The construction of communication models at the micro‐/nanoscale involving abiotic nanodevices and living organisms has the potential to open a wide range of applications in biomedical and ...communication technologies. However, this area remains almost unexplored. Herein, we report, as a proof of concept, a stimuli‐responsive interactive paradigm of communication between yeasts (as a model microorganism) and enzyme‐controlled Janus Au–mesoporous silica nanoparticles. In the presence of the stimulus, the information flows from the microorganism to the nanodevice, and then returns from the nanodevice to the microorganism as a feedback.
If yeasts could talk: An interactive paradigm of communication between yeasts and enzyme‐controlled Janus Au–mesoporous silica nanoparticles is reported. The fluorescent signal from the microorganism (corresponding to the production of green fluorescent protein) is governed by the biunivocal communication with the nanodevice through enzymatic reactions and the exchange of chemical messengers.
Helicobacter pylori (H. pylori) is a recalcitrant pathogen, which can cause gastric disorders. During the past decades, polypharmacy‐based regimens, such as triple and quadruple therapies have been ...widely used against H. pylori. However, polyantibiotic therapies can disturb the host gastric/gut microbiota and lead to antibiotic resistance. Thus, simpler but more effective approaches should be developed. Here, some recent advances in nanostructured drug delivery systems to treat H. pylori infection are summarized. Also, for the first time, a drug release paradigm is proposed to prevent H. pylori antibiotic resistance along with an IVIVC model in order to connect the drug release profile with a reduction in bacterial colony counts. Then, local delivery systems including mucoadhesive, mucopenetrating, and cytoadhesive nanobiomaterials are discussed in the battle against H. pylori infection. Afterward, engineered delivery platforms including polymer‐coated nanoemulsions and polymer‐coated nanoliposomes are poposed. These bioinspired platforms can contain an antimicrobial agent enclosed within smart multifunctional nanoformulations. These bioplatforms can prevent the development of antibiotic resistance, as well as specifically killing H. pylori with no or only slight negative effects on the host gastrointestinal microbiota. Finally, the essential checkpoints that should be passed to confirm the potential effectiveness of anti‐H. pylori nanosystems are discussed.
Here, some novel strategies are proposed for future of H. pylori treatment using nanomedicines. For effective smart multifunctional nanosystems based on polymer‐coated nanoemulsions and polymer‐coated nanoliposomes, it is necessary to prevent the early release of therapeutic cargos in the acidic pH, to protect them against enzymes and acidic microenvironment, and precisely target H. pylori in its survival zone (basic pH).
Here, a new bio‐inspired nanoarchitectonics approach for the design of optical probes is presented. It is based on nanodevices that combine 1) an enzymatic receptor subunit, 2) a signaling subunit ...(consisting of a labeled reporter attached to a silica surface), and 3) a mechanism of communication between the two sites based on the production of chemical messengers by the enzymatic subunit, which induces the detachment of the reporter molecules from the silica surface. As a proof of concept, a urea nanosensor based on the release of Alexa‐Fluor‐647‐labeled oligonucleotide from enzyme‐functionalized Janus gold–mesoporous‐silica nanoparticles (Au–MSNPs) was developed. The Janus particles were functionalized on the silica face with amino groups to which the labeled oligonucleotides were attached by electrostatic interactions, whereas the gold face was used for grafting urease enzymes. The nanodevice was able to release the fluorescent oligonucleotide through the enzyme‐mediated hydrolysis of urea to ammonia and the subsequent deprotonation of amino groups on the silica face. This simple nanodevice was applied for the fluorometric detection of urea in real human blood samples and for the identification of adulterated milk. Given the large variety of enzymes and reporter species that could be combined, this is a general new paradigm that could be applied to the design of a number of optical probes for the detection of target analytes.
Designing biosensors: A new paradigm for the design of optical sensors based on nanodevices incorporating an enzymatic receptor subunit and a hybrid signaling subunit that communicate through chemical messengers is presented. As a proof of concept, a urea nanosensor based on the release of an oligonucleotide labeled with Alexa Fluor 647 from urease‐functionalized Janus gold–mesoporous‐silica nanoparticles (Au–MSNPs) was developed.
Harnessing interactions of functional nano‐compartments to generate larger particle assemblies allows studying diverse biological behaviors based on their population states and can lead to the ...development of smart materials. Herein, thiol‐functionalized polymersome nanoreactors are utilized as responsive organelle‐like nano‐compartments—with inherent capacity to associate into larger aggregates in response to change in the redox state of their environment—to study the kinetics of cascade reactions and explore functions of their collective under different population states. Two nanoreactor populations, glucose oxidase‐ and horseradish peroxidase‐loaded polymersomes, are prepared, and the results of their cascading upon addition of glucose are investigated. The kinetics of resorufin production in associated polymersomes and non‐associated polymersome populations are compared, observing a decreased rate upon association. For the associated populations, faster chemical cascading is found when the two types of nanoreactors are associated in a concerted step, as compared to sequential association. The addition of competing agents such as catalase impacts the communication between non‐associated polymersomes, whereas such an effect is less pronounced for the associated ones. Altogether, the results showcase the impact of collective associations on enzymatic cascading between organelle‐like nanoreactors.
Herein, thiol‐functionalized semipermeable polymersomal nanoreactors that are able to collectively associate, depending on their redox state, are presented. Using these responsive organelle‐like nano‐compartments, two types of communicating nanoreactors loaded with complementary enzyme molecules (glucose oxidase and horseradish peroxidase) are prepared, that are utilized to study the kinetics of cascade reactions (resorufin production) under different population states.
Janus gold nanostar–mesoporous silica nanoparticle (AuNSt–MSNP) nanodevices able to release an entrapped payload upon irradiation with near infrared (NIR) light were prepared and characterized. The ...AuNSt surface was functionalized with a thiolated photolabile molecule (5), whereas the mesoporous silica face was loaded with a model drug (doxorubicin) and capped with proton‐responsive benzimidazole‐β‐cyclodextrin supramolecular gatekeepers (N 1). Upon irradiation with NIR‐light, the photolabile compound 5 photodissociated, resulting in the formation of succinic acid, which induced the opening of the gatekeeper and cargo delivery. In the overall mechanism, the gold surface acts as a photochemical transducer capable of transforming the NIR‐light input into a chemical messenger (succinic acid) that opens the supramolecular nanovalve. The prepared hybrid nanoparticles were non‐cytotoxic to HeLa cells, until they were irradiated with a NIR laser, which led to intracellular doxorubicin release and hyperthermia. This induced a remarkable reduction in HeLa cells viability.
NIR‐light irradiation of a Janus gold nanostar–mesoporous silica nanoparticle nanodevice induced succinic acid generation and doxorubicin release due to the dethreading of a supramolecular nanovalve.
'Communication' between abiotic nanoscale chemical systems is an almost-unexplored field with enormous potential. Here we show the design and preparation of a chemical communication system based on ...enzyme-powered Janus nanoparticles, which mimics an interactive model of communication. Cargo delivery from one nanoparticle is governed by the biunivocal communication with another nanoparticle, which involves two enzymatic processes and the interchange of chemical messengers. The conceptual idea of establishing communication between nanodevices opens the opportunity to develop complex nanoscale systems capable of sharing information and cooperating.
A novel organic–inorganic hybrid compound, named (1-phenylpiperazinium) trihydrogen triphosphate, with the formula (C
10
H
15
N
2
)
2
H
3
P
3
O
10
has been obtained by low speed of evaporation of a ...mixture of an alcoholic solution of 1-phenylpiperazine and triphosphoric acid H
5
P
3
O
10
at room temperature after using the ion exchange chemical procedure. To carry out a detailed crystallographic structure analysis, single-crystal X-ray diffraction has been reported. In the molecular arrangement, the different entities are held together through N–H
…
O, O–H
…
O, and C-H
…
O hydrogen bonds, building up a three-dimensional packing. Powder X-ray diffraction analysis is acquired to confirm the purity of the product. The nature and the proportion of intermolecular interactions were investigated by Hirshfeld surface analysis. In order to support the experimental results, a density functional theory (DFT) calculation was performed, using the Becke-3-parameter-Lee–Yang–Parr (B3LYP) function with LANL2DZ basis set, and the data indicate much agreement between the experimental and the theoretical results. Thus, the physicochemical properties were studied employing a variety of techniques (FTIR, NMR, UV–visible, and photoluminescence). To get an insight of the possible employment of the present material in biology, cell viability assays were performed.
Poly(ethylene glycol)‐block‐poly(lactide) (PEG‐b‐PLA) micro‐ and nanoparticles (NPs) have been intensively investigated for applications in biomedicine, due to their inherent biocompatibility and ...biodegradability, which allows them to be used as sustained release systems. Current methods for preparing PEG‐b‐PLA NPs typically require two different steps that include polymer synthesis and NP assembly, with the necessary intermediate polymer purification and the use of a variety of organic solvents in the process. In order to facilitate the biomedical application of PEG‐b‐PLA NPs, it is of great interest to develop a strategy to formulate the NPs in a simplified manner. Here, we report a straightforward method to construct PEG‐b‐PLA NPs through a sequential two‐step process without intermediate work‐up, which involves synthesizing the polymer in a water‐miscible organic solvent that is, N,N‐dimethylformamide (DMF), followed by addition of water to the polymer solution. In this way, large NPs (~600 nm) were prepared. We comprehensively characterized the NPs using turbidity studies, dynamic light scattering (DLS), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) techniques. We further demonstrated the ability of the NPs to encapsulate drugs, exemplified in the immunotherapeutic agent rapamycin, with relatively high encapsulation efficiency. In vitro drug release tests showed that rapamycin‐encapsulating NPs had comparable sustained‐release profiles at different pH conditions, highlighting the broad application window of our NP platform. Moreover, in vitro T cell suppression assays revealed that rapamycin‐loaded NPs exhibited similar inhibitory performance to free rapamycin on CD8+ cells at all rapamycin concentrations and on CD4+ cells at high and intermediate rapamycin concentrations, while the performance of the NPs was superior on CD4+ at low rapamycin concentration. Overall, this work provides a route for the scalable synthesis of biocompatible PEG‐b‐PLA NPs, which can be extended to other polymeric NPs, with potential in biomedical applications such as immunotherapy.
This work reports a new gated nanodevice for acetylcholine‐triggered cargo delivery. We prepared and characterized Janus Au–mesoporous silica nanoparticles functionalized with acetylcholinesterase on ...the Au face and with supramolecular β‐cyclodextrin:benzimidazole inclusion complexes as caps on the mesoporous silica face. The nanodevice is able to selectively deliver the cargo in the presence of acetylcholine via enzyme‐mediated acetylcholine hydrolysis, locally lowering the pH and opening the supramolecular gate. Given the key role played by ACh and its relation with Parkinson's disease and other nervous system diseases, we believe that these findings could help design new therapeutic strategies.
Janus Au–mesoporous silica nanoparticles functionalized with acetylcholinesterase on the Au face and with supramolecular β‐cyclodextrin:benzimidazole inclusion complexes as caps on the mesoporous silica face were made and characterized. The nanodevice is able to selectively deliver cargo in the presence of acetylcholine via enzyme‐mediated acetylcholine hydrolysis, locally lowering pH and opening the supramolecular gate.
Within many chemical and biological systems, both synthetic and natural, communication via chemical messengers is widely viewed as a key feature. Often known as
such communication has been a concern ...in the fields of synthetic biologists, nanotechnologists, communications engineers, and philosophers of science. However, interactions between these fields are currently limited. Nevertheless, the fact that the same basic phenomenon is studied by all of these fields raises the question of whether there are unexploited interdisciplinary synergies. In this paper, we summarize the perspectives of each field on molecular communications, highlight potential synergies, discuss ongoing challenges to exploit these synergies, and present future perspectives for interdisciplinary efforts in this area.
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