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ACS Sustainable Chemistry & Engineering · 2021 · IF 8.198

Spontaneous In Situ Surface Alloying of Li-Zn Derived from a Novel Zn2+-Containing Solid Polymer Electrolyte for Steady Cycling of Li Metal Battery

Zhen Zeng,Shang Wang,Jun Cheng,Guangmei Hou,Deping Li,Guifang Han,Lijie Ci

Solid polymer electrolytes (SPEs) are preferable in the pursuit for developing high-energy Li metal batteries due to their inherent flexibility and intimate contact with electrodes. However, continuous interfacial parasitic reactions and undesired Li dendrite growth caused by inhomogeneous plating/stripping of Li+ result in rapid deterioration of an SPE/Li interface. Herein, a novel Zn2+-containing SPE (SPE-xZn) with anionic groups partially tethered on the polymer chains is developed to meet these challenges. During cycling, Zn2+ cations inside the SPE-xZn will gradually migrate to the surface of a Li electrode and then evolve to a Li-Zn alloy layer, where Li+ can diffuse more efficiently. Meanwhile, owing to the electrostatic interaction, the immobilized anionic groups within SPE-xZn can alleviate local concentrated Li+ flux. The synergistic effects of an in situ formed alloy layer and unique macromolecular structure can promote uniform plating/stripping of Li, thus yielding a more stable SPE-xZn/Li interface. Therefore, steady cycling over 300 h at 0.2 mA cm–2 is achieved by Li/SPE-5Zn/Li, and an impressive capacity retention of 87.3% at 0.5 C after 800 cycles is realized by LFP/SPE-5Zn/Li with an average Coulombic efficiency of 99.90%.

研究领域: 材料科学 · 电化学 · 电池技术
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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

Environmentally Friendly High-Near-Infrared Reflectance Blue Pigment YIn0.9–xMn0.1MxO3−δ Based on Li/Zn Doping

Meiqi Zhang,Luo Feng,Zhiyuan Zeng,Yijie Yang,Xiaoqi Sun

In this work, the Li/Zn-doped near-infrared reflective inorganic blue pigment YIn0.9–xMn0.1MxO3−δ (M = Li/Zn, x = 0–0.4) was synthesized by the high-temperature solid-state reaction method. The phase structures, morphologies, color properties and optical properties of synthetic pigments were characterized by X-ray diffractometer (XRD), scanning electron microscope (SEM), CIE1976 color space system, UV–vis-NIR spectrophotometer, and other instruments. All the doped samples have a hexagonal structure with space group P63cm (185). Compared with YIn0.9Mn0.1O3 (b* = −45.91), Li/Zn doped pigments have richer blue hues (b* is ranged from −29.59 to −55.14), which can meet the needs of public’s demands for blue hues. The NIR solar reflectance (R*) of all the samples are above 70%, and the highest R* with different doping concentrations can reach 86% (M = Li, x = 0.2), which is about 16% higher than YIn0.9Mn0.1O3. YIn0.9–xMn0.1MxO3−δ (M = Zn/Li, x = 0–0.4) are indicated to possess higher near-infrared solar reflectivity than other blue compounds, including commercial products. The surface temperature difference between the Li-doped (x = 0.2)/Zn-doped (x = 0.1) paints and commercial ultramarine paint can reach about 20 and 10 °C, respectively. The above properties ensure the potential applications of environmentally friendly YIn0.9–xMn0.1MxO3−δ pigments with a rich blue-hue in the field of energy-saving materials.

CAS / MDL: 1314-36-9
研究领域: 材料科学 · 环境科学
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

High-performance all-solid-state lithium batteries enabled by high-conductivity free-standing sulfide electrolyte membrane and Li-Zn/LiCl bifunctional interphase

Jingguang Yi,Shuai Shi,Qi Liu,Tianxiang Yang

All-solid-state lithium batteries (ASSLBs) empolying sulfide solid electrolyte and lithium metal anode can afford improved energy density and safety. However, their large-scale application is hampered by the rigidity of ceramic–based electrolyte and the inevitable growth of lithium dendrites . Herein, a novel, flexible, high-conductivity and free-standing sulfide electrolyte membrane (Li 6 PS 5 Cl-polypropylene carbonate6, (LPSCl-PPC6)) with a thickness of 60 μm is prepared via methodology of blade coating and hot pressing, which exhibits a high Li + conductivity (3.1 × 10 −3  S cm −1  at 25 °C) and a wide electrochemical window (4.7 V vs Li + /Li) at 25 °C. Additionally, a bifunctional interphase with Li-Zn/LiCl is implanted on lithium metal surface to enhance the stability of electrolyte/lithium anode, which effectively prevents the growth of lithium dendrites and the internal short circuit of lithium symmetric battery. Benefiting from the synergistic effect, the assembled ASSLBs of S-CNTs/LPSCl-PPC6/Li-Zn/LiCl|Li and LLZO@NCM93/LPSCl-PPC6/Li-Zn/LiCl|Li exhibit high initial capacity of 1183.5 mAh g −1 (193.6 mAh g −1 ) and exceptionally cyclic stability with capacity retention of 89.2% over 150 cycles at 0.05C (93.2% over 100 cycles at 0.1C). This highly conductive sulfide-based composite electrolyte and interface engineering provides a promising strategy for achieving high performance ASSLBs.

研究领域: 材料科学 · 储能技术 · 电化学 · 固体离子学 · 锂电池
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Journal of Materials Chemistry A · 2024 ·Vol. 12 ·期 45 ·31570-31580 · IF 10.7

A mortise–tenon-like ionic/electronic conductive interface facilitates long-cycle solid-state lithium metal batteries

Guoxiang Zheng,Yifan Jin,Michal Sedlačík,Elif Vargun,Yifan Zhang,Ying He,Petr Saha,Qilin Cheng

Solid-state lithium metal batteries (SSLMBs) with high energy density and superior safety have been recognized as next-generation energy storage systems and have attracted a lot of attention. Garnet-type oxide solid-state electrolytes, especially Li6.4La3Zr1.4Ta0.6O12 (LLZTO), with high ionic conductivity, low activation energy and superior stability with Li, are among the most promising solid-state electrolyte materials. However, high interfacial resistance, uneven lithium deposition and lithium dendrite growth between Li/LLZTO interfaces have hindered the industrialization of SSLMBs. In this work, a novel mortise–tenon-like hybrid ionic/electronic conductive interface (Li/LZFC@LLZTO) is constructed, which is composed of LiF, LiCl, and a Li–Zn alloy through an in situ transformation reaction. As expected, the interfacial impedance of Li|LZFC@LLZTO|Li is significantly reduced from 128 Ω cm2 to 2.7 Ω cm2, the critical current density increases from 0.3 mA cm−2 to 2.1 mA cm−2, and a prominent cycling performance of 6600 h at 0.2 mA cm−2 or 900 h at 0.4 mA cm−2 is achieved. Consequently, both the Li|LZFC@LLZTO|LiFePO4 and Li|LZFC@LLZTO|LiNi0.8Co0.1Mn0.1O2 full cells exhibit excellent rate performance. Furthermore, Li|LZFC@LLZTO|LiFePO4 can maintain a high discharge specific capacity close to 140 mA h g−1 at 0.2C after 150 cycles of stable cycling. This work lays the foundation for developing garnet-based SSLMBs with high critical current density, low interfacial impedance and long-term cycling performance.

研究领域: 材料科学 · 储能系统 · 电池技术
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