Leveraging Metal Nodes in Metal-Organic Frameworks for Advanced Anodic Hydrazine Oxidation Assisted Seawater Splitting

作者：Xu, Xuefei; Chen, Hsiao-Chien; Li, Linfeng; Humayun, Muhammad; Zhang, Xia; Sun, Huachuan; Debecker, Damien P.; Zhang, Wenjun; Dai, Liming^*; Wang, Chundong^*

来源：ACS Nano, 2023, 17(11): 10906-10917.

DOI：10.1021/acsnano.3c02749

• metal-organic frameworks
• metal nodes
• electronic structure
• hydrogen evolution reaction
• hydrazine oxidation reaction

Metal-organic frameworks (MOFs) show great promisefor electrocatalysisowing to their tunable ligand structures. However, the poor stabilityof MOFs impedes their practical applications. Unlike the general pathwayfor engineering ligands, we report herein an innovative strategy forleveraging metal nodes to improve both the catalytic activity andthe stability. Our electrolysis cell with a NiRh-MOF||NiRh-MOF configurationexhibited 10 mA cm(-2) at an ultralow cell voltageof 0.06 V in alkaline seawater (with 0.3 M N2H4), outperforming its counterpart benchmark Pt/C||Pt/C cell (0.12V). Impressively, the incorporation of Rh into a MOF secured a robuststability of over 60 h even when working in the seawater electrolyte.Experimental results and theoretical calculations revealed that Rhatoms serve as the active sites for hydrogen evolution while Ni nodesare responsible for the hydrazine oxidation during the hydrazine oxidationassisted seawater splitting. This work provides a paradigm for greenhydrogen generation from seawater.

• 单位
  华中科技大学