Low temperature catalysts are attracting increasing attention in the selective catalytic reduction(SCR)of NO with NH3.Mn Ox-decorated Mg Al layered double oxide(Mn/Mg Al-LDO)was synthesized via a facile fast pour assi...Low temperature catalysts are attracting increasing attention in the selective catalytic reduction(SCR)of NO with NH3.Mn Ox-decorated Mg Al layered double oxide(Mn/Mg Al-LDO)was synthesized via a facile fast pour assisted co-precipitation(FP-CP)process.Compared to the Mn/Mg Al-LDO obtained via slow drop assisted coprecipitation(SD-CP)method,the Mn/Mg Al-LDO(FP-CP)has excellent activity.The Mn/Mg Al-LDO(FP-CP)catalyst was shown to possess a high NO conversion rate of 76%-100%from 25 to 150℃,which is much better than the control Mn/Mg Al-LDO(SD-CP)(29.4%-75.8%).In addition,the Mn/Mg Al-LDO(FP-CP)offered an enhanced NO conversion rate of 97%and a N2selectivity of 97.3%at 100℃;the NO conversion rate was 100%and the N2selectivity was 90%at 150℃with a GHSV of 60,000 h^-1.The Mn/Mg Al-LDO(FP-CP)catalyst exhibited a smaller fragment nano-sheet structure(sheet thickness of 7.23 nm).An apparent lattice disorder was observed in the HRTEM image confirming the presence of many defects.The H2-TPR curves show that the Mn/Mg Al-LDO(FP-CP)catalyst has abundant reducing substances.Furthermore,the enhanced surface acidity makes the NH3concentration of the Mn/Mg Al-LDO(FP-CP)catalyst lower than 100 ml·m^-3after the reaction from 25 to 400℃.This can effectively reduce the ammonia escape rate in the SCR reaction.Thus,the Mn/Mg Al-LDO(FP-CP)catalyst has potential applications in stationary industrial installations for environmentally friendly ultra-low temperature SCR.展开更多
Owing to the serious potential side-effects on the environment and human health,the rapid detection and removal of antibiotics have become an important research focus.In this work,four zinc-based metal-organic framewo...Owing to the serious potential side-effects on the environment and human health,the rapid detection and removal of antibiotics have become an important research focus.In this work,four zinc-based metal-organic frameworks(MOFs)with different functional groups,i.e.,Zn-MOF,Zn-MOF-CH_(3),Zn-MOF-NO_(2),Zn-MOF-COOH,were utilized for the construction of LDO/MOF composite materials with a nickel-iron-cobalt-based layered double oxide,NiFeCo-LDO.The results showed that the LDO/MOF composites not only had high sensitivity in detecting sulfonamide and quinolone antibiotics,but also had an appreciable ability to adsorb them from wastewater.The maximum adsorption capacities of all the four types of LDO@Zn-MOFs to all antibiotics can at least reach 150 mg/g,and the limits of detection in relation to all four antibiotics were at least as low as 100μg/L.Our work suggested the dual-function extraction performance can be attributed to the synergistic effects between the LDO and the MOFs.Moreover,the strong ferromagnetism derived from the LDO provided great convenience for the separation and regeneration of the LDO/MOF composites.展开更多
In this paper, the superhydrophobic polyurethane sponge(SS-PU) was facilely fabricated by etching with Jones reagent to bind the nanoparticles of Ni-Co double layered oxides(LDOs) on the surface, and following modific...In this paper, the superhydrophobic polyurethane sponge(SS-PU) was facilely fabricated by etching with Jones reagent to bind the nanoparticles of Ni-Co double layered oxides(LDOs) on the surface, and following modification with n-dodecyl mercaptan(DDT). This method provides a new strategy to fabricate superhydrophobic PU sponge with a water contact angle of 157° for absorbing oil with low cost and in large scale. It exhibits the strong absorption capacity and highly selective characteristic for various kinds of oils which can be recycled by simple squeezing. Besides, the as-prepared sponge can deal with the floating and underwater oils, indicating its application value in handling oil spills and domestic oily wastewater. The good self-cleaning ability shows the potential to clear the pollutants due to the ultralow adhesion to water. Especially, the most important point is that the superhydrophobic sponge can continuously and effectively separate the oil/water mixture against the condition of turbulent disturbance by using our designed device system, which exhibit its good superhydrophobicity, strong stability.Furthermore, the SS-PU still maintained stable absorption performance after 150 cycle tests without losing capacity obviously, showing excellent durability in long-term operation and significant potential as an efficient absorbent in large-scale dispose of oily water.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
Acidification of paper-based relics is a common problem,leading to their degradation and eventual loss.Paper deacidification is highly dependent on a limited variety of alkaline materials,and the development of new ma...Acidification of paper-based relics is a common problem,leading to their degradation and eventual loss.Paper deacidification is highly dependent on a limited variety of alkaline materials,and the development of new materials that are safe,efficient and easy-to-prepare is highly demanded to ensure a high level of safety and effective protection of paper-based relic.This study proposes the introduction of layered double hydroxide(LDH)and its calcined product,mixed metal oxide(layered double oxide(LDO)),as innovative protective materials for the deacidification of paper with varying levels of acidity.The results demonstrate that treatment with Mg-Al LDH/LDO can effectively modify the p H of acidic paper(e.g.,pH~4.0–6.4)to a neutral or weakly basic state,maintaining this desirable p H range even under long-term accelerated aging condition.Remarkably,LDH proves to be well-suited for the protection of slightly acidified paper(e.g.,pH>5.5),while LDO serves as an especially option for the deacidification of severely acidified paper(e.g.,pH≤5.5).During aqueous deacidification,due to the memory effect of the LDH-based materials,LDO is converted to rehydrated LDH,which creates a mild and appropriate alkaline retention in the paper,avoiding damage caused by strong alkalinity such as cellulose degradation and pigment fading during subsequent long-term natural preservation of the paper.Furthermore,Mg-Al LDH/LDO materials also exhibit flame-retardant and bacteriostatic properties.This opens up opportunities for the safe,efficient and multifunctional protection of acidified paper-based relics.展开更多
A series of MgAl-layered double oxides（LDO） doped with different rare-earth elements（Y, La, and Ce）were synthesized by the calcination of Mg-Al layered double hydroxides, and Ru, which were used to prepare ammonia...A series of MgAl-layered double oxides（LDO） doped with different rare-earth elements（Y, La, and Ce）were synthesized by the calcination of Mg-Al layered double hydroxides, and Ru, which were used to prepare ammonia synthesis catalysts. The as-obtained oxides and catalysts were characterized by XRD,TEM, TPD, TPR and XPS to understand their catalytic performances in ammonia synthesis. The H_2-TPR and HRTEM studies reveal that Ru/Y-LDO catalyst possesses more active Ru metal and small particle size.The XPS demonstrates that the electronic interaction between Y and Ru metals is stronger, which can be tentatively explained by most of Y inserted into the hydrotalcites structure. CO_2-TPD demonstrates that Ru/Y-LDO catalyst shows stronger basic site densities than catalysts doped with Ce and La. Higher activity of the Ru/Y-LDO catalyst can be attributed to smaller particle size, more active metal（Ru） and strong Ru-support interaction.展开更多
The use of non-noble nickel-based catalysts for low temperature CO methanation has been a challenge in recent years.Herein,MgAl layered double oxides sample with high dispersion synthesized by a facile N-(2-Hydroxyeth...The use of non-noble nickel-based catalysts for low temperature CO methanation has been a challenge in recent years.Herein,MgAl layered double oxides sample with high dispersion synthesized by a facile N-(2-Hydroxyethyl)ethylenediaminetriacetic acid assisted wetness impregnation approach,demonstrates much superior catalytic activity and exceptional stability for CO methanation in comparison with the classical Ni/MgAl-LDO catalyst prepared by the ordinary wetness impregnation method.HRTEM results showed that N-(2-Hydroxyethyl)ethylenediaminetriacetic acid played a positive role in the dispersion of Ni,as well as Ni-support interaction.Well-dispersed Ni particles with a size of about 5 nm were formed in the presence of N-(2-Hydroxyethyl)ethylenediaminetriacetic acid.Compared to the Ni/MgAl-LDO prepared by conventional impregnation method,the NH-Ni/MgAl-LDO exhibited superior catalytic performance,especially excellent thermal stability.The NH-Ni30/MgAl-LDO catalyst was found to keep a 70%CO conversion even at 160◦C which demonstrates its good low temperature performance.From the in situ FTIR observations,this good performance at low temperatures may be linked to the delocalization of electrons around CO caused by surface hydroxyl groups.展开更多
基金supported by Science and Technology Innovation Talents Program of Bingtuan(No.2019CB025)Major Scientific and Technological Project of Bingtuan(No.2018AA002)。
文摘Low temperature catalysts are attracting increasing attention in the selective catalytic reduction(SCR)of NO with NH3.Mn Ox-decorated Mg Al layered double oxide(Mn/Mg Al-LDO)was synthesized via a facile fast pour assisted co-precipitation(FP-CP)process.Compared to the Mn/Mg Al-LDO obtained via slow drop assisted coprecipitation(SD-CP)method,the Mn/Mg Al-LDO(FP-CP)has excellent activity.The Mn/Mg Al-LDO(FP-CP)catalyst was shown to possess a high NO conversion rate of 76%-100%from 25 to 150℃,which is much better than the control Mn/Mg Al-LDO(SD-CP)(29.4%-75.8%).In addition,the Mn/Mg Al-LDO(FP-CP)offered an enhanced NO conversion rate of 97%and a N2selectivity of 97.3%at 100℃;the NO conversion rate was 100%and the N2selectivity was 90%at 150℃with a GHSV of 60,000 h^-1.The Mn/Mg Al-LDO(FP-CP)catalyst exhibited a smaller fragment nano-sheet structure(sheet thickness of 7.23 nm).An apparent lattice disorder was observed in the HRTEM image confirming the presence of many defects.The H2-TPR curves show that the Mn/Mg Al-LDO(FP-CP)catalyst has abundant reducing substances.Furthermore,the enhanced surface acidity makes the NH3concentration of the Mn/Mg Al-LDO(FP-CP)catalyst lower than 100 ml·m^-3after the reaction from 25 to 400℃.This can effectively reduce the ammonia escape rate in the SCR reaction.Thus,the Mn/Mg Al-LDO(FP-CP)catalyst has potential applications in stationary industrial installations for environmentally friendly ultra-low temperature SCR.
基金support from the National Natural Science Foundation of China(Nos.22276080,21605105)the Foreign Expert Project,China(No.G2022014096L)+1 种基金the Natural Science Foundation of Jiangsu Province,China(No.BK20211340)Graduate Research and Practice Innovation Program of Jiangsu Province,China(No.KYCX22_3835).
文摘Owing to the serious potential side-effects on the environment and human health,the rapid detection and removal of antibiotics have become an important research focus.In this work,four zinc-based metal-organic frameworks(MOFs)with different functional groups,i.e.,Zn-MOF,Zn-MOF-CH_(3),Zn-MOF-NO_(2),Zn-MOF-COOH,were utilized for the construction of LDO/MOF composite materials with a nickel-iron-cobalt-based layered double oxide,NiFeCo-LDO.The results showed that the LDO/MOF composites not only had high sensitivity in detecting sulfonamide and quinolone antibiotics,but also had an appreciable ability to adsorb them from wastewater.The maximum adsorption capacities of all the four types of LDO@Zn-MOFs to all antibiotics can at least reach 150 mg/g,and the limits of detection in relation to all four antibiotics were at least as low as 100μg/L.Our work suggested the dual-function extraction performance can be attributed to the synergistic effects between the LDO and the MOFs.Moreover,the strong ferromagnetism derived from the LDO provided great convenience for the separation and regeneration of the LDO/MOF composites.
基金the financial support from National Key Research & Development Program of China (2017B0602702)。
文摘In this paper, the superhydrophobic polyurethane sponge(SS-PU) was facilely fabricated by etching with Jones reagent to bind the nanoparticles of Ni-Co double layered oxides(LDOs) on the surface, and following modification with n-dodecyl mercaptan(DDT). This method provides a new strategy to fabricate superhydrophobic PU sponge with a water contact angle of 157° for absorbing oil with low cost and in large scale. It exhibits the strong absorption capacity and highly selective characteristic for various kinds of oils which can be recycled by simple squeezing. Besides, the as-prepared sponge can deal with the floating and underwater oils, indicating its application value in handling oil spills and domestic oily wastewater. The good self-cleaning ability shows the potential to clear the pollutants due to the ultralow adhesion to water. Especially, the most important point is that the superhydrophobic sponge can continuously and effectively separate the oil/water mixture against the condition of turbulent disturbance by using our designed device system, which exhibit its good superhydrophobicity, strong stability.Furthermore, the SS-PU still maintained stable absorption performance after 150 cycle tests without losing capacity obviously, showing excellent durability in long-term operation and significant potential as an efficient absorbent in large-scale dispose of oily water.
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support from the National Key R&D Program of China(No.2022YFF0904200)Shanghai Rising-Star Program(No.23QA1404100)Key Laboratory of Pulp and Paper Science and Technology of Ministry of Education of China(No.KF201921)。
文摘Acidification of paper-based relics is a common problem,leading to their degradation and eventual loss.Paper deacidification is highly dependent on a limited variety of alkaline materials,and the development of new materials that are safe,efficient and easy-to-prepare is highly demanded to ensure a high level of safety and effective protection of paper-based relic.This study proposes the introduction of layered double hydroxide(LDH)and its calcined product,mixed metal oxide(layered double oxide(LDO)),as innovative protective materials for the deacidification of paper with varying levels of acidity.The results demonstrate that treatment with Mg-Al LDH/LDO can effectively modify the p H of acidic paper(e.g.,pH~4.0–6.4)to a neutral or weakly basic state,maintaining this desirable p H range even under long-term accelerated aging condition.Remarkably,LDH proves to be well-suited for the protection of slightly acidified paper(e.g.,pH>5.5),while LDO serves as an especially option for the deacidification of severely acidified paper(e.g.,pH≤5.5).During aqueous deacidification,due to the memory effect of the LDH-based materials,LDO is converted to rehydrated LDH,which creates a mild and appropriate alkaline retention in the paper,avoiding damage caused by strong alkalinity such as cellulose degradation and pigment fading during subsequent long-term natural preservation of the paper.Furthermore,Mg-Al LDH/LDO materials also exhibit flame-retardant and bacteriostatic properties.This opens up opportunities for the safe,efficient and multifunctional protection of acidified paper-based relics.
基金Project supported by the Natural Science Foundation of Fujian Province(2014J01043)the National Natural Science Foundation of China(21203028)PetroChina Innovation Foundation(2016D-5007-0504)
文摘A series of MgAl-layered double oxides（LDO） doped with different rare-earth elements（Y, La, and Ce）were synthesized by the calcination of Mg-Al layered double hydroxides, and Ru, which were used to prepare ammonia synthesis catalysts. The as-obtained oxides and catalysts were characterized by XRD,TEM, TPD, TPR and XPS to understand their catalytic performances in ammonia synthesis. The H_2-TPR and HRTEM studies reveal that Ru/Y-LDO catalyst possesses more active Ru metal and small particle size.The XPS demonstrates that the electronic interaction between Y and Ru metals is stronger, which can be tentatively explained by most of Y inserted into the hydrotalcites structure. CO_2-TPD demonstrates that Ru/Y-LDO catalyst shows stronger basic site densities than catalysts doped with Ce and La. Higher activity of the Ru/Y-LDO catalyst can be attributed to smaller particle size, more active metal（Ru） and strong Ru-support interaction.
基金National Natural Science Foundation of China(No.22068034)International Science and Technology Cooperation Project of Shihezi University(No.GJHZ201804)+1 种基金International Science and Technology Cooperation Project of Bingtuan(No.2018BC002)Science and Technology Innovation Talents Program of Bingtuan(No.2019CB025).
文摘The use of non-noble nickel-based catalysts for low temperature CO methanation has been a challenge in recent years.Herein,MgAl layered double oxides sample with high dispersion synthesized by a facile N-(2-Hydroxyethyl)ethylenediaminetriacetic acid assisted wetness impregnation approach,demonstrates much superior catalytic activity and exceptional stability for CO methanation in comparison with the classical Ni/MgAl-LDO catalyst prepared by the ordinary wetness impregnation method.HRTEM results showed that N-(2-Hydroxyethyl)ethylenediaminetriacetic acid played a positive role in the dispersion of Ni,as well as Ni-support interaction.Well-dispersed Ni particles with a size of about 5 nm were formed in the presence of N-(2-Hydroxyethyl)ethylenediaminetriacetic acid.Compared to the Ni/MgAl-LDO prepared by conventional impregnation method,the NH-Ni/MgAl-LDO exhibited superior catalytic performance,especially excellent thermal stability.The NH-Ni30/MgAl-LDO catalyst was found to keep a 70%CO conversion even at 160◦C which demonstrates its good low temperature performance.From the in situ FTIR observations,this good performance at low temperatures may be linked to the delocalization of electrons around CO caused by surface hydroxyl groups.
