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Schematic representation of synthetic methods for the preparation of Cell@LDH biohybrid materials by a) adsorption, b) layer-by-layer deposition and c) direct coprecipitation. 

Schematic representation of synthetic methods for the preparation of Cell@LDH biohybrid materials by a) adsorption, b) layer-by-layer deposition and c) direct coprecipitation. 

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This review highlights the current research on the interactions between biological cells and Layered Double Hydroxides (LDH). The as-prepared biohybrid materials appear extremely attractive in diverse fields of application relating to health care, environment and energy production. We describe how thanks to the main features of biological cells and...

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... to better control the biohybrid nanostructura- tion and the amount of immobilized biological cells, other soft chemical routes have been investigated by our group to prepare biological cells/LDH assemblies such as layer-by-layer deposition and direct coprecipitation, as illustrated in Fig- ure 3. Starting from colloidal solution of LDH nanoparticles, we succeeded to prepare bacteria@LDH biohybrid thin films. [58] The layer-by-layer assembly technique relying on the sequential adsorption on a substrate was implemented from LDH nanosheets and Pseudomonas sp. strain ADP through an alternate immersion of a substrate in different solutions. [58] The layer-by-layer technique, [79] leading to nanostructured thin films is well-known to favor electrostatic interactions between positively-charged layers and negatively-charge mol- ecules. By this way, nanostructured Pseudomonas sp. strain ADP@LDH thin films were developed (Figure 3). The assembly process was efficiently monitored by UV-vis spectroscopy evidencing an increase of the deposited amount upon successive cycles while the biological activity is confirmed by chronoamperometry (see part ...
Context 2
... to better control the biohybrid nanostructura- tion and the amount of immobilized biological cells, other soft chemical routes have been investigated by our group to prepare biological cells/LDH assemblies such as layer-by-layer deposition and direct coprecipitation, as illustrated in Fig- ure 3. Starting from colloidal solution of LDH nanoparticles, we succeeded to prepare bacteria@LDH biohybrid thin films. [58] The layer-by-layer assembly technique relying on the sequential adsorption on a substrate was implemented from LDH nanosheets and Pseudomonas sp. strain ADP through an alternate immersion of a substrate in different solutions. [58] The layer-by-layer technique, [79] leading to nanostructured thin films is well-known to favor electrostatic interactions between positively-charged layers and negatively-charge mol- ecules. By this way, nanostructured Pseudomonas sp. strain ADP@LDH thin films were developed (Figure 3). The assembly process was efficiently monitored by UV-vis spectroscopy evidencing an increase of the deposited amount upon successive cycles while the biological activity is confirmed by chronoamperometry (see part ...

Citations

... Layered double hydroxide (LDH) can adsorb most bacteria and viruses in water (You et al., 200;Forano et al., 2018), although this fact was not covered in the review by Sellaoui et al. (2021). LDH is harmless to humans and is used in pharmaceuticals (Forano et al., 2018). ...
... Layered double hydroxide (LDH) can adsorb most bacteria and viruses in water (You et al., 200;Forano et al., 2018), although this fact was not covered in the review by Sellaoui et al. (2021). LDH is harmless to humans and is used in pharmaceuticals (Forano et al., 2018). It is also effective in adsorbing bacteria such as Escherichia coli (E. ...
... coli.: ATCC 15597 and 13706) and Bacillus subtilis (Jin et al., 2007;Liu et al., 2013), along with bacteriophage viruses like MS2 and øX174 (You et al., 2003;Park et al., 2012) from water. This adsorption ability is due to the positive charge of LDH, which attracts the negatively charged surfaces of most bacteria and viruses through electrostatic forces (Liu et al., 2013;Forano et al., 2018). However, due to the powdery nature of LDH, its utilization in batch or column methods presents inherent difficulties, thus limiting the practical application of LDH in POU water treatment methods (Dou et al., 2022). ...
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Waterborne pathogens from poor sanitation are the main cause of drinking water problems facing humanity in the 21 st century, leading to infections and diarrhea. This results in over half a million deaths annually, with most of them occurring in developing countries such as Indonesia. Due to the lack of access to centralized water treatment facilities, point-of-use (POU) systems have been suggested as an important solution for water treatment in developing communities. These systems are user-friendly, low-cost, low-maintenance, and do not depend on the power grid. Importantly, they treat and reduce the number of pathogens in the water supply, and many POU systems have been implemented and used by communities on a household scale. However, the POU system has limitations that hinder its implementation in Indonesia. To examine and evaluate the technology implemented in POU systems, this review focuses on systems that can serve households or communities. The advantages, disadvantages, and limitations of technology that have existed in the last decade are explained. By taking the case of Indonesia, it is hoped that this review can provide an evaluation and illustration of its application in similar developing countries. Another affordable technological solution suggested that could benefit people relying on unsafe water sources.
... However, when LDH is utilized for drug delivery, the drug loading capacity is limited by the limited interlayer spacing (≈2 nm) and the high charge intensity between the layers. [105,106] Zhang et al. [107] constructed ultra-thin LDH nanosheets (P-LDH) using polymer assisted synthesis method. As shown in Figure 4f, the drug loading capacity of P-LDH was much greater than that of traditional multi-layer LDH. ...
Article
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Cancer is one of the most serious diseases challenging human health and life span. Cancer has claimed millions of lives worldwide. Early diagnosis and effective treatment of cancer are very important for the survival of patients. In recent years, 2D nanomaterials have shown great potential in the development of anticancer treatment by combining their inherent physicochemical properties after surface modification. 2D nanomaterials have attracted great interest due to their unique nanosheet structure, large surface area, and extraordinary physicochemical properties. This article reviews the advantages and application status of emerging 2D nanomaterials for targeted tumor synergistic therapy compared with traditional therapeutic strategies. In order to investigate novel potential anticancer strategies, this paper focuses on the surface modification, cargo delivery capability, and unique optical properties of emerging 2D nanomaterials. Finally, the current problems and challenges in cancer treatment are summarized and prospected.
... The profuse clinical application scope withal toxicity screening for the successful bench-to-bedside translation of LDHs. Therefore, much effort has been taken to understand the bio-nano interaction of LDHs at the in-vitro level, individually focusing on different cell systems depending upon the chosen bio-application [17]. Alongside, the increased usage of LDHs for various applications has raised concerns about exposure toxicity, and many studies have been reported on the effect of different types of LDHs at in-vivo levels including aquatic systems [18][19][20]. ...
... The toxicity of LDHs is variably dependable on the composition of both cation-anion, concentration, particle size, physico-chemical parameters, and exposed cell type [17]. On a previous toxicity evaluation by Baek et al., Mg-Al-CO 3 LDHs showed higher ROS production and oxidative stress in in-vitro model compared to the chloride-incorporated counterpart. ...
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LDHs, 2D (two-dimensional) clay material with memory effect clutches noteworthy properties like high surface area, ion-exchange capacity, tunable properties and possibility for wide elemental as well as anion combinations. A variety of LDHs are being explored for profuse applications including catalysis, absorbent material, flame retardants, drug delivery, polymer additives and bone regeneration. Recent research updates reveal the promising potential of LDHs in bone tissue engineering and are expected to grab a major hold in futuristic medicare. There have been tremendous efforts concentrated on fine-tuning the LDHs properties by controlling the growth parameters to improve its multi-functionality. In this study, an effort has been made to synthesize and characterize Zn–Al LDHs via the co-precipitation method with control over the nucleation and hydrothermal growth steps. The interactions of the fabricated Zn–Al LDHs with human osteoblast (HOS) cells were explored in the context of bone regeneration applications. The effect of Zn–Al LDHs on the mitochondrial function of HOS cells was examined. The study also evaluated the potential of LDHs to trigger apoptosis by using DNA fragmentation as the marker. The potential impact of positively charged LDHs on negatively charged DNA was also probed using the DNA laddering assay, as an audit on genotoxic potential. Graphical abstract
... Adsorption offers a practical means of disinfection by effectively eliminating bacteria and viruses from water (Sellaoui et al. 2021). Layered double hydroxides (LDHs) are potent adsorbents with demonstrated capacity to adsorb a wide spectrum of bacteria and viruses from water (You et al. 2003;Forano et al. 2018). The adsorption is primarily because of the electrostatic attraction between the positively charged LDH and negatively charged microbial surfaces, which is enhanced by anion exchange, OH-exchange, hydrogen bonding, and polar interactions (Liu et al. 2013). ...
... The adsorption is primarily because of the electrostatic attraction between the positively charged LDH and negatively charged microbial surfaces, which is enhanced by anion exchange, OH-exchange, hydrogen bonding, and polar interactions (Liu et al. 2013). LDH is nontoxic to humans and is used in pharmaceutical applications (Forano et al. 2018). The unique trait of LDH as an immobilization medium is intriguing because the bacteria adsorbed onto it remain viable and activated (Forano et al. 2018). ...
... LDH is nontoxic to humans and is used in pharmaceutical applications (Forano et al. 2018). The unique trait of LDH as an immobilization medium is intriguing because the bacteria adsorbed onto it remain viable and activated (Forano et al. 2018). However, in batch or column water treatment, the powdery nature of LDH poses challenges, hindering its application for POU treatment (Dou et al. 2022). ...
Article
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Point-of-use (POU) drinking water treatment is crucial for residents in resource-constrained areas. This study introduces a layered double hydroxide (LDH) foil, an innovative POU device that eliminates waterborne pathogens via adsorption. It is an aluminum foil coated with magnesium–aluminum (Mg–Al)-type LDH, a recognized human-safe pathogen adsorbent. Its sheet-like morphology enables easy retrieval of inherently powdered LDH from post-disinfected water. Coating with Mg–Al LDH foils was accomplished by immersing aluminum foils in alkaline magnesium solutions, resulting in the on-surface formation of LDH. Using 12 distinct alkaline magnesium solutions, 12 types of LDH foils were prepared. Most LDH foils demonstrated >99% removal of Escherichia coli (DH5α strain) within 3–24 h when 100 mL of water was inoculated with DH5α at approximately 103 colony-forming units (CFU)/mL was agitated with a 25-cm2 LDH foil piece. The LDH foil with the highest efficacy had a maximum adsorption capacity of approximately 1.3 × 106 CFU per 1-cm2 LDH foil. Furthermore, the LDH foil was regenerated by submersing it in the alkaline solution during its preparation, enabling multiple reuses. Owing to its straightforward production and application, the LDH foil holds substantial promise as a convenient-to-use adsorbent for batch water disinfection, such as jug water, in rural households.
... The adsorption force is Coulombic because LDHs have positive charges, whereas the surfaces of most bacteria and viruses are negatively charged (Liu et al. 2013). LDH is safe for human consumption and finds applications in the pharmaceutical industry as well (Hoyo 2007;Forano et al. 2018). Recently, Mg-Al type LDH was formed directly on the surface of an aluminum alloy plate by treating it with a solution of Mg (Fukugaichi et al. 2022). ...
... For both LDH foils, the LDH appeared to adhere firmly to the surface, and no detachment was observed. Although Mg-Al LDH is safe for humans (Hoyo 2007;Forano et al. 2018), the dissolution of surface LDH following prolonged immersion in water needs to be further investigated to ensure safety during long-term use. ...
... When LDH-foil-5 was added to the test solution, the viable count of DH5α decreased from approximately 10 3 CFU mL À1 to 134 CFU mL À1 after 10 min, then further decreased to 14 CFU mL À1 after 1 h and reached almost zero (0.25 CFU mL À1 ) after 24 h. As LDH is known to be harmless to bacteria (Forano et al. 2018), it is reasonable to assume that the reduction in viable count was exclusively attributed to the adsorption of DH5αassume that the decrease in the viable count was solely due to the adsorption of DH5α. The alive of adsorbed DH5α on the LDH foil was confirmed by the numerous colonies observed by naked eyes on the LDH foils when putting in a lisogeny broth agar, then incubated at 37°C for 24 h, after taking out from the test solutions. ...
Article
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The contamination of drinking water by pathogens poses a serious health hazard in developing countries. Herein, a simple sanitization tool for drinking water is proposed using layered double hydroxide (LDH), which adsorbs most pathogens with its positive charges. By immersing aluminum foil in a mixture of seawater and NaOH without heating, a Mg–Al type LDH was directly formed and adhered to the surface (LDH foil). An LDH foil of 20 cm2 was shaken in 100 mL of test water containing Escherichia coli (DH5α) for up to 24 h and manually removed from the water. The initial viable count of approximately 103 CFU mL−1 decreased to 14 CFU mL−1 in 1 h, reaching 0.25 CFU mL−1 in 24 h; without the LDH foil, the variation 980–1,270 CFU mL−1. The simplicity in its development and use makes LDH foil a promising tool for sanitizing household water among rural residents. HIGHLIGHTS A foil with Mg–Al LDH directly formed on the surface was created from aluminum foil (LDH foil).; LDH foil adsorbed most of the Escherichia coli species (DH5α) from water.; LDH foil is easily removed from treated water.; LDH foil has the potential to be a sanitization tool for batch water, such as household jug water.;
... The higher surface area, rheological, and adsorption properties are preferred for a wide range of applications. Moreover, the chemically inert nature of these materials makes them more biocompatible [102]. ...
Article
The death caused by multidrug-resistant pathogens is increasing day by day, and it needs special attention due to the challenges faced by the world health care systems. Hence, there is an urgent need to develop novel materials for antimicrobial and drug delivery applications due to the emergence of multidrug-resistant microbial pathogens. The innovations in polymer nanotechnology have paved the way to explore their applications in biomedical and other industrial sectors. Two-dimensional (2D) materials are ultrathin nanomaterials that receive great attention due to the degree of anisotropy, a higher surface area, antimicrobial activity, and a drug-carrying capacity. These easily tunable materials can be functionalized with any material of interest that makes them superior to others. The polymer nanocomposites based on 2D materials can have significant potential in drug delivery and antimicrobial applications. Hence, this review will give an overview of different types of 2D nanomaterials, their properties, their interaction with biological systems, their antimicrobial mechanisms, antiviral properties, 2D material-based viral detection, their interaction with surfaces, immunomodulating effect, biocompatibility, 2D materials and inflammation, polymer composites based on 2D materials, and their antimicrobial as well as biomedical applications.
... mg/L) . Lastly, LDHs show low toxicity to humans (e.g., Forano et al., 2018;Mishra et al., 2018). However, as far as we know, there is only a single ecotoxicological study of LDHs (Cu-Mg-Fe) on freshwater organisms, which is chemically different from Zn-Al LDH-NO 3 . ...
Article
Layered double hydroxides (LDHs) are stimuli-responsive anionic nanoclays. The vast possibilities of using LDHs can lead to their existence in the ecosystem, raising a question of potential ecological concern. However, little is known about the effect of these nanomaterials on freshwater organisms. The present study aimed to assess the ecotoxicological effects of Zinc-Aluminium LDH-nitrate (ZnAl LDH-NO3) in zebrafish (Danio rerio) early life stages. The endpoints measured were mortality, malformations and hatching rate after exposure of D. rerio embryos and larvae to ZnAl LDH-NO3 following the OECD 236 guideline. The behavioral, biochemical (markers of oxidative stress and neurotoxicity), and molecular (at DNA level) alterations were also assessed using sub-lethal concentrations. No observable acute effects were detected up to 415.2 mg LDH/L while the 96 h-LC50 was estimated as 559.9 mg/L. Tested LDH caused malformations in D. rerio embryos, such as pericardial edema, incomplete yolk sac absorption and tail deformities (96 h-EC50 = 172.4 mg/L). During the dark periods, the locomotor behavior in zebrafish larvae was affected upon ZnAl LDH-NO3 exposure. However, no significant biochemical and molecular changes were recorded. The present findings suggest that ZnAl LDH-NO3 can be regarded as a non-toxic nanomaterial towards D. rerio (E/LC50 > > 100 mg/L) although impairment of the locomotion behavior on zebrafish embryos can be expected at concentrations below 100 mg/L.
... The structural M n+ ions allocated in the hydroxylated layers can add functionality to LDH as follow: zinc, magnesium, and iron ions, natural elements in bone tissue, can be incorporated in scaffolds for bone tissue engineering [135]; copper and zinc for antimicrobial therapies concerning skin wound healing [148,149]; aluminum in vaccine carriers [150]; iron, copper, or manganese biomaterials for Fenton-like catalytic reactions applied in chemodynamic therapy (CDT), endogenously activated, or photodynamic therapy (PDT) and sonodynamic therapy (SDT), endogenously activated [151]. ...
Article
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The development of biomaterials has a substantial role in pharmaceutical and medical strategies for the enhancement of life quality. This review work focused on versatile biomaterials based on nanocomposites comprising organic polymers and a class of layered inorganic nanoparticles, aiming for drug delivery (oral, transdermal, and ocular delivery) and tissue engineering (skin and bone therapies). Layered double hydroxides (LDHs) are 2D nanomaterials that can intercalate anionic bioactive species between the layers. The layers can hold metal cations that confer intrinsic biological activity to LDHs as well as biocompatibility. The intercalation of bioactive species between the layers allows the formation of drug delivery systems with elevated loading capacity and modified release profiles promoted by ion exchange and/or solubilization. The capacity of tissue integration, antigenicity, and stimulation of collagen formation, among other beneficial characteristics of LDH, have been observed by in vivo assays. The association between the properties of biocompatible polymers and LDH-drug nanohybrids produces multifunctional nanocomposites compatible with living matter. Such nanocomposites are stimuli-responsive, show appropriate mechanical properties, and can be prepared by creative methods that allow a fine-tuning of drug release. They are processed in the end form of films, beads, gels, monoliths etc., to reach orientated therapeutic applications. Several studies attest to the higher performance of polymer/LDH-drug nanocomposite compared to the LDH-drug hybrid or the free drug.
... LDHs are considered as efficient delivery agents for various biomolecules into cells during treatment of different diseases [3,131,132]. Conjugation of bio-active compounds with the LDH carrier involves interfacial interaction between the host and guest, i.e., adsorption on either the outer surface or within the layers. ...
Article
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Layered double hydroxides (LDHs) are appealing nanomaterials for (bio)medical applications and their potential is three-fold. One can gain advantage of the structure of LDH frame (i.e., layered morphology), anion exchanging property towards drugs with acidic character and tendency for facile surface modification with biopolymers. This review focuses on the third aspect, as it is necessary to evaluate the advantages of polymer adsorption on LDH surfaces. Beside the short discussion on fundamental and structural features of LDHs, LDH-biopolymer interactions will be classified in terms of the effect on the colloidal stability of the dispersions. Thereafter, an overview on the biocompatibility and biomedical applications of LDH-biopolymer composite materials will be given. Finally, the advances made in the field will be summarized and future research directions will be suggested.
... As investigations on nanocarrier increased, there arose safety issues of the nanomaterials depending on their physicochemical properties. In fact, there have been lots of researches to reveal the low or no cytotoxicity of LDH particles (Choi et al., , 2008Choi and Choy, 2011a;Yang et al., 2016;Forano et al., 2018). Typically, Choi et al. reported that the LDH particles did not induce serious suppression in cultured cell lines of human normal lung cells (L− 132), human lung epithelial carcinoma cells (A549), hepatoblastoma cells (HepG2), and breast adenocarcinoma cells (MCF-7) (Choi et al., , 2008 and that the LDH particles injected to BALB/c mice in suspension states exhibit neither significant pathological manifestation nor toxic signals in systemic level (Choi et al., 2008Yu et al., 2013). ...
Article
Biological behavior of layered double hydroxide (LDH) toward human blood cells was evaluated with respect to the particle size and surface charge parameters. Three kinds of LDHs with different particle sizes were prepared by different synthesis routes and surface charge of the LDH was controlled by coating with citrate, malate or serine. Powder X-ray diffraction patterns and scanning electron microscopic (SEM) analyses indicated that the three LDHs before surface coating had average diameter ~ 160 nm, ~ 340 nm and ~ 1980 nm with well-crystallized hydrotalcite-like structure. According to zeta potential measurement, the surface coating with citrate, malate, and serine gave controlled zeta potential of −15.28 mV, 5.68 mV, and 36.5 mV, respectively. It was confirmed that all the six LDH samples regardless of size and surface charge did not induce serious hemolysis toward human red blood cells (RBCs), of which the value was less than 2.5% even in a high administration concentration of 10 mg/mL. However, the LDH with the largest size showed statistically a higher hemolysis ratio than the others at the high administration dose and long exposure time. The SEM showed that the large LDH particles induced membrane disruption by direct attack, while most of the LDH particles were softly landed on the RBC surface. Comparative SEM study suggested that the membrane interaction of LDH toward RBC was different from that with adherent cells. The adherent cells showed massive attachment of LDH particles on membrane periphery with active endocytosis. It was therefore concluded that LDH particles with moderate size are highly compatible to human blood cells.