Low-overpotential layered hydroxides(LDHs)with high theoretical capacity are promising electrodes for supercapaterry and oxygen evolution reaction;however,the low electronic conductivity and insufficient active sites ...Low-overpotential layered hydroxides(LDHs)with high theoretical capacity are promising electrodes for supercapaterry and oxygen evolution reaction;however,the low electronic conductivity and insufficient active sites of bulk LDHs increase the internal resistance and reduce the capacity and oxygen-production efficiency of electrodes.Herein,we prepared a polyaniline-coated Ni-Co-layered double hydroxide intercalated with MoO_(4)^(2−)(M-LDH@PANI)composite electrode using a two-step method.As the amount of MoO_(4)^(2−)in the LDH increases,acicular microspheres steadily evolve into flaky microspheres with a high surface area,providing more active electrochemical sites.Moreover,the amorphous PANI coating of M-LDH boosts the electronic conductivity of the composite electrode.Accordingly,the M-LDH@PANI at an appropriate level of MoO_(4)^(2−)exhibits significantly enhanced energy storage and catalytic performance.Experimental analyses and theoretical calculations reveal that a small amount of MoO_(4)^(2−)is conducive to the expansion of LDH interlayer spacing,while an excessive amount of MoO_(4)^(2−)combines with the H atoms of LDH,thus competing with OH^(−),resulting in reduced electrochemical performance.Moreover,M-LDH flaky microspheres can efficiently modulate deprotonation energy,greatly accelerating surface redox reactions.This study provides an explanation for an unconventional mechanism,and a method for the modification of LDH-based materials for anion intercalation.展开更多
Layered intercalated functional materials of layered double hydroxide type are an important class of functional materials developed in recent years. Based on long term studies on these materials in the State Key Labor...Layered intercalated functional materials of layered double hydroxide type are an important class of functional materials developed in recent years. Based on long term studies on these materials in the State Key Laboratory of Chemical Resource Engineering in Beiiing University of Chemical Technology, the orinciole for the design of controlled intercalation processes in the light of tuture production processing requirements has been developed. Intercalation assembly methods and technologies have been invented to control the intercalation process for preparing layered intercalated materials with various structures and functions.展开更多
The hydrotalcite-like compound [Zn2Al·（OH）6] NO3·nH2O and [Mg2Al·（OH）6] NO3·nH2O （shorted as ZnA1-NO3 and MgAl-NO3） was intercalated with the chelating agent EDTA （Ethylenediaminetetraacetic...The hydrotalcite-like compound [Zn2Al·（OH）6] NO3·nH2O and [Mg2Al·（OH）6] NO3·nH2O （shorted as ZnA1-NO3 and MgAl-NO3） was intercalated with the chelating agent EDTA （Ethylenediaminetetraacetic Acid） and EDDS （N, N＇-1, 2-Ethanediylbis-1-Aspartic Acid） by anion exchange. The materials synthesized in this work were characterized by chemical analysis, FT-IR （Fourier Transform Infrared Spectroscopy）, SEM （Scanning Electron Microscopy） and XRD （Powder X-ray Diffraction） to confirm their properties. In order to discuss the adsorption capacity of LDHs （Layered Double Hydroxides）, the adsorption experiment was investigated under the optimum condition （10 mg, 25℃ and 100 μg·L-1）. The amount of metallic ions adsorbed by LDHs intercalated with EDTA and precursor LDHs were determined by ICP-AES （Inductively Coupled Plasma-Atomic Emission Spectrometry） and AAS （Atomic Absorption Spectrometry）. The intercalation of EDTA leads to improve the adsorption capacity of LDHs. LDHs intercalated with chelating agents have generally high affinity for removing metallic ions, and they can be efficient adsorbents for metallic ions.展开更多
文摘Low-overpotential layered hydroxides(LDHs)with high theoretical capacity are promising electrodes for supercapaterry and oxygen evolution reaction;however,the low electronic conductivity and insufficient active sites of bulk LDHs increase the internal resistance and reduce the capacity and oxygen-production efficiency of electrodes.Herein,we prepared a polyaniline-coated Ni-Co-layered double hydroxide intercalated with MoO_(4)^(2−)(M-LDH@PANI)composite electrode using a two-step method.As the amount of MoO_(4)^(2−)in the LDH increases,acicular microspheres steadily evolve into flaky microspheres with a high surface area,providing more active electrochemical sites.Moreover,the amorphous PANI coating of M-LDH boosts the electronic conductivity of the composite electrode.Accordingly,the M-LDH@PANI at an appropriate level of MoO_(4)^(2−)exhibits significantly enhanced energy storage and catalytic performance.Experimental analyses and theoretical calculations reveal that a small amount of MoO_(4)^(2−)is conducive to the expansion of LDH interlayer spacing,while an excessive amount of MoO_(4)^(2−)combines with the H atoms of LDH,thus competing with OH^(−),resulting in reduced electrochemical performance.Moreover,M-LDH flaky microspheres can efficiently modulate deprotonation energy,greatly accelerating surface redox reactions.This study provides an explanation for an unconventional mechanism,and a method for the modification of LDH-based materials for anion intercalation.
基金Supported by the National Key Technologies R＆D Program （2011BAE28B01） and the National Natural Science Foundation of China （21276016）.
文摘Layered intercalated functional materials of layered double hydroxide type are an important class of functional materials developed in recent years. Based on long term studies on these materials in the State Key Laboratory of Chemical Resource Engineering in Beiiing University of Chemical Technology, the orinciole for the design of controlled intercalation processes in the light of tuture production processing requirements has been developed. Intercalation assembly methods and technologies have been invented to control the intercalation process for preparing layered intercalated materials with various structures and functions.
文摘The hydrotalcite-like compound [Zn2Al·（OH）6] NO3·nH2O and [Mg2Al·（OH）6] NO3·nH2O （shorted as ZnA1-NO3 and MgAl-NO3） was intercalated with the chelating agent EDTA （Ethylenediaminetetraacetic Acid） and EDDS （N, N＇-1, 2-Ethanediylbis-1-Aspartic Acid） by anion exchange. The materials synthesized in this work were characterized by chemical analysis, FT-IR （Fourier Transform Infrared Spectroscopy）, SEM （Scanning Electron Microscopy） and XRD （Powder X-ray Diffraction） to confirm their properties. In order to discuss the adsorption capacity of LDHs （Layered Double Hydroxides）, the adsorption experiment was investigated under the optimum condition （10 mg, 25℃ and 100 μg·L-1）. The amount of metallic ions adsorbed by LDHs intercalated with EDTA and precursor LDHs were determined by ICP-AES （Inductively Coupled Plasma-Atomic Emission Spectrometry） and AAS （Atomic Absorption Spectrometry）. The intercalation of EDTA leads to improve the adsorption capacity of LDHs. LDHs intercalated with chelating agents have generally high affinity for removing metallic ions, and they can be efficient adsorbents for metallic ions.
