In organic photovoltaics, morphological control of donor and acceptor domains on the nanoscale is key for efficient exciton diffusion and dissociation, carrier transport, and suppression of recombination losses. To realise this, here, we demonstrated a double-fibril network based on ternary donor:acceptor morphology with multi-length scales constructed by combining ancillary conjugated polymer crystallizers and non-fullerene acceptor filament assembly. Using this approach, we achieved an average power conversion efficiency of 19.3% (certified 19.2%). The success lies in the good match between the photoelectric parameters and the morphological characteristic lengths, which utilizes the excitons and free charges efficiently. This strategy leads to enhanced exciton diffusion length (hence exciton dissociation yield) and reduced recombination rate, hence minimizing photon-to-electron losses in the ternary devices as compared to their binary counterparts. The double-fibril network morphology strategy minimizes losses and maximizes the power output, offering the possibility towards 20% power conversion efficiencies in single-junction organic photovoltaics. MainOrganic semiconductors offer the advantage of high optical absorption and tunable energy levels, enabling thin-film solar cells with high light-to-electron conversion efficiencies over a wide range of wavelengths [1][2][3][4] . Desipte recent progresses, the performance of organic solar cells (OSCs) is still limited by non-ideal exciton and charge transport, which depend not only on the electronic structure of organic semiconductors but also on the nanostructure that is formed by material crystallization and phase separation in a bulk heterojunction (BHJ) setting [5][6][7][8] . A suitable sized phase-separated morphology that balances crystalline region and mixing domain on the nanoscale is therefore needed to further push the power conversion efficiency (PCE) of OSCs, however it is a
Novel porous ZnO/ZnFe2O4/C octahedra with hollow interiors are fabricated by a facile self-sacrificing template method involving the refluxing synthesis of hollow, metal-organic framework octahedra in solution and subsequent thermal annealing in N2 . When evaluated as an anode material for lithium-ion batteries, these porous hollow ZnO/ZnFe2O4/C octahedra exhibit significantly enhanced electrochemical performances with high rate capability, high capacity, and excellent cycling stability.
Rh-based heterogeneous catalysts generally have limited selectivity relative to their homogeneous counterparts in hydroformylation reactions despite of the convenience of catalyst separation in heterogeneous catalysis. Here, we develop CoO-supported Rh single-atom catalysts (Rh/CoO) with remarkable activity and selectivity towards propene hydroformylation. By increasing Rh mass loading, isolated Rh atoms switch to aggregated clusters of different atomicity. During the hydroformylation, Rh/CoO achieves the optimal selectivity of 94.4% for butyraldehyde and the highest turnover frequency number of 2,065 h−1 among the obtained atomic-scale Rh-based catalysts. Mechanistic studies reveal that a structural reconstruction of Rh single atoms in Rh/CoO occurs during the catalytic process, facilitating the adsorption and activation of reactants. In kinetic view, linear products are determined as the dominating products by analysing reaction paths deriving from the two most stable co-adsorbed configurations. As a bridge of homogeneous and heterogeneous catalysis, single-atom catalysts can be potentially applied in other industrial reactions.
Hydrogen energy-based electrochemical energy conversion technologies offer the promise of enabling a transition of the global energy landscape from fossil fuels to renewable energy. Here, we present a comprehensive review of the fundamentals of electrocatalysis in alkaline media and applications in alkaline-based energy technologies, particularly alkaline fuel cells and water electrolyzers. Anion exchange (alkaline) membrane fuel cells (AEMFCs) enable the use of nonprecious electrocatalysts for the sluggish oxygen reduction reaction (ORR), relative to proton exchange membrane fuel cells (PEMFCs), which require Pt-based electrocatalysts. However, the hydrogen oxidation reaction (HOR) kinetics is significantly slower in alkaline media than in acidic media. Understanding these phenomena requires applying theoretical and experimental methods to unravel molecularlevel thermodynamics and kinetics of hydrogen and oxygen electrocatalysis and, particularly, the proton-coupled electron transfer (PCET) process that takes place in a proton-deficient alkaline media. Extensive electrochemical and spectroscopic studies, on single-crystal Pt and metal oxides, have contributed to the development of activity descriptors, as well as the identification of the nature of active sites, and the rate-determining steps of the HOR and ORR. Among these, the structure and reactivity of interfacial water serve as key potential and pH-dependent kinetic factors that are helping elucidate the origins of the HOR and ORR activity differences in acids and bases. Additionally, deliberately modulating and controlling catalyst−support interactions have provided valuable insights for enhancing catalyst accessibility and durability during operation. The design and synthesis of highly conductive and durable alkaline membranes/ionomers have enabled AEMFCs to reach initial performance metrics equal to or higher than those of PEMFCs. We emphasize the importance of using membrane electrode assemblies (MEAs) to integrate the often separately pursued/optimized electrocatalyst/support and membranes/ionomer components. Operando/in situ methods, at multiscales, and ab initio simulations provide a mechanistic understanding of electron, ion, and mass transport at catalyst/ionomer/membrane interfaces and the necessary guidance to achieve fuel cell operation in air over thousands of hours. We hope that this Review will serve as a roadmap for advancing the scientific understanding of the fundamental factors governing electrochemical energy conversion in alkaline media with the ultimate goal of achieving ultralow Pt or precious-metal-free highperformance and durable alkaline fuel cells and related technologies.
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