Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability cau...Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability caused by detrimental chlorine chemistry.Herein,we present our recent discovery that the incorporation of Ce into Ni Fe layered double hydroxide nanosheet array on Ni foam(Ce-Ni Fe LDH/NF)emerges as a robust electrocatalyst for seawater oxidation.During the seawater oxidation process,CeO_(2)is generated,effectively repelling Cl^(-)and inhibiting the formation of Cl O-,resulting in a notable enhancement in the oxidation activity and stability of alkaline seawater.The prepared Ce-Ni Fe LDH/NF requires only overpotential of 390 m V to achieve the current density of 1 A cm^(-2),while maintaining long-term stability for 500 h,outperforming the performance of Ni Fe LDH/NF(430 m V,150 h)by a significant margin.This study highlights the effectiveness of a Ce-doping strategy in augmenting the activity and stability of materials based on Ni Fe LDH in seawater electrolysis for oxygen evolution.展开更多
The aim of this paper is to investigate the effect of nitrite intercalated Mg-Al layered double hydroxides(Mg-Al LDH-NO_(2))on mortar durability under the coexisting environment of Cl−and SO_(4)^(2-).Cl−and SO_(4)^(2-...The aim of this paper is to investigate the effect of nitrite intercalated Mg-Al layered double hydroxides(Mg-Al LDH-NO_(2))on mortar durability under the coexisting environment of Cl−and SO_(4)^(2-).Cl−and SO_(4)^(2-) binding properties of Mg-Al LDH-NO_(2) in simulated concrete pore solutions,Cl−and SO_(4)^(2-) diffusion properties of mortars with Mg-Al LDHNO 2 were examined.The steel corrosion and resistance of mortar against SO_(4)^(2-) attack were also evaluated.The results indicate that Mg-Al LDH-NO_(2) can effectively adsorb the Cl−and SO_(4)^(2-) in simulated concrete pore solution,and inhibit the diffusion of Cl−and SO_(4)^(2-) into cement mortars.The presence of SO_(4)^(2-) can greatly affect the uptake amount of Cl−,and there is a coupled effect of Cl−and SO_(4)^(2-) on their penetration into mortar specimens.In addition,Mg-Al LDH-NO_(2) can greatly upgrade the resistance of mortars against SO_(4)^(2-) attack and well prevent the steel from corrosion.However,Cl−will aggravate the SO_(4)^(2-) attack and SO_(4)^(2-) can initially decrease and then increase the steel corrosion.展开更多
Mg-Al layered double hydroxide intercalated with CO_(3)^(2-)(CO_(3)·Mg-Al LDH) is effective for treating HCl exhaust gas.HCl reacts with CO_(3)^(2-) in CO_(3)·Mg-Al LDH, resulting in the formation of Cl·...Mg-Al layered double hydroxide intercalated with CO_(3)^(2-)(CO_(3)·Mg-Al LDH) is effective for treating HCl exhaust gas.HCl reacts with CO_(3)^(2-) in CO_(3)·Mg-Al LDH, resulting in the formation of Cl·Mg-Al LDH.We propose that CO_(2) can be used for the desorption of Cl^(-)from Cl·Mg-Al LDH to regenerate CO_(3)·Mg-Al LDH.Herein,we studied the desorption of a from CI-Mg-Al LDH by adding water to Cl·Mg-Al LDH and blowing CO_(2) into it.We also analyzed the effects of temperature and water addition speed on the desorption of CI^(-)from Cl·Mg-Al LDH.Our results show that the added water adhered to CI·Mg-Al LDH and that CO_(2) in the gaseous phase was dissolved in this adhered water,thus generating CO_(3)^(2-).Therefore,anion exchange occurred between CO_(3)^(2-) and Cl^(-)in the Cl·Mg-Al LDH,thus desorbing Cl^(-).展开更多
Rationally manipulating surface reconstruction of catalysts for water oxidation,inducing formation and dynamic accumulation of catalytically active centers still face numerous challenges.Herein,the introduction of[Cr(...Rationally manipulating surface reconstruction of catalysts for water oxidation,inducing formation and dynamic accumulation of catalytically active centers still face numerous challenges.Herein,the introduction of[Cr(C_(2)O_(4))_(3)]^(3-)into NiFe LDHs by intercalation engineering to promote surface reconstruction achieves an advanced oxygen evolution reaction(OER)activity.In view of the weak electronegativity of Cr^(3+) in[Cr(C_(2)O_(4))_(3)]^(3-),the intercalation of[Cr(C_(2)O_(4))_(3)]^(3-)is expected to result in an electron-rich structure of Fe sites in NiFe LDHs,and higher valence state of Ni can be formed with the charge transfer between Fe and Ni.The optimized electronic structure of NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs with more active Ni^(3+) species and the expedited dynamic generation of Ni^(3+) (Fe)OOH phase during the OER process contributed to its excellent catalytic property,revealed by in situ X-ray absorption spectroscopy,Raman spectroscopy,and quasi-in situ X-ray photoelectron spectroscopy.With the modulated electronic structure of metal sites,NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs exhibited promoted OER property with a lower overpotential of 236 mV at the current density of 10 mA cm^(-2).This work illustrates the intercalation of conjugated anion to dynamically construct desired Ni^(3+) sites with the optimal electronic environment for improved OER electrocatalysis.展开更多
The thermodynamic instability of zinc anodes in aqueous electrolytes leads to issues such as corrosion,hydrogen evolution reactions(HER), and dendrite growth, severely hindering the practical application of zinc-based...The thermodynamic instability of zinc anodes in aqueous electrolytes leads to issues such as corrosion,hydrogen evolution reactions(HER), and dendrite growth, severely hindering the practical application of zinc-based aqueous energy storage devices. To address these challenges, this work proposes a dualfunction zinc anode protective layer, composed of Zn-Al-In layered double oxides(ILDO) by rationally designing Zn-Al layered double hydroxides(Zn-Al LDHs) for the first time. Differing from previous works on the LDHs coatings, firstly, the ILDO layer accelerates zinc-ion desolvation and also captures and anchors SO_(4)^(2-). Secondly, the in-situ formation of the Zn-In alloy phase effectively lowers the nucleation energy barrier, thereby regulating zinc nucleation. Consequently, the zinc anode with the ILDO protective layer demonstrates long-term stability exceeding 1900 h and low voltage hysteresis of 7.5 m V at 0.5 m A cm^(-2) and 0.5 m A h cm^(-2). Additionally, it significantly enhances the rate capability and cycling performance of Zn@ILDO//MnO_(2) full batteries and Zn@ILDO//activated carbon zinc-ion hybrid capacitors.This simple and effective dual-function protective layer strategy offers a promising approach for achieving high-performance zinc-ion batteries.展开更多
The title compound, [HgI2（C12H8N4S）], has been synthesized and characterized by single-crystal X-ray diffraction analysis. It crystallizes in monoclinic, space group P21/n with a = 14.086（2）, b = 6.0365（6）, c = ...The title compound, [HgI2（C12H8N4S）], has been synthesized and characterized by single-crystal X-ray diffraction analysis. It crystallizes in monoclinic, space group P21/n with a = 14.086（2）, b = 6.0365（6）, c = 20.286（2）°A,β= 108.818（5）°, V = 1632.7（3）°A^3, Mr = 694.67, Z = 4, D, = 2.826 g/cm^3,μ= 13.331 mm^-1, F（000） = 1240, S = 1.108, the final R = 0.0438 and wR = 0.0934 for 3085 observed reflections （I〉 2σ（I））. The Hg（Ⅱ） atom is coordinated by two 2,5-bis（4-pyridyl）-1,3,4-thiadiazole （L） molecules and two iodine anions in a distorted tetrahedral coordination geometry. Mercury atoms are linked by the organic ligands to form a one-dimensional zigzag chain. It is noteworthy that such 1D zigzag chains are extended into a two-dimensional double layer framework through I…I interactions展开更多
In the paper entitled"Efficient adsorption of Mn(Ⅱ)by layered double hydroxides intercalated with di ethylenetriaminepentaacetic acid and the mechanistic study"in Journal of Environmental Sciences,volume 85...In the paper entitled"Efficient adsorption of Mn(Ⅱ)by layered double hydroxides intercalated with di ethylenetriaminepentaacetic acid and the mechanistic study"in Journal of Environmental Sciences,volume 85,page 56-65,there were problems with mathematical notation and dimensional errors in the calculation for Giibbs free energy.In Section 2.5:Adsorption isotherms and thermodynamics studies,authors calculated the Gibbs free energy change(△G°)展开更多
基金support from the Free Exploration Project of Frontier Technology for Laoshan Laboratory(No.16-02)the National Natural Science Foundation of China(Nos.22072015 and 21927811)。
文摘Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability caused by detrimental chlorine chemistry.Herein,we present our recent discovery that the incorporation of Ce into Ni Fe layered double hydroxide nanosheet array on Ni foam(Ce-Ni Fe LDH/NF)emerges as a robust electrocatalyst for seawater oxidation.During the seawater oxidation process,CeO_(2)is generated,effectively repelling Cl^(-)and inhibiting the formation of Cl O-,resulting in a notable enhancement in the oxidation activity and stability of alkaline seawater.The prepared Ce-Ni Fe LDH/NF requires only overpotential of 390 m V to achieve the current density of 1 A cm^(-2),while maintaining long-term stability for 500 h,outperforming the performance of Ni Fe LDH/NF(430 m V,150 h)by a significant margin.This study highlights the effectiveness of a Ce-doping strategy in augmenting the activity and stability of materials based on Ni Fe LDH in seawater electrolysis for oxygen evolution.
基金Project(51478164)supported by the National Natural Science Foundation of ChinaProject(BK20181306)supported by Natural Science Foundation of Jiangsu Province,China。
文摘The aim of this paper is to investigate the effect of nitrite intercalated Mg-Al layered double hydroxides(Mg-Al LDH-NO_(2))on mortar durability under the coexisting environment of Cl−and SO_(4)^(2-).Cl−and SO_(4)^(2-) binding properties of Mg-Al LDH-NO_(2) in simulated concrete pore solutions,Cl−and SO_(4)^(2-) diffusion properties of mortars with Mg-Al LDHNO 2 were examined.The steel corrosion and resistance of mortar against SO_(4)^(2-) attack were also evaluated.The results indicate that Mg-Al LDH-NO_(2) can effectively adsorb the Cl−and SO_(4)^(2-) in simulated concrete pore solution,and inhibit the diffusion of Cl−and SO_(4)^(2-) into cement mortars.The presence of SO_(4)^(2-) can greatly affect the uptake amount of Cl−,and there is a coupled effect of Cl−and SO_(4)^(2-) on their penetration into mortar specimens.In addition,Mg-Al LDH-NO_(2) can greatly upgrade the resistance of mortars against SO_(4)^(2-) attack and well prevent the steel from corrosion.However,Cl−will aggravate the SO_(4)^(2-) attack and SO_(4)^(2-) can initially decrease and then increase the steel corrosion.
文摘Mg-Al layered double hydroxide intercalated with CO_(3)^(2-)(CO_(3)·Mg-Al LDH) is effective for treating HCl exhaust gas.HCl reacts with CO_(3)^(2-) in CO_(3)·Mg-Al LDH, resulting in the formation of Cl·Mg-Al LDH.We propose that CO_(2) can be used for the desorption of Cl^(-)from Cl·Mg-Al LDH to regenerate CO_(3)·Mg-Al LDH.Herein,we studied the desorption of a from CI-Mg-Al LDH by adding water to Cl·Mg-Al LDH and blowing CO_(2) into it.We also analyzed the effects of temperature and water addition speed on the desorption of CI^(-)from Cl·Mg-Al LDH.Our results show that the added water adhered to CI·Mg-Al LDH and that CO_(2) in the gaseous phase was dissolved in this adhered water,thus generating CO_(3)^(2-).Therefore,anion exchange occurred between CO_(3)^(2-) and Cl^(-)in the Cl·Mg-Al LDH,thus desorbing Cl^(-).
基金support from the National Natural Science Foundation of China(51402100,21905088,21573066 and U19A2017)the Provincial Natural Science Foundation of Hunan(2020JJ5044,2022JJ10006)。
文摘Rationally manipulating surface reconstruction of catalysts for water oxidation,inducing formation and dynamic accumulation of catalytically active centers still face numerous challenges.Herein,the introduction of[Cr(C_(2)O_(4))_(3)]^(3-)into NiFe LDHs by intercalation engineering to promote surface reconstruction achieves an advanced oxygen evolution reaction(OER)activity.In view of the weak electronegativity of Cr^(3+) in[Cr(C_(2)O_(4))_(3)]^(3-),the intercalation of[Cr(C_(2)O_(4))_(3)]^(3-)is expected to result in an electron-rich structure of Fe sites in NiFe LDHs,and higher valence state of Ni can be formed with the charge transfer between Fe and Ni.The optimized electronic structure of NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs with more active Ni^(3+) species and the expedited dynamic generation of Ni^(3+) (Fe)OOH phase during the OER process contributed to its excellent catalytic property,revealed by in situ X-ray absorption spectroscopy,Raman spectroscopy,and quasi-in situ X-ray photoelectron spectroscopy.With the modulated electronic structure of metal sites,NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs exhibited promoted OER property with a lower overpotential of 236 mV at the current density of 10 mA cm^(-2).This work illustrates the intercalation of conjugated anion to dynamically construct desired Ni^(3+) sites with the optimal electronic environment for improved OER electrocatalysis.
基金Natural Science Foundation of Hunan Province (No.2020JJ4734)High Performance Computing Center of Central South University。
文摘The thermodynamic instability of zinc anodes in aqueous electrolytes leads to issues such as corrosion,hydrogen evolution reactions(HER), and dendrite growth, severely hindering the practical application of zinc-based aqueous energy storage devices. To address these challenges, this work proposes a dualfunction zinc anode protective layer, composed of Zn-Al-In layered double oxides(ILDO) by rationally designing Zn-Al layered double hydroxides(Zn-Al LDHs) for the first time. Differing from previous works on the LDHs coatings, firstly, the ILDO layer accelerates zinc-ion desolvation and also captures and anchors SO_(4)^(2-). Secondly, the in-situ formation of the Zn-In alloy phase effectively lowers the nucleation energy barrier, thereby regulating zinc nucleation. Consequently, the zinc anode with the ILDO protective layer demonstrates long-term stability exceeding 1900 h and low voltage hysteresis of 7.5 m V at 0.5 m A cm^(-2) and 0.5 m A h cm^(-2). Additionally, it significantly enhances the rate capability and cycling performance of Zn@ILDO//MnO_(2) full batteries and Zn@ILDO//activated carbon zinc-ion hybrid capacitors.This simple and effective dual-function protective layer strategy offers a promising approach for achieving high-performance zinc-ion batteries.
基金This work was supported by the 973 Program of the MOST (001CB108906) and the Natural Science Foundation of Fujian Province (2005HZ01-1)
文摘The title compound, [HgI2（C12H8N4S）], has been synthesized and characterized by single-crystal X-ray diffraction analysis. It crystallizes in monoclinic, space group P21/n with a = 14.086（2）, b = 6.0365（6）, c = 20.286（2）°A,β= 108.818（5）°, V = 1632.7（3）°A^3, Mr = 694.67, Z = 4, D, = 2.826 g/cm^3,μ= 13.331 mm^-1, F（000） = 1240, S = 1.108, the final R = 0.0438 and wR = 0.0934 for 3085 observed reflections （I〉 2σ（I））. The Hg（Ⅱ） atom is coordinated by two 2,5-bis（4-pyridyl）-1,3,4-thiadiazole （L） molecules and two iodine anions in a distorted tetrahedral coordination geometry. Mercury atoms are linked by the organic ligands to form a one-dimensional zigzag chain. It is noteworthy that such 1D zigzag chains are extended into a two-dimensional double layer framework through I…I interactions
基金funded by the National Natural Science Foundation of China(Nos.31971551,31470573 and 31070478)the Tianjin Key Projects of Scientific and Technological Support(Nos.17YFZCNC00220 and 18YFZCNC01270)
文摘In the paper entitled"Efficient adsorption of Mn(Ⅱ)by layered double hydroxides intercalated with di ethylenetriaminepentaacetic acid and the mechanistic study"in Journal of Environmental Sciences,volume 85,page 56-65,there were problems with mathematical notation and dimensional errors in the calculation for Giibbs free energy.In Section 2.5:Adsorption isotherms and thermodynamics studies,authors calculated the Gibbs free energy change(△G°)
