INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Zunpeng Hu,Senjie Dong,Quanfeng He,Zihao Chen,Ding Yuan
Developing electrocatalysts that integrate the merits of the hollow structure and heterojunction is an attractive but still challenging strategy for addressing the sluggish kinetics of oxygen evolution reaction (OER) in many renewable energy technologies. Herein, a 3D hierarchically flexible self-supporting electrode with a hollow heterostructure is intentionally constructed by assembling thin NiFe layered double hydroxide (LDH) nanosheets on the surface of metal–organic framework-derived hollow NiCo2O4 nanoflake arrays (NiCo2O4@NiFe-LDH) for rechargeable Zn–air batteries (ZABs). Theoretical calculations demonstrate that the interfacial electron transfer from NiFe-LDH to NiCo2O4 induces the electronic modulation, improves the conductivity, and lowers the reaction energy barriers during OER, ensuring high catalytic activity. Meanwhile, the 3D hierarchically hollow nanoarray architecture can afford plentiful catalytic active sites and short mass-/charge-transfer pathways. As a result, the obtained catalyst exhibits remarkable OER electrocatalytic performance, showing low overpotentials (only 231 mV at 10 mA cm–2, 300 mV at 50 mA cm–2) and robust stability. When assembling liquid and flexible solid-state ZABs with NiCo2O4@NiFe-LDH as the OER catalyst, the ZABs achieve excellent power density, high specific capacity, superior cycle durability, and good bending flexibility, exceeding the RuO2 + Pt/C benchmarks and other previously reported self-supporting catalysts. This work not only constructs an advanced hollow heterostructured catalyst for sustainable energy systems and wearable electronic devices but also provides insights into the role of interfacial electron modulation in catalytic performance enhancement.
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高影响因子
Nanomaterials
·
2018
·Vol. 8
·期 2
·113
·
IF 3.504
Lijun Wang,Yusen Wang,Xiaoxia Wang,Xiaolan Feng,Xiao Ye,Jie Fu
Layered double hydroxides (LDHs) have been widely used as an important subset of solid base catalysts. However, developing low-cost, small-sized LDH nanoparticles with enhanced surface catalytic sites remains a challenge. In this work, silica aerogel (SA)-supported, small-sized Mg–Al LDH nanosheets were successfully prepared by one-pot coprecipitation of Mg and Al ions in an alkaline suspension of crushed silica aerogel. The supported LDH nanosheets were uniformly dispersed in the SA substrate with the smallest average radial diameter of 19.2 nm and the thinnest average thickness of 3.2 nm, both dimensions being significantly less than those of the vast majority of LDH nanoparticles reported. The SA/LDH composites also showed large pore volume (up to 1.3 cm3·g) and pore diameter (>9 nm), and therefore allow efficient access of reactants to the edge catalytic sites of LDH nanosheets. In a base-catalyzed Henry reaction of benzaldehyde with nitromethane, the SA/LDH catalysts showed high reactant conversions and favorable stability in 6 successive cycles of reactions. The low cost of the SA carrier and LDH precursors, easy preparation method, and excellent catalytic properties make these SA/LDH composites a competitive example of solid-base catalysts.Keywords:layered double hydroxides;nanocatalysts;mesoporous silica;support;solid base
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2018
·
IF 3.779
Ziqiang Ai,Changqing Liu,Qiwu Zhang,Jun Qu,Zhao Li,Xiaoman He
In this study, a mechanochemical route to promote the adsorption of the precursor of Zn-Al layered double hydroxide (LDH) was introduced, in which ZnO and SiO 2 were added to Zn basic carbonate and Al hydroxide that were first dry milled into an activated state as a precursor for a LDH phase. The samples prepared in this way were characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR) and Scanning electron microscopy (SEM). The precursors showed a high adsorption rate when added with the oxides. 10% addition of ZnO gave a maximum MO removal efficiency of 96.91% (193.82 mg/g at initial MO concentration of 160 mg/L), 16.46% higher than the sample without addition. Addition of SiO 2 at 25% allowed MO removal efficiency reaching 88.90% (222.25 mg/g, at initial MO concentration of 200 mg/L), 19.26% higher than the no additive sample. The improvement in the adsorption performance could be attributed to the effective dispersion of the precursor's agglomeration phenomenon. Discussion was performed based on the characterized features of the samples and fitting results on several adsorption models.
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DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 32
·12168-12176
·
IF 4.052
Hanchun Xia,Geng Li,Haoran Cai,Xiaolong Li,Peiheng Sun,Peijia Wang,Jiajie Huang,Liang Wang,Desuo Zhang,Yefeng Yang,Jie Xiong
The development of flexible energy storage devices for portable and wearable electronics has aroused increasing interest. In this work, three-dimensional hierarchical NiCo2O4@NiMn-LDH nanowire/nanosheet arrays have been successfully fabricated on carbon cloth through a facile hydrothermal and calcination synthetic method. Benefiting from the sophisticated hybrid nanoarchitectures with desirable structure and components, the optimized NiCo2O4@NiMn-LDH hybrid electrode is found to deliver a remarkable specific capacity of 278 mA h g−1 at 2 mA cm−2 and a good rate capability of 89.1% retention at 20 mA cm−2. Detailed analysis of the reaction kinetics for the hybrid electrode clearly indicates the dominant diffusion-controlled contribution to the total capacity. In addition, a flexible solid-state hybrid supercapacitor is assembled by taking NiCo2O4@NiMn-LDH and activated carbon as the cathode and anode, respectively, which manifests a maximum energy density of 47 W h kg−1 at a power density of 357 W kg−1 as well as an excellent long-term cycling stability (95.6% retention after 5000 cycles over 8 mA cm−2). Our work demonstrates the great potential of this core/shell hybrid nanostructure as an advanced battery-type electrode for high-performance flexible energy storage devices.
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高影响因子
ACS Applied Materials & Interfaces
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2017
·
IF 7.504
Yanna Wang,Liguang Dou,Hui Zhang
A series of novel nanosheet array-like catalysts Pdx/rGO@CoAl-LDH (x = 0.0098–1.9, refers to Pd loading in wt % on ICP, rGO: reduced graphene oxide, LDH: layered double hydroxide) were first prepared via a simple and green lattice atomic-confined in situ reduction of oxidative Pd precursors by the evenly atomic-dispersed reductive Co2+ sites on LDH layers of a nanohybrid rGO@CoAl-LDH with hexagonal LDH nanoplates (∼73 × 7 nm) interdigitated vertical to the surfaces of rGO layer in both sides, fabricated through a simple citric acid-assisted aqueous-phase coprecipitation method. The as-obtained Pd catalysts possess clean Pd nanoclusters (NCs) with tunable sizes in 1.3–1.8 nm on varied Pd loadings. All the Pdx/rGO@CoAl-LDH catalysts show excellent activities for the Heck reaction, and the Pd0.0098/rGO@CoAl-LDH with the ultrafine Pd NCs of 1.3 ± 0.2 nm yields a maximum turnover frequency of 160 000 h–1 over a heterogeneous catalyst so far. The excellent activities can be attributed to the ultrasmall Pd NCs with high dispersion and clean Pd surfaces, increased electron transfer capacity and surface area, and remarkable Pd–CoAl-LDH—rGO three-phase synergistic effect of the present unique nanosheet array-like Pd NCs catalysts. Moreover, the catalyst Pd0.33/rGO@CoAl-LDH shows a broad range of substrate applicability and can be reused more than five runs without obvious loss of activity, giving the present catalysts long-term stability. These findings make the rGO@CoAl-LDH hybrid prepared by a facile and scalable synthesis route a universal green platform to support other noble or nonprecious metal NCs via lattice atomic-confined in situ reduction strategy to construct more desired heterogeneous catalysts.
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CORROSION SCIENCE
·
2024
·
IF 7.4
Jingjing Wang,Yanhui Cao,Junhao Xue,Xinyue Zhang,Yu Liang,Kaifeng Chen,Congshu Huang,Dajiang Zheng
The in-depth influence mechanism of the functional groups and conjugated structure of aromatic inhibitor on the corrosion protection ability of CaAl layered double hydroxide (CaAl-LDH) in epoxy coatings was investigated by performing the inhibitor modification using three typical aromatic inhibitors. The electrochemistry impedance spectroscopy (EIS) measurement demonstrated that CaAl-LDH-MBT showed superior protection for carbon steel in epoxy coatings. Density functional theory (DFT) calculation and molecular dynamic (MD) simulation indicated that the aromatic conjugated structure with larger π electron clouds and heteroatoms with lone pair electrons would contribute to the enhanced corrosion protection.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhibin Chen,Jinke Wang,Lin Lu,Thee Chowwanonthapunya,Weiting Chen,Zongbao Li,Lingwei Ma,Dawei Zhang
A corrosion-oriented self-healing coating system relying on metal–organic framework (MOF) based nanofiller is designed for aluminum alloy protection. The nanofiller is comprise of ZnMg MOF nanoparticle as a framework, salicylaldoxime corrosion inhibitors inside the MOF, and a polydopamine layer on the MOF surface. The Al 3+ ions generated from the aluminum alloy substrate at the damaged coating area can etch the nanofiller, causing the collapse of the nanofiller and releasing the corrosion inhibitors to suppress the corrosion process in time. Subsequently, Zn 2+ and Mg 2+ ions from the nanofiller co-precipitate with Al 3+ to form a dense AlZnMg layered double hydroxide (LDH) film, which provides further protection performance at the exposed alloy surface. Electrochemical impedance spectroscopy results demonstrate that the intact MOF@S/P coating exhibits a remarkable corrosion resistance property. For the damaged coating, the self-healing performance originated from the formation of LDH layer and the release of corrosion inhibitors gradually took effect, with the |Z| 0.01Hz value increasing 2.27 times within 14 days. Moreover, under near-infrared irradiation, the photothermal effect of polydopamine will accelerate the release of corrosion inhibitor, the formation of LDH film, as well as the shape memory effect of coating defect for an efficient recovery of the corrosion resistance property. This novel coating system enables a corrosion-driven and location-specific repair with in-situ deposition of both an inhibitor film and an LDH film. As the first work to fully utilize and consume nanofillers on demand, this approach prevents inadequate use of healing agents, addressing a significant challenge in corrosion-driven self-healing coatings. The self-healing mechanism ensures target-oriented corrosion protection that makes the most efficient use of the healing substances.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 28
·17574-17585
·
IF 10.7
Xinping Yang,Shucheng Li,Yan Zhang,Fagui Qiu,Yanbin Sun,Weikun Ning,Qinglong Tao,Wenqing Li,Shiding Miao
Nickel–iron layered bimetallic hydroxides (Ni3Fe LDHs) are regarded as excellent materials for electrodes for electrolyzing water but still require high overpotentials because of their weak adsorption/desorption of oxygen intermediates by metal–oxygen bonding (M–O). Herein, the rare earth element thulium (Tm) was selected for incorporation into Ni3Fe LDH owing to its particular electronic structure of 4f136s2, and the composite LDH was regulated using an electron-compensated buffer to avoid the overoxidation of M–O and was proven to be an excellent OER electrocatalyst. By further loading platinum (Pt) on the Tm-doped LDH (Ni3Fe LDH/NiFe2O4/Pt–Tm), the HER performance was also found to be greatly improved, and overall water splitting catalysts could be constructed utilizing the two types of Ni3Fe LDH-based materials. The state-of-the-art optimized Ni3Fe LDH/NiFe2O4/Pt–Tm composite in 1.0 M KOH solution achieved an OER overpotential as low as 224.0 mV at a current density of 10.0 mA cm−2, which was one of the lowest among previously reported LDHs, with a Tafel slope of 54.81 mV dec−1 and a turnover frequency (0.1969 s−1). For HER catalysis, Ni3Fe LDH/NiFe2O4/Pt–Tm exhibited an even lower overpotential of 125.0 mV (vs. 238.0 mV for bare Ni3Fe LDH) at 10.0 mA cm−2, and only 1.69 V was required to drive overall water splitting. The electrocatalytic stability was evaluated for 5000 cycles of cyclic voltammetry scanning and chronoamperometry tests. Raman and XPS spectra confirmed that structural regulation promoted the generation of NiOOH and the adsorption of intermediates. In particular, oxygen vacancies and unsaturated ligands were preserved, providing abundant active sites for electrocatalysis.
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Nano Research
·
2024
·
IF 9.5
Su Jihao,Yang Ling,Yu Dengbin,Dong Shaojun
A significant challenge in developing high-performance hybrid supercapacitors (HSCs) is the need to reasonably construct advanced architectures that consist of various components and exhibit superior electrochemical capacitance performance. The FeCoNi-layered double hydroxide (FeCoNi-LDH) porous material has a specific capacitance of 1960 F·g −1 when used as the anode material at 1 A·g −1 . The FeCoNi-LDH material exhibits nanoplates with a distinct spindle morphology on their surface. Due to the combined action of the three metals and abundant oxygen vacancies, they exhibit unique rate performance and cycle stability. The electronic structure of LDH and the regulation of oxygen vacancy were confirmed by density functional theory (DFT) calculations. This suggests that the strength of hydroxide can reduce the energy required for oxygen vacancy formation in FeCoNi-LDH nanosheets and enhance ion and charge transfer, as well as electrolyte adsorption on the electrode surface. The FeCoNi-LDH//activated carbon (AC) HSC has an energy density of 53.2 Wh·kg −1 at a power density of 800 W·kg −1 , surpassing other devices composed of comparable materials during the same timeframe. This study made significant advances in the design and synthesis of a ternary LDH porous structure with distinct oxygen vacancies, as well as its potential application in electrochemical energy storage.
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Journal of Energy Storage
·
2024
·
IF 8.9
Yu-Gang Fu,Yi-Han Li,Qiu-Feng Lü
Nickel‑cobalt layered double hydroxide (NiCo-LDH) has received much attention in the field of supercapacitor electrodes due to its multiple oxidation states and good electrochemical activity. However, NiCo-LDH often suffers from structural instability and low conductivity in practical applications. In this study, sea urchin-like structural NiCo-LDH coated cobalt‑nitrogen co-doped carbon (NiCo-LDH@Co-NC-x) electrode materials were prepared by in situ growth of NiCo-LDH on the surface of cobalt‑nitrogen co-doped carbon nanosheets (Co-NC) using a one-step hydrothermal method. The results show that the NiCo-LDH@Co-NC-2 electrode material exhibits excellent electrochemical performance, its specific capacitance is up to 1909 F g −1 at a current density of 1 A g −1 , and capacitance retention of 69.5 % (only 26.2 % for NiCo-LDH) can be achieved after 10,000 cycles at a current density of 10 A g −1 . This is because the abundant and uniformly distributed Co nanoparticles on Co-NC provide nucleation sites for the in-situ growth of NiCo-LDH, effectively improving the interface binding between Co-NC and NiCo-LDH, enhancing the structural stability of NiCo-LDH, and ensuring highly efficient electron transport throughout the NiCo-LDH@Co-NC-2 electrode. An asymmetric supercapacitor (NiCo-LDH@Co-NC-2//AC) was further assembled with NiCo-LDH@Co-NC-2 and activated carbon (AC) as positive and negative electrodes, respectively, achieving an energy density as high as 36.8 Wh kg −1 at a power density of 750 W kg −1 . These findings suggest that the NiCo-LDH@Co-NC-2 composite can be a promising candidate for high-performance supercapacitor electrode.
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LWT-FOOD SCIENCE AND TECHNOLOGY
·
2024
·
IF 6
Yuanyi Wu,Yumei Xiao,Yang Ju,Yanque Sun,Jialin He,Tian Liu,Miao He,Kaiyong Wang,Yi Yang
The determination of gallic acid (GA), one of the most prevalent antioxidants in various plants, provides information for food nutrition evaluation. A novel colorimetric, fluorescent, and smartphone multi-mode GA sensing platform based on Fe 3 O 4 @Co/Ni/Al-layered double hydroxide (LDH) nanospheres was designed in this study. The core-shell magnetic Fe 3 O 4 @Co/Ni/Al-LDH nanospheres were synthesized through a simple co-precipitation approach. They showed dominate peroxidase-like activities capable of oxidizing 3,3′,5,5′-tetramethylbenzidine (TMB) into a blue colored oxidation oxTMB. Meanwhile, the generated oxTMB could quench the fluorescence of neutral red via the inner filter effect. GA acted as an inhibitor to prevent the oxidation of TMB to oxTMB and restoring the fluorescence of neutral red. Under optimized conditions, the linear ranges were 0.5–120 μmol/L with detection limits of 0.137–0.415 μmol/L. Besides, the sensor exhibited good selectivity toward GA over various interferents. Moreover, it was successfully utilized to analyze GA in tea beverages with ideal recoveries of 92.8–105%, demonstrating good reliability and stability in practical applications. This study provided Fe 3 O 4 @Co/Ni/Al-LDH nanospheres as candidate nanozymes for the construction of biosensors. The multi-mode self-checking function and the “turn on” fluorescent sensing strategy offered this sensor superior anti-interference ability, and opens up a new strategy for the determination of antioxidants in foods.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Guangyao Yang,Weiliang Peng,Jianwei Ye,Renzong Hu,Qiying Han,Sen Li,Bin Yuan
Although low-cost nickel-iron layered double hydroxide (NiFe LDH) has admirable electrolytic activity for oxygen evolution reaction (OER), the high energy barrier of hydrogen adsorption restricts its application as a bifunctional catalyst for alkaline overall water-splitting. Herein, sulfur (S) and phosphorus (P) elements have been co-introduced into a NiFe LDH on a nickel-iron foam (NIF) via sulfurating and phosphorizing co-thermal treatment, whereupon the phase composition and electronic structure are optimized, forming the (S, P)-NiFe LDH/NIF bifunctional catalyst. Benefiting from the synergy effect caused by the multiphasic interfaces, the (S, P)-NiFe LDH/NIF surprisingly exhibits an ultra-low overpotential of only 29 mV to induce hydrogen evolution reaction (HER) at a current density of 10 mA cm −2 , showing outstanding HER performance. In addition, the obtained catalyst also shows remarkable OER performance with an overpotential of only 190 mV at a current density of 10 mA cm −2 . Moreover, the symmetric electrolyzer assembled by the bifunctional (S, P)-NiFe LDH/NIF catalysts can deliver a current density of 100 mA cm −2 at a cell voltage of only 1.75 V, and maintain the reaction activity continuously for up to 200 h, showing excellent overall water-splitting performance. This work is expected to provide a new insight for designing and synthesizing bifunctional electrocatalysts based on low-cost NiFe LDH, further promoting and realizing the large-scale water-electrolysis.
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