPs by taking advantage of the increasing surface-to-volume ratio and hence enhanced utilization of the Pt atoms.…”

Section: Introductionmentioning

confidence: 99%

Oxygen Reduction Reaction Catalyzed by Carbon-Supported Platinum Few-Atom Clusters: Significant Enhancement by Doping of Atomic Cobalt

Nichols

Mercado

et al. 2020

Research

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Oxygen reduction reaction (ORR) plays an important role in dictating the performance of various electrochemical energy technologies. As platinum nanoparticles have served as the catalysts of choice towards ORR, minimizing the cost of the catalysts by diminishing the platinum nanoparticle size has become a critical route to advancing the technological development. Herein, first-principle calculations show that carbon-supported Pt9 clusters represent the threshold domain size, and the ORR activity can be significantly improved by doping of adjacent cobalt atoms. This is confirmed experimentally, where platinum and cobalt are dispersed in nitrogen-doped carbon nanowires in varied forms, single atoms, few-atom clusters, and nanoparticles, depending on the initial feeds. The sample consisting primarily of Pt2~7 clusters doped with atomic Co species exhibits the best mass activity among the series, with a current density of 4.16 A mgPt−1 at +0.85 V vs. RHE that is almost 50 times higher than that of commercial Pt/C.

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“…Combining above‐characterized results and electrocatalytic OER and HER activities of series of samples ST‐150–400, it is thus considered that the excellent electrocatalytic OER and HER property of as‐prepared sample at a proper calcining temperature should give the credit to the co‐existence of Ni and NiO and a special hierarchical fiber‐like morphology, which is also verified by others. [ 27 ]…”

Section: Resultsmentioning

confidence: 99%

“…Combining above-characterized results and electrocatalytic OER and HER activities of series of samples ST-150-400, it is thus considered that the excellent electrocatalytic OER and HER property of as-prepared sample at a proper calcining temperature should give the credit to the co-existence of Ni and NiO and a special hierarchical fiber-like morphology, which is also verified by others. [27] Subsequently, samples SM-0.00-2.00 were used to further investigate the effect of CF amount on electrocatalytic performance of as-prepared samples. Their corresponding electrocatalytic OER and HER behaviors are shown in Figure 8.…”

Section: Electrocatalytic Performancementioning

confidence: 99%

Biomass‐Templated Preparation of Hierarchically Multi‐Functional Ni/NiO@C Hollow‐Fibers

Wang

Luo

et al. 2020

Part & Part Syst Charact

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core-shelled Ni/NiO nanowires via an N 2 H 4 ⋅H 2 O reduction method for microstructure and magnetic property investigations. [17] In addition, some carbon modified NiO/Ni materials were also prepared. [8-11,19,20] Chinnappan et al. synthesized C@NiO/Ni nanofibers via an electrospinning method for hydrogen evolution reaction. [11] Lv et al. prepared a series of MOF-derived NiO/Ni@C magnetic composites with chestnut shelllike hollow sphere structure for arsenic removal. [15] Nevertheless, it can be found that many methods are complicated, highcost, harm to the environment, thereby limiting their large-scale production and application. Currently, biomass template-assisted method has attracted extensive attention of researchers because it endows materials with diverse morphologies and improved performances. There are many biomass templates used, such as eggshell membrane, [12] ginkgo leaves, [22] chicken feathers, [23] cotton fibers, [24] pomelo-orange peels, [25,26] etc. Among them, cotton fiber (CF) consisting of cellulose and hemicellulose and pectin, contains abundant polar/active groups including-OH,-NH, and-C-O/N-C (seen in Figure S1, Supporting Information), making it well H 2 O-wet, swell, easily removed under air atmosphere. Thus, it is used as a vital template to give as-obtained material fibrous morphology and improved property. Herein, two series of hollow fibered Ni/NiO@C composites were successfully fabricated via a novel template-assisted dipping/adsorbing and calcining method by using CF as a multifunctional template and Ni(NO 3) 2 •6H 2 O as Ni source without any other additives, such as reducer, alkali agents, and extra carbon (C) source (Figure 1). During the preparation process, Ni 2+ ions were firstly adsorbed on the surface of wetting and swelling CFs to produce the precursors (Ni 2+ /CF), and then the precursors were calcined under an air condition to obtain target Ni/NiO@C material. It is worth pointing out that the asprepared materials show good magnetic, adsorptive, and electrolysis properties. 2. Results and Discussion 2.1. SEM and TEM Analyses Considering ST-200 sample delivered the best magnetic, adsorptive, and electrocatalytic properties, we thus take it as a Two series of hierarchically Ni/NiO@C hollow-fibers with magnetic, adsorptive, and electrocatalytic oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) properties are successfully prepared via a facile and green cotton fiber (CF)-templated dipping/adsorbing-calcining strategy. The effect of calcination temperature and CF amount on morphologies, components, and properties of the as-prepared materials is investigated. The results demonstrate that a proper CF template can endow the as-obtained materials with hierarchically hollow-fiber morphology and multi-components (Ni 0 , NiO, and C) at a certain calcination temperature, therefore providing excellent magnetic, adsorptive, and electrocatalytic OER and HER properties. Specifically, the unique hierarchical morphology and synergistic effect between Ni 0 and NiO remar...

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Boosting alkaline hydrogen evolution: the dominating role of interior modification in surface electrocatalysis

Abstract: Alkaline hydrogen evolution reaction (A-HER) holds great promise for clean hydrogen fuel generation but its practical utilization is severely hindered by the sluggish kinetics for water dissociation in alkaline solutions....

Cited by 94 publications

References 50 publications

A fundamental viewpoint on the hydrogen spillover phenomenon of electrocatalytic hydrogen evolution

A fundamental viewpoint on the hydrogen spillover phenomenon of electrocatalytic hydrogen evolution

Oxygen Reduction Reaction Catalyzed by Carbon-Supported Platinum Few-Atom Clusters: Significant Enhancement by Doping of Atomic Cobalt

Biomass‐Templated Preparation of Hierarchically Multi‐Functional Ni/NiO@C Hollow‐Fibers

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