Search

The practical application of lithium–sulfur batteries (LSBs) is severely hindered by the undesirable shuttling of lithium polysulfides (LiPSs) and sluggish redox kinetics of sulfur species. Herein, a series of ultrathin single‐atomic tungsten‐doped Co3O4 (Wx‐Co3O4) nanosheets as catalytic additives in the sulfur cathode for LSBs are rationally designed and synthesized. Benefiting from the enhanced catalytic activity and optimized electronic structure by W doping, the Wx‐Co3O4 not only reduces the shuttling of LiPSs but also decreases the energy barrier of sulfur redox reactions of sulfur species, leading to accelerated electrode kinetic. As a result, LSB cathodes with the use of 5.0 wt% W0.02‐Co3O4 as the electrocatalyst show the high reversible capacities of 1217.0 and 558.6 mAh g−1 at 0.2 and 5.0 C, respectively, and maintain a high reversible capacity of 644.6 mAh g−1 at 1.0 C (1.0 C = 1675 mA g−1) after 500 cycles. With a high sulfur loading of 5.5 mg cm−2 and electrolyte–electrode ratio of 8 μLelectrolyte mgsulfur−1, the 5.0 wt% W0.02‐Co3O4‐based sulfur cathode also retains a high reversible areal capacity of 3.86 mAh cm−2 at 0.1 C after 50 cycles with an initial capacity retention of 84.7%. [ABSTRACT FROM AUTHOR]

Recently, a new seeding growth approach for perovskite thin films is reported to significantly enhance the device performance of perovskite solar cells. This work unveils the intermediate structures and the corresponding growth kinetics during conversion to perovskite crystal thin films assisted by seeding PbS nanocrystals (NCs), using time‐resolved grazing‐incidence X‐ray scattering. Through analyses of time‐resolved crystal formation kinetics obtained from synchrotron X‐rays with a fast subsecond probing time resolution, an important "catalytic" role of the seed‐like PbS NCs is clearly elucidated. The perovskite precursor‐capped PbS NCs are found to not only accelerate the nucleation of a highly oriented intermediate phase, but also catalyze the conversion of the intermediate phase into perovskite crystals with a reduced activation energy Ea = 47 (±5) kJ mol−1, compared to 145 (±38) kJ mol−1 for the pristine perovskite thin film. The reduced Ea is attributed to a designated crystal lattice alignment of the perovskite nanocrystals with perovskite cubic crystals; the pivotal heterointerface alignment of the perovskite crystals coordinated by the Pb NCs leads to an improved film surface morphology with less pinholes and enhanced crystal texture and thermal stability. These together contribute to the significantly improved photovoltaic performance of the corresponding devices. [ABSTRACT FROM AUTHOR]