Gradient‐Concentration Design of Stable Core–Shell Nanostructure for Acidic Oxygen Reduction Electrocatalysis

Lyu, Xiao; Jia, Yi; Mao, Xin; Li, Daohao; Li, Gen; Zhuang, Linzhou; Wang, Xin; Yang, Dongjiang; Wang, Qiang; Du, Aijun; Yao, Xiangdong

doi:10.1002/adma.202003493

Cited by 94 publications

(63 citation statements)

References 43 publications

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“…Non-Noble Metals (Fe, Ni, Cu, Sn): Fe (Downshift of ε d ): Construction of holes on the carbon substrate induces the favorable manipulation of the electronic structures of the Fe-N 4 sites for the Fe-N-G-p electrocatalyst, as reported by Li et al [190] The unique configurations of the Fe-N-G-p electrocatalyst cause the downshift of the d-band center, which weakens the bonding strength between the * CO intermediates and the active sites (Figure 18a). DFT-based calculations Pt 75 Co 25 /C(500) None 2.06@0.9 V versus RHE 0.97@0.9 V versus RHE 0.1 m HClO 4 Pt Downshift [180] PtML IrNi/C None ≈0.6@0.9 V versus RHE ≈1.35@0.9 V versus RHE 0.1 m HClO 4 Pt Downshift [181] PtNiRu-IL/C None 2.26@0.9 V versus RHE 1.31@0.9 V versus RHE 0.1 m HClO 4 Pt Downshift [182] Pt/BC None 7.1@0.9 V versus RHE 0.209@0.9 V versus RHE 0.1 m HClO 4 Pt [111] PtCu/C 0.942 0.42@0.9 V versus RHE 1.2@0.9 V versus RHE 0.1 m HClO 4 Pt Upshift [183] PtNi-BNCs/C None 5.16@0.9 V versus RHE 3.52@0.9 V versus RHE 0.1 m HClO 4 Pt Downshift [169] TePtCo 0.924 1.15@0.9 V versus RHE 0.7@0.9 V versus RHE 0.1 m HClO 4 Pt Downshift [184] Pt/22L-Ti 3 C 2 None 0.1@0.9 V versus RHE 0.04@0.9 V versus RHE 0.1 m HClO 4 Pt Downshift [107] Pt-Ni@PtD/G 0.829 0.098@0.9 V versus RHE 0.061@0.9 V versus RHE 0.1 m HClO 4 Pt Ni Upshift [89] reveal the facile desorption of the * CO from the catalyst surface, which offers more fresh sites for the generation of CO, and thus accelerates the reaction kinetics. The electrocatalytic performance for the Fe-N-G-p indicates a high FE of 94% with a CO partial current density of 4.5 mA cm -2 at the potential of −0.58 V versus RHE and a high TOF value of 1630 h -1 (Figure 18b).…”

Section: Ag (Upshift Of ε D )mentioning

confidence: 99%

Descriptors for the Evaluation of Electrocatalytic Reactions: d‐Band Theory and Beyond

Jiao

Huang

2021

Adv Funct Materials

272

136

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Closing the carbon-, hydrogen-, and nitrogen cycle with renewable electricity holds promises for the mitigation of the facing environment and energy crisis, along with the continuing prosperity of the human society. Descriptors bridge the gap between the physicochemical factors of electrocatalysts and their boosted activity and serve as guiding principles during the rational design of electrocatalysts. The optimal adsorption strength of key intermediates is potentially accessed under the tendentious guidelines proposed by indicators, such as d-band center, ΔG H , E O* , coordination number (CN), bond length, etc. Here, in this review, a comprehensive summary of the recent advances achieved regarding the descriptors during the rational design of electrocatalysts that aims for the recycling of C/H/N-containing chemicals is offered. The review is initiated by providing the necessity of the development of efficient electrocatalysts and then the physics behind the d-band center is introduced. Then a summary of the recent progress relating to the development of electrocatalysts under the guidance of descriptors is reviewed. Following that, an extended discussion regarding the experimental or theoretical characterization of the d-band center and the descriptors beyond it is provided. Finally, perspectives and challenges in this area are offered.

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Section: Ag (Upshift Of ε D )mentioning

confidence: 99%

Descriptors for the Evaluation of Electrocatalytic Reactions: d‐Band Theory and Beyond

Jiao

Huang

2021

Adv Funct Materials

272

136

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“…[113] Lyu et al reported the gradient alloying of PtNi alloy with Pt-rich skin. [114] Then, the researchers applied acid leaching to partially dealloy the minor nickel atoms on the surface to generate defective Pt-rich skeleton shell. A surfactant-modified HNO 3 dealloying approach was also developed to obtain {111} and {100} facets and step/kink sites enriched nanoporous Au with the assistance of pyrogallol and sodium citrate, respectively.…”

Section: (De)alloyingmentioning

confidence: 99%

Multidimensional Nonstoichiometric Electrode Materials for Electrochemical Energy Conversion and Storage

Liu

Jinhan

et al. 2021

Advanced Energy Materials

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number of compounds deviate from definite composite. For example, Wüstite type FeO was found to occur in varied Fe/O ratios with Fe vacancies over a narrow limit in nature, [2,3] while stoichiometric form of FeO was obtained only under high pressure. [4] With the discovery of more chemical compounds with compositions deviating from their stoichiometric counterparts, a new family of materials, which is now recognized as nonstoichiometric material (NMs) or berthollides in honor of Berthollet, has drawn increasing research interest in materials chemistry.Structurally, nonstoichiometry can be induced from defect engineering, element doping, or substitution. [5,6] Although the resulting composition and elemental ratio are allowed to vary in a wide range, the phase and space group of nonstoichiometric compounds are generally identical to the parent stoichiometric counterparts. The type of nonstoichiometry is multidimensional, ranging from point defects (vacancy, substitution or interstitial), local defect (Frenkel pair or cation mixing), linear substitution (typically in layered compounds) to surface defect, bulk composition variation, and spatially dependent concentration gradient. [7] Thermodynamically, deviation from stoichiometry is always accompanied by the change in the system Gibbs free energy and/or redox of characteristic ions, which would endow the materials with multiple physicochemical features in modulating electronic structures, chemical valence, charge storage, carrier diffusion, and stability. [8][9][10][11] Since nonstoichiometry widely exists in many types of compounds including oxides, nitrides, carbides, sulfides, and alloys, it is desirable to develop deep understanding over the fundamental origin, related features, and their contributions to practical functionality.In the context of developing renewable energy conversion and storage, functional electrode materials are crucial to determine the electrochemical performance, stability, and cost. [11,12] In electrocatalysis, exploring highly active electrode materials for hydrogen evolution reaction (HER), oxygen reduction reaction (ORR), and oxygen evolution reaction (OER) is a key to boost the performance of water splitting, fuel cell, and metalair battery. [13][14][15] Meanwhile, electrochemical nitrogen reduction reaction (NRR) under ambient conditions provides a promising pathway of ammonia synthesis from N 2 and H 2 O alternative to the traditional contaminative Haber-Bosch process. [16] For batteries, the cell voltage, reversible capacity, and cycling Nonstoichiometry plays an important role in determining physicochemical properties such as conductivity, activity, and stability due to the compositioninduced change in phase, local atomic environment, and electronic structure. A variety of materials with nonstoichiometry have emerged in electrochemical energy conversion and storage, which necessitates a solid understanding of their formation mechanism and structure-function relationship. This review presents a summary of the progress made in this ...

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“…One of the important points that is limiting the use of bimetallic catalysts is the leaching of the alloying component, which results in the poisoning of the proton-exchange membrane and the degradation of the membrane electrode assembly (MEA) [7,8]. Therefore, one of the current research areas of the present paper is the catalyst's synthesis with nanoparticles of the following structures: core-shell [4,[9][10][11], gradients [12,13], hollow [14][15][16], porous frameworks [17,18], nanowires, and nanodendrites [19][20][21]. The key components of such catalysts are nanoparticles with a platinum shell, which protects the d-metal core from dissolution during the fuel cell operation.…”

Section: Introductionmentioning

confidence: 99%

Influence of Electrochemical Pretreatment Conditions of PtCu/C Alloy Electrocatalyst on Its Activity

et al. 2021

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A carbon supported PtCux/C catalyst, which demonstrates high activity in the oxygen electroreduction and methanol electrooxidation reactions in acidic media, has been obtained using a method of chemical reduction of Pt (IV) and Cu (2+) in the liquid phase. It has been found that the potential range of the preliminary voltammetric activation of the PtCux/C catalyst has a significant effect on the de-alloyed material activity in the oxygen electroreduction reaction (ORR). High-resolution transmission electron microscopy (HRTEM) demonstrates that there are differences in the structures of the as-prepared material and the materials activated in different potential ranges. In this case, there is practically no difference in the composition of the PtCux-y/C materials obtained after activation in different conditions. The main reason for the established effect, apparently, is the reorganized features of the bimetallic nanoparticles’ surface structure, which depend on the value of the limiting anodic potential in the activation process. The effect of the activation conditions on the catalyst’s activity in the methanol electrooxidation reaction is less pronounced.

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Gradient‐Concentration Design of Stable Core–Shell Nanostructure for Acidic Oxygen Reduction Electrocatalysis

Abstract: Article type: Communication Gradient-concentration design of stable core-shell nanostructure for acidic oxygen reduction electrocatalysis

Cited by 94 publications

References 43 publications

Descriptors for the Evaluation of Electrocatalytic Reactions: d‐Band Theory and Beyond

Descriptors for the Evaluation of Electrocatalytic Reactions: d‐Band Theory and Beyond

Multidimensional Nonstoichiometric Electrode Materials for Electrochemical Energy Conversion and Storage

Influence of Electrochemical Pretreatment Conditions of PtCu/C Alloy Electrocatalyst on Its Activity

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