The aqueous ammonium ion hybrid supercapacitor (AIHSC) for dual-energy storage mechanisms of bulk intercalation and bulk adsorption has attracted extensive attention from researchers in the field of energy storage. However, AIHSC currently lacks sufficiently effective anode materials with high capacitance and stability. Pre-intercalated MXene electrodes have demonstrated high-capacity advantages in the fields of magnesium and zinc ion energy storage, but there have been no research reports in the field of AIHSC. Here, for the first time, pre-intercalated MXene was used as the anode material for AIHSC, and a high-performance multifunctional AIHSC was constructed by combining it with multi-walled carbon nanotubes-FeFe(CN) 6 cathode. A series of characterizations and theoretical calculations show that pre-intercalated strategies can effectively enhance the electrochemical properties of MXene. As a result, the pre-intercalated MXene anode shows a superior ammonium storage capacitance of 252 F g −1 and a high stability of 6000 cycles. The quasi-solid-state AIHSC also displays the excellent electrochemical performance and can be directly used as a pressure sensor to monitor external pressure changes and human limb movements. This study provides a viable path to the effective development of high-performance multifunctional AIHSCs and their anodes.
Three-dimensional lead halide hybrids exhibit excellent photophysical properties but suffer from inherent instability. In contrast, two-dimensional layered lead halides offer enhanced environmental stability, yet their strongly bound excitons restrict efficient charge transport. Here we present a covalent intercalation strategy involving the benchmark photosensitizer [Ru(bpy) 3 ] 2+ into a layered lead halide framework, featuring cationic [Pb 23 X 42 ] 4+ (X − = Cl − or Br − ) layers pillared by [Ru(bpy) 3 ] 2+ ligands via Pb 2+ -carboxylate coordination. This hybrid material achieves nearly full visible-light absorption and efficient photoinduced charge transfer from [Ru(bpy) 3 ] 2+ to the lead halide layers. This affords efficient CO 2 -to-CO photoreduction with an apparent quantum efficiency of ~3.0% at 500 nm, exceeding the performance of all previously reported organolead halide photocatalysts. Mechanistic studies indicate that the [Ru(bpy) 3 ] 2+ ligands enhance charge transport to Pb 2+ sites, facilitating CO 2 activation and reducing the reaction barrier for the *COOH intermediate. This work establishes a paradigm for intercalation chemistry in robust layered lead halide hybrids.
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