Quaternary FeCoNiMn-Based Nanocarbon Electrocatalysts for Bifunctional Oxygen Reduction and Evolution: Promotional Role of Mn Doping in Stabilizing Carbon

Gupta, Shiva; Zhao, Shuai; Wang, Xiao Xia; Hwang, Sooyeon; Karakalos, Stavros; Devaguptapu, Surya V.; Mukherjee, Shreya; Su, Dong; Xu, Hui; Wu, Gang

doi:10.1021/acscatal.7b02949

Cited by 140 publications

(76 citation statements)

References 47 publications

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“…From Figure 2a, two characteristic carbon resonances around 1600 cm −1 (G band) and 1380 cm −1 (D band) are dominant, which correspond to the planar motion of sp 2 ‐hybridized carbon atoms in an ideal plane and at the edge, respectively . The ratio of the intensities of the two peaks ( I D / I G ) indicates the overall degree of graphitization in carbon.…”

Section: Resultsmentioning

confidence: 99%

Atomically Dispersed Single Ni Site Catalysts for Nitrogen Reduction toward Electrochemical Ammonia Synthesis Using N₂ and H₂O

et al. 2020

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Ammonia (NH3) electrosynthesis gains significant attention as NH3 is essentially important for fertilizer production and fuel utilization. However, electrochemical nitrogen reduction reaction (NRR) remains a great challenge because of low activity and poor selectivity. Herein, a new class of atomically dispersed Ni site electrocatalyst is reported, which exhibits the optimal NH3 yield of 115 µg cm−2 h−1 at –0.8 V versus reversible hydrogen electrode (RHE) under neutral conditions. High faradic efficiency of 21 ± 1.9% is achieved at ‐0.2 V versus RHE under alkaline conditions, although the ammonia yield is lower. The Ni sites are stabilized with nitrogen, which is verified by advanced X‐ray absorption spectroscopy and electron microscopy. Density functional theory calculations provide insightful understanding on the possible structure of active sites, relevant reaction pathways, and confirm that the Ni‐N3 sites are responsible for the experimentally observed activity and selectivity. Extensive controls strongly suggest that the atomically dispersed NiN3 site‐rich catalyst provides more intrinsically active sites than those in N‐doped carbon, instead of possible environmental contamination. This work further indicates that single‐metal site catalysts with optimal nitrogen coordination is very promising for NRR and indeed improves the scaling relationship of transition metals.

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Section: Resultsmentioning

confidence: 99%

Atomically Dispersed Single Ni Site Catalysts for Nitrogen Reduction toward Electrochemical Ammonia Synthesis Using N₂ and H₂O

et al. 2020

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“…On the other hand, the range of the precursors' content, variety, and ratios is larger than that in other methods theoretically, offering more choices for fabricating electrocatalysts. For example, the mixture method has been proposed for synthesizing a quaternary FeCoNiMn‐based nanocarbon electrocatalyst containing more species of TM compared to the other method 64. Furthermore, the role of various metals can also be researched by adjusting the ratios of the precursors, revealing that Fe, Co, and Ni catalyzed the formation of the porous carbon bases and the formation of the active sites, whereas Mn was highly effective in catalyzing the formation of the highly ordered and fewer‐defect graphite‐like carbon.…”

Section: Synthetic Strategies For Porous Carbon Nanostructures Decoramentioning

confidence: 99%

Efficient Oxygen Reduction Catalysts of Porous Carbon Nanostructures Decorated with Transition Metal Species

Huang

Shen

Zhang

et al. 2019

Advanced Energy Materials

200

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Developing substitutes of noble metal catalysts toward oxygen reduction reaction (ORR) at the cathode is of vital importance for promoting low‐temperature polymer electrolyte membrane fuel cells. Transition metal species have been one of the hot areas of interest due to their low cost, high activity, and long‐term stability. The design of porous carbon nanostructures decorated with transition metal species plays a vital role in enhancing ORR catalytic performance. Here, the recent breakthroughs in porous carbon nanostructures decorated with transition metal species (including nanoparticles and atomically dispersed supported metal) are discussed. The porous nanostructures can provide large surface area as well as abundant pore channels, leading to sufficient exposure of active sites and efficient mass transfer. These nanostructures can be synthesized by several approaches, including the templated method, the self‐templated method, the impregnation process, and so on. Furthermore, the ORR performance and the exploration of active sites are also discussed for further enhancement of the ORR catalysts. Finally, the challenges and prospects are discussed, which would push forward the development of ORR catalysts in the near future.

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“…Therefore, numerous carbon‐based nanomaterials have been developed to replace the Pt based composites . Among them, the nitrogen species coordinated first‐row transition metal (e.g., Co, Ni, and Fe) atoms in carbons (M–N–C) are widely considered as promising electrocatalysts for ORR . The M–N–C materials are usually recognized as single‐atom catalysts (SACs), since isolated N‐bonded metals atoms are embedded in carbons.…”

Section: Methodsmentioning

confidence: 99%

N,P Co‐Coordinated Manganese Atoms in Mesoporous Carbon for Electrochemical Oxygen Reduction

Zhu

Amal

2019

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The increasing interest in fuel cell technology encourages the development of efficient and low‐cost electrocatalysts to replace the Pt based materials for catalyzing the cathodic oxygen reduction reaction (ORR). In the present work, a nitrogen and phosphorus co‐coordinated manganese atom embedded mesoporous carbon composite (MnNPC‐900) is successfully prepared via a polymerization of o‐phenylenediamine followed by calcination at 900 °C. The MnNPC‐900 composite shows a high ORR activity in alkaline media, offering an onset potential of 0.97 V, and a half‐wave potential of 0.84 V (both vs reversible hydrogen electrode) with a loading of 0.4 mg cm−2. This performance not only exceeds its phosphorus‐free counterpart (MnNC‐900), but also is comparable to the Pt/C catalyst under identical measuring conditions. The significantly enhanced ORR performance of MnNPC‐900 can be ascribed to: i) the introduction of phosphorus assists the generation of mesopores during the pyrolysis and endows the MnNPC‐900 composite with large surface area and pore volume, thus facilitating the mass transfer process and increases the number of exposed active sites. ii) The formation of N,P co‐coordinated atomic‐scale Mn sites (MnNxPy), which modifies the electronic configuration of the Mn atoms and thereby boosts the ORR catalytic activity.

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Quaternary FeCoNiMn-Based Nanocarbon Electrocatalysts for Bifunctional Oxygen Reduction and Evolution: Promotional Role of Mn Doping in Stabilizing Carbon

Cited by 140 publications

References 47 publications

Atomically Dispersed Single Ni Site Catalysts for Nitrogen Reduction toward Electrochemical Ammonia Synthesis Using N₂ and H₂O

Atomically Dispersed Single Ni Site Catalysts for Nitrogen Reduction toward Electrochemical Ammonia Synthesis Using N₂ and H₂O

Efficient Oxygen Reduction Catalysts of Porous Carbon Nanostructures Decorated with Transition Metal Species

N,P Co‐Coordinated Manganese Atoms in Mesoporous Carbon for Electrochemical Oxygen Reduction

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Quaternary FeCoNiMn-Based Nanocarbon Electrocatalysts for Bifunctional Oxygen Reduction and Evolution: Promotional Role of Mn Doping in Stabilizing Carbon

Cited by 140 publications

References 47 publications

Atomically Dispersed Single Ni Site Catalysts for Nitrogen Reduction toward Electrochemical Ammonia Synthesis Using N2 and H2O

Atomically Dispersed Single Ni Site Catalysts for Nitrogen Reduction toward Electrochemical Ammonia Synthesis Using N2 and H2O

Efficient Oxygen Reduction Catalysts of Porous Carbon Nanostructures Decorated with Transition Metal Species

N,P Co‐Coordinated Manganese Atoms in Mesoporous Carbon for Electrochemical Oxygen Reduction

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Product

Resources

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Atomically Dispersed Single Ni Site Catalysts for Nitrogen Reduction toward Electrochemical Ammonia Synthesis Using N₂ and H₂O

Atomically Dispersed Single Ni Site Catalysts for Nitrogen Reduction toward Electrochemical Ammonia Synthesis Using N₂ and H₂O