Polymer electrolytes incorporated with fillers possess immense potential for constructing the fast and selective Li + conduction. However, the inhomogeneous distribution of the fillers usually deteriorates the microdo...
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Polymer electrolytes incorporated with fillers possess immense potential for constructing the fast and selective Li + conduction. However, the inhomogeneous distribution of the fillers usually deteriorates the microdomain consistency of the electrolytes, resulting in uneven Li + flux, and unstable electrode-electrolyte interfaces. Herein, we formulate a solution-process chemistry to in situ construct gel polymer electrolytes (GPEs) with well-dispersed metal–organic frameworks (MOFs), leading to a uniform microdomain structure. Through the integration of X-ray computed tomography analyses and theoretical simulations, our research identifies that the improvement of microdomain consistency in GPEs is beneficial for enhancing its mechanical strength, homogenizing ionic/electronic field distribution and upgrading the interface stability with the elctrodes. Moreover, consistently spread MOFs bind effectively with Lewis-base anions of Li salts, enhancing Li + kinetics. Owing to these advantages, the developed GPEs achieve a high conductivity of 1.51 mS cm −1 and a Li + transference number of 0.66, resulting in exceptional cyclability of lithium metal electrodes (over 1800 hours). Additionally, the solid-state NCM811//Li pouch batteries exhibit an impressive capacity retention of 94.2 % over 200 cycles with an N/P ratio of 1.69. This study emphasizes the significant impact of microdomain structural chemistry on the advancement of solid-state batteries.
The stability and reversibility of Zn anode can be greatly improved by in situ construction of solid electrolyte interphase (SEI) on Zn surface via a low-cost design strategy of ZnSO 4 electrolyte. However, the role o...
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The stability and reversibility of Zn anode can be greatly improved by in situ construction of solid electrolyte interphase (SEI) on Zn surface via a low-cost design strategy of ZnSO 4 electrolyte. However, the role of hydrogen bond acceptor -SO 3 accompanying ZnS formation during SEI reconstruction is overlooked. In this work, we have explored and revealed the new role of -SO 3 and ZnS in the in situ formed sulfide composite SEI (SCSEI) on Zn anode electrochemistry in ZnSO 4 aqueous electrolytes. Structure characterization and DFT demonstrate that the introduction of -SO 3 can not only reduce the dehydration energy of [Zn(H 2 O) 6 ] 2+ , but also enhance the stability of the ZnS/Zn interface and homogenize the ZnS/Zn interface electric field, thereby significantly improving the dynamic kinetics and uniform deposition of Zn 2+ . Owing to the synergistic effect of ZnS and -SO 3 , a high cycling stability of 1500 h with a cumulative-plated capacity of 7.5 Ah cm −2 at 10 mA cm −2 has been achieved within the symmetrical cell. Furthermore, the full cell with NH 4 V 4 O 10 cathode exhibits outstanding cyclic stability, exceeding 2000 cycles at 5 A g −1 and maintaining a Coulombic efficiency of 100 %. These new insights into anionic synergistic strategy could significantly enhance the practical application of zinc-ion batteries.
Proton adsorption on metallic catalysts is a prerequisite for efficient hydrogen evolution reaction (HER). However, tuning proton adsorption without perturbing metallicity remains a challenge. A Schottky catalyst base...
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Proton adsorption on metallic catalysts is a prerequisite for efficient hydrogen evolution reaction (HER). However, tuning proton adsorption without perturbing metallicity remains a challenge. A Schottky catalyst based on metal–semiconductor junction principles is presented. With metallic MoB, the introduction of n‐type semiconductive g‐C 3 N 4 induces a vigorous charge transfer across the MoB/g‐C 3 N 4 Schottky junction, and increases the local electron density in MoB surface, confirmed by multiple spectroscopic techniques. This Schottky catalyst exhibits a superior HER activity with a low Tafel slope of 46 mV dec −1 and a high exchange current density of 17 μA cm −2 , which is far better than that of pristine MoB. First‐principle calculations reveal that the Schottky contact dramatically lowers the kinetic barriers of both proton adsorption and reduction coordinates, therefore benefiting surface hydrogen generation.
Thermal runaway, a major battery safety issue, is triggered when the local temperature exceeds a threshold value resulting from slower heat dissipation relative to heat generation inside the cell. However, improving i...
Thermal runaway, a major battery safety issue, is triggered when the local temperature exceeds a threshold value resulting from slower heat dissipation relative to heat generation inside the cell. However, improving internal heat transfer is challenged by the low thermal conductivity of metal current collectors (CCs) and challenges in manufacturing nonmetal CC foils at large scales. Here we report a rapid temperature-responsive nonmetallic CC that can substitute benchmark Al and Cu foils to enhance battery safety. The nonmetallic CC was fabricated through a continuous thermal pressing process to afford a highly oriented Gr foil on a hundred-meter scale. This Gr foil demonstrates a high thermal conductivity of 1,400.8 W m−1K−1, about one order of magnitude higher than those of Al and Cu foils. Importantly, LiNi0.8Co0.1Mn0.1O2||graphite cells integrated with these temperature-responsive foils show faster heat dissipation, eliminating the local heat concentration and circumventing the fast exothermic aluminothermic and hydrogen-evolution reactions, which are critical factors causing the thermal failure propagation of lithium-ion battery packs.
The exploitation of highly efficient carbon dioxide reduction (CO 2 RR) electrocatalyst for methane (CH 4 ) electrosynthesis has attracted great attention for the intermittent renewable electricity storage but remains...
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The exploitation of highly efficient carbon dioxide reduction (CO 2 RR) electrocatalyst for methane (CH 4 ) electrosynthesis has attracted great attention for the intermittent renewable electricity storage but remains challenging. Here, N-heterocyclic carbene (NHC)-ligated copper single atom site (Cu SAS) embedded in metal–organic framework is reported (2Bn-Cu@UiO-67), which can achieve an outstanding Faradaic efficiency (FE) of 81 % for the CO 2 reduction to CH 4 at −1.5 V vs. RHE with a current density of 420 mA cm −2 . The CH 4 FE of our catalyst remains above 70 % within a wide potential range and achieves an unprecedented turnover frequency (TOF) of 16.3 s −1 . The σ donation of NHC enriches the surface electron density of Cu SAS and promotes the preferential adsorption of CHO* intermediates. The porosity of the catalyst facilitates the diffusion of CO 2 to 2Bn-Cu, significantly increasing the availability of each catalytic center.
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