The electronic structures of graphene nanoflakes (GNFs) were estimated for various shapes, sizes, symmetries, and edge configurations. The Hückel molecular orbital (HMO) method was employed as a convenient way of handling the variety of possible GNF structures, since its simplicity allows the rapid solution of large system problems, such as tailoring optoelectronic characteristics of molecule containing large number of carbon atoms. The HMO method yielded the electronic structures with respect to the energy state eigenvalues, with results comparable to those obtained by other approaches, such as the tightbinding method reported elsewhere. The analyses included the consideration of various types of edge configurations of 68 GNF systems grouped by their geometric shape, reflecting symmetry. It was inferred that GNFs in the small length scale regimes, below 1 nm, which are effectively small polycyclic aromatic hydrocarbon molecules, exhibit the optoelectronic characteristic of quantum dots. This is due to the widely spaced discrete energy states, together with large energy gaps between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO). With increasing size this arrangement evolves into graphene-like ones, as revealed by the narrowing HOMO-LUMO gaps and decreasing energy differences between eigenstates. However, the changes in electronic structure are affected by the symmetries, which are related to the geometric shapes and edge configurations.

As the pace of technological advances accelerates, the role of electrical energy storage has become increasingly important. Among various storage solutions, supercapacitors are garnering significant attention. Their unique attributes, including high power density, rapid charge/discharge capabilities, and extended lifecycle, position them as a promising alternative to conventional batteries. This study investigates the synthesis of a nickel oxide (NiO) and nickel oxide/graphene oxide (NiO/GO) composite using a single-step hydrothermal method, to evaluate their potential as supercapacitor electrode materials. The synthesized NiO, graphene oxide (GO), and NiO/GO composite were comprehensively characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), and Raman spectroscopy to analyze their crystal structures and chemical bonding. The XRD analysis confirmed the formation of an NiO phase with a rhombohedral crystal structure, and no change after GO incorporation. SEM analysis revealed the formation of spherical NiO particles and porous morphology of the NiO/GO composite, which also exhibited a spherical shape. The GO displayed a randomly arranged wrinkled sheet-like structure. Electrochemical analysis of the NiO/GO composite exhibited a remarkable specific capacitance of 893 F g-1 at a current density of 1 A g-1, surpassing that of NiO and GO alone, demonstrating NiO/GO has promising performance for supercapacitor applications. The charge transfer resistance, derived from the Nyquist plot, suggests that the reduction in charge transfer resistance contributed significantly to the improved capacitance. Additional stability studies of over 5,000 cycles at 5 A g-1 revealed an 85 % initial capacitance retention, confirming the advantages of GO inclusion to improve material retention for superior long-term performance. The asymmetric supercapacitor (ASC) assembled using an electrode with the configuration NiO/GO//activated carbon (AC) showed a specific capacitance of 77.8 F g-1 obtained at a current density of 0.5 A g-1.

본 연구에서는 유기계 산화 방지제인 가려진 페놀이 그래프팅된 산화 그래핀(hindered phenol-grafted graphene oxide, HP-GO)을 합성하였고, 이를 도입한 나피온(Nafion) 기반의 복합 막을 제조하여 고분자 전해질 막 연료전지에 응용하 였다. HP-GO는 3,5-디-tert-뷰틸-4-히드록시페닐프로피오닐 클로라이드에 존재하는 염화 카보닐기(carbonyl chloride)와 GO에 존재하는 히드록시간의 치환 반응을 통해 합성되었으며, 합성된 HP-GO를 고분자 기지체 대비 0.01~0.5 wt%까지 포함하는 복합 막을 제조하여 순수 Nafion과의 물성 차이를 비교하였다. 특정 함량의 HP-GO가 첨가된 복합 막은 순수 Nafion에 비해 우수한 인장강도와 수분 흡수율 및 치수안정성을 나타내었다. 특히 HP-GO의 산화 방지 특성으로 인해 HP-GO가 첨가된 복 합 막은 장시간의 펜톤 평가(Fenton’s test) 이후 순수 Nafion 대비 높은 산화 안정성을 나타내었다. 또한 HP-GO에 의한 향상 된 수분 흡수율에 의해 복합 막은 전 습도 구간에서 순수 Nafion 대비 우수한 수소 이온 전도도를 나타내었다.

본 연구에서는 산화 방지 특성이 있는 가려진 페놀기를 도입한 산화 그래핀(hindered phenol-grafted graphene oxide, HP-GO)을 합성한 후 탄화수소계 고분자인 sulfonated poly(arylene ether sulfone) (SPAES)을 기지체로 사용한 복합 막을 제조하여 고분자 연료전지 시스템에 응용하고자 하였다. HP-GO는 GO 표면의 하이드록시기(hydroxy group)와 HP의 염화 카 보닐(carbonyl chloride) 간의 친핵성 아실치환 반응을 통해 합성되었으며, HP-GO의 비율을 다르게 첨가한 복합 막을 제조한 후 선형 SPAES 막과의 비교를 통해 성능 특성 변화를 확인하였다. 특정 함량의 HP-GO를 첨가한 복합 막의 경우 선형 SPAES 막에 비해 체적 안정성과 기계적 강도 및 수소 이온 전도도가 증가된 것을 확인할 수 있었으며, 펜톤 평가(Fenton’s test) 진행 후 막 분해 시간 및 잔여 막 무게 비율이 증가되는 경향을 통해 화학적 내구성 역시 증가한 것을 확인할 수 있었다.