查看更多>>摘要:Traditional CuxO (x = 1, 2) electrodes exhibit excellent specific capacity, but the poor stress-buffering performance and inferior conductivity hinder its further application. To solve these issues, herein, we develop a built-in bifunctional ultrafine Cu nanocrystalline networks hybridized 3D hollow nanoporous CuxO (BUCN@3D-HN CuxO) integrated anode by a facile gas-phase Kirkendall effect. The 3D hollow nanoporous (3D-HN) structure can bidirectionally retard the change of stress, while the built-in ultrafine Cu nanocrystalline networks (BUCN) own the effect of providing rapid internal electron transport across the active/inert Cu/CuxO system. Benefiting from the synergistic effect of the excellent stress-buffering ability and improved electronic conductivity, the designed BUCN@3D-HN CuxO electrode delivers a high initial reversible capacity of 1.67 mAh cm- 2 under the current density of 1 mA cm- 2. Besides, a high capacity retention of 0.96 mAh cm- 2 with a high capacity retention ratio of 85.7 % is achieved even after 800 cycles at a high rate of 4 mA cm- 2. This work provides a facile yet effective method to prepare hollow nanoporous electrodes and emphasizes the significance of active/inert system, which may shed light on the design of other high-performance electrodes beyond Lithium-ion batteries.
查看更多>>摘要:In the transition to a CO2-neutral circular economy, innovative solutions for e-fuels production are imperative. This study delineates the potential of molten carbonate electrolysis, utilizing a reversible molten carbonate fuel cell technology, recognized for its efficacy in large-scale electrical power generation and CO2 capture, to steer a groundbreaking pathway to e-fuels production through molten carbon electrolyzer modality. By meticulously scrutinizing the rMCFC's electrochemical behavior under assorted thermal-flow parameters, we offer an incisive analysis of its operation in the electrolysis mode, thereby unveiling a promising avenue for high-efficiency gaseous fuel production through electrochemical reactions. The experimental study includes current-voltage assessments and electrochemical impedance spectroscopy analysis, providing an elucidative view of the cell's performance landscape. Moreover, SEM microscopy was employed in both pre- and post-mortem stages, facilitating a deep understanding of material degradation mechanisms. Our results not only enhance the contemporary comprehension of reversible cell operations but also delineate the pivotal operating parameters that are conducive to optimizing both fuel cell and electrolysis modes, signposting a highly promising route to efficient and sustainable e-fuels production for the future circular economy. This study stands as a critical milestone in harnessing the molten carbonate electrolysis technology as a corner stone on the roadmap towards achieving a high-efficiency e-fuels production ecosystem.
Kim, JaeminYang, SonggeZhong, YuTompsett, Geoffrey...
1.1-1.11页
查看更多>>摘要:High-entropy oxides (HEOs) are emerging as promising cathode materials for Li-ion batteries (LIBs) due to their stable solid-state phase and compositional flexibility. Herein, we investigate the structural and electrochemical properties of a novel non-equimolar high-entropy cathode material, termed high-entropy Li-rich layered oxide (HE-LLO, Li1.15Na0.05Ni0.19Mn0.56Fe0.02Mg0.02Al0.02O1.97F0.03), in comparison to a pristine Li-rich layered oxide (PR-LLO, Li1.2Ni0.2Mn0.6O2). The incorporation of multiple cations (Na+, Al3+, Mg2+, Fe3+) and anion (F-) into HE-LLO introduces compositional diversity, enhancing structural stability through the entropy stabilization effect. Theoretical calculations confirm a significantly higher configurational entropy in HE-LLO compared to PRLLO, supporting its high-entropy nature. Electrochemical evaluations demonstrate that HE-LLO exhibits considerable capacity retention, preserving 76.8 % of its discharge capacity at 0.5C after 200 cycles, compared to only 36.2 % for PR-LLO. Even under high-temperature conditions, HE-LLO outperformed PR-LLO, maintaining 76.1 % of its discharge capacity after 100 cycles at 5C, while PR-LLO retained only 12.4 %. These enhancements are attributed to the improved phase reversibility and higher Li+ ion diffusion coefficients of HE-LLO, validated by ex-situ characterizations using a synchrotron X-ray technique, along with density functional theory (DFT) calculations. These findings highlight the promise of non-equimolar HEOs as a novel design strategy for highperformance cathode materials.