Department of Physics , Chalmers University of Technology , 412 96 Göteborg , Sweden.
Center for Electron Nanoscopy , Technical University of Denmark , 2800 Kongens Lyngby , Denmark.
ACS Sens. 2019 May 24;4(5):1424-1432. doi: 10.1021/acssensors.9b00610. Epub 2019 May 10.
Hydrogen sensors are a prerequisite for the implementation of a hydrogen economy due to the high flammability of hydrogen-air mixtures. They are to comply with the increasingly stringent requirements set by stakeholders, such as the automotive industry and manufacturers of hydrogen safety systems, where sensor deactivation is a severe but widely unaddressed problem. In response, we report intrinsically deactivation-resistant nanoplasmonic hydrogen sensors enabled by a rationally designed ternary PdAuCu alloy nanomaterial, which combines the identified best intrinsic attributes of the constituent binary Pd alloys. This way, we achieve extraordinary hydrogen sensing metrics in synthetic air and poisoning gas background, simulating real application conditions. Specifically, we find a detection limit in the low ppm range, hysteresis-free response over 5 orders of magnitude hydrogen pressure, subsecond response time at room temperature, long-term stability, and, as the key, excellent resistance to deactivating species like carbon monoxide, notably without application of any protective coatings. This constitutes an important step forward for optical hydrogen sensor technology, as it enables application under demanding conditions and provides a blueprint for further material and performance optimization by combining and concerting intrinsic material assets in multicomponent nanoparticles. In a wider context, our findings highlight the potential of rational materials design through alloying of multiple elements for gas sensor development, as well as the potential of engineered metal alloy nanoparticles in nanoplasmonics and catalysis.
由于氢气-空气混合物的高可燃性，氢气传感器是实施氢能经济的前提条件。它们必须符合汽车行业和氢气安全系统制造商等利益相关者提出的日益严格的要求，在这些行业中，传感器失活是一个严重但广泛未得到解决的问题。有鉴于此，我们报告了一种通过合理设计的三元 PdAuCu 合金纳米材料实现的固有抗失活纳米等离子体氢气传感器，该材料结合了组成二元 Pd 合金的已确定的最佳固有属性。通过这种方式，我们在模拟实际应用条件的合成空气和中毒气体背景下实现了非凡的氢气传感指标。具体而言，我们发现其在低 ppm 范围内具有检测极限，在 5 个数量级的氢气压力下无滞后响应，在室温下具有亚秒级的响应时间，长期稳定性，以及作为关键的，对像一氧化碳这样的失活物质具有出色的抵抗力，重要的是，无需应用任何保护涂层。这是光学氢气传感器技术的重要进步，因为它能够在苛刻的条件下应用，并通过组合和协调多组分纳米颗粒中的固有材料资产，为进一步的材料和性能优化提供了蓝图。在更广泛的背景下，我们的研究结果强调了通过多种元素合金化进行气体传感器开发的合理材料设计的潜力，以及工程金属合金纳米粒子在纳米等离子体学和催化中的潜力。
