In situ molecular-level synthesis of N, S co-doped carbon as efficient metal-free oxygen redox electrocatalysts for rechargeable Zn–Air batteries

Lyu, Dandan; Yao, Sixian; Bahari, Yaser; Hasan, Syed Waqar; Pan, Chan; Zhang, Xiaoran; Ye, Feng; Tian, Zhi Qun; Shen, Pei Kang

doi:10.1016/j.apmt.2020.100737

Cited by 25 publications

(20 citation statements)

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“…According to our previous research results on N, S–C metal free oxygen electrocatalysts, we selected the carbon atom between the N and S in N, S–C layer as the adsorption active site. [ 51 ] The adsorption model of oxygen intermediates for Co 9 S 8 (4 4 0)@N, S–C and Co 9 S 8 (3 1 1)@N, S–C is shown in Figure S18 in the Supporting Information. The free energy is calculated of the oxygenated intermediate species in ORR and OER process use the above models.…”

Section: Resultsmentioning

confidence: 99%

N, S Codoped Carbon Matrix‐Encapsulated Co₉S₈ Nanoparticles as a Highly Efficient and Durable Bifunctional Oxygen Redox Electrocatalyst for Rechargeable Zn–Air Batteries

Lyu

Yao

Ali

et al. 2021

Advanced Energy Materials

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117

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Herein, a N, S co-doped carbon encapsulating Co 9 S 8 nanoparticles (Co 9 S 8 @N, S-C) catalyst is successfully synthesized by a new precursor of Co-pyridine coordinated-polymer consisting of 2,6-diacetylpyridine and 4,4′-dithiodianiline. Benefiting from the abundant pore-structure (average pore-size ≈25nm) and unique electronic-properties of the Co 9 S 8 and N, S-C layer, the as-prepared Co 9 S 8 @N, S-C exhibits rapid oxygen reduction reaction (ORR) kinetics with high electron transfer number of ≈3.998 and demonstrates a low overpotential of 304 mV for the oxygen evolution reaction (OER). It exhibits a small potential difference of 0.647V for overall ORR/OER activity, outperforming most of the non-precious metal-catalysts previously reported. The rechargeable Zn-Air battery test further demonstrates its excellent activity and stability, in which the battery delivers a maximum power density output of 259 mW cm −2 , a specific capacity of 862 mAh g Zn −1 , and after continuous 110 h operation the charge-discharge round-trip efficiency only reduces by 4.83%. Theoretical calculation studies show that the surface N, S-C layers and Co 9 S 8 can adjust each other's Fermi levels, so that the adsorption energy of Co 9 S 8 @N, S-C on O intermediate is more favorable than using Co 9 S 8 and N, S-C alone. This study reveals the structure-function relationship of coated-nanostructures with multifunctional electrocatalytic properties, and provides a feasible strategy for the design of non-noble metal-catalysts.

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Section: Resultsmentioning

confidence: 99%

N, S Codoped Carbon Matrix‐Encapsulated Co₉S₈ Nanoparticles as a Highly Efficient and Durable Bifunctional Oxygen Redox Electrocatalyst for Rechargeable Zn–Air Batteries

Lyu

Yao

Ali

et al. 2021

Advanced Energy Materials

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117

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“…Along with the monodoped carbon catalysts discussed above, co‐doping of carbon materials with two or more different heteroatoms can further enhance the catalytic performance of the carbon catalysts by increasing the total number of active sites and through possible synergistic effects. [ 47 ] So far, co‐doping studies have been focused on co‐doping of N‐doped carbon materials with a second element, such as B, [ 69–76 ] S, [ 77–88 ] P, [ 89–106 ] and, to a less extent, Cl, [ 107 ] and Si. [ 108,109 ] A few reports on the co‐doping of carbon materials with three elements, such as N–P–S, [ 110,111 ] N–P–B, [ 112,113 ] N–P–F, [ 114 ] and N–S–F, [ 115 ] have recently appeared.…”

Section: Co‐doped C‐mfecsmentioning

confidence: 99%

“…Besides ORR, N and S co‐doped carbon materials were also applied as bifunctional electrocatalysts for Zn–air batteries [ 81,82 ] and water splitting reactions. [ 77,78,83 ] Recently, Lyu et al.…”

Section: Co‐doped C‐mfecsmentioning

confidence: 99%

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Non‐N‐Doped Carbons as Metal‐Free Electrocatalysts

Wang

Liu

Dai

2020

Advanced Sustainable Systems

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Ten years have passed since the discovery of the first nitrogen‐doped carbon‐based metal‐free catalyst for the oxygen reduction reaction, which opened a new field of catalysis toward a large variety of important applications, ranging from energy conversion and storage to environmental remediation. Various heteroatom‐doped carbons, beyond nitrogen‐doping (N‐doping), with distinctive features have also been developed for many specific reactions of practical significance (e.g., oxygen reduction (ORR), water splitting (OER and HER), CO2 reduction (CO2RR), and N2 reduction (NRR)). However, the topic of metal‐free non‐N‐doped carbon electrocatalysts has not been reviewed till now. This article aims to review recent advances in non‐N‐doped carbon electrocatalysts with an emphasis on their synthesis, catalytic mechanisms, and catalytic performance in various electrochemical reactions, including the ORR, OER, HER, H2O2 production, NRR, and CO2RR. Like N‐doping, boron‐doping, phosphorus‐doping, and fluorine‐doping are found to show similar catalytic efficiency for the ORR, OER, and HER. However, oxygen‐doping and boron‐doping are particularly favorable for the selective production of H2O2 and NH3, respectively, exceeding the performance of N‐doping. Along with the timely and critical overview on the non‐N‐doped carbon electrocatalysts, current challenges and future perspectives for this emerging field are also discussed.

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“…Metal-free nanocarbons doped with heteroatoms (such as N, O, P, S, B, and F) have been widely regarded as the most promising ORR electrocatalysts because of their superior activity, excellent durability, tunable geometric/electronic structures, and sur-/interface properties, and cost-effectiveness [15][16][17][18][19][20]. Among them, the N-doped nanocarbons are the most widely studied because they can activate the ORR process by providing the donor electrons to adjacent carbon atoms [21,22].…”

Section: Introductionmentioning

confidence: 99%

2D Zinc-Based Metal–Organic Complexes Derived N-Doped Porous Carbon Nanosheets as Durable Air Cathode for Rechargeable Zn–Air Batteries

et al. 2022

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The defect and N-doping engineering are critical to developing the highly efficient metal-free electrocatalysts for oxygen reduction reaction (ORR), mainly because they can efficiently regulate the geometric/electronic structures and sur-/interface properties of the carbon matrix. Herein, we provide a facile and scalable strategy for the large-scale synthesis of N-doped porous carbon nanosheets (NPCNs) with hierarchical pore structure, only involving solvothermal and pyrolysis processes. Additionally, the turnover frequency of ORR (TOFORR) was calculated by taking into account the electron-transfer number (n). Benefiting from the trimodal pore structures, high specific surface area, a higher pore volume, high-ratio mesopores, massive vacancies/long-range structural defects, and high-content pyridinic-N (~2.1%), the NPCNs-1000 shows an excellent ORR activity (1600 rpm, js = ~5.99 mA cm−2), a selectivity to four-electron ORR (~100%) and a superior stability in both the three-electrode tests (CP test for 7500 s at 0.8 V, Δjs = ~0.58 mA cm−2) and Zn–Air battery (a negligible loss of 0.08 V within 265 h). Besides, the experimental results indicate that the enhancement of ORR activity mainly originates from the defects and pyridinic-N. More significantly, this work is expected to realize green and efficient energy storage and conversion along with the carbon peaking and carbon neutrality goals.

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In situ molecular-level synthesis of N, S co-doped carbon as efficient metal-free oxygen redox electrocatalysts for rechargeable Zn–Air batteries

Cited by 25 publications

References 50 publications

N, S Codoped Carbon Matrix‐Encapsulated Co₉S₈ Nanoparticles as a Highly Efficient and Durable Bifunctional Oxygen Redox Electrocatalyst for Rechargeable Zn–Air Batteries

N, S Codoped Carbon Matrix‐Encapsulated Co₉S₈ Nanoparticles as a Highly Efficient and Durable Bifunctional Oxygen Redox Electrocatalyst for Rechargeable Zn–Air Batteries

Non‐N‐Doped Carbons as Metal‐Free Electrocatalysts

2D Zinc-Based Metal–Organic Complexes Derived N-Doped Porous Carbon Nanosheets as Durable Air Cathode for Rechargeable Zn–Air Batteries

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In situ molecular-level synthesis of N, S co-doped carbon as efficient metal-free oxygen redox electrocatalysts for rechargeable Zn–Air batteries

Cited by 25 publications

References 50 publications

N, S Codoped Carbon Matrix‐Encapsulated Co9S8 Nanoparticles as a Highly Efficient and Durable Bifunctional Oxygen Redox Electrocatalyst for Rechargeable Zn–Air Batteries

N, S Codoped Carbon Matrix‐Encapsulated Co9S8 Nanoparticles as a Highly Efficient and Durable Bifunctional Oxygen Redox Electrocatalyst for Rechargeable Zn–Air Batteries

Non‐N‐Doped Carbons as Metal‐Free Electrocatalysts

2D Zinc-Based Metal–Organic Complexes Derived N-Doped Porous Carbon Nanosheets as Durable Air Cathode for Rechargeable Zn–Air Batteries

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N, S Codoped Carbon Matrix‐Encapsulated Co₉S₈ Nanoparticles as a Highly Efficient and Durable Bifunctional Oxygen Redox Electrocatalyst for Rechargeable Zn–Air Batteries

N, S Codoped Carbon Matrix‐Encapsulated Co₉S₈ Nanoparticles as a Highly Efficient and Durable Bifunctional Oxygen Redox Electrocatalyst for Rechargeable Zn–Air Batteries