Edge-sited Fe-N4 atomic species improve oxygen reduction activity via boosting O2 dissociation

Ma, Ruguang; Lin, Gaoxin; Ju, Qiangjian; Tang, Wei; Chen, Gen; Chen, Zhenhua; Liu, Qian; Yang, Minghui; Lu, Yunfeng; Wang, Yuandong

doi:10.1016/j.apcatb.2020.118593

Cited by 67 publications

(31 citation statements)

References 46 publications

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“…However, the application of ZAB is greatly limited duo to the sluggish kinetics at the air electrode, which highly depends on the expensive Ptgroup catalysts 3,4 . To address these issues, many researches have spent energy to study low-cost and high-efficiency catalysts to replace noble metal Pt/RuO2 [5][6][7] . Usually, a large number of active sites and high activity of active species are indispensable for efficient catalysts.…”

Section: Introductionmentioning

confidence: 99%

Co<sub>2</sub>P@P-Doped 3D Porous Carbon for Bifunctional Oxygen Electrocatalysis

Xiao¹,

Pei²,

Hu³

et al. 2020

Acta Physico Chimica Sinica

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The existing energy and environmental issues are the primary issues that restrict the continual development of the mankind. Cost-effective energy storage and conversion devices have attracted significant attention. Rechargeable zinc-air batteries (ZABs) are widely studied because they are portable, possess high power density, and are environmentally friendly. However, the slow kinetics of the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) limit their practical application. It is crucial to develop dual-functional electrocatalysts with excellent electrocatalytic performance, low price, simple operation, and outstanding stability. Therefore, transition metals and carbon-based materials should be combined. Although Co2P has been widely reported as an efficient OER catalyst, there are few studies based on the ORR activity. Herein, a facile pyrolysis of cobalt salt, phytic acid, and k-carrageenan aerogel was carried out on Co2P nanoparticles within P-doped porous carbon (Co2P-PCA-800), showing enhanced ORR activity. The resulting composite (Co2P-PCA-800) with a three-dimensional (3D) hierarchical porous architecture exhibited outstanding ORR activity with a high half-wave potential (E1/2) of approximately 0.84 V, which is comparable to that of Pt/C. Simultaneously, we fabricated phosphorus-doped porous carbon (PCA) and cobalt-doped porous carbon (Co-CA) to compare the effect of structural morphology on the catalytic performance. Studies have found that a regular interconnected porous structure can be beneficial for mass transfer and can ensure uniform distribution of ion current, thereby resulting in increased number of effective active sites. The outstanding ORR activity mainly results from the synergistic effect of the 3D honeycomb hierarchical porous structure and positively charged Co2P nanoparticles encapsulated in P-doped carbon. In addition, the 3D honeycomb porous carbon structure not only facilitates mass transfer and accelerates electron transfer but also protects the cobalt phosphide. Finally, we assembled a rechargeable ZAB with Co2P-PCA-800 as the air cathode catalyst. Compared with precious metal catalysts, the catalyst has considerable charge-discharge performance and energy density as well as higher specific capacity and better cycle stability. We believe that this study will provide a significant direction for solving energy and environmental issues.

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Section: Introductionmentioning

confidence: 99%

Co<sub>2</sub>P@P-Doped 3D Porous Carbon for Bifunctional Oxygen Electrocatalysis

Xiao¹,

Pei²,

Hu³

et al. 2020

Acta Physico Chimica Sinica

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“…The latter underwent a first pyrolysis treatment (900 °C, Ar atmosphere) during which a black powder of the desired pre-catalyst was formed. Its subsequent treatment with a 2 M NaOH solution at 80 °C was employed to etch and remove the silica template 46 before submitting the sample to a second pyrolysis step (see the Experimental section for details). During the thermal phases, Zn was vaporized leaving behind micropore channels while Fe atoms remained trapped in the C/N matrix as stable FeN x moieties ( vide infra ).…”

Section: Resultsmentioning

confidence: 99%

Inducing atomically dispersed Cl–FeN₄ sites for ORRs in the SiO₂-mediated synthesis of highly mesoporous N-enriched C-networks

et al. 2022

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“…The selected nitrogen functional groups are electron-accepting groups, which are more likely to accept the electron and generate electrostatic interactions with adsorbates. As shown in Table S1, the electron of BSUs has been redistributed caused by N atoms doping, as well as the electron distribution of carbon atoms at the edges of the pore has been changed, which leaded to the increase of EI contribution [56,57]. In addition, the N atoms in BSU-Pyrrolic and BSU-NH 2 exhibit a high electronegativity than that of other functional groups, which make the other atoms around them strongly electronegative or electropositive.…”

Section: Ei Contributionmentioning

confidence: 99%

Influence of functional groups and pore sizes in porous carbon for methanol acetone adsorptive separation based on molecular simulation

Chen

Liu

et al. 2021

J Mater Sci

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In order to investigate the optimal nitrogen functional group and the most suitable pore size for the efficient adsorptive separation of methanol-acetone mixed vapor, a series of theoretical calculations, including Grand Canonical Monte Carlo (GCMC) simulation and density functional theory (DFT) calculation, were carried out to determine the adsorptive separation properties of AC-Rs (AC = activated carbon, R = Pyridinic, -NH 2 , Pyrrolic, Quaternary) with different pore sizes (0.6-8.0 nm). The results showed AC-Pyridinic had the highest methanol-acetone adsorption capacities (14.64 mol/kg for acetone and 26.35 mol/kg for methanol at their respective saturation pressures). The high adsorption energies, the hydrogen bonding interaction between the pyridinic nitrogen and hydrogen of methanol's hydroxyl group, and electrostatic interaction between the pyridinic nitrogen and carbon of acetone's carbonyl group were crucial factors for that. In the case of methanol-acetone separation, the methanol molecular aggregation resulted in an increase in methanol-acetone selectivities on AC-Rs. Interestingly, AC-Pyridinic still showed the highest methanol-acetone selectivity. Furthermore, the pore with 3.5 nm and 3.0 nm were optimal for methanol and acetone adsorption respectively, in which AC-Pyridinic exhibited superior capture capacities (23.19 mmol/g for methanol at 16 kPa and 11.64 mmol/g for acetone at 30 kPa). And with a 6 nm pore size, AC-Pyridinic had the highest selectivity (* 5.0). The mesopore of 2.5-3 nm is suitable for methanol-acetone adsorptive separation taking both adsorption and selectivity performance into consideration. This investigation predicted the functional group and pore sizes with the best modification effect on AC for methanol-acetone adsorptive separation, which sheds light on ways to design a highly efficient adsorbent for gas adsorption and separation.

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Edge-sited Fe-N4 atomic species improve oxygen reduction activity via boosting O2 dissociation

Cited by 67 publications

References 46 publications

Co<sub>2</sub>P@P-Doped 3D Porous Carbon for Bifunctional Oxygen Electrocatalysis

Co<sub>2</sub>P@P-Doped 3D Porous Carbon for Bifunctional Oxygen Electrocatalysis

Inducing atomically dispersed Cl–FeN₄ sites for ORRs in the SiO₂-mediated synthesis of highly mesoporous N-enriched C-networks

Influence of functional groups and pore sizes in porous carbon for methanol acetone adsorptive separation based on molecular simulation

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Edge-sited Fe-N4 atomic species improve oxygen reduction activity via boosting O2 dissociation

Cited by 67 publications

References 46 publications

Co<sub>2</sub>P@P-Doped 3D Porous Carbon for Bifunctional Oxygen Electrocatalysis

Co<sub>2</sub>P@P-Doped 3D Porous Carbon for Bifunctional Oxygen Electrocatalysis

Inducing atomically dispersed Cl–FeN4 sites for ORRs in the SiO2-mediated synthesis of highly mesoporous N-enriched C-networks

Influence of functional groups and pore sizes in porous carbon for methanol acetone adsorptive separation based on molecular simulation

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Inducing atomically dispersed Cl–FeN₄ sites for ORRs in the SiO₂-mediated synthesis of highly mesoporous N-enriched C-networks