Kim Minhyun, Park Seyeon, Ahn Jaewan, Baek Jong Won, Kim Dong-Ha, Shin Hamin, Ko Jaehyun, Song Lu, Park Chungseong, Shin Euichul, Kim Il-Doo
Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea.
Department of Materials Science and Chemical Engineering, Hanyang University, Ansan 15588, Republic of Korea.
ACS Sens. 2024 Dec 27;9(12):6492-6501. doi: 10.1021/acssensors.4c01852. Epub 2024 Nov 1.
Perovskite oxides are promising candidates for chemiresistive-type gas sensors owing to their exceptional thermal and chemical stability during solid-gas reactions. However, perovskites suffer from critical issues such as low surface area and poor surface activity, which negatively influence the sensing characteristics. While metal nanoparticles can be incorporated in perovskites to improve their reactivity, the fundamental incompatibility between catalytic metals and perovskite oxides often leads to substantial structural degradation as well as phase instability. Herein, we overcome this challenge through the introduction of an intermediary phase that forms coherent interfaces with both the perovskite phase and catalyst metals. Specifically, we present the case study of p-type LaCaFePtO perovskite, whose hole accumulation layer was modulated by the incorporation of metal-organic framework (MOF)-derived n-type α-FeO nanoparticles decorated with highly dispersed Pt catalysts. The resulting composite exhibited significantly improved surface activity over the nonmodified LaCaFeO perovskite, leading to exceptional chemiresistive sensing performance toward acetone gas (/ = 39.8 toward 10 ppm of acetone at 250 °C) with high cross-sensitivity against interfering gases. Importantly, our findings reaffirm the critical influence of interfacial engineering in facilitating surface chemical reactions on perovskite oxides and, by doing so, effectively provide a general synthetic guideline to the design of perovskite-based chemiresistors.
钙钛矿氧化物因其在固气反应中具有出色的热稳定性和化学稳定性,是用于化学电阻型气体传感器的有前途的候选材料。然而,钙钛矿存在诸如低表面积和差的表面活性等关键问题,这些问题会对传感特性产生负面影响。虽然可以将金属纳米颗粒掺入钙钛矿中来提高其反应活性,但催化金属与钙钛矿氧化物之间的根本不相容性通常会导致大量的结构降解以及相不稳定。在此,我们通过引入一种与钙钛矿相和催化剂金属均形成相干界面的中间相来克服这一挑战。具体而言,我们展示了p型LaCaFePtO钙钛矿的案例研究,其空穴积累层通过掺入用高度分散的Pt催化剂修饰的金属有机框架(MOF)衍生的n型α-FeO纳米颗粒进行调制。所得复合材料相对于未改性的LaCaFeO钙钛矿表现出显著改善的表面活性,从而对丙酮气体具有出色的化学电阻传感性能(在250°C下对10 ppm丙酮的/=39.8),对干扰气体具有高交叉敏感性。重要的是,我们的研究结果再次证实了界面工程在促进钙钛矿氧化物表面化学反应方面的关键影响,并且通过这样做,有效地为基于钙钛矿的化学电阻器的设计提供了一般合成指南。