Alternative view of oxygen reduction on porous carbon electrocatalysts: The substance of complex oxygen-surface interactions

Falco, Giacomo de; Florent, Marc; Jagiełło, Jacek; Cheng, Yongqiang; Daemen, Luke L.; Ramirez‐Cuesta, Anibal J.; Bandosz, Teresa J.

doi:10.1016/j.isci.2021.102216

Cited by 14 publications

(17 citation statements)

References 60 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Proton exchange membrane fuel cells (PEMFCs) have aroused increasing attention as one of the most promising renewable energy conversion systems on account of their high energy conversion efficiency, low operation temperature, and environmentally benign products [1][2][3]. As a crucial cathode reaction in PEMFCs, the oxygen reduction reaction (ORR) has attracted enormous research interest [4][5][6][7][8][9]. However, the overall efficiency of energy conversion is limited due to the intricate reaction process and inherently sluggish reaction kinetics of ORR.…”

Section: Introductionmentioning

confidence: 99%

Cyanogel-Derived Synthesis of Porous PdFe Nanohydrangeas as Electrocatalysts for Oxygen Reduction Reaction

et al. 2021

View full text Add to dashboard Cite

It is important to develop cost-efficient electrocatalysts used in the oxygen reduction reaction (ORR) for widespread applications in fuel cells. Palladium (Pd) is a promising catalyst, due to its more abundant reserves and lower price than platinum (Pt), and doping an earth-abundant 3d-transition metal M into Pd to form Pd–M bimetallic alloys may not only further reduce the use of expensive Pd but also promote the electrocatalytic performance of ORR, owing to the synergistic effect between Pd and M. Here we report a cyanogel-derived synthesis of PdFe alloys with porous nanostructure via a simple coinstantaneous reduction reaction by using K2PdIICl4/K4FeII(CN)6 cyanogel as precursor. The synthesized PdFe alloys possess hydrangea-like morphology and porous nanostructure, which are beneficial to the electrochemical performance in ORR. The onset potential of the porous PdFe nanohydrangeas is determined to be 0.988 V, which is much more positive than that of commercial Pt/C catalyst (0.976 V) and Pd black catalyst (0.964 V). Resulting from the unique structural advantages and synergetic effect between bimetals, the synthesized PdFe nanohydrangeas with porous structure have outstanding electrocatalytic activity and stability for ORR, compared with the commercial Pd black and Pt/C.

show abstract

Section: Introductionmentioning

confidence: 99%

Cyanogel-Derived Synthesis of Porous PdFe Nanohydrangeas as Electrocatalysts for Oxygen Reduction Reaction

et al. 2021

View full text Add to dashboard Cite

show abstract

“…Besides the advantages of heteroatom doping, de Falco et al demonstrated the additional benefit of the suitable pore structure in the ORR. The synergy of ultramicropores and hydrophobic surface rich in ether groups and/or electrons enhances the electrocatalytic efficiency of carbon materials and may result in an ORR performance similar to that measured on Pt/C with a 4 electron transfer mechanism [26].…”

Section: Introductionmentioning

confidence: 83%

“…As has been recently pointed out, ultramicropores work as pseudocatalytic centers for ORR by promoting strong O2 adsorption. The thus facilitated O=O bond splitting orientates the ORR through a 4e − reduction mechanism [26]. Figure 11b implies that in case of CA the 4e − route is indeed the dominant pathway.…”

Section: Electrocatalytic Applicationmentioning

confidence: 91%

Biomass Related Highly Porous Metal Free Carbon for Gas Storage and Electrocatalytic Applications

et al. 2021

View full text Add to dashboard Cite

In this paper we report the synthesis of a N, S co-doped metal free carbon cryogel obtained from a marine biomass derived precursor using urea as nitrogen source. Natural carrageenan intrinsically contains S and inorganic salt. The latter also serves as an activating agent during the pyrolytic step. The overall 11.6 atomic % surface heteroatom concentration comprises 5% O, 4.6% N and 1% S. The purified and annealed final carbon (CA) has a hierarchical pore structure of micro-, meso- and macropores with an apparent surface area of 1070 m2/g. No further treatment was applied. The gas adsorption potential of the samples was probed with H2, CO2 and CH4, while the electrocatalytic properties were tested in an oxygen reduction reaction. The atmospheric CO2 and CH4 storage capacity at 0 °C in the low pressure range is very similar to that of HKUST-1, with the CO2/CH4 selectivity below 20 bar, even exceeding that of the MOF, indicating the potential of CA in biogas separation. The electrocatalytic behavior was assessed in an aqueous KOH medium. The observed specific gravimetric capacitance 377 F/g was exceeded only in B, N dual doped and/or graphene doped carbons from among metal free electrode materials. The CA electrode displays almost the same performance as a commercial 20 wt% Pt/C electrode. The oxygen reduction reaction (ORR) exhibits the 4-electron mechanism. The 500-cycle preliminary stability test showed only a slight increase of the surface charge.

show abstract

“…It is because the developed surface area leads to a high dispersion and large quantity of the latter. The porosity, and especially ultramicropores, has also been indicated as advancing the ORR performance of carbon-based catalysts by promoting strong O 2 adsorption leading to oxygen–oxygen bond splitting and its reduction and protonation in an alkaline electrolyte. ,− Nevertheless, from the viewpoints of a circular economy and cost-effectiveness, acid washing is not a desired procedure. Recently, we have shown that equally good ORR catalysts to those acid-washed biosolid-based ones and even to porous carbons can be obtained by a simple pyrolysis of biosolid alone, with a specific modification of the process conditions (time and heating rate) .…”

Section: Introductionmentioning

confidence: 99%

Complexity of Biosolid-Derived Electrocatalysts Grants Their Excellent Performance in Oxygen Reduction Reaction

Falco

Florent

Bandosz

2022

ACS Appl. Energy Mater.

Self Cite

View full text Add to dashboard Cite

A class of oxygen reduction reaction (ORR) catalysts was derived from surfactant-modified biosolid by a simple pyrolysis of mixtures at 950 °C. Two nonionic surfactants of long and short chains (F127 and P123) were added to biosolids in various amounts to modify surface features. These features (porosity, texture, and chemistry) were extensively characterized by various methods, and then an ORR efficiency in an alkaline electrolyte was evaluated. The modification increased surface areas and pore volumes by about 30% compared to the material obtained from biosolid alone, resulting in micro/mesoporous solids. The treatment also changed surface chemistry, increased the content of a carbon phase, and led to the formation of metal carbides. These changes resulted in a high catalytic activity with the electron-transfer number practically equal to 4 and a kinetic current density of 42.5 mA/cm2. The performance varied depending on the type of surfactant added and its amount. The results suggested that the interplay of surface chemistry (catalytic metals, nitrogen-based sites, carbides, and the type and chemistry of the carbon phase) and the dispersion of catalytic sites (the extent of porosity development) were responsible for the excellent catalytic activity. The source of the catalysts and their performance indicates a new direction for the sustainable use of municipal wastes.

show abstract

Alternative view of oxygen reduction on porous carbon electrocatalysts: The substance of complex oxygen-surface interactions

Cited by 14 publications

References 60 publications

Cyanogel-Derived Synthesis of Porous PdFe Nanohydrangeas as Electrocatalysts for Oxygen Reduction Reaction

Cyanogel-Derived Synthesis of Porous PdFe Nanohydrangeas as Electrocatalysts for Oxygen Reduction Reaction

Biomass Related Highly Porous Metal Free Carbon for Gas Storage and Electrocatalytic Applications

Complexity of Biosolid-Derived Electrocatalysts Grants Their Excellent Performance in Oxygen Reduction Reaction

Contact Info

Product

Resources

About