Search Results (4)

In this study, density functional theory (DFT) was used to investigate the influence of temperature on the performance of a novel Cu-nitrogen-doped graphene Cu₂-N₈/Gr nanocomposite as a catalyst for the oxygen reduction reaction (ORR) in fuel cell applications. Our DFT calculations, conducted using Gaussian 09w with the 3–21G/B3LYP basis set, focus on the Cu-nitrogen-doped graphene nanocomposite cathode catalyst, exploring its behavior at three distinct temperatures: 298.15 K, 353.15 K, and 393.15 K, under acidic conditions. Our analysis of formation energies indicates that the structural stability of the catalyst remains unaffected as the temperature varies within the potential range of 0–7.21 V. Notably, the stability of the ORR steps experiences a marginal decrease with increasing temperature, with the exception of the intermediate OH + H₂O (*OH + H + *OH). Interestingly, the optimization reveals the absence of single OH and H₂O intermediates during the reactions. Furthermore, the OH + H₂O step is optimized to form the OH + H + OH intermediate, featuring the sharing of a hydrogen atom between dual OH intermediates. Free energy calculations elucidate that the catalyst supports spontaneous ORR at all temperatures. The highest recorded maximum cell potential, 0.69 V, is observed at 393.15 K, while the lowest, 0.61 V, is recorded at 353.15 K. In particular, the Cu₂-N₈/Gr catalyst structure demonstrates a reduced favorability for the H₂O₂ generation at all temperatures, resulting in the formation of dual OH intermediates rather than H₂O₂. In conclusion, at 393.15 K, Cu₂-N₈/Gr exhibits enhanced catalyst performance compared to 353.15 K and 298.15 K, making it a promising candidate for ORR catalysis in fuel cell applications. Full article

To develop high-performance microwave absorption materials with the features of lightweight, thin thickness, broad bandwidth, and strong absorption, an ultralight Ni₃S₂@N, S-codoped graphene aerogel with a density of 13.5 mg/cm³ has been fabricated by the use of metal-organic frameworks (MOFs) to directly initiate the gelation of graphene oxide strategy. In such a strategy, dual-functional 1D Ni-MOF nanorods not only act as the gelation agent but also afford the doping elements (N and S) originated from the organic species and the precursor for metal sulfide. Due to the synergistic effects of good impedance matching and multiple losses, the optimal reflection loss (RL) of as-prepared Ni₃S₂@N, S-codoped graphene aerogel reaches −46.9 dB at 17.1 GHz with only 2.0 mm and ultralow filling content (1.75 wt%). The maximum effective absorption bandwidth (EAB) reaches 6.3 GHz (11.7–18.0 GHz) at 2.38 mm, covering the whole Ku band. Moreover, the value of EAB with the RL less than −30 dB can be tuned to 12.2 GHz (5.8–18 GHz) at the absorber thickness ranging from 1.9 to 5.0 mm. This work provides insight for rational design and fabrication of multicomponent-containing graphene aerogels, showing the potential application in lightweight and high-performance microwave absorption. Full article

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. Full article

A series of PdSn binary catalysts with varied molar ratios of Pd to Sn are synthesized on B and N dual-doped graphene supporting materials. The catalysts are characterized by X-ray diffraction (XRD) and Transmission electron microscopy (TEM). Formic acid electro-oxidation reaction is performed on these catalysts, and the results reveal that the optimal proportion of Pd:Sn is 3:1. X-ray photoelectron spectroscopy (XPS) measurements show that when compared with 3Pd1Sn/graphene, B and N co-doping into the graphene sheet can tune the electronic structure of graphene, favoring the formation of small-sized metallic nanoparticles with good dispersion. On the other hand, when compared with the monometallic counterparts, the incorporation of Sn can generate oxygenated species that help to remove the intermediates, exposing more active Pd sites. Moreover, the electrochemical tests illustrate that 3Pd1Sn/BN-G catalyst with a moderate amount of Sn exhibits the best catalytic activity and stability on formic acid electro-oxidation, owing to the synergistic effect of the Sn doping and the B, N co-doping graphene substrate. Full article