天津大学凌涛团队报道，将Fe–N–C单原子催化剂转化为，质子交换膜燃料电池用的新型FeN_xSe_y簇催化剂。相关论文于2025年1月21日发表在《德国应用化学》杂志上。

Fe-N-C催化剂是质子交换膜燃料电池（PEMFC）中，最有前途的铂催化剂替代品，但其高性能在器件中不能保持足够长的时间。在Fe-N-C催化剂中构建不同于方形平面Fe-N 4构型的，新型铁配位环境有望打破电流稳定性的限制，但这方面的研究仍未得到充分探索。

研究团队报道了Fe-N-C转化为一种新的FeN_xSe_y催化剂，其中Fe位是由N和Se原子三维共配的。FeN_xSe_y催化剂表现出比Fe-N-C催化剂更好的4e^- ORR活性和选择性。具体来说，FeN_xSe_y上H₂O₂和·OH自由基的产率分别只有Fe-N-C上的1/4和1/3。

因此，FeN_xSe_y催化剂表现出出色的稳定性，在10,000次循环后，在E1/2中仅损失10 mV，远远小于Fe-N-C催化剂（56 mV），代表了迄今为止报道的最稳定的无Pt催化剂。此外，在H₂O₂存在下，三维共配结构抑制了Fe的脱金属。结果表明，FeN_xSe_y基PEMFC表现出优异的耐久性，在加速耐久性测试后，电流密度衰减显著低于Fe-N-C为基础器件。

附：英文原文

Title: Converting Fe–N–C single-atom catalyst to a new FeNxSey cluster catalyst for proton-exchange membrane fuel cells

Author: Yang Zhao, Pengfei Yin, Yuanyuan Yang, Ruguang Wang, Cairong Gong, Jisi Li, Jiaxin Guo, Quanlu Wang, Tao Ling

Issue&Volume: 2025-01-21

Abstract: Fe–N–C catalyst is the most promising alternative to platinum catalyst for proton-exchange membrane fuel cells (PEMFCs), however its high performance cannot be maintained for a long enough time in device. The construction of a new Fe coordination environment that is different from the square-planar Fe–N 4 configuration in Fe–N–C catalyst is expected to break current stability limits, which however remains unexplored. Here, we report the conversion of Fe–N–C to a new FeNxSey catalyst, where the Fe sites are three-dimensionally (3D) co-coordinated by N and Se atoms. The FeNxSey catalyst exhibits much better 4e– ORR activity and selectivity than the Fe–N–C catalyst. Specifically, the yields of H2O2 and ·OH radicals on FeNxSey are only one-quarter and one-third of that on Fe–N–C, respectively. Therefore, the FeNxSey catalyst exhibits outstanding stability, losing only 10 mV in E1/2 after 10,000 cycles, much smaller than that of the Fe–N–C catalyst (56 mV), representing the most stable Pt-free catalysts ever reported. Moreover, the 3D co-coordination structure inhibits the Fe demetallization in the presence of H2O2. As a result, the FeNxSey based PEMFC shows excellent durability, with the current density attenuation significantly lower than that of the Fe–N–C based device after accelerated durability testing.

DOI: 10.1002/anie.202419501

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202419501