Search

Liquid metals (LMs) are electronic liquid with enigmatic interfacial chemistry and physics. These features make them promising materials for driving chemical reactions on their surfaces for designing nanoarchitectonic systems. Herein, we showed the interfacial interaction between eutectic gallium-indium (EGaIn) liquid metal and graphene oxide (GO) for the reduction of both substrate-based and free-standing GO. NanoIR surface mapping indicated the successful removal of carbonyl groups. Based on the gained knowledge, a composite consisting of assembled reduced GO sheets on LM microdroplets (LM-rGO) was developed. The LM enforced Ga3+ coordination within the rGO assembly found to modify the electrochemical interface for selective dopamine sensing by separating the peaks of interfering biologicals. Subsequently, paper-based electrodes were developed and modified with the LM-rGO that presented the compatibility of the assembly with low-cost commercial technologies. The observed interfacial interaction, imparted by LM's interfaces, and electrochemical performance observed for LM-rGO will lead to effective functional materials and electrode modifiers.

Self-assembly is ubiquitous in nature. It is of great significance to use simple self-assembly structure to realize the complex functions of natural self-assembly system, that is, to construct nanoarchitectonic functional materials. This chapter summarized recent developments of self-assembling peptide-based nanoarchitectonics, where peptides serve as the template to modulate the assembly of various species in a controlled and flexible manner. Mechanisms of regulating the peptide-based self-assembly were detailed. Importantly, the peptides also guided efficient construction of nanoarchitectonics with desired functionalities, and recent findings of the self-assembling peptides in phototherapy and biomimetic photosynthetic systems were discussed. This chapter aims to provide guidance for the design of novel peptide-modulated materials by understanding the role of peptides in the assembly process.

The fabrication of peptide-based molecular architectonics and nanoarchitectonics in high-precision, environment-friendly, and low-cost synthesis has drawn significant importance because of their irresistible applications in chemistry, biology, material sciences, and medicine. These new ways for the creation of nanostructured advance functional materials from assembly of molecular building blocks have appeared as the next-generation approach beyond nanotechnology. Generally two distinct schools of thoughts, the “top-down” approach and the “bottom-up” approach, have been employed to fabricate molecular architectonics and nanoarchitectonics. The noncovalent interactions such as hydrogen bonding, hydrophobic, π-π stacking, and van der Waals interactions play very important role to achieve the production of nanoarchitectonics from the molecular building blocks. In addition, the self-immobilization based on self-assembly and array formation of building blocks results in nanoarchitectures with soft functions. Among all building blocks, amino acids, peptides, and peptide mimetics are highly promising owing to their wide structural diversity, self-assembly propensities, biocompatibility, and biodegradability. The layer-by-layer assemblies, Langmuir-Blodgett films, nanoporous materials, soft rods, and nanotubes are some of the best architectures for controllable functions. Moreover, the balance between these noncovalent interactions can tune the shape, size, and morphology of the nanoarchitectonics. Artificial enzymes and enzyme mimics are briefly analyzed as examples of biology’s adaptive properties and applications. This chapter mainly focuses on the role of amino acids or small peptides as building blocks to form nanoarchitectonics. Emphasis will be given on both advantages and limitations. The recent advances and future scope in this area will be discussed briefly.

Dynamics of charged fullerene in a surface layer of fullerite is studied under the influence of neutral or charged particles of the gas phase surrounding the fullerite material. The translational displacements of the nodes of the crystal lattice structure are determined by the equations of motion of the centers of mass of fullerenes. Central fullerene, which is described as a discrete set of sixty carbon atoms, plays a special role in the presented mathematical model. Angular oscillations and rotations of the central fullerene are described by the dynamic Euler equations. All other fullerenes have a centrally symmetric field of the potential of interaction with the surrounding atoms and molecules. In this regard, we use the hybrid discrete–continuous mathematical model with four potentials that describe the interactions between the surrounding fullerenes, smoothed fullerene and an atom, a pair of atoms, and electric charges. The results of a numerical study of influence of the Coulomb interaction on the rotational and translational motion of the C60 fullerene are presented.

Printed flexible sensors have the potential to be seamlessly applied to soft and irregularly shaped surfaces such as human skin or textile fabrics. Owing to its varied range of applications in the field of flexible and wearable electronics, soft robotics, human–machine interaction, and biomedical devices, it is required of these sensors to be flexible and stretchable conforming to the arbitrary surfaces of their soft or stiff counterparts. The challenges in maintaining the fundamental features of these sensors, such as flexibility, sensitivity, repeatability, linearity, and durability, are tackled by the progress in the fabrication techniques and customization of the material properties. As a result, materials and structures for innovative flexible sensors, as well as their integration into systems, continue to be in the spotlight of research. This chapter outlines the current state of flexible sensor technologies and the impact of material developments on this field. Special attention is given to stress, strain, temperature, chemical, electropotential, and magnetic sensors, as well as their respective applications.

Materials science and chemistry have played a central and significant role in advancing our society. With the shift toward sustainable living, it is anticipated that the development of functional materials will continue to be vital for sustaining life on our planet. In the recent decades, rapid progress has been made in materials science and chemistry owing to the advances in experimental, analytical, and computational methods, thereby producing several novel and useful materials. However, most problems in material development are highly complex. In this review article, we discuss the best strategy for the development of functional materials via the implementation of three key concepts: nanotechnology as a game changer, nanoarchitectonics as an integrator, and materials informatics as a super accelerator. Discussions from conceptual viewpoints and exemplified recent developments, chiefly focused on nanoporous materials, are presented. We anticipate that coupling these three strategies together will open advanced routes for the swift designing and exploratory search of functional materials truly useful for solving real-world problems. These novel strategies will result in the evolution of nanoporous functional materials. This article is protected by copyright. All rights reserved.

Lung cancer (LC) is heading up as a substantial cause of mortality worldwide. Despite enormous progress in cancer management, LC remains a crucial problem for oncologists due to the lack of early diagnosis and precise treatment. In this context, numerous early diagnosis and treatment approaches for LC at the cellular level have been developed using advanced nanomaterials in the last decades. Amongst this, graphene quantum dots (GQDs) as a novel fluorescent material overwhelmed the horizons of materials science and biomedical fields due to their multifunctional attributes. Considering the complex nature of LC, emerging diagnostic and therapeutic (Theranostics) strategies using GQDs proved to be an effective way for the current practice in LC. In this line, we have abridged various approaches used in the LC theranostics using GQDs and its surface-engineered motif. The admirable photophysical attributes of GQDs realised in photolytic therapy (PLT), hyperthermia therapy (HTT), and drug delivery have been discussed. Furthermore, we have engrossed the impasse and its effects on the use of GQDs in cancer treatments from cellular level (in vivo-in vitro) to clinical. Inclusively, this review will be an embodiment for the scientific fraternity to design and magnify their view for the theranostic application of GQDs in LC treatment.

Nanoarchitectonics has been recently proposed as a post-nanotechnology concept. It is the methodology to produce functional materials from nanoscale units. Carbon-based materials are actively used in nanoarchitectonics approaches. This review explains several recent examples of energy and related applications of carbon materials from the viewpoint of the nanoarchitectonics concept. Explanations and discussions are described according to the classification of carbon sources for nanostructured materials: (i) carbon nanoarchitectonics from molecules and supramolecular assemblies; (ii) carbon nanoarchitectonics from fullerenes; (iii) carbon nanoarchitectonics from biomass; and (iv) carbon nanoarchitectonics with composites and hybrids. Functional carbon materials can be nanoarchitected through various processes, including well-skilled organic synthesis with designed molecular sources; self-assembly of fullerenes under various conditions; practical, low-cost synthesis from biomass; and hybrid/composite formation with various carbon sources. These examples strikingly demonstrate the enormous potential of nanoarchitectonics approaches to produce functional carbon materials from various components such as small molecules, fullerene, other nanocarbons, and naturally abundant biomasses. While this review article only shows limited application aspects in energy-related usages such as supercapacitors, applications for more advanced cells and batteries, environmental monitoring and remediation, bio-medical usages, and advanced devices are also expected.

Halloysite is a promising building block in nanoarchitectonics of functional materials, especially in the development of novel biomaterials and smart coatings. Understanding the behavior of materials produced using halloysite nanotubes within living organisms is essential for their safe applications. In this study, quantum dots of different compositions were synthesized on the surface of modified clay nanotubes, and the biodistribution of this hybrid material was monitored within Caenorhabditis elegans nematodes. The influence of the modification agent as well as the particles’ composition on physicochemical properties of hybrid nanomaterials was investigated. Several microscopy techniques, such as fluorescence and dark-field microscopy, were compared in monitoring the distribution of nanomaterials in nematodes’ organisms. The effects of QDs-halloysite composites on the nematodes’ life cycle were investigated in vivo. Our fluorescent hybrid probes induced no acute toxic effects in model organisms. The stable fluorescence and low toxicity towards the organisms suggest that the proposed synthesis procedure yields safe nanoarchitectonic materials that will be helpful in monitoring the behavior of nanomaterials inside living cells and organisms.

As a typical battery-type material, CuCo2 S4 is a promising candidate for supercapacitors due to the high theoretical specific capacity. However, its practical application is plagued by inherently sluggish ion diffusion kinetics and inferior electrical transport properties. Herein, sulfur vacancies are incorporated in CuCo2 S4 hollow nanoarchitectures (HNs) to accelerate redox reactivity. Experimental analyses and theoretical investigations uncover that the generated sulfur vacancies increase the active electron states, reduce the adsorption barriers of electrolyte ions, and enrich reactive redox species, thus achieving enhanced electrochemical performance. Consequently, the deficient CuCo2 S4 with optimized vacancy concentration presents a high specific capacity of 231 mAh g-1 at 1 A g-1 , a ≈1.78 times increase compared to that of pristine CuCo2 S4 , and exhibits a superior rate capability (73.8% capacity retention at 20 A g-1 ). Furthermore, flexible solid-state asymmetric supercapacitor devices assembled with the deficient CuCo2 S4 HNs and VN nanosheets deliver a high energy density of 61.4 W h kg-1 at 750 W kg-1 . Under different bending states, the devices display exceptional mechanical flexibility with no obvious change in CV curves at 50 mV s-1 . These findings provide insights for regulating electrode reactivity of battery-type materials through intentional nanoarchitectonics and vacancy engineering.

In this work, the nanoarchitectonics approach to synthesize a new functional material with certain configurations and hierarchical motifs of the multifunctional initiators of surface-initiated radical polymerization (MPIs) on surface of multi-wall carbon nanotubes (MWCNTs) was realized. The presence of covalently-linked MPIs on the surfaces of amine functionalized MWCNTs was confirmed by Raman spectroscopy and thermal analysis. Nanocomposites of polybutylene terephthalate – poly(tetramethylene oxide) – (PBT/PTMO) with modified nanotubes show higher values of Young's modulus, elongation at break, and crystallization temperature in comparison to non-modified ones.

Next-generation desalination technologies are needed to meet the increasing demand for clean water. Capacitive deionization (CDI) is a thermodynamically efficient technique to treat non-potable water with relatively low salinity. The salt removal capacity and rate of CDI are highly dependent on the electrode materials, which are preferentially porous to store ions through electrosorption and/or redox reactions. Metal-organic frameworks (MOFs) with "infinite" combinations of transition metals and organic linkers simplify the production of carbonaceous materials often with redox-active components after pyrolysis. MOFs-derived materials show great tunability in both compositions and structures but require further refinement to improve CDI performance. This review article summarizes recent progress in derivatives of MOFs and MOF-like materials used as CDI electrodes, focusing on the structural and compositional material considerations as well as the processing parameters and electrode architectures of the device. Furthermore, the challenges and opportunities associated with this research area are also discussed.

Poly(vinylidene fluoride) (PVDF) membranes are a commonly used cheap material and have been widely used in wastewater treatment. In this study, a simple strategy was proposed to construct PVDF-g-PEG membranes with an interpenetrating network structure by simulating plant roots for the treatment of oil/water emulsion. Meanwhile, the hydrophilicity, antifouling, and mechanical properties of the membrane were improved. A series of chemical and physical characterization methods were used to verify the successful formation of a PVDF-g-PEG layer on the membrane surface. The effects of graft modifier content on the crystallization behavior, microstructure, and membrane permeability were studied. When the optimized membrane (m-PVDF-2) was applied to the treatment of oily wastewater, its separation performance was significantly better than that of the blank PVDF membrane, and the oil removal rate was over 99.3%. BSA and oil contamination were nearly reversible, and excellent oil resistance to high-viscosity oil was also observed. The method reported in this article is a one-step, simple method for constructing hydrophilic and oil-resistant PVDF membranes without any intermediate additives and harmful or costly catalysts. They can be used as an ideal material for preparing efficient oil–water separation membranes.

The development in the area of novel anticancer prodrugs (conjugates and complexes) has attracted growing attention from many research groups. The dangerous side effects of currently used anticancer drugs, including cisplatin and other platinum based drugs, as well their systemic toxicity is a driving force for intensive search and presents a safer way in delivery platform of active molecules. Silicon based nanocarriers play an important role in achieving the goal of synthesis of the more effective prodrugs. It is worth to underline that silicon based platform including silica and silsesquioxane nanocarriers offers higher stability, biocompatibility of such the materials and pro-longed release of active platinum drugs. Silicon nanomaterials themselves are well-known for improving drug delivery, being themselves non-toxic, and versatile, and tailored surface chemistry. This review summarizes the current state-of-the-art within constructs of silicon-containing nano-carriers conjugated and complexed with platinum based drugs. Contrary to a number of other reviews, it stresses the role of nano-chemistry as a primary tool in the development of novel prodrugs.

Hypothesis Nanocarbon/polymeric 3D porous composites have been widely developed as piezoresistive sensors due to their improved performances. Functionalized nanocarbon is usually used to allow its adsorption on the surface of porous polymeric material. However, both the functionalization and the surface localized distribution of the nanomaterial can limit the nanocarbon effect on conductivity and mechanical stability of the material thus affecting piezoresistive performances. Experiments A novel nanoarchitectonics strategy to prepare an elastomeric/carbon nanotubes (CNTs) 3D porous piezoresistive nanocomposite is developed. The fabrication route does not require complex apparatus and CNTs chemical functionalization. Moreover, foams of any shape and dimensions can be produced with neither complex machinery and procedures nor wastes production. Findings The obtained material is characterized by the presence of well dispersed pristine CNTs on both surface and bulk of the polymeric matrix. The foam exhibited improved piezoresistive properties with excellent compressive stress (>150 kPa), sensitivity at low displacement (29 kPa−1) and limit of detection for both pressure (2 Pa) and extension (130 nm). These excellent features could allow the use of the as prepared nanocomposite in different applications ranging from wearable devices to robotic or infrastructure monitoring with outstanding flexibility.

Composite, helical nanostructures formed using cooperative interactions of liquid crystals and Au nanoparticles were studied using a scanning transmission electron microscopy (STEM) mode. The investigated helical assemblies exhibit long-range hierarchical order across length scales, as a result of the crystallization (freezing) directed growth mechanism of nanoparticle-coated twisted nanoribbons and their ability to form organized bundles. Here, STEM methods were used to reproduce the 3D structure of the Au nanoparticle double helix.

Molecular machines are often regarded as molecular artworks and sometimes as fancy molecular toys. However, many researchers strive to operate molecular machines as useful tools for realistic practical applications. In this perspective article, shifting the working environment of molecular machines from solution to interfacial media is discussed from the viewpoint of their evolution from scientific toys to useful tools. Following a short description of traditional research into molecular machines in solution and their nanotechnological manipulation on clean solid surfaces, pioneering research into molecular machine operation at dynamic interfaces, such as liquid surfaces, is discussed, along with cutting-edge research into molecular machine functions in living cells and their models. Biomolecular machines within organisms are the products of evolution over billions of years. We may nanoarchitect such sophisticated functional systems with artificial molecular machines within much shorter periods., Molecular machines can be made more useful with interfacial nanoarchitectonics.

Diagnosis of cancer using electroanalytical methods can be achieved at low cost and in rapid assays, but this may require the combination with data treatment for determining biomarkers in real samples. In this paper, we report an immunomagnetic nanoparticle-based microfluidic sensor (INμ-SPCE) for the amperometric detection of the prostate-specific antigen (PSA) biomarker, the data of which were treated with information visualization methods. The INμ-SPCE consists of eight working electrodes, reference and counter electrodes. On the working electrodes, magnetic nanoparticles with secondary antibodies with the enzyme horseradish peroxidase were immobilized for the indirect detection of PSA in a sandwich-type procedure. Under optimal conditions, the immunosensor could operate within a wide range from 12.5 to 1111 fg·L−1, with a low detection limit of 0.062 fg·L−1. Multidimensional projections combined with feature selection allowed for the distinction of cell lysates with different levels of PSA, in agreement with results from the traditional enzyme-linked immunosorbent assay. The approaches for immunoassays and data processing are generic, and therefore the strategies described here may provide a simple platform for clinical diagnosis of cancers and other types of diseases.

Cell surface engineering, as a practical manifestation of nanoarchitectonics, is a powerful tool to modify and enhance properties of live cells. In turn, cells may serve as sacrificial templates to fabricate cell-mimicking materials. Herein we report a facile method to produce cell-recognising silica imprints capable of the selective detection of human cells. We used HeLa cells to template silica inorganic shells doped with halloysite clay nanotubes. The shells were destroyed by sonication resulting in the formation of polydisperse hybrid imprints that were used to recognise HeLa cells in liquid media supplemented with yeast. We believe that methodology reported here will find applications in biomedical and clinical research.

Peptide-based supramolecular hydrogels, as a new type of biological nanoarchitectonic structure, hold great promise for a wide range of biomedical and nanotechnological applications, such as tissue engineering, drug delivery, and electronic and photonic energy storage. In this work, a cyclic dipeptide (CDP) cyclo-(Trp-Tyr) (C-WY), which has exceptional structural rigidity and high stability, is selected as a hydrogelator for the formation of supramolecular hydrogels. The unique hydrogen bonding in C-WY endows a high propensity for self-assembly and the resulting hydrogels are revealed to be crystalline. The crystalline hydrogels possess excellent mechanical capacity and superior tolerance to various harsh conditions, including in the presence of charged biopolymers, extreme acid/base environments, and changing thermal conditions. Such high tolerance enables the crystalline hydrogels to be applied in the complex and harsh environments of electrochemistry. In addition, this study demonstrates that the self-assembly of cyclic dipeptides results in highly robust hydrogels which can be applied for electrochemical applications such as electrochemical supercapacitors.

An emerging concept, nanoarchitectonics, raises the stage of nanotechnology to materials productions with nanoscale precisions through inclusion of the other research fields. In this review article, we exemplify nanocarbon assembly and composite as successful products of the nanoarchitectonics concept. Nanocarbon materials are representative objects to demonstrate the wide possibilities of functional varieties through structural fabrication using uni-elemental zero-dimensional objects such as fullerenes, one-dimensional carbon nanotube, two-dimensional graphene, and three dimensional assemblies and composites. Here, several related examples are introduced according to classification with (i) self-assembly mainly with liquid–liquid interfacial precipitation, (ii) process-based assembly mainly with layer-by-layer assembly, and (iii) composite formation mainly with metal oxides. The research efforts in self-assembly and process-assembly somehow still stay at challenging and basic stages. In contrast, research examples on composites of nanocarbon materials with various metal oxides are aiming to practical applications especially in energy-related applications, but the latter composite approaches do not have features of precise structure controls, yet. Therefore, more aggressive introduction of the nanoarchitectonics concept to these practical composite approaches is necessary for further possibilities to create materials with much more advanced performances.

Design of a Pt-based catalyst with desired nanoarchitectonics highly favors an enhanced electrocatalytic performance. Herein unique yolk–shell structures containing a Pt core and a mesoporous bimet...

Crystalline poly- and oligosaccharides such as cellulose can form extremely robust assemblies, whereas the construction of self-assembled materials from such molecules is generally difficult due to their complicated chemical synthesis and low solubility in solvents. Enzyme-catalyzed oligomerization-induced self-assembly has been shown to be promising for creating nanoarchitectured crystalline oligosaccharide materials. However, the controlled self-assembly into organized hierarchical structures based on a simple method is still challenging. Herein, we demonstrate that the use of organic solvents as small-molecule additives allows for control of the oligomerization-induced self-assembly of cellulose oligomers into hierarchical nanoribbon network structures. In this study, we dealt with the cellodextrin phosphorylase-catalyzed oligomerization of phosphorylated glucose monomers from ᴅ-glucose primers, which produce precipitates of nanosheet-shaped crystals in aqueous solution. The addition of appropriate organic solvents to the oligomerization system was found to result in well-grown nanoribbon networks. The organic solvents appeared to prevent irregular aggregation and subsequent precipitation of the nanosheets via solvation for further growth into the well-grown higher-order structures. This finding indicates that small-molecule additives provide control over the self-assembly of crystalline oligosaccharides for the creation of hierarchically structured materials with high robustness in a simple manner.

Much attention has been paid to the synthesis of low-dimensional materials from small units such as functional molecules. Bottom-up approaches to create new low-dimensional materials with various functional units can be realized with the emerging concept of nanoarchitectonics. In this review article, we overview recent research progresses on materials nanoarchitectonics at two-dimensional liquid interfaces, which are dimensionally restricted media with some freedoms of molecular motion. Specific characteristics of molecular interactions and functions at liquid interfaces are briefly explained in the first parts. The following sections overview several topics on materials nanoarchitectonics at liquid interfaces, such as the preparation of two-dimensional metal-organic frameworks and covalent organic frameworks, and the fabrication of low-dimensional and specifically structured nanocarbons and their assemblies at liquid–liquid interfaces. Finally, interfacial nanoarchitectonics of biomaterials including the regulation of orientation and differentiation of living cells are explained. In the recent examples described in this review, various materials such as molecular machines, molecular receptors, block-copolymer, DNA origami, nanocarbon, phages, and stem cells were assembled at liquid interfaces by using various useful techniques. This review overviews techniques such as conventional Langmuir–Blodgett method, vortex Langmuir–Blodgett method, liquid–liquid interfacial precipitation, instructed assembly, and layer-by-layer assembly to give low-dimensional materials including nanowires, nanowhiskers, nanosheets, cubic objects, molecular patterns, supramolecular polymers, metal-organic frameworks and covalent organic frameworks. The nanoarchitecture materials can be used for various applications such as molecular recognition, sensors, photodetectors, supercapacitors, supramolecular differentiation, enzyme reactors, cell differentiation control, and hemodialysis.

As an emerging concept for the development of new materials with nanoscale features, nanoarchitectonics has received significant recent attention. Among the various approaches that have been developed in this area, the fixed-direction construction of functional materials, such as layered fabrication, offers a helpful starting point to demonstrate the huge potential of nanoarchitectonics. In particular, the combination of nanoarchitectonics with layer-by-layer (LbL) assembly and a large degree of freedom in component availability and technical applicability would offer significant benefits to the fabrication of functional materials. In this Minireview, recent progress in LbL assembly is briefly summarized. After introducing the basics of LbL assembly, recent advances in LbL research are discussed, categorized according to physical, chemical, and biological innovations, along with the fabrication of hierarchical structures. Examples of LbL assemblies with graphene oxide are also described to demonstrate the broad applicability of LbL assembly, even with a fixed material.

The construction of flexible electrochemical devices for energy storage and generation is of utmost importance in modern society. In this article, we report on the synthesis of flexible MoS2-based composite paper by high-energy shear force milling and simple vacuum filtration. This composite material combines high flexibility, mechanical strength and good chemical stability. Chronopotentiometric charge–discharge measurements were used to determine the capacitance of our paper material. The highest capacitance achieved was 33 mF·cm−2 at a current density of 1 mA·cm−2, demonstrating potential application in supercapacitors. We further used the material as a cathode for the hydrogen evolution reaction (HER) with an onset potential of approximately −0.2 V vs RHE. The onset potential was even lower (approximately −0.1 V vs RHE) after treatment with n-butyllithium, suggesting the introduction of new active sites. Finally, a potential use in lithium ion batteries (LIB) was examined. Our material can be used directly without any binder, additive carbon or copper current collector and delivers specific capacity of 740 mA·h·g−1 at a current density of 0.1 A·g−1. After 40 cycles at this current density the material still reached a capacity retention of 91%. Our findings show that this composite material could find application in electrochemical energy storage and generation devices where high flexibility and mechanical strength are desired.Keywords: flexible composites; hydrogen evolution reaction (HER); lithium ion batteries (LIBs); molybdenum disulfide; nanoarchitectonics; supercapacitors

A highly active surface-enhanced Raman scattering (SERS) substrate was developed by facile deposition of silver nanoparticles onto cellulose fibers of ordinary laboratory filter paper. This was achieved by means of the silver mirror reaction in a manner to control both the size of the silver nanoparticles and the silver density of the substrate. This paper-based substrate is composed of a particle-on-fiber structure with the unique three-dimensional network morphology of the cellulose matrix. For such a SERS substrate with optimized size of the silver nanoparticles (ca. 70 nm) and loading density of silver (17.28 wt %), a remarkable detection limit down to the sub-attomolar (1 × 10−16 M) level and an enhancement factor of 3 × 106 were achieved by using Rhodamine 6G as the analyte. Moreover, this substrate was applied to monitor the molecular recognition through multiple hydrogen bonds in between nucleosides of adenosine and thymidine. This low-cost, highly sensitive, and biocompatible paper-based SERS substrate holds considerable potentials for the detection and analyses of chemical and biomolecular species.

This review focuses on the design of poly(N-isopropylacrylamide) (PIPAAm)-grafted surfaces for cell sheet preparation and manipulation, which are revolutionary tools for the creation of transplanta...

Although porous materials based on coordination compounds, including metal-organic frameworks (MOFs) and porous coordination polymers (PCPs), have well-defined pore structures and promising propert...

Enzyme mimics have broad applications in catalysis and can assist elucidation of the catalytic mechanism of natural enzymes. However, challenges arise from the design of catalytic sites, the selection of host molecules, and their integration into active three-dimensional structures. Herein, we describe the development of a photooxidase mimic by synergetic molecular self-assembly. 9-Fluorenylmethyloxycarbonyl-l-histidine undergoes efficient co-assembly with phthalocyanine into nanovesicles with tunable particle size and membrane thickness. The obtained nanovesicles can be used as catalysts for reactive-oxygen-mediated photosensitive oxidation with improved efficiency and stability. This work highlights the co-assembly of simple building blocks into a supramolecular photocatalyst, which might give insight into possible evolutionary paths of photocatalytic membrane systems, and might allow facile transfer into photosensitive nanoreactors or artificial organelles.

The development of science and technology of advanced materials using nanoscale units can be conducted by a novel concept involving combination of nanotechnology methodology with various research disciplines, especially supramolecular chemistry. The novel concept is called ‘nanoarchitectonics’ where self-assembly processes are crucial in many cases involving a wide range of component materials. This review of self-assembly processes re-examines recent progress in materials nanoarchitectonics. It is composed of three main sections: (1) the first short section describes typical examples of self-assembly research to outline the matters discussed in this review; (2) the second section summarizes self-assemblies at interfaces from general viewpoints; and (3) the final section is focused on self-assembly processes at interfaces. The examples presented demonstrate the strikingly wide range of possibilities and future potential of self-assembly processes and their important contribution to materials nanoarchitectonics. The research examples described in this review cover variously structured objects including molecular machines, molecular receptors, molecular pliers, molecular rotors, nanoparticles, nanosheets, nanotubes, nanowires, nanoflakes, nanocubes, nanodisks, nanoring, block copolymers, hyperbranched polymers, supramolecular polymers, supramolecular gels, liquid crystals, Langmuir monolayers, Langmuir–Blodgett films, self-assembled monolayers, thin films, layer-by-layer structures, breath figure motif structures, two-dimensional molecular patterns, fullerene crystals, metal–organic frameworks, coordination polymers, coordination capsules, porous carbon spheres, mesoporous materials, polynuclear catalysts, DNA origamis, transmembrane channels, peptide conjugates, and vesicles, as well as functional materials for sensing, surface-enhanced Raman spectroscopy, photovoltaics, charge transport, excitation energy transfer, light-harvesting, photocatalysts, field effect transistors, logic gates, organic semiconductors, thin-film-based devices, drug delivery, cell culture, supramolecular differentiation, molecular recognition, molecular tuning, and hand-operating (hand-operated) nanotechnology., Graphical Abstract

Two-dimensional metal oxide nanosheets are versatile materials for constructing artificial photosynthetic systems that can carry out photocatalytic processes such as water splitting and CO2 fixatio...

Self-assembly is omnipresent in nature. While natural self-assembly systems are complicated in structure, the simplification of natural systems while maintaining their inherent functionalities has ...

The shape-controlled synthesis of bimetallic Pt-based nanoarchitectonics has attracted considerable interest due to their remarkable electrocatalytic activity for the oxygen reduction reaction (ORR). In this work, we report a direct method for the fabrication of unique bimetallic AuPt nanobrick spherical nanoarchitectonics (AuPt NSNs) in aqueous solution. Benefiting from their rugged surfaces and bimetallic compositions, AuPt NSNs exhibit excellent electrocatalytic performance for the ORR. The proposed method is very useful for the fabrication of metallic nanoarchitectonics with rugged surfaces.

The discovery and development of novel approaches, materials and manufacturing processes in the field of energy are compelling increasing recognition as a major challenge for contemporary societies. The performance and lifetime of energy devices are critically dependent on nanoscale interfacial phenomena. From the viewpoint of materials design, the improvement of current technologies inevitably relies on gaining control over the complex interface between dissimilar materials. In this sense, interfacial nanoarchitectonics with polymer brushes has seen growing interest due to its potential to overcome many of the limitations of energy storage and conversion devices. Polymer brushes offer a broad variety of resources to manipulate interfacial properties and gain molecular control over the synergistic combination of materials. Many recent examples show that the rational integration of polymer brushes in hybrid nanoarchitectures greatly improves the performance of energy devices in terms of power density, lifetime and stability. Seen in this light, polymer brushes provide a new perspective from which to consider the development of hybrid materials and devices with improved functionalities. The aim of this review is therefore to focus on what polymer brush-based solutions can offer and to show how the practical use of surface-grafted polymer layers can improve the performance and efficiency of fuel cells, lithium-ion batteries, organic radical batteries, supercapacitors, photoelectrochemical cells and photovoltaic devices. Fil: Giussi, Juan Martín. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina Fil: Cortez, María Lorena. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina Fil: Marmisollé, Waldemar Alejandro. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina Fil: Azzaroni, Omar. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina

The development of coordination polymers (CPs) originated from crystal engineering, which mainly focuses on crystals and their physico-chemical properties. This has now reached molecular- and nanoengineering, which push these CPs into practical applications. Depending on the application, the deformability of CPs becomes an important issue. To use CP films in flexible devices, it is necessary to develop CP films that can be bent/stretched. The present review illustrates how nanotechnology and supramolecular chemistry work cooperatively to make CP films soft through numerous procedures. These soft films show non-interrupted performances under mechanical deformation, demonstrating that CPs can be used in next-generation flexible devices.

Multifunctional energy storage devices can greatly impact public safety and flexible electronics. For example, mechanically strong energy devices can prevent catastrophic failure in batteries or act as structural elements, simultaneously dissipating energy and bearing a load. Herein we report on a nanoarchitectonics approach, which implements an optimal experimental design framework to optimize the electrochemical and mechanical properties of a composite electrode. First, functional analysis was used to determine the weight percentages of the electrode components as control variables of interest in this material system. A utility function was then developed to measure the trade-offs between the electrochemical and mechanical properties. Finally, Gaussian process regression was used to model initial experimental data and optimal compositions were predicted using expected improvement acquisition methods.

A new conceptual paradigm that combines nanotechnology and other research disciplines, called “nanoarchitectonics”, has been established. Nanoarchitectonics can be achieved with contributions of atomic/molecular level manipulation, chemical synthesis/modification, self-organization/self-assembly, field-controlled arrangement, material fabrication, and bio-related techniques together with advanced knowledge and skills in nanoscience and nanotechnology. In particular, the dynamic nature of the nanoarchitectonics concept accords with soft material functionalization. Therefore, the nanoarchitectonics concept provides rational strategies to create functional materials with deep relations with molecular system designs that are especially useful for the development of novel functions of soft materials. In this review article, recent research efforts on soft material nanoarchitectonics at interfacial media are mainly focused. The presented examples are classified according to the following processes: (i) from molecules to two-dimensional material systems at the air–water interface; (ii) from interfacial assembly to hierarchical nanostructures with layer-by-layer assembly; (iii) from interfacial assembly to hierarchical nanostructures at the liquid–liquid interface; (iv) from material systems to life control at the interface.

Solvent-free functional fluidic materials have recently attracted considerable attention owing to their high deformability and facile processability. The counterintuitive softness of functional organic molecules/materials that are intrinsically rigid, such as polycyclic hydrocarbons, aromatic macrocycles, fullerenes, and conjugated polymers, is a significant advantage towards various softness-oriented applications. For example, the development of optoelectronically active fluids has shifted the attention from hard matter-based devices that barely bend and stretch under actions required in flexible/stretchable electronics. This minireview presents a summary of the latest reports and current challenges of functional molecular/polymeric fluids from their molecular engineering approaches or the nanoarchitectonics of functional fluids to the state-of-the-art functions derived from the fluids.

The ability to produce structural color from inherently colorless materials, similar to that in butterfly wings and beetle shells, has attracted considerable research interest over the last three decades. Despite their extraordinary properties and performances, the field of structural colors based on inherently functional 2D materials only took off recently. In this minireview, we highlight the diversity of 2D materials utilized for achieving structural coloration in different architectures. We summarize the large tunability of photonic architectures based on 2D materials and emphasize their extraordinary dynamic response induced by external stimuli. Subsequently, recent strategies to tailor their properties with molecular and structural approaches are discussed. Finally, we point out promising future directions in this emerging field.