Harnessing the interplay of Fe–Ni atom pairs embedded in nitrogen-doped carbon for bifunctional oxygen electrocatalysis

Zhu, Xiaofeng; Zhang, Detao; Chen, Chih‐Jung; Zhang, Qingran; Liu, Ru‐Shi; Xia, Zhaoqiang; Dai, Liming; Amal, Rose; Lu, Xunyu

doi:10.1016/j.nanoen.2020.104597

Cited by 259 publications

(195 citation statements)

References 49 publications

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“…[4] In addition, the presence of dual TM-N x species will also facilitate the ORR process synergistically via an optimized adsorption/desorption process, as reported previously. [27,28,29] As a consequence, the obtained SA-CoCu@Cu/CoNP catalyst exhibits a remarkable ORR activity as well as long-term durability in alkaline media (0.1 m KOH with a pH value of 13), showing the onset potenital of 0.98 V and the half-wave potential of 0.88 V (vs reversible hydrogen electrode), which are even superior to the commercially available Pt/C catalyst (20 wt% of Pt, purchased from Sigma Aldrich). The excellent ORR activity is mainly ascribed to the presence of electron-rich CoN x sites, which result in an optimized binding energy that benefits the adsorption/desorption of the reaction intermediates.…”

Section: Introductionmentioning

confidence: 99%

Electronically Modified Atomic Sites Within a Multicomponent Co/Cu Composite for Efficient Oxygen Electroreduction

Zhang

Kumar

Zhu

et al. 2021

Advanced Energy Materials

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Moreover, the stability issues of Pt-based catalysts (e.g., the crystallite dissolution and nanoparticle agglomeration) have also jeopardized the reliability of power systems including ORR as a half reaction. [7,8] In these regards, there is a general call for the replacement of the Pt-based composites with cost-effective, durable and highly active ORR catalysts.During the past few years, nitrogencoordinated transition metal species (TM-N x ) that are embedded within a carbon matrix have emerged as a class of promising catalysts for ORR, owing to their high activity, maximum utilization of the metal species and distinct configurations of active sites. Among them, the Fe-N-C catalysts demonstrate an exceptional ORR catalytic activity that is even comparable to the Pt/C benchmark. [9,10] Nevertheless, the usual insufficient durability of the Fe-N x species under long-term ORR operation has severely impeded their potential for commercial perspectives. [11] Although the actual degradation mechanism of Fe-N x centers is still under debate, it is clear that the reactive oxygen species (ROS) generated during the "electro-Fenton" process in the presence of Fe species and hydrogen peroxide tend to cause corrosion or oxidation of carbon that leads to the cleavage of Fe-N bond and the eventual decay of activity. [12,13] By contrast, CoN x -containing materials would have less deleterious effects in this regard and appear to be promising alternatives to the Fe-N-C catalysts in various applications, [14] as reported recently. [15,16] Nonetheless, despite significant progress in preparation methods, [17,18] it is still extremely challenging for CoN x -containing catalysts to be applied in large scale due to i) their insufficient activity compared with the Pt-based catalysts; [14,19] and ii) the relatively high percentage of H 2 O 2 produced during ORR that results in a lower energy efficiency and possible catalyst corrosion. [4,20,21,22] Thus, it is necessary to develop a strategy to enhance the catalytic ORR performance of the Co-N-based composites meanwhile suppress the H 2 O 2 production on them. [23] Herein, Cu species are introduced to mitigate the activity and high H 2 O 2 selectivity issues of Co-N based composites. For the first time, the different roles of CuN x and CoN x moieties in ORR have been investigated within a multicomponent Co/ Cu catalyst, both experimentally and theoretically. Atomically dispersed CuN x sites are proposed to be effective in reducing Rational design of cost-effective and active electrocatalysts is an essential step toward the large-scale realization of hydrogen fuel cells and metal-air batteries. Its success requires a drastic improvement in the kinetics of the cathodic oxygen reduction reaction (ORR). Herein, a novel ORR catalyst formed by encapsulating thin Cu layer decorated Co nanoparticles inside graphitic carbon layers that are embedded with abundant CoN x and CuN x atomic sites (denoted as SA-CoCu@Cu/CoNP), is reported. The multicomponent SA-CoCu@Cu/CoNP composite exhibits a r...

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Section: Introductionmentioning

confidence: 99%

Electronically Modified Atomic Sites Within a Multicomponent Co/Cu Composite for Efficient Oxygen Electroreduction

Zhang

Kumar

Zhu

et al. 2021

Advanced Energy Materials

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“…The charge distribution between the Fe–Ni atom pairs can mutually tune the electronic structure of both Fe and Ni sites, modifying the binding energy of the oxygen‐containing intermediates and facilitating OER and ORR kinetics. [ 145,146 ]…”

Section: Electrochemical Applications Of Macsmentioning

confidence: 99%

Multiatom Catalysts for Energy‐Related Electrocatalysis

Peng

Feng

Yan

et al. 2020

Advanced Sustainable Systems

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Multiatom catalysts (MACs) with isolated monodisperse active sites comprising two to tens of metal atoms have attracted intensive research attention and industrial interest. With the combination of high atom utilization and well‐defined molecule‐like electronic structure, MACs show great potential for applications in a wide range of electrochemical catalytic reactions. This review aims to discuss the recent progress of MACs in energy‐related electrocatalysis. Critical issues, including the synthesis and characterization of the MACs, will be showcased. Moreover, recent advances are highlighted in the design and synthesis of MACs with a well‐controlled structure and composition to achieve enhanced catalytic performance in energy‐related electrocatalysis. Current challenges and future prospects for MACs are also presented to shed light on the rational design of MACs as potential industrialized catalysts in the future.

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“…This would modulate the adsorption energy of reaction intermediates, which enhances the catalytic efficiency and thereby the battery performance (Figure 6B,C). Further example, the formed bond between the atomic Fe and Ni allows the charge redistribution among the metallic centers 132 . Indeed, this charge redistribution imposes a mutual enhancement on both Fe and Ni, which accounts for the improved ORR and OER activity, respectively.…”

Section: Tm/carbon Hybrids For Oxygen Electrocatalystsmentioning

confidence: 99%

Transition metal/carbon hybrids for oxygen electrocatalysis in rechargeable zinc‐air batteries

Douka

Yang

Huang

et al. 2020

EcoMat

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Zinc‐air batteries (ZABs) could be an ideal candidate for challenging energy conversion and storage technology. Usually, the crucial oxygen reduction reaction and oxygen evolution reaction are naturally lethargic and require efficient catalysts to kinetically boost the energy conversion processes to achieve the practicable ZABs application. Transition‐metal/carbon hybrid catalysts show excellent potentials in electrocatalysis, and they have been developed into cost‐effective and scalable oxygen electrocatalyst alternatives for expensive and scarcer noble metal ones in rechargeable ZABs. Herein we summarize recent achievements in transition metal/carbon hybrids for oxygen electrocatalysis. These catalysts mainly fall into two categories by the integrated metal/metal oxides nanoparticles and atomically dispersed transition metal/carbon matrix. We focus on the relationship between structure and performance with their synthesis strategies. Their application in rechargeable ZABs are also comprehensively discussed. Finally, the perspectives on transition metal/carbon hybrids for oxygen electrocatalysis are presented for the future challenges in rechargeable ZABs.

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Harnessing the interplay of Fe–Ni atom pairs embedded in nitrogen-doped carbon for bifunctional oxygen electrocatalysis

Cited by 259 publications

References 49 publications

Electronically Modified Atomic Sites Within a Multicomponent Co/Cu Composite for Efficient Oxygen Electroreduction

Electronically Modified Atomic Sites Within a Multicomponent Co/Cu Composite for Efficient Oxygen Electroreduction

Multiatom Catalysts for Energy‐Related Electrocatalysis

Transition metal/carbon hybrids for oxygen electrocatalysis in rechargeable zinc‐air batteries

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