Anticorrosive Copper Current Collector Passivated by Self‐Assembled Porous Membrane for Highly Stable Lithium Metal Batteries

Abstract

The regulation of lithium plating/stripping behavior is considered to be critical for next-generation safe and high-energy-density lithium metal batteries. Lithium deposition with maximum granular size and minimum microstructural tortuosity can significantly improve the lithium plating/stripping efficiency. Here, a self-assembled organosilane layer with nanopores is constructed on Cu current collector surface via a thiol-Cu reaction. In contrast to typical stacked-particle morphology with small grain size and high specific area in ether electrolyte, dough-like and lateral-growth lithium deposition can be plated on the modified Cu current collector due to the low surface energy of a lithiophilic SiOSi membrane. The planar and dense lithium deposition contributes to the stable implementation of up to near 500 cycles in full cells with high-loading LiFePO 4 cathode. Anticorrosion in rigorous Cl-ion containing solution can even be achieved due to the corrosive repellency of hydrophobic organosilane. A high Coulombic efficiency (97.12%) is remained after corroding for 300 min. Moreover, the irreversible capacity loss caused by galvanic corrosion, an ignored but crucial aspect, has been significantly suppressed due to the passivation of high-redox-potential Cu by organosilane coating.

Facile Electroless Plating Method to Fabricate a Nickel–Phosphorus-Modified Copper Current Collector for a Lean Lithium-Metal Anode

“…Similarly, a higher percentage of SO x F y in S 2p spectra (peaks at 167.8 eV) derived from the decomposition of LiTFSI salts is detected on bare Cu. An additional SO x at 164.4 eV with a much reduced amount is detected on NiP@Cu, suggesting suppressed decomposition of lithium salts in the electrolyte . The percentage of Li–S in the inorganic Li x S component is increased from 48 to 65%, which indicates that −S atoms are prone to bond with Li atoms to form inorganic Li x S in the SEI layer on the NiP@Cu sample .…”

“…An additional SO x at 164.4 eV with a much reduced amount is detected on NiP@Cu, suggesting suppressed decomposition of lithium salts in the electrolyte. 47 The percentage of Li−S in the inorganic Li x S component is increased from 48 to 65%, which indicates that −S atoms are prone to bond with Li atoms to form inorganic Li x S in the SEI layer on the NiP@Cu sample. 48 Furthermore, the percentage of RO−Li species (∼528.4 eV), which is related to the side reactions between lithium and the electrolyte, in the NiP@Cu sample is reduced.…”

High‐Concentration Additive and Triiodide/Iodide Redox Couple Stabilize Lithium Metal Anode and Rejuvenate the Inactive Lithium in Carbonate‐Based Electrolyte

“…present high interfacial energy, Young's modulus and Li-ion conductivity, which boost the lateral growth of Li deposition and significantly restrain the dendrite growth and the derivation of dead Li 0 . [10] In spite of superior compatibility against metallic Li, LiNO 3 -modified ether-based electrolytes are still not appreciated due to their limited oxidative stability (<4 V) and conventional carbonate-based electrolytes (≈4.3 V) are still prospective candidates for high-voltage battery in short-term future. [11] Although considered to be the one of the most successful additive in ether-based electrolyte, the application of LiNO 3 in carbonatebased electrolyte has been shelved frequently due to low solubility (≈0.01 mg mL −1 ).…”

Rationalized design of hyperbranched trans-scale graphene arrays for enduring high-energy lithium metal batteries

“…S22, where the charge/discharge plateaus are well retained during cycling without obvious increase in overpotential. When comparing with the recently reported Li metal full cells (14,16,19,(37)(38)(39)(40)(41)(42)(43)(44)(45)(46)(47)(48)(49)(50)(51)(52), the Li-HVDG||LFP cell in this work is more appropriately positioned at a high areal capacity, low N/P ratio, and low E/C ratio (Fig. 6D and table S1), highly desirable for achieving a high practical energy density.…”