JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 10
·4225-4235
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IF 3.5
Yang Xingchen,Fan Zhitian,Ni Rui,Zheng Long,Lu Haiyan
The original MOFs exhibit poor electrochemical performance when used as electrode materials for supercapacitors. To improve their conductivity and stability, in situ growth of high specific capacitance and conductivity layered double hydroxide (LDH) on the MOFs surface is an ideal approach. In this study, we employed the MOF as a template and employed a secondary hydrothermal synthesis method to enable in situ growth of NiCo-LDH on the surface of the MOF. The utilization of the MOF template enhances the stability of NiCo-LDH, while the flower-like structure of LDH exposes more active sites. By optimizing the Ni:Co molar ratio to 1:2 and the urea:NH 4 F molar ratio to 2:1, the resulting material exhibits higher specific capacitance and improved cycle stability. Specifically, at a current density of 1 A g −1 , the specific capacitance reaches 1674 F g −1 . At a current density of 5 A g −1 , the capacity retention rate after 2000 cycles is 80%. When NiCo-LDH/HKUST-1 is assembled with activated carbon as a supercapacitor, it exhibits a significant energy density of 33.96 Wh kg −1 and a power density of 745.4 W kg −1 . This work provides a novel approach for utilizing MOF-based composite materials as positive electrode materials for supercapacitors. Graphical Abstract
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Journal of Central South University
·
2024
·Vol. 31
·期 4
·1292-1305
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IF 3.7
Hou Jin-feng,Sun Qian,Hao Xiu-zhen
Heavy metal composite pollution is becoming increasingly serious. In this study, CaAl-layered double hydroxide (CaAl-LDH) was prepared using the facile co-precipitating method, and was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), fourier transform infrared (FTIR) spectroscopy and X-ray photoelectron spectroscopy (XPS). Lead(II), Cd(II), and As(V) were selected as the representative heavy metals to evaluate the adsorption capability of the synthesized CaAl-LDH by the batch experiments. The maximal adsorption capability of CaAl-LDH for Pb(II), Cd(II), and As(V) was 786.6, 437.2 and 72.9 mg/g, respectively. The adsorption mechanism of Pb, Cd and As may be surface precipitation, isomorphic substitution and ion exchange within the interlayer spaces of LDH, respectively. In conclusion, this experiment provides a LDH material with fast and efficient adsorption performance for both anionic and cationic metals, indicating its potential for practical application in the remediation of heavy metal composite pollution.
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Emerging Contaminants
·
2024
·
IF 5.3
Yuxuan Zhang,Kai He,Long Chen,Wen Liu,Jinlong Yuan,Yaotong Gao,Yuanfeng Qi,Bingjun Liu
Residual enrofloxacin (ENR) exposed in aqueous environments is challenging to the ecosphere. In this work, a layered double hydroxide CoAl-LDH was used to activate the common oxidizing agent persulfate (PS) for photodegradation of ENR, and the degradation pathways of ENR were scrutinized and elucidated. The results indicated that, under the optimal conditions obtained through orthogonal experiments, even though the degradation rate of ENR was as high as 97.72%, the removal of total organic carbon (TOC) from the system was only about 30%. Eleven probable reaction pathways were categorized, and thirty-one types of intermediates were identified in participating in the complex degradation process. The major products of ENR were P4 (C 17 H 20 FN 3 O 3 ), P22 (C 19 H 22 FN 3 O 4 ), P19 (C 17 H 18 FN 3 O 3 ), which are mainly derived from the cleavage of the piperazine groups and quinolone rings. Density functional theory (DFT) calculations of the Fukui index for ENR revealed that the two N atoms in the piperazine ring were the core reactive sites in triggering the degradation chains, which were sensitive for electrophilic attack by the dominant radicals (•OH and SO 4 • - ) generated from the composite PS-UV-CoAl-LDH system.
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APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Jie Yang,Lixia Ma,Yuqi Zhang,Xuqian Zhao,Shouren Zhang,Luo Huang,Yunpeng Fang,Xiaojie Zhou,Jianghao Kang,Ruibin Jiang
The design of low-cost and highly efficient bifunctional electrocatalyst towards oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is challengeable, which limits the commercial application of rechargeable zinc-air battery. Herein, an efficient ORR and OER bifunctional electrocatalyst (NiFe-LDH/F x −FeN 4 /C) is composed of nickel/iron-based heterostructures sparsely grown on carbon black (CB) with single FeN 4 sites. The NiFe-LDH/F x − FeN 4 /C electrocatalysts are prepared through the pyrolysis of hemin chloride adsorbed on CB, followed by in-situ hydrothermal growth of NiFe-LDH/F x heterostructures. The NiFe-LDH/F x heterostructures are composed of NiFe-LDH, (NH 4 ) 3 FeF 6 , and NiF 2 . The elevated valence states of Fe and Ni in heterostructures significantly increase the OER activity. The mesopores and large pores of the NiFe-LDH/F x − FeN 4 /C facilitate the exposure of active sites and enhance mass transfer. These features contribute to the outstanding bifunctional activity of NiFe-LDH/F x − FeN 4 /C, achieving a half-wave potential of 0.906 V for the ORR, an OER overpotential of 246 mV at 10 mA cm −2 , and an extremely small voltage gap of 0.57 V. Additionally, the NiFe-LDH/F x − FeN 4 /C-based RZAB also exhibits a peak power density of 209 mW cm −2 and charging/discharging cycling stability for 445 h. This work establishes a novel strategy for the preparation of highly efficient bifunctional electrocatalysts through in-situ growth and heterostructure engineering.
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Materials Today Communications
·
2025
·
IF 4.5
Zhou Jie,Siyuan Jin,Ruizhi Wu,Xiaochun Ma,Haoran Wang,Mengyao Pang,Zhe Yu,Wang Guixiang,Jinghuai Zhang,Boris Krit,Sergey Betsofen,Neshchimenko Vitalii,Buzikov Ruslan,Min Qiu,Yurong Yang,Jiaming Chen
Due to the poor corrosion resistance of Mg-Li alloys and the limited effectiveness of single surface treatment methods, developing a composite coating is essential to significantly enhance the corrosion protection. In this study, a stable ceramic coating was fabricated on the surface of a Mg-Li alloy by micro-arc oxidation with regulation of the concentration of ZnO nanoparticles added to the electrolyte. Layered double hydroxides (LDH) was subsequently prepared on the coating surface by modulating the hydrothermal temperature, contributing to blocking the micropores and cracks to enhance the compactness of the coating. Additionally, a low-surface-energy hexadecyltrimethoxysilane (HDTMS) was selected to self-assemble on a rough micro/nano structured MAO/LDH coating to obtain a superhydrophobic surface The composite coating exhibited exceptional corrosion resistance, with the R ct value increasing by four orders of magnitude compared to the substrate and the Y 0 (CPE out ) reduced to the 10 -9 range. Furthermore, the coating keeps almost non-corrosion morphology after 7 days of immersion in 3.5% NaCl solution, which is attributed to the combined effects of the superhydrophobicity of HDTMS, the physical barrier effect and chloride ion trapping ability of LDHs, and the reduction in porosity achieved through the incorporation of nano-ZnO in MAO coating.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yawen Xu,Ye Li,Yizhi Du,Jinlong Zhang,Siyi Li,Chao Zhang,Xiaoli Ren,Zhiqiang Xu,Bing Xue,Fangfei Li
In this work, a W O bond-enriched NiFe layered double hydroxide composite (NiFe-LDH@NWT) was synthesized as a high-performance electrocatalyst for the oxygen evolution reaction (OER) in alkaline media. The incorporation of W O bonds effectively modulates the local electronic environment and surface charge distribution of the NiFe-LDH, thereby enhancing its intrinsic activity and interfacial reactivity. Electrochemical measurements reveal that NiFe-LDH@NWT delivers low overpotentials of 236 mV at current densities of 100 mA cm −2 , respectively, with a small Tafel slope of 33.53 mV dec −1 , indicating favorable reaction kinetics. In addition, the electrochemically active surface area (ECSA) reaches 7.82 mF cm −2 , confirming the increased density of accessible active sites upon W O bond integration. Notably, the catalyst maintains excellent operational stability for over 1000 h at a current density of 100 mA cm −2 . These findings highlight a promising strategy to tailor the physicochemical properties of LDH-based catalysts, providing valuable insights into the rational design of stable and efficient OER systems for water-splitting applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Ruoxuan Zheng,Wan-Lei Zhao,Hongqiang Li,Hanbin Hu,Tong Lin,Wei Chen,Yu-Fei Song
The effective removal of Cu 2+ ions from contaminated wastewater is greatly significant for environmental remediation. Herein, the PAN@LDH-Hpdc (PAN = polyacrylonitrile; LDH = layered double hydroxide; Hpdc = pyrazole-3,5-dicarboxylate) was prepared using the “Seeds Embedded-Epitaxial Growth-Ion exchange” strategy. Benefiting from the high surface area and abundant exposed active sites, the PAN@LDH-Hpdc showed the removal efficiency of 99.6 % in 25 min, and the Cu 2+ ions (10 ppm) can be decreased to reach the WHO drinking water standard in 10 min. When the concentration of Cu 2+ ions was ∼ 1000 ppm, the adsorption capacity of PAN@LDH-Hpdc was as high as 200.0 mg/g. In addition, the PAN@LDH-Hpdc exhibited high selectivity for Cu 2+ ions with the removal efficiency of 99.9 % in the mixed solution containing Na + , Mg 2+ , K + , Ca 2+ , Cu 2+ , Ni 2+ , Zn 2+ and Co 2+ ions. The adsorption mechanisms of PAN@LDH-Hpdc involved the coordination by the intercalated Hpdc anions and surface adsorption by the LDH laminate.
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RSC Advances
·
2025
·Vol. 15
·期 7
·5277-5285
·
IF 4.6
Dongfeng Shi,Xiyin Mao,Min Fei,Cong Liang,Yuyang Luo,Zhidan Xu,Liyong Hu
Antibiotics are frequently detected in aquatic environments, posing potential risks to ecological systems and human health. Among the various treatment strategies, advanced oxidation processes (AOPs) utilizing peroxymonosulfate (PMS) activation stand out due to their ease of activation and potent oxidative capabilities. This study synthesized manganese–iron–copper layered double hydroxides coupled with graphene oxide (MnFeCu-LDH/GO) using eco-friendly transition metals. Optimal conditions of pH 7, 298 K, and 0.2 g L−1 dosage of both catalyst and PMS achieved 98% CTC removal in 30 minutes. The composite was employed for the degradation of chlortetracycline (CTC) through PMS activation. Reactive oxygen species (ROS), including 1O2, ˙OH, and SO4˙−, were identified and quantified through trapping and quenching experiments, and 1O2 was identified, to be the most significant contributor to degradation. The catalyst demonstrated excellent reusability, maintaining high degradation efficiency after five cycles. These findings suggest that MnFeCu-LDH/GO-activated PMS is a promising method for mitigating antibiotic contamination in water.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Wenqian Zhu,Wenhe Yu,Zehong Yin,Fengzhu Lv,Jiajing Feng
Tetracycline hydrochloride (TC) water pollution poses a serious threat to human health. Preparation of a high-efficiency TC treatment agent is one of the key tasks in TC wastewater treatment. The present work innovatively designed and successfully prepared a three-dimensional layered double hydroxide nanocage (H-NiCo-LDH) to efficiently remove TC through synergistic adsorption and non-photocatalytic degradation. The nanocage structure, derived from Co-ZIF through the Kirkendall effect, featured ultrathin nanosheets with a high specific surface area of 659 m2 g−1 and abundant oxygen vacancies (Ovs). The material showed excellent TC removal performance in a wide pH (5–11) and temperature (5–45 °C) range, and the removal rate of 20 mg L−1 of TC reached 99.6% in 5 min. In addition, the maximum removal amount reached 630 mg g−1, which was higher than that of most reported LDHs. The removal mechanism was confirmed to be the combined effect of adsorption and 1O2 driven degradation. Remarkably, the degradation pathway, independent of light, relied on Ov-mediated dissolved oxygen. Liquid chromatography-mass spectrometry (LC-MS) gave the primary intermediates of TC degradation, and toxicity assessment showed that the degradation process decreased the environmental risks of TC. The work provides a paradigm for designing self-sustaining catalysts for antibiotic removal in complex aquatic environments.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Guoying Yang,Yijin Song,Songde Han,Zhen-Zhen Xue,De-Xuan Liu,Ani Wang,Guoming Wang
Assembling a heterostructure is an effective strategy for enhancing the electrocatalytic activity of hybrid materials. Herein, CoFe-layered double hydroxide and Co-metal–organic framework (CoFe-LDH/Co-MOF) hollow heterostructure nanorod arrays are synthesized. First, [Co(DIPL)(H3BTC)(H2O)2]n [named as Co-MOF, DIPL = 2,6-di(pyrid-4-yl)-4-phenylpyridine, H3BTC = 1,3,5-benzenetricarboxylic acid] crystalline materials with a uniform hollow structure were prepared on the nickel foam. The CoFe-LDH/Co-MOF composite perfectly inherits the original hollow nanorod array morphology after the subsequent electrodeposition process. Optimized CoFe-LDH/Co-MOF hollow heterostructure nanorod arrays display excellent performance in oxygen evolution reaction (OER) with ultralow overpotentials of 215 mV to deliver current densities of 10 mA cm–2 and maintain the electrocatalytic activity for a duration as long as 220 h, ranking it one of the non-noble metal-based electrocatalysts for OER. Density functional theory calculations validate the reduction in free energy for the rate-determining step by the synergistic effect of Co-MOF and CoFe-LDH, with the increased charge density and noticeable electron transfer at the Co–O site, which highlights the capability of Co-MOF to finely adjust the electronic structure and facilitate the creation of active sites. This work establishes an experimental and theoretical basis for promoting efficient water splitting through the design of heterostructures in catalysts.
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Sustainable Materials and Technologies
·
2025
·
IF 9.2
Jingyuan Wei,Yanhui Song,Manyuan Gan,Guodong An,Yongqing Shen,Xiaohui Zhao,Yi Zhang,Peizhi Liu,Bingshe Xu,Junjie Guo
Modifying the catalyst's electronic structure is essential for improving the hydrazine oxidation reaction (HzOR) and alkaline hydrogen evolution reaction (HER), but it is still very difficult. We have developed a new heterostructured electrocatalyst in this work using Ru nanosheets and NiCo layered double hydroxides (LDH). In-situ Raman and theoretical studies show that the heterostructure of Ru/NiCo LDH lowers absorption of hydrogen's Gibbs free energy and the d-band center of Ru/NiCo LDH (from −1.7250 to −1.3341 eV), causing the directed development of interfacial H 2 O (ΔG H* , from 1.65 to 0.23 eV). With an overpotential of 19 and 75 mV to achieve 10 and 100 mA cm −2 for HER, these beneficial characteristics provide the Ru/NiCo LDH with exceptional electrocatalytic capabilities. For HzOR, 10 and 100 mA cm −2 may be produced using just −118 and−112 mV, respectively. The Ru/NiCo LDH electrolyzer also only needs 22 and 223 mV to produce 10 and 100 mA cm −2 , respectively. This work lays the groundwork for developing bifunctional catalysts for the green hydrogen industry.
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KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.2
Liu Xilin,Yang Fuwei,Yao Zhiqian,Wang Xuan,Liu Pengfei,Li Jiayin,Zhou Hu
Immobilizing the activator on the carrier is an effective strategy to solve the difficult recovery and secondary pollution of activator in advanced oxidation process. In this study, cobalt–aluminum-layered double hydroxide (activator) was immobilized on a PU membrane carrier (Co–Al-LDH@PU membrane) by a hydrothermal in situ growth technique to form a recyclable peroxymonosulfate (PMS) activator. The as-prepared Co–Al-LDH@PU membrane exhibited an excellent ability to activate PMS for the removal of tetracycline hydrochloride (TC). 97.20% of TC (30 mg L −1 ) was eliminated with Co–Al-LDH@PU membrane (3 × 3 cm 2 ) and 1.6 mM PMS at pH 5.5 in 30 min. Singlet oxygen ( 1 O 2 ) was verified as dominant reactive oxygen species responsible for TC removal via quenching tests. Mechanism investigation suggested that the redox cycle of Co 2+ /Co 3+ on the surface of Co–Al-LDH@PU membrane was crucial for PMS activation. Meanwhile, Co–Al-LDH@PU membrane displayed the ideal reusability and versatility.
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