Dispersing the minuscule mass loading without hampering the high catalytic activity and long-term stability of a noble metal catalyst results in its ultimate efficacy for the electrochemical hydrogen evolution reaction (HER). Despite being the most efficient HER catalyst, the use of Pt is curtailed due to its scarcity and tendency to leach out in the harsh electrochemical reaction environment. In this study, we combined F-doped tin(IV) oxide (F-SnO 2 ) aerogel with Pt catalyst to prevent metallic corrosion and to achieve abundant Pt active sites (approximately 5 nm clusters) with large specific surface area (321 cm 2 •g −1 ). With nanoscopic Pt loading inside the SnO 2 aerogel matrix, the as-synthesized hybrid F-SnO 2 @Pt possesses a large specific surface area and high porosity and, thus, exhibits efficient experimental and intrinsic HER activity (a low overpotential of 42 mV at 10 mA•cm −2 in 0.5 M sulfuric acid), a 22-times larger turnover frequency (11.2 H 2 •s −1 ) than that of Pt/C at 50 mV, and excellent robustness over 10,000 cyclic voltammetry cycles. The existing metal support interaction and strong intermolecular forces between Pt and F-SnO 2 account for the catalytic superiority and persistence against corrosion of F-SnO 2 @Pt compared to commercially used Pt/C. Density functional theory analysis suggests that hybridization between the Pt and F-SnO 2 orbitals enhances intermediate hydrogen atom (H*) adsorption at their interface, which improves the reaction kinetics.
High‐energy‐density battery‐type materials have sparked considerable interest as supercapacitors electrode; however, their sluggish charge kinetics limits utilization of redox‐active sites, resulting in poor electrochemical performance. Here, the unique core–shell architecture of metal organic framework derived N–S codoped carbon@CoxSy micropetals decorated with Nb‐incorporated cobalt molybdate nanosheets (Nb‐CMO4@CxSyNC) is demonstrated. Coordination bonding across interfaces and π–π stacking interactions between CMO4@CxSy and N and, S–C can prevent volume expansion during cycling. Density functional theory analysis reveals that the excellent interlayer and the interparticle conductivity imparted by Nb doping in heteroatoms synergistically alter the electronic states and offer more accessible species, leading to increased electrical conductivity with lower band gaps. Consequently, the optimized electrode has a high specific capacity of 276.3 mAh g−1 at 1 A g−1 and retains 98.7% of its capacity after 10 000 charge–discharge cycles. A flexible quasi‐solid‐state SC with a layer‐by‐layer deposited reduced graphene oxide /Ti3C2TX anode achieves a specific energy of 75.5 Wh kg−1 (volumetric energy of 1.58 mWh cm−3) at a specific power of 1.875 kWh kg−1 with 96.2% capacity retention over 10 000 charge–discharge cycles.
Ultra‐high energy density battery‐type materials are promising candidates for supercapacitors (SCs); however, slow ion kinetics and significant volume expansion remain major barriers to their practical applications. To address these issues, hierarchical lattice distorted α‐/γ‐MnS@CoxSy core‐shell heterostructure constrained in the sulphur (S), nitrogen (N) co‐doped carbon (C) metal‐organic frameworks (MOFs) derived nanosheets (α‐/γ‐MnS@CoxSy@N, SC) have been developed. The coordination bonding among CoxSy, and α‐/γ‐MnS nanoparticles at the interfaces and the π–π stacking interactions developed across α‐/γ‐MnS@CoxSy and N, SC restrict volume expansion during cycling. Furthermore, the porous lattice distorted heteroatom‐enriched nanosheets contain a sufficient number of active sites to allow for efficient electron transportation. Density functional theory (DFT) confirms the significant change in electronic states caused by heteroatom doping and the formation of core‐shell structures, which provide more accessible species with excellent interlayer and interparticle conductivity, resulting in increased electrical conductivity. . The α‐/γ‐MnS@CoxSy@N, SC electrode exhibits an excellent specific capacity of 277 mA hg−1 and cycling stability over 23 600 cycles. A quasi‐solid‐state flexible extrinsic pseudocapacitor (QFEPs) assembled using layer‐by‐layer deposited multi‐walled carbon nanotube/Ti3C2TX nanocomposite negative electrode. QFEPs deliver specific energy of 64.8 Wh kg−1 (1.62 mWh cm−3) at a power of 933 W kg−1 and 92% capacitance retention over 5000 cycles.
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