High-entropy layered hydroxides(HELHs),an emerging frontier in entropy-stabilized materials derived from layered double hydroxides(LDHs),have captivated attention with their unparalleled tunability,thermodynamic stabi...High-entropy layered hydroxides(HELHs),an emerging frontier in entropy-stabilized materials derived from layered double hydroxides(LDHs),have captivated attention with their unparalleled tunability,thermodynamic stability,and electrochemical performance.The integration of the high-entropy concept into LDHs empowers HELHs to surmount the constraints of conventional materials through compositional diversity,structurally disordered configurations,and synergistic multi-element interactions.This review systematically embarks on their synthesis methodologies,functional mechanisms,and applications in energy conversion/storage and biomedicine.Advanced synthesis strategies,such as plasma-assisted hydrothermal methods,facilitate precise control over HELH architectures while supporting scalable production.HELHs demonstrate superior electrochemical performance in critical reactions,including oxygen evolution reaction,water oxidation,hydrogen evolution,and glucose electrooxidation.Future directions encompass integrating in situ characterization with simulations,leveraging machine learning for composition screening,and expanding HELHs application through interdisciplinary collaborations.This work establishes a comprehensive roadmap for advancing HELHs as next-generation multifunctional platforms for sustainable energy and biomedical technologies.展开更多
NiFe layered double hydroxide(NiFe LDH)has emerged as a promising catalyst for the oxygen evolution reaction(OER);however,its hydrogen evolution reaction(HER)activity remains suboptimal due to unfavorable electronic s...NiFe layered double hydroxide(NiFe LDH)has emerged as a promising catalyst for the oxygen evolution reaction(OER);however,its hydrogen evolution reaction(HER)activity remains suboptimal due to unfavorable electronic structures,particularly the d-electron density of metal sites,which impede water dissociation and lead to poor hydrogen adsorption/desorption capabilities.Herein,we introduce an efficient cooperative d-electron density regulation(CDDR)engineering to comprehensively optimize the delectron density of NiFe LDH by grafting MoO_(x) -modified NiFe LDH nanosheets onto porous nickel particles(PNPs).The PNPs facilitate d-electron density modulation along the edges of the nanosheets,while the MoO_(x) species enable d-electron density modulation across the plane of the nanosheets,thus cooperatively constructing enriched d-electron density in NiFe LDH.Theoretical studies validate the CDDR process and reveal that the enriched d-electron density accelerates water dissociation and optimizes the hydrogen adsorption behavior of NiFe LDH.As a result,the engineered catalyst exhibits significantly improved HER activity,achieving an ultra-low overpotential of 38 mV at 10 mA cm^(-2)in 1 M KOH.Additionally,the CDDR-optimized catalyst also exhibits good OER performance,demonstrating excellent bifunctional performance for overall water splitting in both alkaline freshwater and seawater electrolytes.This work presents a novel CDDR strategy for engineering NiFe LDH into efficient HER catalysts without compromising its OER activity,potentially paving the way for the development of active and robust electrocatalysts for sustainable energy applications.展开更多
A method for the effective in-situ formation of boron-containing Mg-Al layered double hydroxides(LDHs)was developed for boron removal and stabilization.The influence of the B/Al molar ratio and pH on the formation of ...A method for the effective in-situ formation of boron-containing Mg-Al layered double hydroxides(LDHs)was developed for boron removal and stabilization.The influence of the B/Al molar ratio and pH on the formation of Mg-Al-B–LDHs was investigated.Compared with the adsorption method,under a high B/Al ratio,the coprecipitation method increased the boron sorption density from 0.256 to 0.472 of Al.The Toxicity Characteristic Leaching Procedure showed that the boron-coprecipitated LDHs exhibited higher stability than the boron-adsorption LDHs.The synthesized LDH samples were characterized by X-ray diffraction,X-ray photoelectron spectroscopy,and solid-state 11B-NMR.The results showed that boron was effectively incorporated into the LDH structure for the coprecipitation method.Combined with the experimental results,a potential in-situ formation pathway for Mg-Al-B–LDHs was elucidated through density functional theory calculations.The boron tended to directly incorporate into the LDH structure in the coprecipitation method,whereas it was predominantly adsorbed on the LDH surface in the adsorption method.The adsorption energy demonstrated that boron preferentially bonded to Mg^(2+)sites on the surface.The mechanism of boron incorporation in the LDHs for the coprecipitation method involved precipitation of amorphous aluminum hydroxide,layered boehmite transformation,nucleation,and layer stacking.During these processes,boron formed complexes to enhance its stability.Residual boron underwent further reactions with the LDHs,including surface adsorption and ion exchange.These findings provide theoretical insight into the effective removal and long-term immobilization of boron in landfill leachate self-remediation processes.展开更多
Owing to its excellent eco-friendliness and facile water elution properties,aluminum-based lithium adsorbents have attracted a surge of interest for selectively extracting Li^(+)from Salt Lake brines,which account for...Owing to its excellent eco-friendliness and facile water elution properties,aluminum-based lithium adsorbents have attracted a surge of interest for selectively extracting Li^(+)from Salt Lake brines,which account for more than 60%of the global lithium resources.However,structural collapse,facile deactivation during desorption process,and ultra-low actual adsorption capacity limit its further large-scale application,particularly in low-grade sulfate-type brines.Herein,considering its advantages,limitations,and structural features,the structural collapse of the aluminum-based lithium adsorbent was effectively suppressed by the in situ intercalation of VO_(3)^(-)and V_(2)O_(7)^(4-)into the interlayer of[LiAl_(2)(OH)_(6)]^(+).Evidently,the initial adsorption capacity andα_(Mg)^(Li)of as-configured adsorbents powder are 14.96 mg g^(-1) and 192.42 in real sulfate-type West Taijinar Salt Lake brines following NaCl salts removal with 800 mg L^(-1) Li^(+)and 9.56 g L^(-1) SO_(4)^(2-).Furthermore,the initial and retained adsorption capacities of these novel adsorbents granulate in brines after 100 adsorption/desorption cycles are 26.68 and 10.36 mg g^(-1),respectively,which are almost 10 times higher than those of industrially utilized products.Based on experiments and density functional theory calculations,the process and mechanism of anion intercalation control were preliminarily elucidated.Furthermore,research findings indicate that intercalated anions can influence not only interlayer interactions but also the backbone strength of LDH-type adsorbents.This work significantly overcomes the major utilization challenges of aluminum-based lithium adsorbents,thereby enabling the high-efficiency and stable extraction of Li^(+)from low-grade brines,including sulfate-type brines.展开更多
CoFe bimetallic hydroxides(CoFe BMHs)find wide applications as excellent catalysts in the field of water splitting.However,no study has systematically investigated the influence of the morphologies of CoFe BMHs on cat...CoFe bimetallic hydroxides(CoFe BMHs)find wide applications as excellent catalysts in the field of water splitting.However,no study has systematically investigated the influence of the morphologies of CoFe BMHs on catalyst performance.In this study,CoFe BMH nanoflowers(CoFe BMH NFs),CoFe BMH nanosheets(CoFe BMH NSHs),CoFe BMH nanorods(CoFe BMH NRs),and CoFe BMH nanospheres(CoFe BMH NSPs)were prepared on nickel foam via a hydrothermal method.CoFe BMH NSHs exhibited the most beneficial catalytic activity.At a current density of 100 mA·cm^(-2),its overpotential for oxygen evolution reaction(OER)was 282 mV,and the overall water splitting voltage was 2.05 V.The double-layer charging capacitance(Cdl)value of CoFe BMH NSHs was the largest in CoFe BMHs,which proves that CoFe BMH NSHs have the largest active area.Furthermore,the active site in the OER process was metal oxyhydroxide(MOOH)through in situ Raman characterization,and the generation of the active substance was an irreversible process.This work provides important insights into the design of catalyst morphologies and offers valuable guidelines for the enhancement of the performance of other catalysts.展开更多
Electrically driven water splitting is an efficient method for green hydrogen production;however,its practical application is substantially constrained by the kinetically sluggish anodic oxygen evolution reaction(OER)...Electrically driven water splitting is an efficient method for green hydrogen production;however,its practical application is substantially constrained by the kinetically sluggish anodic oxygen evolution reaction(OER).Ruthenium(Ru)and its oxides are widely recognized as highly active OER catalysts.Although Ru is significantly cheaper than iridium(Ir),further reducing its content remains desirable.Herein,atomically dispersed Ru is doped into iron-nickel layered double hydroxides(Ru-FeNi-LDH)to decrease the Ru usage.We found that the Ru doping limit is roughly 9 wt%,and the Ru doping content significantly alters the OER kinetics-note that the high Ru concentration remarkably damages the Ru-FeNi-LDH structure and leads to agglomeration formation.By optimizing the Ru doping content to 3.3 wt%,the Ru-FeNi-LDH presents a low overpotential of 230 mV to reach a current density of 10 mA cm^(-2) in 1 M KOH,which is far better than the reference FeNi-LDH(280 mV)and RuO_(2)(350 mV).In the overall water splitting test,the current density of 10 mA cm^(-2) can be reached at a low voltage of 1.52 V,with stable operation for 80 h.Interestingly,Ru and Fe form an asymmetric Ru-Fe dipole,which is likely doped together into the LDH because the content of Fe instead of Ni is dependent on Ru content in experimental results.The electron-deficient feature of the Ru-Fe dipole thus facilitates the OER process.This work demonstrates a dual-transition metal synergy,providing a design strategy for OER and related catalysts.展开更多
Layered double hydroxides(LDHs)are potential cathode materials for aqueous magnesium-ion batteries(AMIBs).However,the low capacity and sluggish kinetics significantly limit their electrochemical performance in AMIBs.H...Layered double hydroxides(LDHs)are potential cathode materials for aqueous magnesium-ion batteries(AMIBs).However,the low capacity and sluggish kinetics significantly limit their electrochemical performance in AMIBs.Herein,we find that oxygen vacancies can significantly boost the capacity,electrochemical kinetics,and structure stability of LDHs.The corresponding structure-performance relationship and energy storage mechanism are elaborated through exhaustive in/ex-situ experimental characterizations and density functional theory(DFT)calculations.Specially,in-situ Raman and DFT calculations reveal that oxygen vacancies elevate orbital energy of O 2p and electron density of O atoms,thereby enhancing the orbital hybridization of O 2p with Ni/Co 3d.This facilitates electron transfer between O and adjacent Ni/Co atoms and improves the covalency of Ni–O and Co–O bonds,which activates Ni/Co atoms to release more capacity and stabilizes the Ov-NiCo-LDH structure.Moreover,the distribution of relaxation times(DRT)and molecular dynamics(MD)simulations disclose that the enhanced d-p orbital hybridization optimizes the electronic structure of Ov-NiCo-LDH,which distinctly reduces the diffusion energy barriers of Mg^(2+)and improves the charge transfer kinetics of Ov-NiCo-LDH.Consequently,the assembled Ov-NiCo-LDH//active carbon(AC)and Ov-NiCo-LDH//perylenediimide(PTCDI)AMIBs can both deliver high specific discharge capacity(182.7 and 59.4 mAh g^(−1)at 0.5 A g^(−1),respectively)and long-term cycling stability(85.4%and 89.0%of capacity retentions after 2500 and 2400 cycles at 1.0 A g^(−1),respectively).In addition,the practical prospects for Ov-NiCo-LDH-based AMIBs have been demonstrated in different application scenarios.This work not only provides an effective strategy for obtaining high-performance cathodes of AMIBs,but also fundamentally elucidates the inherent mechanisms.展开更多
Noble metal-loaded layered hydroxides exhibit high efficiency in electrocatalyzing water splitting.However,their widespread use as bifunctional electrocatalysts is hindered by low metal loading,inefficient yield,and c...Noble metal-loaded layered hydroxides exhibit high efficiency in electrocatalyzing water splitting.However,their widespread use as bifunctional electrocatalysts is hindered by low metal loading,inefficient yield,and complex synthesis processes.In this work,platinum atoms were anchored onto nickel-iron layered double hydroxide/carbon nanotube(LDH/CNT)hybrid electrocatalysts by using a straightforward milling technique with K_(2)Pt Cl_(6)·6H_(2)O as the Pt source.By adjusting the Pt-to-Fe ratio to 1/2 and 1/10,excellent electrocatalysts—Pt_(1/6)-Ni_(2/3)Fe_(1/3)-LDH/CNT and Pt_(1/30)-Ni_(2/3)Fe_(1/3)-LDH/CNT—were achieved with superior performance in hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),outperforming the corresponding commercial Pt/C(20 wt%)and Ru O_(2)electrocatalysts.The enhanced electrochemical performance is attributed to the modification of Pt's electronic structure,which exhibits electron-rich states for HER and electrondeficient states for OER,significantly boosting Pt's electrochemical activity.Furthermore,the simple milling technology for controlling Pt loading offers a promising approach for scaling up the production of electrocatalysts.展开更多
Mobilization of arsenic under anaerobic conditions is of great concern in arsenic contaminated soils and sediments. Bacterial reduction of As(V) and Fe(III) influences the cycling and partitioning of arsenic betwe...Mobilization of arsenic under anaerobic conditions is of great concern in arsenic contaminated soils and sediments. Bacterial reduction of As(V) and Fe(III) influences the cycling and partitioning of arsenic between solid and aqueous phase. We investigated the impact of bacterially mediated reductions of Fe(III)/Al hydroxides-bound arsenic(V) and iron(III) oxides on arsenic release. Our results suggested that As(V) reduction occurred prior to Fe(III) reduction, and Fe(III) reduction did not enhance the release of arsenic. Instead, Fe(III) hydroxides retained their dissolved concentrations during the experimental process, even though the new iron mineral-magnetite formed. In contrast, the release of reduced As(III) was promoted greatly when aluminum hydroxides was incorporated. Thus, the substitution of aluminum hydroxides may be responsible for the release of arsenic in the contaminated soils and sediments, since aluminum substitution of Fe(III) hydroxides universally occurs under natural conditions.展开更多
Colored layered double hydroxides (LDHs) can be synthesized by introducing colored cations such as Fe^3+ and Cr^3 +, which call be used as thermal stabilizers for polyvinyl chloride (PVC). The yellowish Mg/Fe an...Colored layered double hydroxides (LDHs) can be synthesized by introducing colored cations such as Fe^3+ and Cr^3 +, which call be used as thermal stabilizers for polyvinyl chloride (PVC). The yellowish Mg/Fe and bluish Mg/Cr LDHs are prepared by the co-precipitation method. The results show that the MgsCr_ CO3 and Mg3Fe_ CO3 colored layered double hydroxides can stabilize PVC for more than 30 min under the thermal aging temperature of 180 ℃. The preparation can use cheap Mg(OH) 2 instead of MgCl2, which produces a much smaller amount of the by-product NH4Cl. It is known that NH4Cl is a cheap fertilizer that is difficult to sell; therefore, the preparation is much greener and more economic than the one using magnesium salt.展开更多
ZnO/NiO/ZnAl2O4 mixed-metal oxides were successfully synthesized through a hydrotalcite-like precursor route, in which appropriate amounts of metal salts solutions were mixed to obtain a new series of ZnNiAl layered d...ZnO/NiO/ZnAl2O4 mixed-metal oxides were successfully synthesized through a hydrotalcite-like precursor route, in which appropriate amounts of metal salts solutions were mixed to obtain a new series of ZnNiAl layered double hydroxides(LDHs) as precursors, followed by calcination under different temperatures. The as-obtained samples were characterized by SEM, HRTEM, TEM, XRD, BET, TG-DTA, and UV-Vis spectra techniques. The photocatalytic activities of the samples were evaluated by degradation of methyl orange(MO) under the simulated sunlight irradiation. The effects of Zn/Ni/Al mole ratio and calcination temperature on the composition, morphology and photocatalytic activity of the samples were investigated in detail. The results indicated that compared with ZnNiAl-LDHs, the mixed-metal oxide showed superior photocatalytic performance for the degradation of MO. A maximum of 97.3% photocatalytic decoloration rate within 60 min was achieved from the LDH with the Zn/Ni/Al mole ratio of 2:1:1 and the calcination temperature of 500 ℃, which much exceeded that of Degussa P25 under the same conditions. The possible mechanism of photocatalytic degradation over ZnO/NiO/ZnAl2O4 was discussed.展开更多
Catalytic oxidation is regarded as one of the most promising strategies for volatile organic compounds(VOCs)purification.Mixed metal oxides(MMOs),after topological transformation using layered double hydroxides(LDHs)a...Catalytic oxidation is regarded as one of the most promising strategies for volatile organic compounds(VOCs)purification.Mixed metal oxides(MMOs),after topological transformation using layered double hydroxides(LDHs)as precursors,are extensively used as catalysts for VOCs oxidation due to their uniformity advantage.This review summarizes the developments in the LDH-derived VOCs heterogeneous catalytic oxidation over the last 10 years.Particularly,it addresses the VOCs abatement performance over MMO,noble metal/MMO,core-shell structured MMO,and integral MMO film catalysts originating from LDHs.Moreover,it highlights the water vapor effect and oxidation mechanism.This review indicates that LDH-based catalysts are a category of important VOCs oxidation materials.展开更多
Mg–Al–Fe layered double hydroxides(LDHs) were exfoliated and incorporated in polyether sulfone membranes for the removal of phosphate and fluoride for the first time. The exfoliation methods, coagulation bath, LDH...Mg–Al–Fe layered double hydroxides(LDHs) were exfoliated and incorporated in polyether sulfone membranes for the removal of phosphate and fluoride for the first time. The exfoliation methods, coagulation bath, LDH amount, interfering ions, adsorption isotherm,desorption and reuse of the membranes were investigated. It was found that LDHs could be quickly exfoliated in formamide/N,N-dimethylformamide(DMF) solvent mixtures with sodium carboxymethyl cellulose as a stabilizer. The membranes displayed much higher adsorption capacity for phosphate(5.61 mg/g) and faster adsorption rate than the unexfoliated materials. With increased DMF content in the coagulation bath, the static and dynamic adsorption capacity rose. Interference from Cl-and SO4^(2-)(50 mg/L) on adsorption of phosphates was not apparent. The membranes displayed excellent reusability in dynamic adsorption/desorption. The membranes also showed high adsorption capacity for fluorides(1.61 mg/g).展开更多
Anodic oxidation is a prevalent technique to introduce superior corrosion and wear resistance upon the surface of titanium(Ti)alloys,in which the selection of appropriate electrolytes and defect-sealing strategies is ...Anodic oxidation is a prevalent technique to introduce superior corrosion and wear resistance upon the surface of titanium(Ti)alloys,in which the selection of appropriate electrolytes and defect-sealing strategies is a key.This study aims to address such issues through anodizing Ti-10V-2Fe-3Al alloy in malic acid,followed by a post-sealing treatment with Mg-Al layered double hydroxides(LDHs).The characteristics of the samples were investigated using scanning electron microscopy(SEM),atomic force microscopy(AFM),glow discharge optical emission spectroscopy(GDOES),X-ray diffraction(XRD)and energy-dispersive X-ray spectroscopy(EDS).SEM micrographs reveals that the anodic coating had a surface full of bulges and cracks,and was almost sealed by the following LDHs treatment.XRD pattern indicate that the anodic coating was mainly consisted of amorphous TiO2 with a small fraction of anatase,but its crystallization degree was increased through the post-sealing.Moreover,electrochemical and tribological measurements demonstrate that corrosion current density was 2.8×10-6,2.0×10-7,5.9×10-9A cm-2,and wear rate was 1.45×10-3,1.30×10-4 and 6.90×10-5 mm3 N-1 m-1 for respective bare Ti-10V-2Fe-3Al alloy substrate,anodized specimens without and with the LDHs post treatment.Finally,a plausible wear mechanism was proposed.展开更多
In this study,greatly enhanced Mn(Ⅱ) adsorption was achieved by as-synthesized diethylenetriaminepentaacetate acid intercalated Mg/Al layered double hydroxides (LDHs-DTPA).The adsorption capacity of LDHs-DTPA was 83....In this study,greatly enhanced Mn(Ⅱ) adsorption was achieved by as-synthesized diethylenetriaminepentaacetate acid intercalated Mg/Al layered double hydroxides (LDHs-DTPA).The adsorption capacity of LDHs-DTPA was 83.5 mg/g,which is much higher than that of LDHs-EDTA (44.4 mg/g),LDHs-Oxalate (21.6 mg/g) and LDHs (28.8 mg/g).The adsorption data of aqueous Mn(Ⅱ) using LDHs-DTPA could be well described by the pseudosecond order kinetics and Langrnuir isotherm model.Thermodynamics study results also showed that the adsorption process of Mn(Ⅱ) by LDHs-DTPA was exothermic as indicated by the negative △H value.Furthermore,based on the structural,morphological and thermostable features,as well as FT-IR and XPS characterizations of LDHs-DTPA and the pristine LDHs,the adsorption mechanism of Mn(Ⅱ) was proposed.The carboxyl groups of DTPA were proposed to be the main binding sites for Mn(Ⅱ),and the hydroxyl groups of LDHs also played a minor role in the adsorption process.Among the three common regeneration reagents,0.1 mol/L Na2CO3 was the best for reusing LDHs-DTPA in Mn(Ⅱ) adsorption.Besides,the Mn(Ⅱ) adsorption performance could be hindered in the presence of typical inorganic ions,especially cations.Further specific modifications of LDHs-DTPA are suggested to get more selective adsorption of Mn(ll) in practical applications.展开更多
Layered double hydroxides(LDHs) with the physical property of high ultraviolet(UV)reflectance were used to enhance the anti-UV aging performance of bitumen. In view of the poor compatibility of LDHs with bitumen, thre...Layered double hydroxides(LDHs) with the physical property of high ultraviolet(UV)reflectance were used to enhance the anti-UV aging performance of bitumen. In view of the poor compatibility of LDHs with bitumen, three organic anions, namely, sodium dodecyl benzenesulfonate(SDBS), sodium dodecyl sulfate(SDS) and sodium dodecyl sulfonate(SDSO), were used as modifiers to prepare organic LDHs(OCLDHs) through regeneration process, and the crystal structure, chemical composition, morphological feature and UV shielding capability of synthesized OCLDHs were analyzed. Then the OCLDHs were added into bitumen to evaluate the storage stability and anti-UV aging property of OCLDHs/bitumen composites.The results show that the organic anions are inserted into the interlayers of LDHs, the intercalation expands the interlayer distance of LDHs, makes the particle shapes become more irregular and complicated, and enhances the absorption ability within the range from 200 to 300 nm while has little influence on the UV reflection ability.Result of high temperature storage stability indicates the organic modification ameliorates the compatibility of LDHs with bitumen. Compared with LDHs, OCLDHs decrease the deteriorations of bitumen’s properties during UV exposure test, exhibiting better effect in enhancing anti-UV aging performance of bitumen. Furthermore,among the three OCLDHs, LDHs intercalated by SDBS exhibit the most effective improvement due to the best compatibility with bitumen and comparatively good UV shielding effect.展开更多
One of the fundamental driving forces in the materials science community is the hunt for new materials with specific properties that meet the requirements of rapidly evolving technology.
Soil contamination by heavy metals has presented severe risks to human health through food chain.As one of the most promising remediation technologies,in-situ immobilization strategy has been widely adopted in practic...Soil contamination by heavy metals has presented severe risks to human health through food chain.As one of the most promising remediation technologies,in-situ immobilization strategy has been widely adopted in practice.However,considering the large quantities of contaminated soil,it is still a huge challenge to design low-cost amendments with strong and long-term immobilization ability.Layered double hydroxides(LDHs)have drawn tremendous attention in fundamental research and practical application because of their unique properties.Moreover,owing to its super-stable mineralization effect to heavy metal ions,LDHs have exhibited great potential in the field of soil remediation.In this work,we mainly focused on the scale production strategy of LDHs with low-cost,and its application in soil remediation.Besides,several key challenges in using LDHs as amendments for immobilization of heavy metal ions are presented.We hope that this mini-review could shed light on the sustainable development of LDHs as amendment for heavy metals in future research directions.展开更多
Oxygen evolution reaction(OER) is a bottle-neck process in many sustainable energy conversion systems due to its sluggish kinetics.The development of cost-effective yet efficient electrocatalysts towards OER is highly...Oxygen evolution reaction(OER) is a bottle-neck process in many sustainable energy conversion systems due to its sluggish kinetics.The development of cost-effective yet efficient electrocatalysts towards OER is highly desirable but still a great challenge at current stage.Herein,a new type of hybrid nanostructure,consisting of two-dimensional(2D) Cerium-doped NiFe-layered double hydroxide nanoflakes directly grown on the 2D Ti3C2Tx MXene surface(denoted as NiFeCe-LDH/MXene),is designed using a facile insitu coprecipitation method.The resultant NiFeCe-LDH/MXene hybrid presents a hierarchical nanoporous structure,high electrical conductivity and strong interfacial junction because of the synergistic effect of Ce doping and MXene coupling.As a result,the hybrid catalyst exhibits an excellent catalytic activity for OER,delivering a low onset overpotential of 197 mV and an overpotential of 260 mV at a current density of 10 mA·cm-2 in the alkaline medium,much lower than its pure LDH counterparts and IrO2 catalyst.Besides,the hybrid catalyst also displays a fast reaction kinetics and a remarkable stable durability.Further theoretic studies using density function theory(DFT) methods reveal that Ce doping could effectively narrow the bandgap of NiFe-LDH and reduce the overpotential in OER process.This work may shed light on the exploration of advanced electrocatalysts for renewable energy conversion and storage systems.展开更多
Flexible thin-film supercapacitors with high specific capacitance are highly desirable for modern wearable or micro-sized electrical and electronic applications. In this contribution, Ni-Co hydroxides(NCH)nanosheets...Flexible thin-film supercapacitors with high specific capacitance are highly desirable for modern wearable or micro-sized electrical and electronic applications. In this contribution, Ni-Co hydroxides(NCH)nanosheets were deposited on top of Ni-Cu alloy(NCA)nanowire arrays forming a freestanding thin-film composite electrode with hierarchical structure for supercapacitors.During electrochemical cycling, the dissolution of Cu into Cu ions will create more active sites on NCA, and the redeposited copper oxide can be coated onto NCH, giving rise to substantial increase in specific capacitance with cycling. Meanwhile, NCA and NCH have excellent conductivity, thus leading to excellent rate performance. This flexible thin-film electrode delivers an ultrahigh initial specific capacitance of 0.63 F·cm^(-2)(or 781.3 F·cm^(-3)).During charge-discharge cycles, the specific capacitance can increase up to 1.18 F·cm^(-2)(or 1475 F·cm^(-3)) along with the“self-etching”process. The electrode presents a better specific capacitance and rate capability compared with previously reported flexible thin-film electrode, and this novel design of etching technique may expand to other binary or ternary materials.展开更多
基金the financial support by Advanced Materials-National Science and Technology Major Project(2024ZD0607400)the National Natural Science Foundation of China(No.52402305)+4 种基金the high-level innovation and entrepreneurship talent project of Qinchuangyuan(No.QCYRCXM-2023-084)the Postdoctoral Fellowship Program of CPSF under Grant Number GZB20230570 and 2024M752552Key projects of Shaanxi Province,China(2023GXLH-001)Natural Science Basic Research Program of Shaanxi(Program No.2024JCYBQN-0494,No.2022TD-27)the State Key Laboratory for Electrical Insulation and Power Equipment(No.EIPE23125)。
文摘High-entropy layered hydroxides(HELHs),an emerging frontier in entropy-stabilized materials derived from layered double hydroxides(LDHs),have captivated attention with their unparalleled tunability,thermodynamic stability,and electrochemical performance.The integration of the high-entropy concept into LDHs empowers HELHs to surmount the constraints of conventional materials through compositional diversity,structurally disordered configurations,and synergistic multi-element interactions.This review systematically embarks on their synthesis methodologies,functional mechanisms,and applications in energy conversion/storage and biomedicine.Advanced synthesis strategies,such as plasma-assisted hydrothermal methods,facilitate precise control over HELH architectures while supporting scalable production.HELHs demonstrate superior electrochemical performance in critical reactions,including oxygen evolution reaction,water oxidation,hydrogen evolution,and glucose electrooxidation.Future directions encompass integrating in situ characterization with simulations,leveraging machine learning for composition screening,and expanding HELHs application through interdisciplinary collaborations.This work establishes a comprehensive roadmap for advancing HELHs as next-generation multifunctional platforms for sustainable energy and biomedical technologies.
基金financially supported from the National Key Research and Development Program of China(2022YFB3803600)the National Natural Science Foundation of China(52301272,22309168,12564025,and 52472205)+7 种基金the Fundamental Research Funds for the Central Universities(CCNU25ZH006)the National College Student Innovation and Entrepreneurship Training Project(202510513082)the Research Program of HBNU(2025X082 and2025Y145)the Foundation of Hubei Key Laboratory of Photoelectric Materials and Devices(PMD202404)the General Program of Open Project of the State Key Laboratory of Precision Welding and Joining of Materials Structures(MSWJ-25M-18)the Key Research Project of Hubei Provincial Department of Education(No.D20252503)the Key Project of Hubei Provincial Natural Science Foundation of China(2025AFD002)the Foundation of National Laboratory of Solid State Microstructures(M37087)。
文摘NiFe layered double hydroxide(NiFe LDH)has emerged as a promising catalyst for the oxygen evolution reaction(OER);however,its hydrogen evolution reaction(HER)activity remains suboptimal due to unfavorable electronic structures,particularly the d-electron density of metal sites,which impede water dissociation and lead to poor hydrogen adsorption/desorption capabilities.Herein,we introduce an efficient cooperative d-electron density regulation(CDDR)engineering to comprehensively optimize the delectron density of NiFe LDH by grafting MoO_(x) -modified NiFe LDH nanosheets onto porous nickel particles(PNPs).The PNPs facilitate d-electron density modulation along the edges of the nanosheets,while the MoO_(x) species enable d-electron density modulation across the plane of the nanosheets,thus cooperatively constructing enriched d-electron density in NiFe LDH.Theoretical studies validate the CDDR process and reveal that the enriched d-electron density accelerates water dissociation and optimizes the hydrogen adsorption behavior of NiFe LDH.As a result,the engineered catalyst exhibits significantly improved HER activity,achieving an ultra-low overpotential of 38 mV at 10 mA cm^(-2)in 1 M KOH.Additionally,the CDDR-optimized catalyst also exhibits good OER performance,demonstrating excellent bifunctional performance for overall water splitting in both alkaline freshwater and seawater electrolytes.This work presents a novel CDDR strategy for engineering NiFe LDH into efficient HER catalysts without compromising its OER activity,potentially paving the way for the development of active and robust electrocatalysts for sustainable energy applications.
基金supported by the research equipment (Nos. G1006,G1010 and G1018) shared in MEXT Project for promoting public utilization of advanced research infrastructure (Program for supporting construction of core facilities)(No. JPMXS0440500023)financial support of the China Scholarship Council.
文摘A method for the effective in-situ formation of boron-containing Mg-Al layered double hydroxides(LDHs)was developed for boron removal and stabilization.The influence of the B/Al molar ratio and pH on the formation of Mg-Al-B–LDHs was investigated.Compared with the adsorption method,under a high B/Al ratio,the coprecipitation method increased the boron sorption density from 0.256 to 0.472 of Al.The Toxicity Characteristic Leaching Procedure showed that the boron-coprecipitated LDHs exhibited higher stability than the boron-adsorption LDHs.The synthesized LDH samples were characterized by X-ray diffraction,X-ray photoelectron spectroscopy,and solid-state 11B-NMR.The results showed that boron was effectively incorporated into the LDH structure for the coprecipitation method.Combined with the experimental results,a potential in-situ formation pathway for Mg-Al-B–LDHs was elucidated through density functional theory calculations.The boron tended to directly incorporate into the LDH structure in the coprecipitation method,whereas it was predominantly adsorbed on the LDH surface in the adsorption method.The adsorption energy demonstrated that boron preferentially bonded to Mg^(2+)sites on the surface.The mechanism of boron incorporation in the LDHs for the coprecipitation method involved precipitation of amorphous aluminum hydroxide,layered boehmite transformation,nucleation,and layer stacking.During these processes,boron formed complexes to enhance its stability.Residual boron underwent further reactions with the LDHs,including surface adsorption and ion exchange.These findings provide theoretical insight into the effective removal and long-term immobilization of boron in landfill leachate self-remediation processes.
基金supported by the Sichuan Provincial Department of Science and Technology Project (2025YFHZ0271).
文摘Owing to its excellent eco-friendliness and facile water elution properties,aluminum-based lithium adsorbents have attracted a surge of interest for selectively extracting Li^(+)from Salt Lake brines,which account for more than 60%of the global lithium resources.However,structural collapse,facile deactivation during desorption process,and ultra-low actual adsorption capacity limit its further large-scale application,particularly in low-grade sulfate-type brines.Herein,considering its advantages,limitations,and structural features,the structural collapse of the aluminum-based lithium adsorbent was effectively suppressed by the in situ intercalation of VO_(3)^(-)and V_(2)O_(7)^(4-)into the interlayer of[LiAl_(2)(OH)_(6)]^(+).Evidently,the initial adsorption capacity andα_(Mg)^(Li)of as-configured adsorbents powder are 14.96 mg g^(-1) and 192.42 in real sulfate-type West Taijinar Salt Lake brines following NaCl salts removal with 800 mg L^(-1) Li^(+)and 9.56 g L^(-1) SO_(4)^(2-).Furthermore,the initial and retained adsorption capacities of these novel adsorbents granulate in brines after 100 adsorption/desorption cycles are 26.68 and 10.36 mg g^(-1),respectively,which are almost 10 times higher than those of industrially utilized products.Based on experiments and density functional theory calculations,the process and mechanism of anion intercalation control were preliminarily elucidated.Furthermore,research findings indicate that intercalated anions can influence not only interlayer interactions but also the backbone strength of LDH-type adsorbents.This work significantly overcomes the major utilization challenges of aluminum-based lithium adsorbents,thereby enabling the high-efficiency and stable extraction of Li^(+)from low-grade brines,including sulfate-type brines.
基金supported by the National Science Fund for Distinguished Young Scholars(No.52025041)the National Natural Science Foundation of China(Nos.52474319,52250091,U2341267,and 52450003)+1 种基金the Fundamental Research Funds for the Central Universities(No.FRF-TP-20-02C2)supported by the Interdisciplinary Research Project for Young Teachers of USTB,China(Fundamental Research Funds for the Central Universities)(No.FRF-IDRY-GD23-003).
文摘CoFe bimetallic hydroxides(CoFe BMHs)find wide applications as excellent catalysts in the field of water splitting.However,no study has systematically investigated the influence of the morphologies of CoFe BMHs on catalyst performance.In this study,CoFe BMH nanoflowers(CoFe BMH NFs),CoFe BMH nanosheets(CoFe BMH NSHs),CoFe BMH nanorods(CoFe BMH NRs),and CoFe BMH nanospheres(CoFe BMH NSPs)were prepared on nickel foam via a hydrothermal method.CoFe BMH NSHs exhibited the most beneficial catalytic activity.At a current density of 100 mA·cm^(-2),its overpotential for oxygen evolution reaction(OER)was 282 mV,and the overall water splitting voltage was 2.05 V.The double-layer charging capacitance(Cdl)value of CoFe BMH NSHs was the largest in CoFe BMHs,which proves that CoFe BMH NSHs have the largest active area.Furthermore,the active site in the OER process was metal oxyhydroxide(MOOH)through in situ Raman characterization,and the generation of the active substance was an irreversible process.This work provides important insights into the design of catalyst morphologies and offers valuable guidelines for the enhancement of the performance of other catalysts.
基金supported by Guangdong Basic and Applied Basic Research Foundation(2022B1515120079)Tertiary Education Scientific research project of Guangzhou Municipal Education Bureau(2024312194)+1 种基金the Science and Technology Projects in Guangzhou(2024A03J0308)the Outstanding Youth Project of Natural Science Foundation of Guangdong Province(2022B1515020020).
文摘Electrically driven water splitting is an efficient method for green hydrogen production;however,its practical application is substantially constrained by the kinetically sluggish anodic oxygen evolution reaction(OER).Ruthenium(Ru)and its oxides are widely recognized as highly active OER catalysts.Although Ru is significantly cheaper than iridium(Ir),further reducing its content remains desirable.Herein,atomically dispersed Ru is doped into iron-nickel layered double hydroxides(Ru-FeNi-LDH)to decrease the Ru usage.We found that the Ru doping limit is roughly 9 wt%,and the Ru doping content significantly alters the OER kinetics-note that the high Ru concentration remarkably damages the Ru-FeNi-LDH structure and leads to agglomeration formation.By optimizing the Ru doping content to 3.3 wt%,the Ru-FeNi-LDH presents a low overpotential of 230 mV to reach a current density of 10 mA cm^(-2) in 1 M KOH,which is far better than the reference FeNi-LDH(280 mV)and RuO_(2)(350 mV).In the overall water splitting test,the current density of 10 mA cm^(-2) can be reached at a low voltage of 1.52 V,with stable operation for 80 h.Interestingly,Ru and Fe form an asymmetric Ru-Fe dipole,which is likely doped together into the LDH because the content of Fe instead of Ni is dependent on Ru content in experimental results.The electron-deficient feature of the Ru-Fe dipole thus facilitates the OER process.This work demonstrates a dual-transition metal synergy,providing a design strategy for OER and related catalysts.
基金financial support of the National Natural Science Foundation of China (22379063)
文摘Layered double hydroxides(LDHs)are potential cathode materials for aqueous magnesium-ion batteries(AMIBs).However,the low capacity and sluggish kinetics significantly limit their electrochemical performance in AMIBs.Herein,we find that oxygen vacancies can significantly boost the capacity,electrochemical kinetics,and structure stability of LDHs.The corresponding structure-performance relationship and energy storage mechanism are elaborated through exhaustive in/ex-situ experimental characterizations and density functional theory(DFT)calculations.Specially,in-situ Raman and DFT calculations reveal that oxygen vacancies elevate orbital energy of O 2p and electron density of O atoms,thereby enhancing the orbital hybridization of O 2p with Ni/Co 3d.This facilitates electron transfer between O and adjacent Ni/Co atoms and improves the covalency of Ni–O and Co–O bonds,which activates Ni/Co atoms to release more capacity and stabilizes the Ov-NiCo-LDH structure.Moreover,the distribution of relaxation times(DRT)and molecular dynamics(MD)simulations disclose that the enhanced d-p orbital hybridization optimizes the electronic structure of Ov-NiCo-LDH,which distinctly reduces the diffusion energy barriers of Mg^(2+)and improves the charge transfer kinetics of Ov-NiCo-LDH.Consequently,the assembled Ov-NiCo-LDH//active carbon(AC)and Ov-NiCo-LDH//perylenediimide(PTCDI)AMIBs can both deliver high specific discharge capacity(182.7 and 59.4 mAh g^(−1)at 0.5 A g^(−1),respectively)and long-term cycling stability(85.4%and 89.0%of capacity retentions after 2500 and 2400 cycles at 1.0 A g^(−1),respectively).In addition,the practical prospects for Ov-NiCo-LDH-based AMIBs have been demonstrated in different application scenarios.This work not only provides an effective strategy for obtaining high-performance cathodes of AMIBs,but also fundamentally elucidates the inherent mechanisms.
基金supported by the Natural Science Foundation of Henan(242300421230)the Young Teacher Fundamental Research Cultivation Program of Zhengzhou University(JC23557030)the National Natural Science Foundation of China(U21A20281 and 22208322)。
文摘Noble metal-loaded layered hydroxides exhibit high efficiency in electrocatalyzing water splitting.However,their widespread use as bifunctional electrocatalysts is hindered by low metal loading,inefficient yield,and complex synthesis processes.In this work,platinum atoms were anchored onto nickel-iron layered double hydroxide/carbon nanotube(LDH/CNT)hybrid electrocatalysts by using a straightforward milling technique with K_(2)Pt Cl_(6)·6H_(2)O as the Pt source.By adjusting the Pt-to-Fe ratio to 1/2 and 1/10,excellent electrocatalysts—Pt_(1/6)-Ni_(2/3)Fe_(1/3)-LDH/CNT and Pt_(1/30)-Ni_(2/3)Fe_(1/3)-LDH/CNT—were achieved with superior performance in hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),outperforming the corresponding commercial Pt/C(20 wt%)and Ru O_(2)electrocatalysts.The enhanced electrochemical performance is attributed to the modification of Pt's electronic structure,which exhibits electron-rich states for HER and electrondeficient states for OER,significantly boosting Pt's electrochemical activity.Furthermore,the simple milling technology for controlling Pt loading offers a promising approach for scaling up the production of electrocatalysts.
基金supported by the National Natural Science Foundation of China (No. 40925011)the Chinese Academy of Sciences (No. KZCX2-YW-446)
文摘Mobilization of arsenic under anaerobic conditions is of great concern in arsenic contaminated soils and sediments. Bacterial reduction of As(V) and Fe(III) influences the cycling and partitioning of arsenic between solid and aqueous phase. We investigated the impact of bacterially mediated reductions of Fe(III)/Al hydroxides-bound arsenic(V) and iron(III) oxides on arsenic release. Our results suggested that As(V) reduction occurred prior to Fe(III) reduction, and Fe(III) reduction did not enhance the release of arsenic. Instead, Fe(III) hydroxides retained their dissolved concentrations during the experimental process, even though the new iron mineral-magnetite formed. In contrast, the release of reduced As(III) was promoted greatly when aluminum hydroxides was incorporated. Thus, the substitution of aluminum hydroxides may be responsible for the release of arsenic in the contaminated soils and sediments, since aluminum substitution of Fe(III) hydroxides universally occurs under natural conditions.
基金The Fundamental Research Funds for the Central Universities,the Scientific Innovation Research of College Graduates in Jiangsu Province(No.CXLX12-0105)the Analysis and Test Fund of Southeast University(No.201226)
文摘Colored layered double hydroxides (LDHs) can be synthesized by introducing colored cations such as Fe^3+ and Cr^3 +, which call be used as thermal stabilizers for polyvinyl chloride (PVC). The yellowish Mg/Fe and bluish Mg/Cr LDHs are prepared by the co-precipitation method. The results show that the MgsCr_ CO3 and Mg3Fe_ CO3 colored layered double hydroxides can stabilize PVC for more than 30 min under the thermal aging temperature of 180 ℃. The preparation can use cheap Mg(OH) 2 instead of MgCl2, which produces a much smaller amount of the by-product NH4Cl. It is known that NH4Cl is a cheap fertilizer that is difficult to sell; therefore, the preparation is much greener and more economic than the one using magnesium salt.
基金Project(21306041)supported by the National Natural Science Young Foundation of ChinaProject(21271071)supported by the National Natural Science Foundation of ChinaProject(15A076)supported by the Scientific Research Foundation of Hunan Provincial Education Department of China
文摘ZnO/NiO/ZnAl2O4 mixed-metal oxides were successfully synthesized through a hydrotalcite-like precursor route, in which appropriate amounts of metal salts solutions were mixed to obtain a new series of ZnNiAl layered double hydroxides(LDHs) as precursors, followed by calcination under different temperatures. The as-obtained samples were characterized by SEM, HRTEM, TEM, XRD, BET, TG-DTA, and UV-Vis spectra techniques. The photocatalytic activities of the samples were evaluated by degradation of methyl orange(MO) under the simulated sunlight irradiation. The effects of Zn/Ni/Al mole ratio and calcination temperature on the composition, morphology and photocatalytic activity of the samples were investigated in detail. The results indicated that compared with ZnNiAl-LDHs, the mixed-metal oxide showed superior photocatalytic performance for the degradation of MO. A maximum of 97.3% photocatalytic decoloration rate within 60 min was achieved from the LDH with the Zn/Ni/Al mole ratio of 2:1:1 and the calcination temperature of 500 ℃, which much exceeded that of Degussa P25 under the same conditions. The possible mechanism of photocatalytic degradation over ZnO/NiO/ZnAl2O4 was discussed.
基金supported by the National Key R&D Program of China(2017YFC0211503,2016YFC0207100)the Strategic Priority Research Program(A)of the Chinese Academy of Sciences(XDA23030300)+2 种基金the National Natural Science Foundation of China(21401200,51672273)the Open Research Fund of State Key Laboratory of Multi-phase Complex Systems(MPCS-2017-D-06)the Young Talent Project of the Center for Excellence in Regional Atmospheric Environment,CAS(CERAE201805)~~
文摘Catalytic oxidation is regarded as one of the most promising strategies for volatile organic compounds(VOCs)purification.Mixed metal oxides(MMOs),after topological transformation using layered double hydroxides(LDHs)as precursors,are extensively used as catalysts for VOCs oxidation due to their uniformity advantage.This review summarizes the developments in the LDH-derived VOCs heterogeneous catalytic oxidation over the last 10 years.Particularly,it addresses the VOCs abatement performance over MMO,noble metal/MMO,core-shell structured MMO,and integral MMO film catalysts originating from LDHs.Moreover,it highlights the water vapor effect and oxidation mechanism.This review indicates that LDH-based catalysts are a category of important VOCs oxidation materials.
基金supported by the National Natural Science Foundation of China and Qinghai Qaidam Saline Lake Chemical Science Research Joint Fund (No. U1607109)
文摘Mg–Al–Fe layered double hydroxides(LDHs) were exfoliated and incorporated in polyether sulfone membranes for the removal of phosphate and fluoride for the first time. The exfoliation methods, coagulation bath, LDH amount, interfering ions, adsorption isotherm,desorption and reuse of the membranes were investigated. It was found that LDHs could be quickly exfoliated in formamide/N,N-dimethylformamide(DMF) solvent mixtures with sodium carboxymethyl cellulose as a stabilizer. The membranes displayed much higher adsorption capacity for phosphate(5.61 mg/g) and faster adsorption rate than the unexfoliated materials. With increased DMF content in the coagulation bath, the static and dynamic adsorption capacity rose. Interference from Cl-and SO4^(2-)(50 mg/L) on adsorption of phosphates was not apparent. The membranes displayed excellent reusability in dynamic adsorption/desorption. The membranes also showed high adsorption capacity for fluorides(1.61 mg/g).
基金supported financially by the National Natural Science Foundation of China(Nos.51971040,51701029 and 51531002)the National Key Research and Development Program of China(No.2016YFB0301100)+3 种基金the Chongqing Research Program of Basic Research and Frontier Technology(No.cstc2016jcyjA0388)the China Postdoctoral Science Foundation Funded Project(Nos.2017M620410 and 2018T110942)the Chongqing Postdoctoral Scientific Research Foundation(No.Xm2017010)the Fundamental Research Funds for the Central Universities(No.2018CDGFCL005).
文摘Anodic oxidation is a prevalent technique to introduce superior corrosion and wear resistance upon the surface of titanium(Ti)alloys,in which the selection of appropriate electrolytes and defect-sealing strategies is a key.This study aims to address such issues through anodizing Ti-10V-2Fe-3Al alloy in malic acid,followed by a post-sealing treatment with Mg-Al layered double hydroxides(LDHs).The characteristics of the samples were investigated using scanning electron microscopy(SEM),atomic force microscopy(AFM),glow discharge optical emission spectroscopy(GDOES),X-ray diffraction(XRD)and energy-dispersive X-ray spectroscopy(EDS).SEM micrographs reveals that the anodic coating had a surface full of bulges and cracks,and was almost sealed by the following LDHs treatment.XRD pattern indicate that the anodic coating was mainly consisted of amorphous TiO2 with a small fraction of anatase,but its crystallization degree was increased through the post-sealing.Moreover,electrochemical and tribological measurements demonstrate that corrosion current density was 2.8×10-6,2.0×10-7,5.9×10-9A cm-2,and wear rate was 1.45×10-3,1.30×10-4 and 6.90×10-5 mm3 N-1 m-1 for respective bare Ti-10V-2Fe-3Al alloy substrate,anodized specimens without and with the LDHs post treatment.Finally,a plausible wear mechanism was proposed.
基金supported by the National Natural Science Foundation of China(Nos.21677055 and 21407052)the Key Project in the National Science&Technology Pillar Program during the Twelfth Five-year Plan Period(No.2015BAB01B04)the Fundamental Research Funds for the Central Universities,HUST(Nos.2017KFXKJC004 and 2016YXMS287)
文摘In this study,greatly enhanced Mn(Ⅱ) adsorption was achieved by as-synthesized diethylenetriaminepentaacetate acid intercalated Mg/Al layered double hydroxides (LDHs-DTPA).The adsorption capacity of LDHs-DTPA was 83.5 mg/g,which is much higher than that of LDHs-EDTA (44.4 mg/g),LDHs-Oxalate (21.6 mg/g) and LDHs (28.8 mg/g).The adsorption data of aqueous Mn(Ⅱ) using LDHs-DTPA could be well described by the pseudosecond order kinetics and Langrnuir isotherm model.Thermodynamics study results also showed that the adsorption process of Mn(Ⅱ) by LDHs-DTPA was exothermic as indicated by the negative △H value.Furthermore,based on the structural,morphological and thermostable features,as well as FT-IR and XPS characterizations of LDHs-DTPA and the pristine LDHs,the adsorption mechanism of Mn(Ⅱ) was proposed.The carboxyl groups of DTPA were proposed to be the main binding sites for Mn(Ⅱ),and the hydroxyl groups of LDHs also played a minor role in the adsorption process.Among the three common regeneration reagents,0.1 mol/L Na2CO3 was the best for reusing LDHs-DTPA in Mn(Ⅱ) adsorption.Besides,the Mn(Ⅱ) adsorption performance could be hindered in the presence of typical inorganic ions,especially cations.Further specific modifications of LDHs-DTPA are suggested to get more selective adsorption of Mn(ll) in practical applications.
基金Funded by the National Natural Science Foundation of China(No.51708121)the National Basic Research Program of China(973 Program)(No.2014CB932104)the Educational Research Projects for Young and Middle-Aged Teachers of Education Department of Fujian Province(No.JAT170067)
文摘Layered double hydroxides(LDHs) with the physical property of high ultraviolet(UV)reflectance were used to enhance the anti-UV aging performance of bitumen. In view of the poor compatibility of LDHs with bitumen, three organic anions, namely, sodium dodecyl benzenesulfonate(SDBS), sodium dodecyl sulfate(SDS) and sodium dodecyl sulfonate(SDSO), were used as modifiers to prepare organic LDHs(OCLDHs) through regeneration process, and the crystal structure, chemical composition, morphological feature and UV shielding capability of synthesized OCLDHs were analyzed. Then the OCLDHs were added into bitumen to evaluate the storage stability and anti-UV aging property of OCLDHs/bitumen composites.The results show that the organic anions are inserted into the interlayers of LDHs, the intercalation expands the interlayer distance of LDHs, makes the particle shapes become more irregular and complicated, and enhances the absorption ability within the range from 200 to 300 nm while has little influence on the UV reflection ability.Result of high temperature storage stability indicates the organic modification ameliorates the compatibility of LDHs with bitumen. Compared with LDHs, OCLDHs decrease the deteriorations of bitumen’s properties during UV exposure test, exhibiting better effect in enhancing anti-UV aging performance of bitumen. Furthermore,among the three OCLDHs, LDHs intercalated by SDBS exhibit the most effective improvement due to the best compatibility with bitumen and comparatively good UV shielding effect.
基金supported by the National Natural Science Foundation of China(Grant Nos.21701043,21825201 and U19A2017)the Provincial Natural Science Foundation of Hunan(2019GK2031)+1 种基金the Open Project Program of Key Laboratory of Low Dimensional Materials&Application Technology(Xiangtan University),Ministry of Education,China(No.KF20180202)the China Postdoctoral Science Foundation(Grant Nos.2019 M662766,2019 M662759,2020 M682549,and 2020 M672473)。
文摘One of the fundamental driving forces in the materials science community is the hunt for new materials with specific properties that meet the requirements of rapidly evolving technology.
基金supported by the National Natural Science Foundation of China(21978023)the Fundamental Research Funds for the Central Universities(XK1803-05)+1 种基金the Inno-vative Achievement Commercialization Service-Platform of Indus-trial Catalysis(2019-00900-2-1)the National Basic Research Program of China(2014CB932104)。
文摘Soil contamination by heavy metals has presented severe risks to human health through food chain.As one of the most promising remediation technologies,in-situ immobilization strategy has been widely adopted in practice.However,considering the large quantities of contaminated soil,it is still a huge challenge to design low-cost amendments with strong and long-term immobilization ability.Layered double hydroxides(LDHs)have drawn tremendous attention in fundamental research and practical application because of their unique properties.Moreover,owing to its super-stable mineralization effect to heavy metal ions,LDHs have exhibited great potential in the field of soil remediation.In this work,we mainly focused on the scale production strategy of LDHs with low-cost,and its application in soil remediation.Besides,several key challenges in using LDHs as amendments for immobilization of heavy metal ions are presented.We hope that this mini-review could shed light on the sustainable development of LDHs as amendment for heavy metals in future research directions.
基金supported by the Science Foundation of China University of Petroleum, Beijing (No. 2462017YJRC013)。
文摘Oxygen evolution reaction(OER) is a bottle-neck process in many sustainable energy conversion systems due to its sluggish kinetics.The development of cost-effective yet efficient electrocatalysts towards OER is highly desirable but still a great challenge at current stage.Herein,a new type of hybrid nanostructure,consisting of two-dimensional(2D) Cerium-doped NiFe-layered double hydroxide nanoflakes directly grown on the 2D Ti3C2Tx MXene surface(denoted as NiFeCe-LDH/MXene),is designed using a facile insitu coprecipitation method.The resultant NiFeCe-LDH/MXene hybrid presents a hierarchical nanoporous structure,high electrical conductivity and strong interfacial junction because of the synergistic effect of Ce doping and MXene coupling.As a result,the hybrid catalyst exhibits an excellent catalytic activity for OER,delivering a low onset overpotential of 197 mV and an overpotential of 260 mV at a current density of 10 mA·cm-2 in the alkaline medium,much lower than its pure LDH counterparts and IrO2 catalyst.Besides,the hybrid catalyst also displays a fast reaction kinetics and a remarkable stable durability.Further theoretic studies using density function theory(DFT) methods reveal that Ce doping could effectively narrow the bandgap of NiFe-LDH and reduce the overpotential in OER process.This work may shed light on the exploration of advanced electrocatalysts for renewable energy conversion and storage systems.
基金financially supported by the National Basic Research Program of China(No.2015CB654603)the National Natural Science Foundation of China(No.51572141,51532003)+1 种基金Beijing Nova Program(No.XX2013037)the Research fund of Science and Technology in Shenzhen(No.JSGG20150331155519130)
文摘Flexible thin-film supercapacitors with high specific capacitance are highly desirable for modern wearable or micro-sized electrical and electronic applications. In this contribution, Ni-Co hydroxides(NCH)nanosheets were deposited on top of Ni-Cu alloy(NCA)nanowire arrays forming a freestanding thin-film composite electrode with hierarchical structure for supercapacitors.During electrochemical cycling, the dissolution of Cu into Cu ions will create more active sites on NCA, and the redeposited copper oxide can be coated onto NCH, giving rise to substantial increase in specific capacitance with cycling. Meanwhile, NCA and NCH have excellent conductivity, thus leading to excellent rate performance. This flexible thin-film electrode delivers an ultrahigh initial specific capacitance of 0.63 F·cm^(-2)(or 781.3 F·cm^(-3)).During charge-discharge cycles, the specific capacitance can increase up to 1.18 F·cm^(-2)(or 1475 F·cm^(-3)) along with the“self-etching”process. The electrode presents a better specific capacitance and rate capability compared with previously reported flexible thin-film electrode, and this novel design of etching technique may expand to other binary or ternary materials.