Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)in acidic media is a promising approach to overcome the unavoidable formation of carbonates in alkaline or neutral electrolytes.However,the proton-rich environment ne...Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)in acidic media is a promising approach to overcome the unavoidable formation of carbonates in alkaline or neutral electrolytes.However,the proton-rich environment near the catalyst surface favors hydrogen evolution reactions(HER),leading to lower energy efficiency of the desired products,especially in industrial-level current densities.Here,quaternary ammonium cationic surfactant(cetyltrimethylammonium bromide(CTAB))was introduced into acidic electrolyte to modulate the interfacial microenvironment,which greatly enhanced CO_(2)electroreduction to formic acid(HCOOH)at the Bi/C nanoparticles electrode.Using a Bi/C nanoparticles electrode with CTAB added,constant production of formic acid was enabled with a cathodic energy efficiency of>40%and maximum FE_(HCOOH)(FE=Faradaic efficiency)of 86.2%at−400 mA·cm^(−2)over 24 h.Combined with in-situ attenuated total reflection Fourier transform infrared spectroscopy,the concentration of*OCHO intermediates significantly increased after CTAB modification,confirming that the hydrophobic interface microenvironment formed by dynamic adsorption of positively charged long alkyl chains on Bi/C nanoparticle electrodes inhibited HER and improved the selectivity of CO_(2)RR to HCOOH.展开更多
The electrochemical behaviors of battery chemistry,especially the operating voltage,are greatly affected by the complex electrode/electrolyte interface,but the corresponding basis understanding is still largely unclea...The electrochemical behaviors of battery chemistry,especially the operating voltage,are greatly affected by the complex electrode/electrolyte interface,but the corresponding basis understanding is still largely unclear.Herein,the concept of regulating electrode potential by interface thermodynamics is proposed,which guides the improvement of the energy density of Zn-MnO_(2) battery.A cationic electrolyte strategy is adopted to adjust the charge density of electrical double layer,as well as entropy change caused by desolvation,thus,achieving an output voltage of 1.6 V(vs.Zn^(2+)/Zn)and a capacity of 400 mAh g^(-1).The detailed energy storage behaviors are also analyzed in terms of crystal field and energy level splitting.Furthermore,the electrolyte optimization benefits the efficient operation of Zn-MnO_(2) battery by enabling a high energy density of 532 Wh kg^(-1) based on the mass of cathode and a long cyclic life of more than 500 cycles.This work provides a path for designing high-energy-density aqueous battery via electrolyte strategy,which is expected to be extended to other battery systems.展开更多
针对江铜贵冶电解车间 ISA 法残极大量断落所遇到的问题,结合生产实际操作,了解 ISA 法电解所需阳极板的工艺要求,铜电解的原理以及铜电解过程中电流强度大小、通电时间长短、电解过程中电解液液位停留的时间长短对残极断落的影响,总结...针对江铜贵冶电解车间 ISA 法残极大量断落所遇到的问题,结合生产实际操作,了解 ISA 法电解所需阳极板的工艺要求,铜电解的原理以及铜电解过程中电流强度大小、通电时间长短、电解过程中电解液液位停留的时间长短对残极断落的影响,总结造成残极断落的主要原因并针对原因提出了解决方案,从而保证了系统生产的稳定运行。展开更多
基金supported by the National Natural Science Foundation of China(Nos.52072197,22302108,21971132,and 52272222)Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(No.2023KJ313)+4 种基金Outstanding Youth Foundation of Shandong Province,China(No.ZR2019JQ14)Major Scientific and Technological Innovation Project(No.2019JZZY020405)Major Basic Research Program of Natural Science Foundation of Shandong Province(No.ZR2020ZD09)Natural Science Foundation of Qingdao(No.23-2-1-12-zyyd-jch)Qingdao Postdoctoral Researcher Applied Research Project(No.QDBSH20220202043).
文摘Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)in acidic media is a promising approach to overcome the unavoidable formation of carbonates in alkaline or neutral electrolytes.However,the proton-rich environment near the catalyst surface favors hydrogen evolution reactions(HER),leading to lower energy efficiency of the desired products,especially in industrial-level current densities.Here,quaternary ammonium cationic surfactant(cetyltrimethylammonium bromide(CTAB))was introduced into acidic electrolyte to modulate the interfacial microenvironment,which greatly enhanced CO_(2)electroreduction to formic acid(HCOOH)at the Bi/C nanoparticles electrode.Using a Bi/C nanoparticles electrode with CTAB added,constant production of formic acid was enabled with a cathodic energy efficiency of>40%and maximum FE_(HCOOH)(FE=Faradaic efficiency)of 86.2%at−400 mA·cm^(−2)over 24 h.Combined with in-situ attenuated total reflection Fourier transform infrared spectroscopy,the concentration of*OCHO intermediates significantly increased after CTAB modification,confirming that the hydrophobic interface microenvironment formed by dynamic adsorption of positively charged long alkyl chains on Bi/C nanoparticle electrodes inhibited HER and improved the selectivity of CO_(2)RR to HCOOH.
基金supported by the National Natural Science Foundation of China(52072411,51932011)the Natural Science Foundation of Hunan Province(2021JJ20060)the Fundamental Research Funds for the Central Universities of Central South University(2021zzts0093)。
文摘The electrochemical behaviors of battery chemistry,especially the operating voltage,are greatly affected by the complex electrode/electrolyte interface,but the corresponding basis understanding is still largely unclear.Herein,the concept of regulating electrode potential by interface thermodynamics is proposed,which guides the improvement of the energy density of Zn-MnO_(2) battery.A cationic electrolyte strategy is adopted to adjust the charge density of electrical double layer,as well as entropy change caused by desolvation,thus,achieving an output voltage of 1.6 V(vs.Zn^(2+)/Zn)and a capacity of 400 mAh g^(-1).The detailed energy storage behaviors are also analyzed in terms of crystal field and energy level splitting.Furthermore,the electrolyte optimization benefits the efficient operation of Zn-MnO_(2) battery by enabling a high energy density of 532 Wh kg^(-1) based on the mass of cathode and a long cyclic life of more than 500 cycles.This work provides a path for designing high-energy-density aqueous battery via electrolyte strategy,which is expected to be extended to other battery systems.
文摘针对江铜贵冶电解车间 ISA 法残极大量断落所遇到的问题,结合生产实际操作,了解 ISA 法电解所需阳极板的工艺要求,铜电解的原理以及铜电解过程中电流强度大小、通电时间长短、电解过程中电解液液位停留的时间长短对残极断落的影响,总结造成残极断落的主要原因并针对原因提出了解决方案,从而保证了系统生产的稳定运行。
