Modulation of Single Atomic Co and Fe Sites on Hollow Carbon Nanospheres as Oxygen Electrodes for Rechargeable Zn–Air Batteries

Jose, Vishal; Hu, Huimin; Edison, Eldho; Manalastas, William; Ren, Hao; Kidkhunthod, Pinit; Sreejith, Sivaramapanicker; Jayakumar, Anjali; Nsanzimana, Jean Marie Vianney; Srinivasan, Madhavi; Choi, Jin Ho; Lee, Jong‐Min

doi:10.1002/smtd.202000751

Cited by 204 publications

(108 citation statements)

References 64 publications

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Section: Introductionmentioning

confidence: 99%

“…[2] However, they are known to suffer from ineluctable concerns with regards to scarcity, extreme cost, poor stability in long term usage and poisoning effects from methanol crossover. [3,4] The potential of rechargeable metal-air batteries (metal = Zn, Li, Al, Mg, etc.) in future energy applications can be simply revealed from its high theoretical energy density values, in the range of 1086-11 140 Wh kg -1 .…”

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Highly Efficient Oxygen Reduction Reaction Activity of N‐Doped Carbon–Cobalt Boride Heterointerfaces

Jose

Nsanzimana

et al. 2021

Advanced Energy Materials

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with thermodynamic oxygen to water conversion potential of 1.23 V (vs reversible hydrogen electrode (RHE)). [1] Especially so in recent years, platinum (Pt)-based catalysts are widely utilized as the state of the art catalyst for ORR. [2] However, they are known to suffer from ineluctable concerns with regards to scarcity, extreme cost, poor stability in long term usage and poisoning effects from methanol crossover. [3,4] The potential of rechargeable metal-air batteries (metal = Zn, Li, Al, Mg, etc.) in future energy applications can be simply revealed from its high theoretical energy density values, in the range of 1086-11 140 Wh kg -1 . [5,6] Metal anodes, such as Zn, are earth abundant, cheap, safe for handling, and environmentally benign, favoring suitability of metal-air batteries for domestic and industrial applications. [7,8] Despite the intensive research being undertaken in the field of Zn-air batteries, major degradation issues remain with regards to the following: a) degradation of cathode materials-catalyst, carbon support and binders and b) morphological degradation of Zn anode during repeated cycles. [9] Thus, in order to realize and leverage on the full potential of metal air batteries, the primary task would be to develop highly efficient and stable air cathodes that favor oxygen chemistry, mainly the ORR.Earth abundant metal-based catalysts, like metal oxides, [10] perovskites, [11] spinel type, [12] MXenes , [13,14] and mixed metal oxides [15,16] have been investigated as ORR catalysts. In addition, heteroatom-doped carbon structures containing metallic elements, like cobalt, nickel, and iron, have emerged as promising candidates to replace Pt. Despite intensive research in metal pnictogens and chalcogens over the years, there is a lack in exploration of metal-metalloids, such as amorphous metal borides for the ORR. Transition metal borides show superior oxygen evolution reaction (OER) performance in alkaline solution compared with noble metal catalysts, metal oxides, and metal alloy counterparts. [17] In contrast, transition metal borides undergo severe oxidation, limiting activities that may be derived and consequently, their ORR performance. [18] To date, only J. Ma et al [19] and K. Elumeeva et al [20] reported the usage of CoB as an ORR electrocatalyst, but the performance obtained was not satisfying with those the state-of-the-art catalysts. CoB nanosheets are expected to be highly beneficial for electrochemical applications (for example, ORR) because 1) the synthesis of metal borides by chemical reduction is fast and facile compared with the time consuming synthesis of many other Compositional and structural engineering of metal-metalloid materials can boost their electrocatalytic performance. Herein, a highly efficient and stable electrocatalytic system for the oxygen reduction reaction is obtained by creating heterointerfaces between N-doped carbon and cobalt boride nanosheets. Furthermore, a detailed investigation on the effect of annealing temperature as well as the amount of carbon ...

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Section: Introductionmentioning

confidence: 99%

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confidence: 99%

Highly Efficient Oxygen Reduction Reaction Activity of N‐Doped Carbon–Cobalt Boride Heterointerfaces

Jose

Nsanzimana

et al. 2021

Advanced Energy Materials

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241

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“…Carbon‐based materials play an important role in energy and catalytic applications 33 – 35 . Their excellent design flexibility enables us to fabricate a variety of materials with unique properties 36 – 40 . Herein, we fabricated Zn-based heterogeneous catalysts (Zn/NC-X), in which Zn single sites [Zn δ+ (0 < δ < 2)] were anchored on microporous N-doped carbon (NC).…”

Section: Introductionmentioning

confidence: 99%

Zn-Nx sites on N-doped carbon for aerobic oxidative cleavage and esterification of C(CO)-C bonds

et al. 2021

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Selective cleavage of C-C bonds is very important in organic chemistry, but remains challenging because of their inert chemical nature. Herein, we report that Zn/NC-X catalysts, in which Zn2+ coordinate with N species on microporous N-doped carbon (NC) and X denotes the pyrolysis temperature, can effectively catalyze aerobic oxidative cleavage of C(CO)-C bonds and quantitatively convert acetophenone to methyl benzoate with a yield of 99% at 100 °C. The Zn/NC-950 can be applied for a wide scope of acetophenone derivatives as well as more challenging alkyl ketones. Detail mechanistic investigations reveal that the catalytic performance of Zn/NC-950 can be attributed to the coordination between Zn2+ and N species to change the electronic state of the metal, synergetic effect of the Zn single sites with their surrounding N atoms, as well as the microporous structure with the high surface area and structural defects of the NC.

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“…[3][4][5] Among such catalysts, the most prominent is the iron-based carbon material. [6][7][8][9][10] Nevertheless, the acidic-oxygen reduction activity of existing non-noble metal catalysts is not sufficient to replace Pt catalysts in proton exchange membrane fuel cells (PEMFCs)/metal-air batteries.…”

Section: Introductionmentioning

confidence: 99%

Sulfate Ions Induced Concave Porous S‐N Co‐Doped Carbon Confined FeC_x Nanoclusters with Fe‐N₄ Sites for Efficient Oxygen Reduction in Alkaline and Acid Media

Jin

Zhao

Liang

et al. 2021

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To improve the catalytic activity of the catalysts, it is key to intensifying the intrinsic activity of active sites or increasing the exposure of accessible active sites. In this work, an efficient oxygen reduction electrocatalyst is designed that confines plentiful FeCx nanoclusters with Fe‐N4 sites in a concave porous S‐N co‐doped carbon matrix, readily accessible for the oxygen reduction reaction (ORR). Sulfate ions react with the carbon derived from ZIF‐8 at high temperatures, leading to the shrinkage of the carbon framework and then forming a concave structure with abundant macropores and mesopores with S incorporation. Such an architecture promotes the exposure of active sites and accelerates remote mass transfer. As a result, the catalyst (Fe/S‐NC) with a large number of C‐S‐C, Fe‐N4, and FeCx nanoclusters presents impressive ORR activity and stability. In alkaline media, the half‐wave potential of the best catalyst (Fe/S2‐NC) is 0.91 V, which far exceeds that of commercial platinum carbon (0.85 V), while in acidic media the half‐wave potential reaches 0.784 V, comparable to platinum carbon (0.812 V). Furthermore, for the zinc‐air battery, the outstanding peak power density of Fe/S2‐NC (170 mW cm−2) superior to platinum carbon (108 mW cm−2) also highlights its great application potential.

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Modulation of Single Atomic Co and Fe Sites on Hollow Carbon Nanospheres as Oxygen Electrodes for Rechargeable Zn–Air Batteries

Cited by 204 publications

References 64 publications

Highly Efficient Oxygen Reduction Reaction Activity of N‐Doped Carbon–Cobalt Boride Heterointerfaces

Highly Efficient Oxygen Reduction Reaction Activity of N‐Doped Carbon–Cobalt Boride Heterointerfaces

Zn-Nx sites on N-doped carbon for aerobic oxidative cleavage and esterification of C(CO)-C bonds

Sulfate Ions Induced Concave Porous S‐N Co‐Doped Carbon Confined FeC_x Nanoclusters with Fe‐N₄ Sites for Efficient Oxygen Reduction in Alkaline and Acid Media

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Modulation of Single Atomic Co and Fe Sites on Hollow Carbon Nanospheres as Oxygen Electrodes for Rechargeable Zn–Air Batteries

Cited by 204 publications

References 64 publications

Highly Efficient Oxygen Reduction Reaction Activity of N‐Doped Carbon–Cobalt Boride Heterointerfaces

Highly Efficient Oxygen Reduction Reaction Activity of N‐Doped Carbon–Cobalt Boride Heterointerfaces

Zn-Nx sites on N-doped carbon for aerobic oxidative cleavage and esterification of C(CO)-C bonds

Sulfate Ions Induced Concave Porous S‐N Co‐Doped Carbon Confined FeCx Nanoclusters with Fe‐N4 Sites for Efficient Oxygen Reduction in Alkaline and Acid Media

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Sulfate Ions Induced Concave Porous S‐N Co‐Doped Carbon Confined FeC_x Nanoclusters with Fe‐N₄ Sites for Efficient Oxygen Reduction in Alkaline and Acid Media