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Composite polymer electrolytes (CPEs) are subject to interface incompatibilities due to the space charge layer of ceramic and polymer phases. The intensive dehydrofluorination of poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVDF‐HFP) incorporating Li7La3Zr2O12 (LLZO) significantly compromises electro‐chemo‐mechanical properties and compatibilities with electrodes. Herein, this study addresses the challenges by precisely phosphatizing LLZO surfaces through a surface Li2CO3 mediated chemical reaction. The designed neutral chemical environment of LLZO surfaces ensures high air stability and effective suppression of PVDF‐HFP dehydrofluorination. This greatly facilitates the uniform distribution of ceramic and polymer phases, and fast interfacial Li+ exchange, establishing high‐throughput ion percolation pathways and distinctly enhancing ionic conductivity and transference number. Moreover, the dramatically reduced formation of dehydrofluorination products and an in situ formed interphase layer between phosphatized surface and a Li metal anode stabilize the Li/CPE and cathode/CPE interfaces, which provide a symmetric Li/Li cell and solid‐state Li/LiFePO4 and Li/LiNi0.8Co0.1Mn0.1O2 cells an exceptional cycling performance at room temperature. This study emphasizes the vital importance of achieving electro‐chemo‐mechanical compatibilities for CPEs and provides a new waste to wealth route. [ABSTRACT FROM AUTHOR] more...

Solid-state batteries (SSBs) have been considered the most promising technology because of their superior energy density and safety. Among all the solid-state electrolytes (SEs), Li7script>La3Zr2O12 (LLZO) with high ionic conductivity (3 × 10−4 S/cm) has been widely investigated. However, its large-scale production in ambient air faces a challenge. After air exposure, the generated Li2CO3 layer deteriorates the ionic conductivity and interfacial wettability, thus greatly compromising the electrochemical performance of SSBs. Many works aim to eliminate this layer to recover the pristine LLZO surface. Unfortunately, few articles have emphasized the merits of Li2CO3. In this review, we focus on the two-sidedness of Li2CO3. We discuss the various characteristics of Li2CO3 that can be used and recapitulate the strategies that utilize Li2CO3. Insulating Li2CO3 is no longer an obstacle but an opportunity for realizing intimate interfacial contact, high air stability, and outstanding electrochemical performance. This review aims to offer insightful guidelines for treating air-induced Li2CO3 and lead to developing the enhanced air stability and electrochemical performance of LLZO. [ABSTRACT FROM AUTHOR] more...

The electrosynthesis of multi‐carbon (C2+) alcohols, specifically ethanol and n‐propanol through CO electroreduction (CORR) in H2O, presents a sustainable pathway for intermittent renewable energy storage and a low‐carbon economy. However, achieving high selectivity for alcohol production at industrial current densities is kinetically hampered by side reactions such as ethylene generation and hydrogen evolution reaction, which result from competing adsorption of *CO and *H. In this study, we developed a Cu/Zn alloy catalyst to simultaneously enhance the activity and selectivity for alcohol production by increasing CO capture capacity and enriching active hydrogen on Cu sites. Our findings demonstrate that the Cu/5Zn alloy with a molar ratio of Cu to Zn of 95 : 5 exhibits a Faradaic efficiency of 50 % for the selective electrosynthesis of C2+ alcohols during ampere‐level CO electrolysis. Mechanistic investigations revealed that the Cu/Zn alloy promotes polarized Cu sites, enhancing CO adsorption while facilitating the spillover of hydrogen atoms from Zn to Cu sites, contributing to selective alcohol formation. [ABSTRACT FROM AUTHOR] more...

Solid‐state electrolytes (SSEs) with high ionic conductivity, stability, and interface compatibility are indispensable for high‐energy‐density and long‐life all‐solid‐state batteries (ASSBs), yet there are scarce SSEs with sufficient ionic conductivity and electrochemical stability. In this study, with a high‐entropy SSE (HE‐SSE, Li2.9In0.75Zr0.1Sc0.05Er0.05Y0.05Cl6), we show the high configuration entropy has a thermodynamically positive relationship with the high‐voltage stability. As a result, the ASSBs with HE‐SSE and high‐voltage cathode materials exhibit superior high‐voltage and long‐cycle stability, achieving 250 cycles with 81.4 % capacity retention when charged to 4.8 V (vs. Li+/Li), and even 5000 cycles if charged to 4.6 V (vs. Li+/Li). Experimental characterizations and density functional theory calculations confirm that the HE‐SSE greatly suppresses the high‐voltage degradation of SSE at the interface, promoting the high‐voltage stability coordinately through high entropy and interface stability. The high entropy design offers a general strategy to simultaneously improve the high‐voltage stability and ionic conductivity of SSEs, creating an avenue to building high‐energy and long‐life ASSBs. [ABSTRACT FROM AUTHOR] more...

Li-stuffed battery materials intrinsically have surface impurities, typically Li 2 CO 3 , which introduce severe kinetic barriers and electrochemical decay for a cycling battery. For energy-dense solid-state lithium batteries (SSLBs), mitigating detrimental Li 2 CO 3 from both cathode and electrolyte materials is required, while the direct removal approaches hardly avoid Li 2 CO 3 regeneration. Here, a decarbonization-fluorination strategy to construct ultrastable LiF-rich interphases throughout the SSLBs by in situ reacting Li 2 CO 3 with LiPF 6 at 60 °C is reported. The fluorination of all interfaces effectively suppresses parasitic reactions while substantially reducing the interface resistance, producing a dendrite-free Li anode with an impressive cycling stability of up to 7000 h. Particularly, transition metal dissolution associated with gas evolution in the cathodes is remarkably reduced, leading to notable improvements in battery rate capability and cyclability at a high voltage of 4.5 V. This all-in-one approach propels the development of SSLBs by overcoming the limitations associated with surface impurities and interfacial challenges., (© 2023 Wiley‐VCH GmbH.) more...