Considerable research efforts have been dedicated to investigating the side reactions and the growth of Zn dendritic in aqueous zinc-ion batteries(AZIBs).The incorporation of organic solvents as additives in electroly...Considerable research efforts have been dedicated to investigating the side reactions and the growth of Zn dendritic in aqueous zinc-ion batteries(AZIBs).The incorporation of organic solvents as additives in electrolytes has yielded highly promising results.Nevertheless,their pervasive use has been hindered by concerns regarding their toxicity,flammability,and economic viability.Herein,we propose the utilization of γ-valerolactone(γ-V),a novel eco-friendly solvent,as an alternative for conventional organic additives to improve the performance of Zn anode.Experimental investigations and theoretical analyses have verified that γ-V additives can diminish the Zn^(2+)-desolvation energy and enhance Zn^(2+) transport kinetics.The adsorbed γ-V molecules modulate the nucleation and diffusion of Zn^(2+),facilitating Zn growth along the(002) crystal plane,thus inhibiting dendrite formation and side reactions.Consequently,the modified electrolyte with 3% γ-V exhibit highly reversible cycling for 2800 h at1 mA cm^(-2) and 1 mA h cm^(-2) in Zn//Zn symmetric cell.The Zn//KVOH coin cells deliver a capacity retention of 74.7% after 1000 cycles at 5 A g^(-1).The Zn//KVOH pouch cells maintain a capacity retention of78.7% over 90 cycles at 3 A g^(-1).Notably,the γ-V additives also effectively alleviate the self-discharge phenomenon.This work provides valuable insights on the development of aqueous zinc-ion batteries with superior safety through the modulation of electrolytes using eco-friendly additives.展开更多
A highly porous nitrogen-doped carbon sphere(NPC)electrocatalyst was prepared through the carbonization of biomass carbon spheres mixed with urea and zinc chloride in N_(2) atmosphere.The sample carbonized at.1000℃ d...A highly porous nitrogen-doped carbon sphere(NPC)electrocatalyst was prepared through the carbonization of biomass carbon spheres mixed with urea and zinc chloride in N_(2) atmosphere.The sample carbonized at.1000℃ demonstrates a superior oxygen reduction reaction(ORR)performance over the Pt/C electrocatalyst,while its contents of pyridinic nitrogen and graphitic nitrogen are the lowest among samples synthesized at the same or lower carbonization temperatures.This unusual result is explained by a space confinement effect from the microporous and mesoporous structures in the microflakes,which induces the further reduction of peroxide ions or other oxygen species produced in the first step reduction to water to have the preferred overall four electron reduction ORR process.This work demonstrates that in addition to the amount or species of its aptive sites,the space confinement can be a new approach to enhance the ORR performance of precious-metal-free,nitrogen-doped carbon electrocatalysts.展开更多
Palladium nanoparticles were deposited on the amine-grafted glass fiber mat (GFM-NH2) catalyst support by a conventional impregnation process followed by the borohydride reduction in aqueous solution at room tempera...Palladium nanoparticles were deposited on the amine-grafted glass fiber mat (GFM-NH2) catalyst support by a conventional impregnation process followed by the borohydride reduction in aqueous solution at room temperature to create the designed Pd/GFM-NH2 catalyst. By the use of large size glass fiber mat without nano/mesopores as the catalyst support, the internal mass transfer limitations due to the existence of nano/mesopores on the catalyst support were eliminated and the Pd/GFM-NH2 catalyst could be easily separated from treated water due to the large size of the catalyst support. Batch experiments demonstrate its good catalytic reduction performance of Cr(VI) with formic acid as the reducing agent. It also demonstrated an efficient Cr(VI) removal and stability in a lab-prepared, packed fixed-bed tube reactor for the continuous treatment of Cr(VI)-containing water. Thus, it has a good potential for the catalytic reduction of Cr(VI) in the water treatment practice.展开更多
基金National Natural Science Foundation of China (Grant No. 52103302, and No. 52070124)Shandong Provincial Natural Science Foundation (ZR2021QB182)+1 种基金Start-up Foundation for Senior Talents of Jiangsu University (21JDG041)China Postdoctoral Science Foundation (2023M731357)。
文摘Considerable research efforts have been dedicated to investigating the side reactions and the growth of Zn dendritic in aqueous zinc-ion batteries(AZIBs).The incorporation of organic solvents as additives in electrolytes has yielded highly promising results.Nevertheless,their pervasive use has been hindered by concerns regarding their toxicity,flammability,and economic viability.Herein,we propose the utilization of γ-valerolactone(γ-V),a novel eco-friendly solvent,as an alternative for conventional organic additives to improve the performance of Zn anode.Experimental investigations and theoretical analyses have verified that γ-V additives can diminish the Zn^(2+)-desolvation energy and enhance Zn^(2+) transport kinetics.The adsorbed γ-V molecules modulate the nucleation and diffusion of Zn^(2+),facilitating Zn growth along the(002) crystal plane,thus inhibiting dendrite formation and side reactions.Consequently,the modified electrolyte with 3% γ-V exhibit highly reversible cycling for 2800 h at1 mA cm^(-2) and 1 mA h cm^(-2) in Zn//Zn symmetric cell.The Zn//KVOH coin cells deliver a capacity retention of 74.7% after 1000 cycles at 5 A g^(-1).The Zn//KVOH pouch cells maintain a capacity retention of78.7% over 90 cycles at 3 A g^(-1).Notably,the γ-V additives also effectively alleviate the self-discharge phenomenon.This work provides valuable insights on the development of aqueous zinc-ion batteries with superior safety through the modulation of electrolytes using eco-friendly additives.
基金supported by the National Natural Science Foundation of China(Grant Nos.51672283 and 51902271)the Fundamental Research Funds for the Central Universities(Grant Nos.A1920502051907-15,2682020CX07,and 2682020CX08)+3 种基金Sichuan Science and Technology Program(Grant Nos.2020YJ0259 and 2020YJ0072)Shandong Provincial Natural Science Foundation(Grant No.ZR2019MEM045)Joint Fund between Shenyang National Laboratory for Materials Science and State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals(Grant No.18LHPY009)Liaoning Baiqianwan Talents Program.
文摘A highly porous nitrogen-doped carbon sphere(NPC)electrocatalyst was prepared through the carbonization of biomass carbon spheres mixed with urea and zinc chloride in N_(2) atmosphere.The sample carbonized at.1000℃ demonstrates a superior oxygen reduction reaction(ORR)performance over the Pt/C electrocatalyst,while its contents of pyridinic nitrogen and graphitic nitrogen are the lowest among samples synthesized at the same or lower carbonization temperatures.This unusual result is explained by a space confinement effect from the microporous and mesoporous structures in the microflakes,which induces the further reduction of peroxide ions or other oxygen species produced in the first step reduction to water to have the preferred overall four electron reduction ORR process.This work demonstrates that in addition to the amount or species of its aptive sites,the space confinement can be a new approach to enhance the ORR performance of precious-metal-free,nitrogen-doped carbon electrocatalysts.
基金supported by the Basic Science Innovation Program of Shenyang National Laboratory for Materials Science(Grant Nos.Y4N56R1161 and Y4N56F2161)the National Natural Science Foundation of China(Grant No.51502305)
文摘Palladium nanoparticles were deposited on the amine-grafted glass fiber mat (GFM-NH2) catalyst support by a conventional impregnation process followed by the borohydride reduction in aqueous solution at room temperature to create the designed Pd/GFM-NH2 catalyst. By the use of large size glass fiber mat without nano/mesopores as the catalyst support, the internal mass transfer limitations due to the existence of nano/mesopores on the catalyst support were eliminated and the Pd/GFM-NH2 catalyst could be easily separated from treated water due to the large size of the catalyst support. Batch experiments demonstrate its good catalytic reduction performance of Cr(VI) with formic acid as the reducing agent. It also demonstrated an efficient Cr(VI) removal and stability in a lab-prepared, packed fixed-bed tube reactor for the continuous treatment of Cr(VI)-containing water. Thus, it has a good potential for the catalytic reduction of Cr(VI) in the water treatment practice.