直接碳氢燃料金属支撑SOFC多层结构阳极及其抗积碳机理研究

Metal-support solid oxide fuel cell (MS-SOFC) has shown the advantages of low cost, easy manufacture, high strength and durability, which is considered as the research hotspot of SOFC. For direct hydrocarbon fueled SOFC, it can decrease the system complexity and cost due to the fuel internal reforming, which will facilitate the commercialization of SOFC technology and has been another research hotspot for SOFC. However, similar to AS-SOFC, the direct hydrocarbon fueled MS-SOFC will encounter the serious anode coking during the long term operation, which will destroy the anode structure and deteriorate the cell performance. This has been the key issue that should be resolved before the practical application of MS-SOFC. In this proposal, we will design a multi-layer structure anode to restrict the coking in anode to increase the stability and durability of MS-SOFC in direct hydrocarbon fuel. The multi-layer anode includes three layer, as internal reforming layer, metal support layer, and functional layer. The BaCeO3/NiCuFe internal reforming layer is constructed on metal support by an in-situ reduce route, which can realize the on-cell reforming efficiently through the optimization of the reforming catalysts. The Ni-Fe metal support will be also optimized with composition and structure. And the carbon deposition behavior on anode and the compression mechanism of carbon deposition will also be analyzed and discussed. The finding of this proposal will be beneficial to the study of high efficient coking-resistant anode for direct hydrocarbon fueled MS-SOFC.

金属支撑固体氧化物燃料电池（MS-SOFC）在成本、制造工艺、机械强度和耐久性等方面具有显著优点，是SOFC领域的研究热点。直接以碳氢化合物为SOFC的燃料，能降低因燃料外部重整带来的系统复杂性及生产成本，是当前SOFC研究另一热点方向。然而，和阳极支撑SOFC一样，直接碳氢燃料MS-SOFC阳极积碳而导致的电池性能衰减和阳极结构破坏，是一个亟待解决的关键难题。本项目针对上述问题，设计多层结构阳极以抑制阳极中的碳沉积现象，提高MS-SOFC在碳氢燃料中的长期稳定性。多层结构阳极包含重整催化层、金属支撑层和阳极功能层。利用原位烧结还原法构建BaCeO3基/NiCuFe重整催化层，实现碳氢燃料的有效重整，并结合Ni-Fe金属支撑体材料优化和结构设计，提高MS-SOFC阳极抗积碳能力。同时深入研究多层阳极上的碳沉积行为程及其抑制机理，为MS-SOFC高效抗积碳阳极设计及材料选择提供科学依据。

直接以碳氢化合物为燃料的金属支撑固体氧化物燃料电池（MS-SOFC）在成本、制造工艺、机械强度和耐久性等方面具有显著优点，且能降低因燃料外部重整带来的系统复杂性及生产成本。然而，和阳极支撑SOFC一样，直接碳氢燃料MS -SOFC阳极积碳而导致的电池性能衰减和阳极结构破坏，是一个亟待解决的关键难题。本项目针对以上技术难点，研发了具有重整催化层的金属支撑SOFC，实现了碳氢燃料的有效原位重整催化，制备了具有优良抗积碳性能的多层结构阳极，提高其在碳氢燃料中的长期稳定性；揭示了多层结构阳极上的碳沉积行为及其抑制机理。本项目所采用的三层结构阳极以提高基于碳氢燃料的金属支撑SOFC的抗积碳性能，利用重整催化层首先实现碳氢燃料的原位重整，而金属支撑层将极大提高阳极的强度、导电性和热循环性，进而在阳极功能层实现燃料气的高效电化学转化，在SOFC结构设计和技术上具有一定的特色和创新，对于解决SOFC的长期稳定性和热循环次数具有重要的参考依据。同时通过实验研究，结合第一性原理计算、原位观察以及电极三维重构等研究手段，综合研究揭示金属支撑SOFC多层结构阳极的积碳行为及抗积碳机理，对于碳氢燃料SOFC的开发，有较好的参考，具有一定的应用前景。基于上述研究成果，已成功开发了基于碳氢燃料的kW级SOFC电堆，运行时间长达1000h以上，向SOFC技术的实用化迈出了坚实的步伐。