The surface chemistry of solid electrolyte interphase is one of the critical factors that govern the cycling life of rechargeable batteries. However, this chemistry is less explored for zinc anodes, owing to their relatively high redox potential and limited choices in electrolyte. Here, we report the observation of a zinc fluoride-rich organic/inorganic hybrid solid electrolyte interphase on zinc anode, based on an acetamide-Zn(TFSI)2 eutectic electrolyte. A combination of experimental and modeling investigations reveals that the presence of anion-complexing zinc species with markedly lowered decomposition energies contributes to the in situ formation of an interphase. The as-protected anode enables reversible (~100% Coulombic efficiency) and dendrite-free zinc plating/stripping even at high areal capacities (>2.5 mAh cm‒2), endowed by the fast ion migration coupled with high mechanical strength of the protective interphase. With this interphasial design the assembled zinc batteries exhibit excellent cycling stability with negligible capacity loss at both low and high rates.
Conventional wisdom is that the MAI and FAI are stable in the solution, but actually they are not. We demonstrated that the MAI first deprotonated to form methylamine (MA), and then MA reacted with FAI to form two condensation products N-methyl FAI and N, N 0 -dimethyl FAI. Moreover, triethyl borate was introduced to stabilize the perovskite precursor solution, which significantly reduced the impure phase in the perovskite film and enhanced the device performance and reproducibility.
Nonflammable functional electrolytes with remarkably interfacial compatibility toward both lithium anodes and high-voltage cathodes are considered as the ultimate pursuit for rechargeable lithium metal battery. For this target, we report a dual-anion deep eutectic solution (D-DES) based on elaborately selected combination of nitrile and functional lithium salts. The interactions of succinonitrile with cation/anion are highlighted by in situ/ex situ measurements, which endow D-DES with excellent ionic conductivity and significantly enhanced interface stability. By using this D-DES, constant Li|Li cycling over 1 year (>10,000 h) under a Li capacity of 5 mA h cm–2 can be achieved. The capacity retention is still over 70% with a high charging voltage of 4.7 V for 500 cycles in LiCoO2|Li battery. Pouch cells with high areal capacity close to practical application also deliver superior safe performance. This study paves a new pathway for designing high-safety electrolyte and boosts the practical application of high-voltage lithium metal battery.
plating/stripping. [7][8][9][10][11][12][13][14][15] As a result, LMB always suffer from rapid capacity deterioration and high safety risk, especially at high charge/discharge rates and over a wide temperature range (from subzero temperatures to high temperatures). Encouragingly, varied strategies have been devoted to explore the Li-dendrite growth mechanism and Li-metal protection. [16][17][18][19][20][21][22][23][24][25][26][27][28][29][30] Wherein, one of the most effective and feasible strategy in protecting Li metal is electrolyte optimization, such as developing ionic liquids, [16] dual-salt electrolytes with additives, [20] gel polymer electrolyte, [18,27,28] concentrated electrolytes, [9,[24][25][26]29,30] etc.Undoubtedly, wide temperature range high-energy LMBs are urgently demanded for special applications, such as carrying out special missions in polar areas, desert areas, snowy mountains region, and outer space. [31] However, the operation of LMBs over a wide temperature range is seldom reported because of the fact that it is a huge challenge to find a compromise between subzero temperature performances and high temperature performances. [31][32][33] At subzero temperatures, due to the significantly reduced Li + conductivity (increased viscosity) of electrolyte and simultaneously increased charge transfer resistances, the severe growth of Li dendrites will become more uncontrolled. [31,34] At high temperatures, the bottlenecks are thermal instability of conventional LiPF 6 salt, severe solid electrolyte interphase (SEI) layer destruction-reformation accompanied by severe gas evolution, and accelerated transition metal dissolution-migration-deposition. [31] Significantly, formulating an electrolyte will play a dominant role in enabling the wide temperature operation of LMBs.Dual-salt electrolyte systems adopting two thermally stable main lithium salts have been proposed to significantly enhance the performances of both LIBs and LMBs. [20,[33][34][35][36][37][38][39][40][41][42] For the wide temperature operation of LIBs, thermally stable lithium borates (such as lithium tetrafluoroborate (LiBF 4 ), lithium bis(oxalato)borate (LiBOB), lithium difluoro(oxalate)borate (LiDFOB), etc.) dissolved in low melting point and high boiling point carbonatebased solvents (such as propylene carbonate (PC, T m = −48.8 °C, T b = 242 °C), ethyl methyl carbonate (EMC, T m = −53 °C, T b = 110 °C), etc.), have been investigated. [33][34][35][36][37][38] Recently, we have reviewed the potential application of functional lithium-borate salts in high performance lithium batteries, [43] and have successfully synthesized a bulky anion lithium trifluoro(perfluoro-tert-butyloxyl)borate (Li[(CF 3 ) 3 COBF 3 ], LiTFPFB), which exhibits high Li + conductivity and oxidation stability, as well as noncorrosivity to In this study, self-synthesized lithium trifluoro(perfluoro-tert-butyloxyl) borate (LiTFPFB) is combined with lithium bis(trifluoromethanesulfonyl) imide (LiTFSI) to formulate a novel 1 m dual-salt electrolyte, which contain...
Photodynamic therapy (PDT) usually aggravates tumor hypoxia, which promotes the survival and metastasis of residue cancer cells; furthermore, although PDT‐induced immunogenic death of cancer cells can induce host antitumor responses, such responses are generally weak and not enough to eliminate the residue cancer cells. Here, metal–organic framework (MOF)‐based nanoparticles to combine PDT, antihypoxic signaling, and CpG adjuvant as an in situ tumor vaccine to boost host anticancer responses after PDT are designed. The MOF‐based nanoparticles are self‐assembled from H2TCPP and zirconium ions with hypoxia inducible factor (HIF) signaling inhibitor (ACF) and immunologic adjuvant (CpG) loading, and hyaluronic acid (HA) coating on the surface. The final nanoparticles (PCN‐ACF‐CpG@HA) can specifically target cancer cells overexpressing CD44 receptor though HA; the aggravated hypoxic survival signaling after PDT can be blocked by ACF to inhibit the HIF‐1α induced survival and metastasis. With the help of CpG adjuvant, the tumor associated antigens generated from PDT‐based cancer cell destruction can initiate strong antitumor immune responses to eliminate residue cancer cells. Taken together, a novel in situ immunostimulatory strategy is designed to synergistically enhance therapeutic effects of PDT by activating host antitumor immune‐responses both in vitro and in vivo, which may have great potential for clinical translation in future.
Gene delivery as a promising and valid tool has been used for treating many serious diseases that conventional drug therapies cannot cure. Due to the advancement of physical technology and nanotechnology, advanced physical gene delivery methods such as electroporation, magnetoporation, sonoporation and optoporation have been extensively developed and are receiving increasing attention, which have the advantages of briefness and nontoxicity. This review introduces the technique detail of membrane perforation, with a brief discussion for future development, with special emphasis on nanoparticles mediated optoporation that have developed as an new alternative transfection technique in the last two decades. In particular, the advanced physical approaches development and new technology are highlighted, which intends to stimulate rapid advancement of perforation techniques, develop new delivery strategies and accelerate application of these techniques in clinic.
Discovering the underlying reason for Li anode failure is ac ritical step towards applications of lithium metal batteries (LMBs). In this work, we conduct deuterium-oxide (D 2 O) titration experiments in an ovel on-line gas analysis mass spectrometry (MS) system, to determine the content of metallic Li and lithium hydride (LiH) in cycled Li anodes disassembled from practical LiCoO 2 /Li LMBs.T he practical cell is comprised of ultrathin Li anode (50 mm), high loading LiCoO 2 (17 mg cm À2 ,2 .805 mAh cm À2)a nd different formulated electrolytes.O ur results suggest that the amount of LiH accumulation is negatively correlated with cyclability of practical LMBs.M ore importantly,w er eveal at emperature sensitive equilibrium (Li + 1/2 H 2 Ð LiH) governing formation and decomposition process of LiH at Li anode.Webelieve that the unusual understanding provided by this study will draw forth more insightful efforts to realizee fficient Li protection and the ultimate applications of "holy grail" LMBs.
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