Ana Belen Jorge

Fe–N-Doped Carbon Capsules with Outstanding Electrochemical Performance and Stability for the Oxygen Reduction Reaction in Both Acid and Alkaline Conditions

High surface area N-doped mesoporous carbon capsules with iron traces exhibit outstanding electrocatalytic activity for the oxygen reduction reaction in both alkaline and acidic media. In alkaline conditions, they exhibit more positive onset (0.94 V vs RHE) and half-wave potentials (0.83 V vs RHE) than commercial Pt/C, while in acidic media the onset potential is comparable to that of commercial Pt/C with a peroxide yield lower than 10%. The Fe-N-doped carbon catalyst combines high catalytic activity with remarkable performance stability (3500 cycles between 0.6 and 1.0 V vs RHE), which stems from the fact that iron is coordinated to nitrogen. Additionally, the newly developed electrocatalyst is unaffected by the methanol crossover effect in both acid and basic media, contrary to commercial Pt/C. The excellent catalytic behavior of the Fe-N-doped carbon, even in the more relevant acid medium, is attributable to the combination of chemical functions (N-pyridinic, N-quaternary, and Fe-N coordination sites) and structural properties (large surface area, open mesoporous structure, and short diffusion paths), which guarantees a large number of highly active and fully accessible catalytic sites and rapid mass-transfer kinetics. Thus, this catalyst represents an important step forward toward replacing Pt catalysts with cheaper alternatives. In this regard, an alkaline anion exchange membrane fuel cell was assembled with Fe-N-doped mesoporous carbon capsules as the cathode catalyst to provide current and power densities matching those of a commercial Pt/C, which indicates the practical applicability of the Fe-N-carbon catalyst.

Synergistic relationship between the three-dimensional nanostructure and electrochemical performance in biocarbon supercapacitor electrode materials

A novel study presented herein correlates the multidimensional morphology with the electrochemical performance of activated bio-carbon materials, for supercapacitor devices over multiple length scales. The optimization of the potassium hydroxide (KOH)/cellulose ratio for supercapacitor electrode materials is related to morphological characteristics and corresponding electrochemical performance, as described in terms of porosity, specific surface area, specific capacitance and electrochemical impedance. KOH/cellulose samples with ratios 0.5 : 1 and 1 : 1 exhibited the best performance, characterized by a hierarchal porous network structure, high surface area and low cell resistance. Compared with the rest of the manufactured samples and commercial activated carbons, Ketjen Black (KB), Norit activated carbon (NAC) and bead-shaped activated carbon (BAC), the former two samples showed better results in three-electrode systems and coin cells, with specific gravimetric capacitances as high as 187 F g−1 at a current density of 1 A g−1. The high performance is attributed to the morphology of the samples that constituted a combination of micro-, meso- and macroporosity which consequently gave high specific surface area, high porosity, low cell resistance and high specific capacitance. This further corroborates the structure-performance relationship observed in the authors model KOH/cellulose system, highlighting that the work can be extended to other similar systems. It is clear that the three-dimensional nanostructure of a material must be understood in its entirety in order to optimize the electrochemical performance.

Pd nanoparticles supported on reduced graphene–E. coli hybrid with enhanced crystallinity in bacterial biomass

A novel method for simultaneous reduction of graphene oxide (GO) and palladium salt, Pd(II), using Escherichia coli (E. coli) in the separate presence of two different mild reducing agents (hydrogen and formate) is investigated to successfully produce reduced GO (rGO)-biomass/Pd hybrid material for potential use as an electrocatalyst. Transmission electron microscopy, X-ray diffraction, thermo-gravimetric analysis, X-ray photoelectron spectroscopy and Raman microscopy demonstrate the successful reduction of Pd(II), GO and the biomass, resulting in the formation of Pd nanoparticles (PdNPs) on an rGO–biomass hybrid. The distribution of the NPs was found to be dependent on the type of reducing agent. PdNPs formed on rGO sheets showed relatively uniform distribution and size control (2–5 nm), whereas PdNPs on the bacterial scaffold were larger (up to 10 nm in size). Raman spectroscopy studies suggest that the presence of Pd leads to oxygen reduction and increased crystallinity in the bacterial biomass. Previous studies have suggested the potential for a bacterially-supported Pd electrocatalyst in fuel cells and, independently, the suitability of rGO as a support for PdNPs. This study confirms the simultaneous bacterial reduction of Pd(II) and GO and the association between the bacterial cells and rGO. We suggest that the simultaneous presence of E. coli and mild reducing agent together with GO and Pd(II) creates an interactive and synergistic environment in a hybrid material to allow (a) better control of PdNP size and distribution both on the inside of the bacterial membrane and on the rGO sheets and (b) increased crystallinity of the bacterial biomass compared to systems with bacteria alone.

Carbon Nitride Materials as Efficient Catalyst Supports for Proton Exchange Membrane Water Electrolyzers

Carbon nitride materials with graphitic to polymeric structures (gCNH) were investigated as catalyst supports for the proton exchange membrane (PEM) water electrolyzers using IrO2 nanoparticles as oxygen evolution electrocatalyst. Here, the performance of IrO2 nanoparticles formed and deposited in situ onto carbon nitride support for PEM water electrolysis was explored based on previous preliminary studies conducted in related systems. The results revealed that this preparation route catalyzed the decomposition of the carbon nitride to form a material with much lower N content. This resulted in a significant enhancement of the performance of the gCNH-IrO2 (or N-doped C-IrO2) electrocatalyst that was likely attributed to higher electrical conductivity of the N-doped carbon support.