Lee Kangpyo, Kang Sukhyun, Ryu Jeong Ho, Jeon Hayun, Kim Minju, Kim Young-Kwang, Song Taeseup, Han HyukSu, Mhin Sungwook, Kim Kang Min
Korea Institute of Industrial Technology, 137-41 Gwahakdanji-ro, Gangneung-si, Gangwon 25440, Republic of Korea.
Department of Energy Engineering, Hanyang University, Seoul 04763, Republic of Korea.
ACS Appl Mater Interfaces. 2023 Dec 20;15(50):58377-58387. doi: 10.1021/acsami.3c13220. Epub 2023 Dec 11.
Alkaline water electrolysis is a vital technology for sustainable and efficient hydrogen production. However, the oxygen evolution reaction (OER) at the anode suffers from sluggish kinetics, requiring overpotential. Precious metal-based electrocatalysts are commonly used but face limitations in cost and availability. Carbon nanostructures, such as carbon nanotubes (CNTs), offer promising alternatives due to their abundant active sites and efficient charge-transfer properties. Surface modification of CNTs through techniques such as pulsed laser ablation in liquid media (PLAL) can enhance their catalytic performance. In this study, we investigate the role of surface-modified carbon (SMC) as a support to increase the active sites of transition metal-based electrocatalysts and its impact on electrocatalytic performance for the OER. We focus on CoO@SMC heterostructures, where an ultrathin layer of CoO is deposited onto SMCs using a combination of PLAL and atomic layer deposition. A comparative analysis with aggregated CoO and CoO@pristine CNTs reveals the superior OER performance of CoO@SMC. The optimized CoO@SMC exhibits a 25.6% reduction in overpotential, a lower Tafel slope, and a significantly higher turnover frequency (TOF) in alkaline water splitting. The experimental results, combined with density functional theory (DFT) calculations, indicate that these improvements can be attributed to the high electrocatalytic activity of CoO as active sites achieved through the homogeneous distribution on SMCs. The experimental methodology, morphology, composition, and their correlation with activity and stability of CoO@SMC for the OER in alkaline media are discussed in detail. This study contributes to the understanding of SMC-based heterostructures and their potential for enhancing electrocatalytic performance in alkaline water electrolysis.
碱性水电解是可持续高效制氢的一项关键技术。然而,阳极的析氧反应(OER)动力学缓慢,需要过电位。常用的贵金属基电催化剂在成本和可用性方面存在局限性。碳纳米结构,如碳纳米管(CNT),由于其丰富的活性位点和高效的电荷转移特性,提供了有前景的替代方案。通过在液体介质中脉冲激光烧蚀(PLAL)等技术对CNT进行表面改性,可以提高其催化性能。在本研究中,我们研究了表面改性碳(SMC)作为载体增加过渡金属基电催化剂活性位点的作用及其对OER电催化性能的影响。我们重点关注CoO@SMC异质结构,其中使用PLAL和原子层沉积相结合的方法将超薄CoO层沉积到SMC上。与聚集的CoO和CoO@原始CNT的对比分析揭示了CoO@SMC优异的OER性能。优化后的CoO@SMC在碱性水分解中过电位降低了25.6%,塔菲尔斜率更低,周转频率(TOF)显著更高。实验结果与密度泛函理论(DFT)计算相结合,表明这些改进可归因于CoO作为活性位点通过在SMC上均匀分布而实现的高电催化活性。详细讨论了CoO@SMC在碱性介质中OER的实验方法、形态、组成及其与活性和稳定性的相关性。本研究有助于理解基于SMC的异质结构及其在碱性水电解中增强电催化性能的潜力。