Gao Yifan, Liang Shuai, Jiang Chengxu, Gu Mengyao, Zhang Quanbiao, Abdelhafiz Ali, Zhang Zhen, Han Ying, Yang Yang, Zhang Xiaoyuan, Liang Peng, Li Ju, Huang Xia
State Key Laboratory of Regional Environment and Sustainability, School of Environment, Tsinghua University, Beijing 100084, China.
Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA 02139, USA.
Sci Adv. 2025 Apr 18;11(16):eads7154. doi: 10.1126/sciadv.ads7154.
Electrocatalysis exhibits certain benefits for water purification, but the low performance of electrodes severely hampers its utility. Here, we report a general strategy for fabricating high-performance three-dimensional (3D) porous electrodes with ultrahigh electrochemical active surface area and single-atom catalysts from earth-abundant elements. We demonstrate a binder-free dual electrospinning-electrospraying (DESP) strategy to densely distribute single atomic Ti and titanium oxycarbide (TiOC) sub-3-nm clusters throughout interconnected carbon nanofibers (CNs). The composite offers ultrahigh conductivity and mechanical robustness (ultrasonication resistant). The resulting TiOC filtration membrane exhibits record-high water purification capability with excellent permeability (~8370 liter m hour bar), energy efficiency (e.g., >99% removal of toxins within 1.25 s at 0.022 kWh·m per order), and erosion resistance. The hierarchical design of the TiOC membrane facilitates rapid and energy-efficient electrocatalysis through both direct electron transfer and indirect reactive oxygen species (O, OH, and O, etc.) oxidations. The electric field-confined DESP strategy provides a general platform for making high-performance 3D electrodes.
电催化在水净化方面展现出一定优势，但电极的低性能严重阻碍了其应用。在此，我们报道一种通用策略，可制备具有超高电化学活性表面积且由储量丰富的元素构成单原子催化剂的高性能三维（3D）多孔电极。我们展示了一种无粘结剂的双静电纺丝 - 电喷雾（DESP）策略，以使单个原子Ti和亚3纳米碳化钛氧基（TiOC）簇密集分布于相互连接的碳纳米纤维（CN）中。该复合材料具有超高电导率和机械强度（耐超声处理）。所得的TiOC过滤膜展现出创纪录的高水净化能力，具有优异的渗透性（约8370升·米⁻¹·小时⁻¹·巴⁻¹）、能源效率（例如，在每级0.022千瓦时·米⁻³的条件下，1.25秒内毒素去除率>99%）以及抗侵蚀性。TiOC膜的分级设计通过直接电子转移和间接活性氧（O、OH和O₂等）氧化促进快速且节能的电催化。电场限制DESP策略为制造高性能3D电极提供了一个通用平台。
