TiO mesoporous crystal has been prepared by one-step corroding process via an oriented attachment (OA) mechanism with SrTiO as precursor. High resolution transmission electron microscopy (HRTEM) and nitrogen adsorption-desorption isotherms confirm its mesoporous crystal structure. Well-dispersed ruthenium (Ru) in the mesoporous nanocrystal TiO can be attained by the same process using Ru-doped precursor SrTiRu O. Ru is doped into lattice of TiO, which is identified by HRTEM and super energy dispersive spectrometer (super-EDS) elemental mapping. X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance spectroscopy (EPR) suggest the pentavalent Ru but not tetravalent, while partial Ti in TiO accept an electron from Ru and become Ti, which is observed for the first time. This Ru-doped TiO performs high activity for electrocatalytic hydrogen evolution reaction (HER) in alkaline solution. First-principles calculations simulate the HER process and prove TiO:Ru with Ru and Ti holds high HER activity with appropriate hydrogen-adsorption Gibbs free energies (Δ G).
Conjugated polymers with high thermoelectric performance enable the fabrication of low-cost, large-area, low-toxicity, and highly flexible thermoelectric devices. However, compared to their p-type counterparts, n-type polymer thermoelectric materials show much lower performance, which is largely due to inefficient doping and a much lower conductivity. Herein, it is reported that the development of a donor-acceptor (D-A) polymer with enhanced n-doping efficiency through donor engineering of the polymer backbone. Both a high n-type electrical conductivity of 1.30 S cm and an excellent power factor (PF) of 4.65 µW mK are obtained, which are the highest reported values among D-A polymers. The results of multiple characterization techniques indicate that electron-withdrawing modification of the donor units enhances the electron affinity of the polymer and changes the polymer packing orientation, leading to substantially improved miscibility and n-doping efficiency. Unlike previous studies in which improving the polymer-dopant miscibility typically resulted in lower mobilities, the strategy maintains the mobility of the polymer. All these factors lead to prominent enhancement of three orders magnitude in both the electrical conductivity and the PF compared to those of the non-engineered polymer. The results demonstrate that proper donor engineering can enhance the n-doping efficiency, electrical conductivity, and thermoelectric performance of D-A copolymers.
The poor ionic conductivity of transition metal oxides (TMOs) is a huge obstacle to their practical application as anodes for lithium-ion batteries (LIBs). Although good performance can be harvested by constructing nanostructures, some other foundmental issues including low tap density and serious electrolyte consumption come along. Herein, inspired by frogspawn, we propose a universal strategy of using lithium salts to assemble TMO nanoparticles into large aggregates to improve their Li + conductivity. In such a frogspawn-like structure, lithium salt networks can not only realize the rapid transmission of Li + but also alleviate the volume change during the charging/discharging process. When Li 3 PO 4 is applied to assemble iron oxides nanoparticles, aggregates with size over 1 μm and tap density up to 1.33 g cm −3 can be obtained, which even hasve an ionic conductivity up to 9.61 × 10 −5 S cm −1 . Fe 3 O 4 was also introduced through reduction to boost electron transfer. Consequently, this carbon-free composite delivered a capacity up to 896 mA h g −1 even after 1000 cycles at 5 A g −1 , which can also be maintained under high mass loading. When using lithium salts such as Li 2 SO 4 , Li 2 CO 3 , LiBO 2 , and LiCl, the corresponding composites also showed similar performance. This strategy is also effective for TMOs such as NiO, Co 3 O 4 , and ZnO, demonstrating the universality of this frogspawninspired design.
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