Rongfang Wang

Enhancing Li⁺ transport within the solid electrolyte interphase while simultaneously inhibiting electron conduction represents an effective strategy to suppress lithium dendrite formation and mitigate interfacial volume fluctuations during charge-discharge cycling, thereby improving the electrochemical performance of lithium metal anodes. In this work, Li₃N with high Li⁺ conductivity and Li₂O with strong electronic insulation were in situ coconstructed into an interwoven SEI architecture using 3-nitro-1,2,4-triazole as a dual nitrogen-oxygen precursor, guided by density functional theory calculations. The formation mechanism of the Li₃N/Li₂O-modified lithium anode (Li₃N/Li₂O-Li) was further elucidated by in situ Raman spectroscopy. Electrochemical measurements reveal that symmetric Li∥Li cells equipped with the Li₃N/Li₂O-Li electrode exhibit a Li⁺ transference number of 0.403, surpassing those of Li₃N-Li (0.334) and bare Li (0.234). In addition, the interfacial charge-transfer resistance is significantly reduced to 53.85 Ω, compared with 77.73 Ω for Li₃N-Li and 94.69 Ω for bare Li. As a result, Li∥Li symmetric cells based on the Li₃N/Li₂O-Li anode achieve an extended cycling lifetime of 800 h at 0.5 mA cm^-2 with 0.5 mAh cm^-2, more than 11 times longer than that of bare Li. Even under more demanding conditions (1 mA cm^-2, 1 mAh cm^-2), stable operation is maintained for 630 h.

Using high-valence metals typically induces lattice distortion and suppresses crystal growth in nickel-based catalysts, leading to the formation of defect-rich amorphous structures. These isotropic amorphous catalysts, characterized by a high density of accessible active sites, hold great promise for the selective oxidation of alcohols to value-added carboxylic acids under mild conditions. Herein, a defect-rich amorphous NiO phase induced high-valence Mo doped is formed via a sequential hydrothermal and air-pyrolysis strategy for the selective oxidation of 1-propanol to propionic acid. Mo doping effectively inhibits the crystallization of, inducing while simultaneously optimizing the electronic structure of the nickel centers. This structural modulation facilitates the in situ generation of the key active species, nickel oxyhydroxide (NiOOH). Consequently, the as-prepared MoOx/NiO/NF electrode achieves a remarkable Faradaic efficiency of 91.94% for propionic acid with a high production rate of 9.98 mol h-1 m-2 at 1.5 V vs. RHE. Furthermore, the catalyst exhibits superior durability, maintaining 93.68% of its initial current density after a 12-hour chronoamperometric test, significantly outperforming the crystalline Ni(OH)2/NF benchmark (77.72%). This work provides a robust strategy for the rational design of high-performance amorphous electrocatalysts and advances the green synthesis of carboxylic acids via electrochemical oxidation.

Although the electrochemical reduction method for synthesizing sodium dithionite (Na₂S₂O₄) provides an environmentally friendly and mild route, its limited Faradaic efficiency at the electrode surface fails to meet the requirements for industrial application. Among the various catalysts explored, copper has exhibited notable catalytic activity toward the electroreduction of NaHSO₃. However, the accumulation of the sulfite radical anion (SO₂*^-) on Cu electrode surfaces severely constrains the efficiency of Na₂S₂O₄ electroproduction. In this work, copper nanoparticles as the primary active component was dispersed on a porous carbon foam, meanwhile, its electronic structure was modulated via introduced cerium with strong electron-withdrawing properties. In a bipolar membrane gap-flow electrolyzer, at a current of 210 mA, the cell voltage required to drive the electroreduction reaction over the Cu-Ce/NC electrode is only 1.53 V. The Cu-Ce/NC electrode achieves a faradaic efficiency as high as 96.7%, corresponding to a power consumption as low as 0.49 kWh·kg^-1. Long-term stability tests demonstrate that the faradaic efficiency for the electrosynthesis of TDS over this electrode remains around 95% after 60 h of continuous operation. In situ Raman spectroscopy confirmed that cerium incorporation effectively suppresses the surface accumulation of SO₂*^- and accelerates the adsorption-conversion of HSO₃^-. This study offers a route for reducing the overpotential in NaHSO₃ electroreduction and opens possibilities for the sustainable recycling of sulfur resources.