Engineering High‐Energy Interfacial Structures for High‐Performance Oxygen‐Involving Electrocatalysis

Guo, Chunxian; Zheng, Yao; Ran, Jingrun; Xie, Fangxi; Jaroniec, Mietek; Qiao, Shi Zhang

doi:10.1002/ange.201701531

Cited by 53 publications

(30 citation statements)

References 34 publications

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“…The Co/ Fe 2p 3/2 peaks of Co/Fe-Se and Co/Fe-O in CoSe 2 -D Fe -V Se exhibit negative shifts to lower binding energies, and those in CoSe 2 -D Fe -V Co show positive shifts to higher binding energies, indicating the reduction and oxidation states of metal sites caused by Se/O and Co vacancies, respectively (Fig. 3c) 31 . The defect structures after CA test at η = 370 mV for 1.5 h were then investigated via electron energy loss spectroscopy (EELS).…”

Section: Resultsmentioning

confidence: 95%

Approaching the activity limit of CoSe2 for oxygen evolution via Fe doping and Co vacancy

et al. 2020

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Electronic structure engineering lies at the heart of efficient catalyst design. Most previous studies, however, utilize only one technique to modulate the electronic structure, and therefore optimal electronic states are hard to be achieved. In this work, we incorporate both Fe dopants and Co vacancies into atomically thin CoSe 2 nanobelts for /coxygen evolution catalysis, and the resulted CoSe 2-D Fe-V Co exhibits much higher catalytic activity than other defect-activated CoSe 2 and previously reported FeCo compounds. Deep characterizations and theoretical calculations identify the most active center of Co 2 site that is adjacent to the V Co-nearest surface Fe site. Fe doping and Co vacancy synergistically tune the electronic states of Co 2 to a near-optimal value, resulting in greatly decreased binding energy of OH* (ΔE OH) without changing ΔE O , and consequently lowering the catalytic overpotential. The proper combination of multiple defect structures is promising to unlock the catalytic power of different catalysts for various electrochemical reactions.

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Section: Resultsmentioning

confidence: 95%

Approaching the activity limit of CoSe2 for oxygen evolution via Fe doping and Co vacancy

et al. 2020

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“…However, they usually suffer issues of high cost, scarcity, and poor stability [8][9][10][11] . On the other hand, ruthenium or iridium oxides (RuO 2 or IrO 2 ) exhibit excellent OER catalytic behavior but relatively poor ORR activity 12,13 . Therefore, it is still a great challenge to prepare low-cost, resource-rich, and robust bifunctional oxygen electrocatalysts with both high OER and ORR catalytic activity for applications in highly efficient regenerative FCs and metal-air batteries to promote their practical applications.…”

Section: Introductionmentioning

confidence: 99%

Monodisperse Co9S8 nanoparticles in situ embedded within N, S-codoped honeycomb-structured porous carbon for bifunctional oxygen electrocatalyst in a rechargeable Zn–air battery

Cao

et al. 2018

NPG Asia Mater

104

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The exploitation of cost-effective, highly active, and robust non-precious metal bifunctional oxygen electrocatalysts for both the oxygen reduction reaction (ORR) and oxygen revolution reaction (OER) is the key to promoting the application of regenerative fuel cells and metal-air batteries. Co 9 S 8 is considered a promising non-precious metal bifunctional oxygen electrocatalyst. However, the electrocatalytic performance of cobalt sulfide-based nanocatalysts is still far from satisfactory because of their poor conductivity, insufficient exposed active sites, and aggregation-prone during continuous work. Herein, based on the inspiration from honeycombs in nature, we synthesized Co 9 S 8 /N, Scodoped honeycomb-structured porous carbon (Co 9 S 8 /NSC) in situ composites via a simple method. Benefiting from the unique honeycomb composite structure composed of monodisperse Co 9 S 8 nanoparticles in situ embedded within the three-dimensional interconnected network carbon matrix with high conductivity, which facilitates not only the electron transport and charge transfer across the interface but also the exposure of active sites and rapid transport of ORR/OER-related species, the obtained Co 9 S 8 /NSC in situ composites exhibit high stability and activity in both the ORR in terms of more a positive half-wave potential (0.88 V vs. RHE) than that (0.86 V vs. RHE) of commercial 20% Pt/C and the OER in terms of a small overpotential (0.41 V vs. RHE) approaching that of commercial IrO 2 (0.39 V vs. RHE) in alkaline electrolytes at 10 mA cm −2 . Thus, as expected, the assembled rechargeable Zn-air batteries based on the bifunctional electrocatalysts exhibit a small discharge/charge overpotential (0.96 V) with a high voltaic efficiency of 55.1% at 10 mA cm −2 and a long-term cycling stability of over 4000 min.

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“…eveloping efficient electrochemical conversion processes is of great significance for storing and utilizing renewable energy 1 . Electrochemical oxygen evolution reaction (OER) plays an essential role in many energy conversion technologies involving metal-air batteries, water splitting, and CO 2 reduction [2][3][4][5] . Unfortunately, the efficiency of OER was limited by its sluggish kinetics and high over-potential.…”

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confidence: 99%

Missing-linker metal-organic frameworks for oxygen evolution reaction

Xue¹,

et al. 2019

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Metal-organic frameworks (MOFs) have been recognized as compelling platforms for the development of miscellaneous applications because of their structural diversity and functional tunability. Here, we propose that the electrocatalytic properties could be well modified by incorporating missing linkers into the MOF. Theoretical calculations suggest the electronic structure of MOFs can be tuned by introducing missing linkers, which improves oxygen evolution reaction (OER) performance of the MOF. Inspired by these aspects, we introduced various missing linkers into a layered-pillared MOF Co2(OH)2(C8H4O4) (termed as CoBDC) to prepare missing-linker MOFs. Transmission electron microscope and synchrotron X-ray measurements confirmed that the missing linkers in the MOF could be introduced and well controlled by our strategy. The self-supported MOF nanoarrays with missing linkers of carboxyferrocene exhibit excellent OER performance with ultralow overpotential of 241 mV at 100 mA cm−2. This work opens a new prospect to develop efficient MOF-based electrocatalysts by introducing missing linkers.

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Engineering High‐Energy Interfacial Structures for High‐Performance Oxygen‐Involving Electrocatalysis

Abstract: Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: http://dx.

Cited by 53 publications

References 34 publications

Approaching the activity limit of CoSe2 for oxygen evolution via Fe doping and Co vacancy

Approaching the activity limit of CoSe2 for oxygen evolution via Fe doping and Co vacancy

Monodisperse Co9S8 nanoparticles in situ embedded within N, S-codoped honeycomb-structured porous carbon for bifunctional oxygen electrocatalyst in a rechargeable Zn–air battery

Missing-linker metal-organic frameworks for oxygen evolution reaction

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