Revealing the key role of non-solvating diluents for fast-charging and low temperature Li-ion batteries

Fast-charging and low temperature operation are of vital importance for the further development of lithium-ion batteries(LIBs),which is hindered by the utilization of conventional carbonate-based electrolytes due to their slow kinetics,narrow operating temperature and voltage range.Herein,an acetonitrile(AN)-based localized high-concentration electrolyte(LHCE)is proposed to retain liquid state and high ionic conductivity at ultra-low temperatures while possessing high oxidation stability.We originally reveal the excellent thermal shielding effect of non-solvating diluent to prevent the aggregation of Li^(+) solvates as temperature drops,maintaining the merits of fast Li transport and facile desolvation as at room temperature,which bestows the graphite electrode with remarkable low temperature performance(264 mA h g^(-1) at-20 C).Remarkably,an extremely high capacity retention of 97%is achieved for high-voltage high-energy graphite||NCM batteries after 250 cycles at-20 C,and a high capacity of 110 mA h g^(-1)(71%of its room-temperature capacity)is retained at-30°C.The study unveils the key role of the non-solvating diluents and provides instructive guidance in designing electrolytes towards fast-charging and low temperature LIBs.

Shorter alkyl chain in thieno[3,4-c]pyrrole-4,6-dione(TPD)-based large bandgap polymer donors – Yield efficient non-fullerene polymer solar cells

Typically,conjugated polymers are composed of conjugated backbones and alkyl side chains.In this contribution,a cost-effective strategy of tailoring the length of alkyl side chain is utilized to design highperforming thieno[3,4-c]pyrrole-4,6-dione(TPD)-based large bandgap polymer donors PBDT-BiTPD(Cχ)(χ=48,52,56),in which x represents the alkyl side chain length in term of the total carbon number.A combination of light absorption,device,and morphology examinations make clear that the shorter alkyl side chains yield(i) higher crystallinity and more predominant face-on crystallite orientation in their neat and BHJ blend films,(ii) higher charge mobilities(6.7×10^(-4) cm~2 V^(-1) s^(-1) for C48 vs.3.2×10^(-4) cm~2 V^(-1) s^(-1) for C56),and negligible charge recombination,consequently,(iii) significantly improved fill-factor(FF) and short current(J_(SC)),while almost the same open circuit voltage(V_(OC)) of ca.0.82 V in their corresponding BHJ devices.In parallel,as alkyl side chain lengths decrease from C56 to C48,power conversion efficiencies(PCEs) increased from 7.8% for C56 to 11.1% for C52,and further to14.1% for C48 in their BHJ solar cells made with a narrow bandgap non-fullerene acceptor Y6.This systematic study declares that shortening the side chain,if providing appropriate solubility in device solution processing solvents,is of essential significance for developing high-performing polymer donors and further improving device photovoltaic performance.

Isolated diatomic Zn-Co metal–nitrogen/oxygen sites with synergistic effect on fast catalytic kinetics of sulfur species in Li-S battery

Lithium-sulfur batteries are severely restricted by low electronic conductivity of sulfur and Li_(2)S,shuttle effect,and slow conversion reaction of lithium polysulfides(LiPSs).Herein,we report a facile and highyield strategy for synthesizing dual-core single-atom catalyst(ZnCoN_(4)O_(2)/CN)with atomically dispersed nitrogen/oxygen-coordinated Zn-Co sites on carbon nanosheets.Based on density functional theory(DFT)calculations and LiPSs conversion catalytic ability,ZnCoN_(4)O_(2)/CN provides dual-atom sites of Zn and Co,which could facilitate Li^(+)transport and Li_(2)S diffusion,and catalyze LiPSs conversion more effectively than homonuclear bimetallic single-atom catalysts or their simple mixture and previously reported singleatom catalysts.Li-S cell with ZnCoN_(4)O_(2)/CN modified separator showed excellent rate performance(789.4 mA h g^(-1)at 5 C)and stable long cycle performance(0.05%capacity decay rate at 6C with 1000cycles,outperforming currently reported single atomic catalysts for LiPSs conversion.This work highlights the important role of metal active centers and provides a strategy for producing multifunctional dual-core single atom catalysts for high-performance Li-S cells.

Synergistic Effect of High Donor Electrolyte and Catalytic Separator for Practical Lithium–Sulfur Batteries

The commercialization of lithium-sulfur(Li-S)batteries has been hampered by the low utilization of S,resulting in low practical energy density and the severe shuttle effect of lithium polysulfides(LiPSs)that leads to poor cycle life.Herein,a combined strategy of electrolyte engineering and separator functionalization was proposed to solve the conflict between high S utilization and cycling life.We have demonstrated that the high donor electrolyte regulates the solvation of LiPSs with the formation of S_(3)^(·-)to induce radical-assisted efficient conversion pathway and threedimensional(3D)Li2S deposition,which greatly enhanced the S utilization while exacerbating the shuttling of LiPSs.Fortunately,the carbon nanosheet-based modified separator with abundant Zn-Co diatomic metal sites efficiently inhibited the shuttling of LiPSs by catalyzing the conversion reaction of LiPSs.Hence,the resulting Li-S battery delivered a remarkably high capacity of 1300 mAh g^(-1) with a high average coulombic efficiency of 99.4% during cycling.Even at a high S mass loading(9.3 mg cm^(-2))and lean electrolyte condition(E/S=3μL mg^(-1)),the Li-S battery still delivered a high capacity of 1088 mAh g^(-1),representing a significant advancement in designing practically high energy Li-S batteries with long cycle life.