Integrated Electrode-Electrolyte Optimization to Manufacture a Real-Life Applicable Aqueous Supercapacitor with Record-Breaking Lifespan

Aqueous supercapacitors(SCs)have been regarded as a promising candidate for commercial energy storage device due to their superior safety,low cost,and environmental benignity.Unfortunately,an age-old challenge of achieving both long electrode lifespan and qualified energy-storage property blocks their practical application.Herein,we develop an electrode-electrolyte integrated optimization strategy to fulfill the real-life device requirements.Electrode optimization simultaneously regulates the nanomorphology and surface chemistry of the tungsten oxide anode,resulting in superior electrochemical performance given by an ideal“bird-nest”structure with optimal oxygen vacancy status;the anodes interact with and are protected from dissolution and structural collapse by the rationally designed hybrid electrolyte with optimized pH and facilitated cation desorption behavior.Collaboratively,a record-breaking durability of no capacitive decay after 250000 cycles is achieved.On the basis of this integrated optimization,the first aqueous pouch SCs with real-life practicability were manufactured by a soft-package encapsulation technique,which can steadily power commercial 3 C products such as tablets and smartphones and maintain safely working against extreme conditions.This work demonstrates the possibility of using aqueous energy storage devices with enhanced safety and lower cost to replace the commercial organic counterparts for wide range of daily applications.

Geometric structures,electronic characteristics,stabilities,catalytic activities,and descriptors of graphene-based single-atom catalysts

Single-atom catalysts(SACs)have been a research hotspot due to their high catalytic activity,selectivity,and atomic utilization rates.However,the theoretical research of SACs is relatively fragmented,which restricts further understanding of SAC stability and activity.To address this issue,we report our analysis of the geometric structures,electronic characteristics,stabilities,catalytic activities,and descriptors of 132 graphene-based singleatom catalysts(M/GS)obtained from density functional theory calculations.Based on the calculated formation and binding energies,a stability map of M/GS was established to guide catalyst synthesis.The effects of metal atoms and support on the charge of metal atoms are discussed.The catalytic activities of M/GS in both nitrogen and oxygen reduction reactions are predicted based on the calculated magnetic moment and the adsorption energy.Combined with the electronegativity and d-band center,a two-dimensional descriptor is proposed to predict the O adsorption energy on M/GS.More importantly,this theoretical study provides predictive guidance for the preparation and rational design of highly stable and active single-atom catalysts using nitrogen doping on graphene.

Unraveling the coordination behavior and transformation mechanism of Cr^(3+) in Fe–Cr redox flow battery electrolytes

Currently,the iron chromium redox flow battery(ICRFB)has become a research hotspot in the energy storage field owing to its low cost and easily-scaled-up.However,the activity of electrolyte is still ambiguous due to its complicated solution environment.Herein,we performed a pioneering investigation on the coordination behavior and transformation mechanism of Cr^(3+)in electrolyte and prediction of impurity ions impact through quantum chemistry computations.Based on the structure and symmetry of electrostatic potential distribution,the activity of different Cr^(3+)complex ions is confirmed as[Cr(H2O)5Cl]^(2+)>[Cr(H2O)4Cl2]+>[Cr(H2O)6]^(3+).The transformation mechanism between[Cr(H2O)6]^(3+)and[Cr(H2O)5Cl]^(2+)is revealed.We find the metal impurity ions(especially Mg^(2+))can exacerbate the electrolyte deactivation by reducing the transformation energy barrier from[Cr(H2O)5Cl]^(2+)(24.38 kcal mol^(−1))to[Cr(H2O)6]^(3+)(16.23 kcal mol^(−1)).The solvent radial distribution and mean square displacement in different solvent environments are discussed and we conclude that the coordination configuration limits the diffusivity of Cr^(3+).This work provides new insights into the activity of electrolyte,laying a fundamental sense for the electrolyte in ICRFB.