Lithium-ion batteries(LIBs)featuring a Ni-rich cathode exhibit increased specific capacity,but the establishment of a stable interphase through the implementation of a functional electrolyte strategy remains challengi...Lithium-ion batteries(LIBs)featuring a Ni-rich cathode exhibit increased specific capacity,but the establishment of a stable interphase through the implementation of a functional electrolyte strategy remains challenging.Especially when the battery is operated under high temperature,the trace water present in the electrolyte will accelerate the hydrolysis of the electrolyte and the resulting HF will further erode the interphase.In order to enhance the long-term cycling performance of graphite/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)LIBs,herein,Tolylene-2,4-diisocyanate(TDI)additive containing lone-pair electrons is employed to formulate a novel bifunctional electrolyte aimed at eliminating H_(2)O/HF generated at elevated temperature.After 1000 cycles at 25℃,the battery incorporating the TDI-containing electrolyte exhibits an impressive capacity retention of 94%at 1 C.In contrast,the battery utilizing the blank electrolyte has a lower capacity retention of only 78%.Furthermore,after undergoing 550 cycles at 1 C under45℃,the inclusion of TDI results in a notable enhancement of capacity,increasing it from 68%to 80%.This indicates TDI has a favorable influence on the cycling performance of LIBs,especially at elevated temperatures.The analysis of the film formation mechanism suggests that the lone pair of electrons of the isocyanate group in TDI play a crucial role in inhibiting the generation of H_(2)O and HF,which leads to the formation of a thin and dense interphase.The existence of this interphase is thought to substantially enhance the cycling performance of the LIBs.This work not only improves the performance of graphite/NCM811 batteries at room temperature and high temperature by eliminating H_(2)O/HF but also presents a novel strategy for advancing functional electrolyte development.展开更多
Fe_(3)O_(4)and Cu_(2)O were successively immobilized on alkali-treated straw,and the magnetically separable straw@Fe_(3)O_(4)/Cu_(2)O composite was obtained.The straw@Fe_(3)O_(4)/Cu_(2)O was characterized by Fourier t...Fe_(3)O_(4)and Cu_(2)O were successively immobilized on alkali-treated straw,and the magnetically separable straw@Fe_(3)O_(4)/Cu_(2)O composite was obtained.The straw@Fe_(3)O_(4)/Cu_(2)O was characterized by Fourier transform infrared spectroscopy,X-ray diffraction,scanning electron microscopy,X-ray photoelectron spectroscopy and vibrating sample magnetometry,respectively.Photocatalytic performance of the straw@Fe_(3)O_(4)/Cu_(2)O was evaluated by measuring the degradation of methyl orange(MO)under irradiation of visible light.The introduction of Fe3O4 not only endowed the straw@Fe_(3)O_(4)/Cu_(2)O with magnetic separation feature but also significantly enhanced photocatalytic activity because Fe3O4 could prevent recombination of hole-electron pairs.The active species capture experiment showed that holes(h+),hydroxyl(∙OH)and superoxide(∙O2ˉ)radicals all took part in the MO degradation.In addition,the photocatalytic mechanism of straw@Fe_(3)O_(4)/Cu_(2)O was proposed based on the experimental results.After five cycles for the photodegradation of MO,the straw@Fe_(3)O_(4)/Cu_(2)O still displayed good photocatalytic activity,suggesting that the as-prepared composite had great potential for practical use in wastewater treatment.展开更多
Electrochemical CO_(2)reduction to C_(2)H_(4)can provide a sustainable route to reduce globally accelerating CO_(2)emissions and produce energy-rich chemical feedstocks.However,the poor selectivity in C_(2)H_(4)electr...Electrochemical CO_(2)reduction to C_(2)H_(4)can provide a sustainable route to reduce globally accelerating CO_(2)emissions and produce energy-rich chemical feedstocks.However,the poor selectivity in C_(2)H_(4)electrosynthesis limits its implementation in industrially interesting processes.Herein,we report a composite structured catalyst composed of Ag and Cu_(2)O with different crystal faces to achieve highly efficient reduction of CO_(2)to C_(2)H_(4).The catalyst composed of Ag and octahedral Cu_(2)O enclosed with(111)facet exhibits the best CO_(2)electroreduction performance,with the Faradaic efficiency(FE)and partial current density reaching 66.8%and 17.8 mA cm2 for C_(2)H_(4)product at-1.2 VRHE in 0.5 M KHCO_(3),respectively.Physical characterization and electrochemical test analysis indicate that the high selectivity for C_(2)H_(4)product stems from the synergistic effect of crystal faces control engineering and tandem catalysis.Specifically,Ag can provide optimal availability of CO intermediate by suppressing hydrogen evolution;subsequently,C-C coupling is promoted on the intimate surface of Cu_(2)O with facetdependent selectivity.The insights gained from this work may be beneficial for designing efficient multicomponent catalysts for improving the selectivity of electrochemical CO_(2)reduction reaction to generate C2þproducts.展开更多
基金financially supported by the Scientific and Technological Plan Projects of Guangzhou City(202103040001),P.R.Chinathe Project of Science and Technology Department of Henan Province(222102240074)the Key Research Programs of Higher Education Institutions of Henan Province(24B150009)。
文摘Lithium-ion batteries(LIBs)featuring a Ni-rich cathode exhibit increased specific capacity,but the establishment of a stable interphase through the implementation of a functional electrolyte strategy remains challenging.Especially when the battery is operated under high temperature,the trace water present in the electrolyte will accelerate the hydrolysis of the electrolyte and the resulting HF will further erode the interphase.In order to enhance the long-term cycling performance of graphite/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)LIBs,herein,Tolylene-2,4-diisocyanate(TDI)additive containing lone-pair electrons is employed to formulate a novel bifunctional electrolyte aimed at eliminating H_(2)O/HF generated at elevated temperature.After 1000 cycles at 25℃,the battery incorporating the TDI-containing electrolyte exhibits an impressive capacity retention of 94%at 1 C.In contrast,the battery utilizing the blank electrolyte has a lower capacity retention of only 78%.Furthermore,after undergoing 550 cycles at 1 C under45℃,the inclusion of TDI results in a notable enhancement of capacity,increasing it from 68%to 80%.This indicates TDI has a favorable influence on the cycling performance of LIBs,especially at elevated temperatures.The analysis of the film formation mechanism suggests that the lone pair of electrons of the isocyanate group in TDI play a crucial role in inhibiting the generation of H_(2)O and HF,which leads to the formation of a thin and dense interphase.The existence of this interphase is thought to substantially enhance the cycling performance of the LIBs.This work not only improves the performance of graphite/NCM811 batteries at room temperature and high temperature by eliminating H_(2)O/HF but also presents a novel strategy for advancing functional electrolyte development.
基金Science and Technology Project from Ministry of Housing and Urban-Rural Development of the People’s Republic of China(No.2014-K7-007)。
文摘Fe_(3)O_(4)and Cu_(2)O were successively immobilized on alkali-treated straw,and the magnetically separable straw@Fe_(3)O_(4)/Cu_(2)O composite was obtained.The straw@Fe_(3)O_(4)/Cu_(2)O was characterized by Fourier transform infrared spectroscopy,X-ray diffraction,scanning electron microscopy,X-ray photoelectron spectroscopy and vibrating sample magnetometry,respectively.Photocatalytic performance of the straw@Fe_(3)O_(4)/Cu_(2)O was evaluated by measuring the degradation of methyl orange(MO)under irradiation of visible light.The introduction of Fe3O4 not only endowed the straw@Fe_(3)O_(4)/Cu_(2)O with magnetic separation feature but also significantly enhanced photocatalytic activity because Fe3O4 could prevent recombination of hole-electron pairs.The active species capture experiment showed that holes(h+),hydroxyl(∙OH)and superoxide(∙O2ˉ)radicals all took part in the MO degradation.In addition,the photocatalytic mechanism of straw@Fe_(3)O_(4)/Cu_(2)O was proposed based on the experimental results.After five cycles for the photodegradation of MO,the straw@Fe_(3)O_(4)/Cu_(2)O still displayed good photocatalytic activity,suggesting that the as-prepared composite had great potential for practical use in wastewater treatment.
基金This work was supported by the University of Science and Technology Beijing.DG acknowledges the financial support from 111 Project(no.B170003)Foshan Science and Technology Innovation Project(no.2018IT100363).
文摘Electrochemical CO_(2)reduction to C_(2)H_(4)can provide a sustainable route to reduce globally accelerating CO_(2)emissions and produce energy-rich chemical feedstocks.However,the poor selectivity in C_(2)H_(4)electrosynthesis limits its implementation in industrially interesting processes.Herein,we report a composite structured catalyst composed of Ag and Cu_(2)O with different crystal faces to achieve highly efficient reduction of CO_(2)to C_(2)H_(4).The catalyst composed of Ag and octahedral Cu_(2)O enclosed with(111)facet exhibits the best CO_(2)electroreduction performance,with the Faradaic efficiency(FE)and partial current density reaching 66.8%and 17.8 mA cm2 for C_(2)H_(4)product at-1.2 VRHE in 0.5 M KHCO_(3),respectively.Physical characterization and electrochemical test analysis indicate that the high selectivity for C_(2)H_(4)product stems from the synergistic effect of crystal faces control engineering and tandem catalysis.Specifically,Ag can provide optimal availability of CO intermediate by suppressing hydrogen evolution;subsequently,C-C coupling is promoted on the intimate surface of Cu_(2)O with facetdependent selectivity.The insights gained from this work may be beneficial for designing efficient multicomponent catalysts for improving the selectivity of electrochemical CO_(2)reduction reaction to generate C2þproducts.
