过氧乙酸预氧化插层膨胀法制备膨胀石墨及对其导电性能的影响

本文以过氧乙酸为预氧化剂、浓硫酸为插层剂,采用化学氧化法制备了不同氧化程度的石墨层间化合物,并对其进行微波膨胀获得膨胀石墨. 本文采用SEM、XRD和FT-IR对石墨层间化合物和膨胀石墨的形貌、结构和含氧官能团的变化进行表征,研究预氧化时间对膨胀石墨膨胀容积及导电性能的影响. 结果表明,当预氧化时间为20 min时插层膨胀最好,获得的膨胀石墨膨胀容积达到275 mL/g,此时所制备的柔性石墨箔电导率达到2000 S/m,表现出极好的导电性能. 本工作为绿色制备具有高膨胀容积的膨胀石墨提供了思路.     

Dual elemental modulation in cationic and anionic sites of the multi-metal Prussian blue analogue pre-catalysts for promoted oxygen evolution reaction

Designing advanced electrocatalysts for the oxygen evolution reaction (OER) is of great significance owing to its crucial role in facilitating the production of clean hydrogen energy via water splitting. To date, it has been widely accepted that a pre-oxidation process with the in-situ generation of the catalytically active high-valence metal sites is essential for promoting the OER behavior of most transition-metal-based OER catalysts, or more felicitously speaking, pre-catalysts. Hence, exploring such pre-catalysts with high pre-oxidation reactivity is of high promise. Herein, we proposed the dual elemental modulation in the cationic and anionic sites of the multi-metal Prussian blue analogue (PBA) pre-catalysts, resulting in promoted OER behavior benefitted from the efficient pre-oxidation ability as well as the multi-metal synergy. Detailed investigations indicate that the Co-containing multi-metallic cations and mixed Fe^IIICo^III cyanide anions in NiCuCo^II–Fe^IIICo^III PBA (denoted as NiCuCo^II–Fe^IIICo^III) are beneficial to OER catalysis owing to the high intrinsic activity guaranteed by the local Co³⁺ active sites as well as the optimal multi-metal synergy. After the facile pre-oxidation process, additional high-valence Ni, Cu and Fe ions can be in-situ formed and serve as the active sites, thereby resulting in significantly improved OER behavior. For example, the OER current density of NiCuCo^II–Fe^IIICo^III exhibits 1.81 times enhancement even after 72 ?h continuous OER catalysis, and the required overpotential for 10 ?mA ?cm^?2 reduces from 288 ?mV for the fresh pre-catalyst to a remarkable record of 251 ?mV after the pre-oxidation-induced activation, making the optimal PBA-based catalyst a promising candidate for efficient and durable water electrolysis.