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We construct a compartmentalized nanoarchitecture to regulate bioenergy level. Glucose dehydrogenase, urease and nicotinamide adenine dinucleotide are encapsulated inside through liquid‐liquid phase separation. ATPase and glucose transporter embedded in hybrid liposomes are attached at the surface. Glucose is transported and converted to gluconic acid catalyzed by glucose dehydrogenase, resulting in an outward proton gradient to drive ATPase for ATP synthesis. In parallel, urease catalyzes hydrolysis of urea to generate ammonia, which leads to an inward proton gradient to drive ATPase for ATP hydrolysis. These processes lead to a change of the direction of proton gradient, thus achieving artificial ATP oscillation. Importantly, the frequency and the amplitude of the oscillation can be programmed. The work explores nanoarchitectonics integrating multiple components to realize artificial and precise oscillation of bioenergy level. [ABSTRACT FROM AUTHOR]

AbstractNanoarchitectonics represents a transformative approach in macromolecular science, extending beyond traditional nanotechnology by emphasizing the precise design and construction of complex materials through controlled molecular interactions. This review explores the integration of nanoarchitectonics with molecular dynamics, a powerful computational tool that enables the prediction and optimization of material behavior at the atomic level. The synergy between these two fields allows for the rational design of smart materials that respond dynamically to environmental stimuli, such as temperature, light and mechanical stress. These materials, including thermo-responsive hydrogels, photochromic polymers and self-healing coatings, demonstrate the significant potential of nanoarchitectonics in creating materials with tailored properties for diverse applications. By leveraging molecular dynamics, researchers can gain insights into the energy landscapes and interaction patterns that drive the self-assembly and functionality of these materials, leading to enhanced performance and novel functionalities. This review also examines the future perspectives of nanoarchitectonics, highlighting the potential of integrating artificial intelligence and machine learning with it to further revolutionize material design. As the field advances, the combination of nanoarchitectonics and molecular dynamics is expected to unlock new possibilities in macromolecular science, offering innovative solutions for applications ranging from biomedical devices to environmental remediation. The review concludes by discussing the challenges and opportunities in translating these innovations from the laboratory to real-world applications, emphasizing the need for interdisciplinary collaboration to fully realize the potential of nanoarchitectonic materials in addressing global challenges. [ABSTRACT FROM AUTHOR]

The recognition of the importance of nanostructures is mainly due to the development of nanotechnology. For further developments in materials sciences, a concept that integrates nanotechnology with material chemistry to fabricate functional materials has to be proposed. Nanoarchitectonics will carry out this task. In nanoarchitectonics, we architect functional material systems from nano-units (atoms, molecules, nanomaterials). The methodology is not specific to any particular material or application. It covers a wide range. Therefore, nanoarchitectonics can be thought of as the method for everything in materials science. As typical demonstrations for usages of nanoarchitectonics, this review paper presents our work on nanoarchitectonics for supercapacitors. We divide it into two categories with different approaches. The first is the development of carbon materials as supercapacitor electrode materials from biomass. The second category is preparing carbon materials using structures created by supramolecular assembly of fullerenes such as C60 and C70. By presenting examples using opposite starting materials, a complex natural material, and an ultimately simple molecule, we will demonstrate the versatility and breadth of possibilities of this approach. [ABSTRACT FROM AUTHOR]

Photothermal conversion of light into heat energy is an intrinsic optical property of metal nanoparticles when irradiated using near-infrared radiation. However, the impact of size and shape on the photothermal behaviour of gold nanomakura particles possessing optical absorption within 600–700 nm as well as on incorporation in hydrogels is not well reported. In this study, nanomakura-shaped anisotropic gold nanoparticles (AuNMs) were synthesized via a surfactant-assisted seed-mediated protocol. Quaternary cationic surfactants having variable carbon tail length (n = 16, 14, 12) were used as capping for tuning the plasmon peak of gold nanomakura within a 600–700 nm wavelength. The aspect ratio as well as anisotropy of synthesized gold nanomakura can influence photothermal response upon near-infrared irradiation. The role of carbon tail length was evident via absorption peaks obtained from longitudinal surface plasmon resonance analysis at 670, 650, and 630 nm in CTAB-AuNM, MTAB-AuNM, and DTAB-AuNM, respectively. Furthermore, the impact of morphology and surrounding milieu of the synthesized nanomakuras on photothermal conversion is investigated owing to their retention of plasmonic stability. Interestingly, we found that photothermal conversion was exclusively assigned to morphological features (i.e., nanoparticles of higher aspect ratio showed higher temperature change and vice versa irrespective of the surfactant used). To enable biofunctionality and stability, we used kappa-carrageenan- (k-CG) based hydrogels for incorporating the nanomakuras and further assessed their photothermal response. Nanomakura particles in association with k-CG were also able to show photothermal conversion, depicting their ability to interact with light without hindrance. The CTAB-AuNM, MTAB-AuNM, and DTAB-AuNM after incorporation into hydrogel beads attained up to ≈17.2, ≈17.2, and ≈15.7 °C, respectively. On the other hand, gold nanorods after incorporation into k-CG did not yield much photothermal response as compared to that of AuNMs. The results showed a promising platform to utilize nanomakura particles along with kappa-carrageenan hydrogels for enabling usage on nanophotonic, photothermal, and bio-imaging applications.

Designing a nanofluidic membrane with high selectivity and fast ion transport property is the key towards high‐performance osmotic energy conversion. However, most of reported membranes can produce power density less than commercial benchmark (5 W/m2), due to the imbalance between ion selectivity and permeability. Here, we report a novel nanoarchitectured design of a heterogeneous membrane with an ultrathin and dense zirconium‐based UiO‐66‐NH2 metal–organic framework (MOF) layer and a highly aligned and interconnected branched alumina nanochannel membrane. The design leads to a continuous trilayered pore structure of large geometry gradient in the sequence from angstrom‐scale to nano‐scale to sub‐microscale, which enables the enhanced directional ion transport, and the angstrom‐sized (~6.6–7 Å) UiO‐66‐NH2 windows render the membrane with high ion selectivity. Consequently, the novel heterogeneous membrane can achieve a high‐performance power of ~8 W/m2 by mixing synthetic seawater and river water. The power density can be largely upgraded to an ultrahigh ~17.1 W/m2 along with ~48.5 % conversion efficiency at a 50‐fold KCl gradient. This work not only presents a new membrane design approach but also showcases the great potential of employing the zirconium‐based MOF channels as ion‐channel‐mimetic membranes for highly efficient blue energy harvesting. [ABSTRACT FROM AUTHOR]

The global threat posed by antimicrobial resistance (AMR) to public health is an immensurable problem. The effectiveness of treating infections would be more at risk in the absence of effective antimicrobials. Researchers have shown an amplified interest in alternatives, such as developing advanced metallic nanohybrids as new therapeutic candidates for antibiotics due to their promising effectiveness against resistant microorganisms. In recent decades, the antimicrobial activity of monometallic nanoparticles has received extensive study and solid proof, providing new opportunities for developing multimetallic nanohybrid antimicrobials. Advanced metallic nanohybrids are an emerging remedy for a number of issues that develop in the field of medicine. Advanced metallic nanohybrids have shown a promising ability to combat resistant microorganisms due to their overall synergistic activity. Formulating advanced multimetallic nanohybrids falling under the umbrella of the growing field of nanoarchitectonics, which extends beyond nanotechnology. The underlying theory of nanoarchitectonics involves utilizing nanoscale units that follow the concepts of nanotechnology to architect nanomaterials. This review focuses on a comprehensive description of antimicrobial mechanisms of metallic nanohybrids and their enabling future insights on the research directions of developing the nanoarchitectonics of advanced multimetallic nanohybrids as novel antibiotics through their synergistic activity. [ABSTRACT FROM AUTHOR]

The characteristic feature of a biofunctional system is that components with various functions work together. These multi-components are not simply mixed together, but are rationally arranged. The fundamental technologies to do this in an artificial system include the synthetic chemistry of the substances that make the component unit, the science and techniques for assembling them, and the technology for analyzing their nanoostructures. A new concept, nanoarchitectonics, can play this role. Nanoarchitectonics is a post-nanotechnology concept that involves building functional materials that reflect the nanostructures. In particular, the approach of combining and building multiple types of components to create composite materials is an area where nanoarchitectonics can be a powerful tool. This review summarizes such examples and related composite studies. In particular, examples are presented in the areas of catalyst & photocatalyst, energy, sensing & environment, bio & medical, and various other functions and applications to illustrate the potential for a wide range of applications. In order to show the various stages of development, the examples are not only state-of-the-art, but also include those that are successful developments of existing research. Finally, a summary of the examples and a brief discussion of future challenges in nanoarchitectonics will be given. Nanoarchitectonics is applicable to all materials and aims to establish the ultimate methodology of materials science. [ABSTRACT FROM AUTHOR]

Nanoscale science is becoming increasingly important and prominent, and further development will necessitate integration with other material chemistries. In other words, it involves the construction of a methodology to build up materials based on nanoscale knowledge. This is also the beginning of the concept of post-nanotechnology. This role belongs to nanoarchitectonics, which has been rapidly developing in recent years. However, the scope of application of nanoarchitectonics is wide, and it is somewhat difficult to compile everything. Therefore, this review article will introduce the concepts of liquid and interface, which are the keywords for the organization of functional material systems in biological systems. The target interfaces are liquid–liquid interface, liquid–solid interface, and so on. Recent examples are summarized under the categories of molecular assembly, metal-organic framework and covalent organic framework, and living cell. In addition, the latest research on the liquid interfacial nanoarchitectonics of organic semiconductor film is also discussed. The final conclusive section summarizes these features and discusses the necessary components for the development of liquid interfacial nanoarchitectonics. [ABSTRACT FROM AUTHOR]

Programmed cell death (PCD) is a controlled and organized form of death regulated by genes, allowing cells to adapt to their environment. Pyroptosis, a recently discovered type of programmed cell death, differs from apoptosis and necrosis. It is characterized by the activation of caspase and the cleavage of gasdermin. Many studies have focused on understanding the mechanisms and roles of pyroptosis, particularly in cancer research. While inducing pyroptosis in tumor cells for cancer treatment is a major research focus, it is equally important to explore methods of reducing pyroptosis in noncancerous diseases. Recent advancements in drug delivery systems, specifically nanoarchitectonics, offer site‐specific targeting, prolonged drug circulation, enhanced efficacy, improved solubility, and better absorption. Although several reviews have described how nanoarchitectonics can trigger pyroptosis in tumor cells, little attention is given to their potential to inhibit pyroptosis in noncancerous diseases. Therefore, it is crucial to bridge this gap and explore the future directions for utilizing nanoarchitectonics as a powerful tool against noncancerous diseases. This review aims to delve into the recent progress made in nanoarchitectonics‐based advanced drug delivery systems for the treatment of noncancerous diseases by reducing pyroptosis, while also highlighting potential future perspectives in this emerging field. [ABSTRACT FROM AUTHOR]

Based on nanoarchitectonics and molecular dynamics simulations, we investigate the structural properties and diffusion pathway of Na atoms in sodium trisilicate over a wide temperature range. The structural and dynamics properties are analyzed through the radial distribution function (RDF), the Voronoi Si- and O-polyhedrons, the cluster function fCL(r), and the sets of fastest (SFA) and slowest atoms (SSA). The results indicate that Na atoms are not placed in Si-polyhedrons and bridging oxygen (BO) polyhedrons; instead, Na atoms are mainly placed in non-bridging oxygen (NBO) polyhedrons and free oxygen (FO) polyhedrons. Here BO, NBO, and FO represent O bonded with two, one, and no Si atoms, respectively. The simulation shows that O atoms in sodium trisilicate undergo numerous transformations: NBF0 ↔ NBF1, NBF1 ↔ NBF2, and BO0 ↔ BO1, where NBF is NBO or FO. The dynamics in sodium trisilicate are mainly distributed by the hopping and cooperative motion of Na atoms. We suppose that the diffusion pathway of Na atoms is realized via hopping Na atoms alone in BO-polyhedrons and the cooperative motion of a group of Na atoms in NBO- and FO-polyhedrons. [ABSTRACT FROM AUTHOR]

Developing electrochemical energy storage and conversion systems, such as capacitors, batteries, and fuel cells is crucial to address rapidly growing global energy demands and environmental concerns for a sustainable society. Significant efforts have been devoted to the structural design and engineering of various electrode materials to improve economic applicability and electrochemical performance. The yolk-shell structures represent a special kind of core-shell morphologies, which show great application potential in energy storage, controlled delivery, adsorption, nanoreactors, sensing, and catalysis. Their controllable void spaces may facilitate the exposure of more ative sites for redox reactions and enhance selective adsorption. Based on different nanoarchitectonic designs and fabrication techniques, the yolk-shell structures with controllable structural nanofeatures and the homo- or hetero-compositions provide multiple synergistic effects to promote reactions on the electrode/electrolyte interfaces. This review is focused on the key structural features of yolk-shell architectures, highlighting the recent advancements in their fabrication with adjustable space and mono- or multi-metallic composites. The effects of tailorable structure and functionality of yolk-shell nanostructures on various electrochemical processes are also summarized.

ABSTRACTExosomes, a type of extracellular vesicles, have attracted considerable attention due to their ability to provide valuable insights into the pathophysiological microenvironment of the cells from which they originate. This characteristic implicates their potential use as diagnostic disease biomarkers clinically, including cancer, infectious diseases, neurodegenerative disorders, and cardiovascular diseases. Aptasensors, which are electrochemical aptamers based biosensing devices, have emerged as a new class of powerful detection technology to conventional methods like ELISA and Western analysis, primarily because of their capability for high-performance bioanalysis. This review covers the current research landscape on the detection of exosomes utilizing nanoarchitectonics strategy for the development of electrochemical aptasensors. Strategies involving signal amplification and biofouling prevention are discussed, with an emphasis on nanoarchitectonics-based bio-interfaces, showcasing their potential to enhance sensitivity and selectivity through optimal conduction and mass transport properties. The ongoing challenges to broaden the clinical applications of these biosensors are also highlighted.

ABSTRACTThe ever-growing use of nature-derived materials creates exciting opportunities for novel development in various therapeutic biomedical applications. Living cells, serving as the foundation of nanoarchitectonics, exhibit remarkable capabilities that enable the development of bioinspired and biomimetic systems, which will be explored in this review. To understand the foundation of this development, we first revisited the anatomy of cells to explore the characteristics of the building blocks of life that is relevant. Interestingly, animal cells have amazing capabilities due to the inherent functionalities in each specialized cell type. Notably, the versatility of cell membranes allows red blood cells and neutrophils’ membranes to cloak inorganic nanoparticles that would naturally be eliminated by the immune system. This underscores how cell membranes facilitate interactions with the surroundings through recognition, targeting, signalling, exchange, and cargo attachment. The functionality of cell membrane-coated nanoparticles can be tailored and improved by strategically engineering the membrane, selecting from a variety of cell membranes with known distinct inherent properties. On the other hand, plant cells exhibit remarkable capabilities for synthesizing various nanoparticles. They play a role in the synthesis of metal, carbon-based, and polymer nanoparticles, used for applications such as antimicrobials or antioxidants. One of the versatile components in plant cells is found in the photosynthetic system, particularly the thylakoid, and the pigment chlorophyll. While there are challenges in consistently synthesizing these remarkable nanoparticles derived from nature, this exploration begins to unveil the endless possibilities in nanoarchitectonics research.

Polyaniline-based atomic switches are material building blocks whose nanoscale structure and resultant neuromorphic character provide a new physical substrate for the development next-generation, nanoarchitectonic-enabled computing systems. Metal ion-doped devices consisting of a Ag/metal ion doped polyaniline/Pt sandwich structure were fabricated using an in situ wet process. The devices exhibited repeatable resistive switching between high (ON) and low (OFF) conductance states in both Ag+ and Cu2+ ion-doped devices. The threshold voltage for switching was>0.8 V and average ON/OFF conductance ratios (30 cycles for 3 samples) were 13 and 16 for Ag+ and Cu2+ devices, respectively. The ON state duration was determined by the decay to an OFF state after pulsed voltages of differing amplitude and frequency. The switching behaviour is analagous to short-term (STM) and long-term (LTM) memories of biological synapses. Memristive behaviour and evidence of quantized conductance were also observed and interpreted in terms of metal filament formation bridging the metal doped polymer layer. The successful realization of these properties within physical material systems indicate polyaniline frameworks as suitable neuromorphic substrates for in materia computing.

Developing inexpensive and efficient catalysts for biomass hydrogenation or hydrodeoxygenation (HDO) is essential for efficient energy conversion. Transition metal phosphides (TMPs), with the merits of abundant active sites, unique physicochemical properties, tunable component structures, and excellent catalytic activities, are recognized as promising biomass hydrogenation or HDO catalytic materials. Nevertheless, the biomass hydrogenation or HDO catalytic applications of TMPs are still limited by various complexities and inherent performance bottlenecks, and thus their future development and utilization remain to be systematically sorted out and further explored. This review summarizes the current popular strategies for the preparation of TMPs. Subsequently, based on the structural and electronic properties of TMPs, the catalytic activity origins of TMPs in biomass hydrogenation or HDO is elucidated. Additionally, the application of TMPs in efficient biomass hydrogenation or HDO catalysis, as well as highly targeted multiscale strategies to enhance the catalytic performance of TMPs, are comprehensively described. Finally, large‐scale amplification synthesis, rational construction of TMP‐based catalysts and in‐depth study of the catalytic mechanism are also mentioned as challenges and future directions in this research field. Expectedly, this review can provide professional and targeted guidance for the rational design and practical application of TMPs biomass hydrogenation or HDO catalysts. [ABSTRACT FROM AUTHOR]

Catalytically driven electrochemical hydrogen evolution reaction (HER) holds immense promise for meeting renewable energy demands. In this study, we have reported highly efficient HER catalyst utilizing a novel electrode composed of titanium (Ti) sheet with gold and iridium oxide (Ti/Au-IrO x), compared to a conventional Pt electrode. The fabrication process involved anodizing a Ti strip to form a TiO 2 film, onto which Au and IrO x particles were sequentially deposited, followed by cathodic and anodic reactions, respectively. The resulting Ti/TiO 2 /Au-IrO x electrode exhibited remarkable efficiency in electrochemical HER, significantly reducing the overpotential. Notably, the catalytic onset potential was recorded at −0.10 V, markedly lower than those observed for Ti, Au, and Au-IrO x electrodes individually. This improvement can be attributed to an increase in the catalytic surface area along with a synergistic effect between the TiO 2 metal sheet and the electronic state of Au, which facilitates the adsorption of hydrogen molecules onto the catalytic surface. Furthermore , the presence of IrO x supports the redox counter-reaction, enhancing overall electrochemical conversion kinetics. Electrokinetic parameters such as turnover frequency (TOF), Tafel slope, and exchange current density (j k) were calculated as 0.334 s−1, 64 mV dec−1, and 0.12 mA cm−2, respectively, outperforming other experimental electrodes in this study and approaching values comparable to those of the Pt electrode (0.354 s−1, 36 mV dec−1, and 1.13 mA cm−2, respectively). Additionally, the Ti/TiO 2 /Au-IrO x electrode exhibited lower resistance for charge transfer (Rct) during HER (0.072 kΩ) compared to other electrodes evaluated. These findings underscore the Ti/TiO 2 /Au-IrO x electrode's potential as a highly efficient catalyst for HER under acidic conditions, offering insights into the intricate mechanisms driving catalytic enhancements beyond mere surface area augmentation. • Ti/TiO2/Au-IrOx electrode is an excellent HER catalyst in an acidic medium. • The Volmer-Heyrovsky step is the rate-determining step with 64 mVdec−1 Tafel slope. • Turnover frequency is 0.334 s−1 which is very close to Pt (0.354 s−1). • The catalytic onset potential recorded at −0.10 V with 1 mA cm−2 current density. [ABSTRACT FROM AUTHOR]

Enhanced bioenergy anabolism through transmembrane redox reactions in artificial systems remains a great challenge. Here, we explore synthetic electron shuttle to activate transmembrane chemo‐enzymatic cascade reactions in a mitochondria‐like nanoarchitecture for augmenting bioenergy anabolism. In this nanoarchitecture, a dendritic mesoporous silica microparticle as inner compartment possesses higher load capacity of NADH as proton source and allows faster mass transfer. In addition, the outer compartment ATP synthase‐reconstituted proteoliposomes. Like natural enzymes in the mitochondrion respiratory chain, a small synthetic electron shuttle embedded in the lipid bilayer facilely mediates transmembrane redox reactions to convert NADH into NAD+ and a proton. These facilitate an enhanced outward proton gradient to drive ATP synthase to rotate for catalytic ATP synthesis with improved performance in a sustainable manner. This work opens a new avenue to achieve enhanced bioenergy anabolism by utilizing a synthetic electron shuttle and tuning inner nanostructures, holding great promise in wide‐range ATP‐powered bioapplications. [ABSTRACT FROM AUTHOR]

The recognition of the importance of nanostructures is mainly due to the development of nanotechnology. For further developments in materials sciences, a concept that integrates nanotechnology with material chemistry to fabricate functional materials has to be proposed. Nanoarchitectonics will carry out this task. In nanoarchitectonics, we architect functional material systems from nano-units (atoms, molecules, nanomaterials). The methodology is not specific to any particular material or application. It covers a wide range. Therefore, nanoarchitectonics can be thought of as the method for everything in materials science. As typical demonstrations for usages of nanoarchitectonics, this review paper presents our work on nanoarchitectonics for supercapacitors. We divide it into two categories with different approaches. The first is the development of carbon materials as supercapacitor electrode materials from biomass. The second category is preparing carbon materials using structures created by supramolecular assembly of fullerenes such as C60 and C70. By presenting examples using opposite starting materials, a complex natural material, and an ultimately simple molecule, we will demonstrate the versatility and breadth of possibilities of this approach.

It has become clear that superior material functions are derived from precisely controlled nanostructures. This has been greatly accelerated by the development of nanotechnology. The next step is to assemble materials with knowledge of their nano-level structures. This task is assigned to the post-nanotechnology concept of nanoarchitectonics. However, nanoarchitectonics, which creates intricate three-dimensional functional structures, is not always easy. Two-dimensional nanoarchitectonics based on reactions and arrangements at the surface may be an easier target to tackle. A better methodology would be to define a two-dimensional structure and then develop it into a three-dimensional structure and function. According to these backgrounds, this review paper is organized as follows. The introduction is followed by a summary of the three issues; (i) 2D to 3D dynamic structure control: liquid crystal commanded by the surface, (ii) 2D to 3D rational construction: a metal–organic framework (MOF) and a covalent organic framework (COF); (iii) 2D to 3D functional amplification: cells regulated by the surface. In addition, this review summarizes the important aspects of the ultimate three-dimensional nanoarchitectonics as a perspective. The goal of this paper is to establish an integrated concept of functional material creation by reconsidering various reported cases from the viewpoint of nanoarchitectonics, where nanoarchitectonics can be regarded as a method for everything in materials science. [ABSTRACT FROM AUTHOR]

Nanotechnology has advanced the techniques for elucidating phenomena at the atomic, molecular, and nano-level. As a post nanotechnology concept, nanoarchitectonics has emerged to create functional materials from unit structures. Consider the material function when nanoarchitectonics enables the design of materials whose internal structure is controlled at the nanometer level. Material function is determined by two elements. These are the functional unit that forms the core of the function and the environment (matrix) that surrounds it. This review paper discusses the nanoarchitectonics of confined space, which is a field for controlling functional materials and molecular machines. The first few sections introduce some of the various dynamic functions in confined spaces, considering molecular space, materials space, and biospace. In the latter two sections, examples of research on the behavior of molecular machines, such as molecular motors, in confined spaces are discussed. In particular, surface space and internal nanospace are taken up as typical examples of confined space. What these examples show is that not only the central functional unit, but also the surrounding spatial configuration is necessary for higher functional expression. Nanoarchitectonics will play important roles in the architecture of such a total system. [ABSTRACT FROM AUTHOR]

The next step in nanotechnology is to establish a methodology to assemble new functional materials based on the knowledge of nanotechnology. This task is undertaken by nanoarchitectonics. In nanoarchitectonics, we architect functional material systems from nanounits such as atoms, molecules, and nanomaterials. In terms of the hierarchy of the structure and the harmonization of the function, the material created by nanoarchitectonics has similar characteristics to the organization of the functional structure in biosystems. Looking at actual biofunctional systems, dynamic properties and interfacial environments are key. In other words, nanoarchitectonics at dynamic interfaces is important for the production of bio-like highly functional materials systems. In this review paper, nanoarchitectonics at dynamic interfaces will be discussed, looking at recent typical examples. In particular, the basic topics of "molecular manipulation, arrangement, and assembly" and "material production" will be discussed in the first two sections. Then, in the following section, "fullerene assembly: from zero-dimensional unit to advanced materials", we will discuss how various functional structures can be created from the very basic nanounit, the fullerene. The above examples demonstrate the versatile possibilities of architectonics at dynamic interfaces. In the last section, these tendencies will be summarized, and future directions will be discussed. [ABSTRACT FROM AUTHOR]

This review comprehensively covers synthetic catalysts for the hydrolysis of biorelevant phosphates and pyrophosphates, which bridge between nanoarchitectonics and biology to construct their interdisciplinary hybrids. In the early 1980s, remarkable catalytic activity of Ce4+ ion for phosphate hydrolysis was found. More recently, this finding has been extended to Ce-based solid catalysts (CeO2 and Ce-based metal-organic frameworks (MOFs)), which are directly compatible with nanoarchitectonics. Monoesters and triesters of phosphates, as well as pyrophosphates, were effectively cleaved by these catalysts. With the use of either CeO2 nanoparticles or elegantly designed Ce-based MOF, highly stable phosphodiester linkages were also hydrolyzed. On the surfaces of all these solid catalysts, Ce4+ and Ce3+ coexist and cooperate for the catalysis. The Ce4+ activates phosphate substrates as a strong acid, whereas the Ce3+ provides metal-bound hydroxide as an eminent nucleophile. Applications of these Ce-based catalysts to practical purposes are also discussed. This review covers recent developments of synthetic catalysts to hydrolyze biorelevant phosphates, which are essential for constructing interdisciplinary hybrids between nanoarchitectonics and biology. [ABSTRACT FROM AUTHOR]

Abstract Advanced materials could perform functions in response to external stimuli. These are responsive materials. In order for us to develop advanced functional systems with a good responsive nature, we need to create a methodology that goes one step further. It is the artificial architecture of functional material systems based on the knowledge of nanotechnology. The task will be fulfilled by the new concept of nanoarchitectonics. Nanoarchitectonics integrates nanotechnology with various material sciences, basic chemistry, microfabrication techniques, and biological processes to architect functional material systems from atomic, molecular, and nanomaterial units. This review will deal with the nanoarchitectonics of responsive materials related with phenomena at interfaces. In order to demonstrate the effectiveness of responsive materials nanoarchitectonics at interfaces for functional systems of various sizes, this review article is organized by size for various functional systems. Specifically, this review has grouped them into (i) molecular level response, (ii) nanodevice level response, (iii) material level response, and (iv) living cell level response. If the social demand for these materials is fully recognized, such development is expected to efficiently progress. This review article would play a role in stimulating such development.

Lateral flow assays (LFAs) are currently the most widely used point-of-care testing technique with remarkable advantages such as simple operation, rapid analysis, portability, and low cost. Traditionally, gold nanoparticles are employed as tracer element in LFAs due to their strong localised surface plasmon resonance. However, this conventional LFA technique based on colorimetric analysis is neither useful to determine critical analytes with desired sensitivity, nor can it quantify the analytes. Various signal amplification strategies have been proposed to improve the sensitivity and the quantitative determination of analytes using LFAs. One of the promising strategies is to enhance the photothermal properties of nanomaterials to generate heat after light irradiation, followed by a temperature measurement to detect and quantify the analyte concentration. Recently, it has been observed that the nanoscale architecture of materials, including size, shape, and nanoscale composition, plays a significant role in enhancing the photothermal properties of nanomaterials. In this review, we discuss the nanoarchitectonics of nanomaterials regarding enhanced photothermal properties and their application in LFAs. Initially, we discuss various important photothermal materials and their classification along with their working principle. Then, we highlight important aspects of the nanoscale architecture (i.e., size, shape, and composition) to enable maximum light-to-heat conversion efficiency. Finally, we discuss some of the recent advances in photothermal LFAs and their application in detecting analytes.

ABSTRACTThis review comprehensively covers synthetic catalysts for the hydrolysis of biorelevant phosphates and pyrophosphates, which bridge between nanoarchitectonics and biology to construct their interdisciplinary hybrids. In the early 1980s, remarkable catalytic activity of Ce4+ ion for phosphate hydrolysis was found. More recently, this finding has been extended to Ce-based solid catalysts (CeO2 and Ce-based metal-organic frameworks (MOFs)), which are directly compatible with nanoarchitectonics. Monoesters and triesters of phosphates, as well as pyrophosphates, were effectively cleaved by these catalysts. With the use of either CeO2 nanoparticles or elegantly designed Ce-based MOF, highly stable phosphodiester linkages were also hydrolyzed. On the surfaces of all these solid catalysts, Ce4+ and Ce3+ coexist and cooperate for the catalysis. The Ce4+ activates phosphate substrates as a strong acid, whereas the Ce3+ provides metal-bound hydroxide as an eminent nucleophile. Applications of these Ce-based catalysts to practical purposes are also discussed.

ABSTRACTPolyaniline-based atomic switches are material building blocks whose nanoscale structure and resultant neuromorphic character provide a new physical substrate for the development next-generation, nanoarchitectonic-enabled computing systems. Metal ion-doped devices consisting of a Ag/metal ion doped polyaniline/Pt sandwich structure were fabricated using an in situ wet process. The devices exhibited repeatable resistive switching between high (ON) and low (OFF) conductance states in both Ag+ and Cu2+ ion-doped devices. The threshold voltage for switching was>0.8 V and average ON/OFF conductance ratios (30 cycles for 3 samples) were 13 and 16 for Ag+ and Cu2+ devices, respectively. The ON state duration was determined by the decay to an OFF state after pulsed voltages of differing amplitude and frequency. The switching behaviour is analagous to short-term (STM) and long-term (LTM) memories of biological synapses. Memristive behaviour and evidence of quantized conductance were also observed and interpreted in terms of metal filament formation bridging the metal doped polymer layer. The successful realization of these properties within physical material systems indicate polyaniline frameworks as suitable neuromorphic substrates for in materia computing.

The layer-by-layer (LbL) technique has been proven to be one of the most versatile approaches in order to fabricate functional nanofilms. The use of simple and inexpensive procedures as well as the possibility to incorporate a very wide range of materials through different interactions have driven its application in a wide range of fields. On the other hand, field-effect transistors (FETs) are certainly among the most important elements in electronics. The ability to modulate the flowing current between a source and a drain electrode via the voltage applied to the gate electrode endow these devices to switch or amplify electronic signals, being vital in all of our everyday electronic devices. In this topical review, we highlight different research efforts to engineer field-effect transistors using the LbL assembly approach. We firstly discuss on the engineering of the channel material of transistors via the LbL technique. Next, the deposition of dielectric materials through this approach is reviewed, allowing the development of high-performance electronic components. Finally, the application of the LbL approach to fabricate FETs-based biosensing devices is also discussed, as well as the improvement of the transistor's interfacial sensitivity by the engineering of the semiconductor with polyelectrolyte multilayers. [ABSTRACT FROM AUTHOR]

In modern materials research, nanotechnology will play a game-changing role, with nanoarchitectonics as an overarching integrator of the field and artificial intelligence hastening its progress as a super-accelerator. We would like to discuss how this schema can be utilized in the context of specific applications, with exemplification using disease diagnosis. In this paper, we focus on early, noninvasive disease diagnosis as a target application. In particular, recent trends in chemosensing in the detection of cancer and Parkinson's disease are reviewed. The concept has been gaining traction as dynamic volatile metabolite profiles have been increasingly associated with disease onset, making them promising diagnostic tools in early stages of disease. We also discuss advances in nanoarchitectonic chemosensors, which are theoretically ideal form factors for diagnostic chemosensing devices. Last but not least, we shine the spotlight on the rise to prominence and emergent contributions of artificial intelligence (AI) in recent works, which have elucidated a strong synergy between chemosensing and AI. The powerful combination of nanoarchitectonic chemosensors and AI could challenge our current notions of disease diagnosis. Disease diagnosis and detection of emerging viruses are important challenges facing society. The parallel development of advanced functional materials for sensing is necessary to support and enable AI methodologies in making technological leaps in applications. The material and structural formative technologies of nanoarchitectonics are critical in meeting these challenges. [ABSTRACT FROM AUTHOR]

The high prevalence of opioid addiction and the shortcomings of systemic opioids has increased the pace of the search for alternative methods of pain management. The local delivery of pain medications has started to be used as a tool for pain management and to decrease the use of systemic opioids for these patients. Here, we explored an in-situ polymerizable hydrogel system for the local delivery of analgesics and nonsteroid anti-inflammatory drugs (NSAID) for orthopaedic applications. We synthesized a series of methacrylated oligomeric polyethylene gly co l- co -lactic acid polymer using microwave radiation for the delivery of bupivacaine hydrochloride as an analgesic and ketorolac tromethamine as an NSAID. We determined drug elution and gel degradation profiles in vitro. Biocompatibility was assessed against osteoblasts in vitro and by histological analysis after subcutaneous implantation for 4 weeks in vivo. Intra-articular and systemic concentrations and pharmacokinetic parameters were estimated using a two-compartment pharmacodynamic model based on in-vitro elution profiles. This type of in-situ applicable hydrogels is promising for extending the local efficacy of pain medication and further reducing the need for opioids. [Display omitted] [ABSTRACT FROM AUTHOR]

We report the development of a novel electrocatalyst composed of nanoarchitectured spinel cobalt manganese oxide and graphene for the oxygen reduction reaction (ORR). A combination of co-precipitation and hydrothermal methods achieved the unique nanoarchitecture of the electrocatalyst. The formation of CoMn2O4 electrocatalyst was confirmed by X-ray diffraction, transmission electron microscopy, and other spectroscopic and microscopic techniques. In addition to synthesizing CoxOy and MnxOy as control electrocatalysts, we created a physical mixture of CoMn2O4 and graphene to investigate the impact of their interface on electrocatalytic activity. Our findings indicate that CoMn2O4/graphene exhibits improved ORR activity, stability, and methanol tolerance in an alkaline medium. This enhancement can be attributed to the synergistic effect and strong interface interaction between CoMn2O4 and graphene. This study demonstrates the potential of the proposed electrocatalyst as a cost-effective and eco-friendly alternative for oxygen reduction in fuel cells applications. [ABSTRACT FROM AUTHOR]

The development of nanotechnology has provided an opportunity to integrate a wide range of phenomena and disciplines from the atomic scale, the molecular scale, and the nanoscale into materials. Nanoarchitectonics as a post-nanotechnology concept is a methodology for developing functional material systems using units such as atoms, molecules, and nanomaterials. Especially, molecular nanoarchitectonics has been strongly promoted recently by incorporating nanotechnological methods into organic synthesis. Examples of research that have attracted attention include the direct observation of organic synthesis processes at the molecular level with high resolution, and the control of organic syntheses with probe microscope tips. These can also be considered as starting points for nanoarchitectonics. In this review, these examples of molecular nanoarchitectonics are introduced, and future prospects of nanoarchitectonics are discussed. The fusion of basic science and the application of practical functional materials will complete materials chemistry for everything.

Based on nanoarchitectonics and molecular dynamics simulations, we investigate the structural properties and diffusion pathway of Na atoms in sodium trisilicate over a wide temperature range. The structural and dynamics properties are analyzed through the radial distribution function (RDF), the Voronoi Si- and O-polyhedrons, the cluster function fCL(r), and the sets of fastest (SFA) and slowest atoms (SSA). The results indicate that Na atoms are not placed in Si-polyhedrons and bridging oxygen (BO) polyhedrons; instead, Na atoms are mainly placed in non-bridging oxygen (NBO) polyhedrons and free oxygen (FO) polyhedrons. Here BO, NBO, and FO represent O bonded with two, one, and no Si atoms, respectively. The simulation shows that O atoms in sodium trisilicate undergo numerous transformations: NBF0 ↔ NBF1, NBF1 ↔ NBF2, and BO0 ↔ BO1, where NBF is NBO or FO. The dynamics in sodium trisilicate are mainly distributed by the hopping and cooperative motion of Na atoms. We suppose that the diffusion pathway of Na atoms is realized via hopping Na atoms alone in BO-polyhedrons and the cooperative motion of a group of Na atoms in NBO- and FO-polyhedrons.

The catalytic conversion of lignocellulose derived products to value added chemicals are of high importance in the quest to solve energy crisis. In this work, we have prepared the phosphomolybdic acid (PMA) supported on boron‐nitride (BN) nanosheets via a facile hydrothermal process. A series of heterogeneous catalysts has been prepared by using varying quantities of BN and PMA. All the catalysts were examined for the conversion of fructose to 5‐hydroxymethylfurfural (5‐HMF) and one of them turns out to be the best catalyst. Different optimizations like catalyst amount, temperature and time have been performed using the best catalyst. Although the catalyst selectively forms 5‐HMF, the yield was relatively low, which could be explained using the zeta potential studies. However, it was interesting to note that an addition of H2SO4 (0.01 M) to the reaction mixture enhances the catalytic activity of the overall process and leads to the formation of levulinic acid (LA) in addition to 5‐HMF, which could be attributed to the increased acidity in the reaction mixture. Overall, this work provides deeper insights on the role of BN, PMA and H2SO4 in the conversion of saccharides to value‐added chemicals. [ABSTRACT FROM AUTHOR]

Nanoarchitectonics is the methodology for production of functional materials from nano‐units. In nanoarchitectonics, the conversion of molecules (chemistry, Chem), the control of nanostructures (nanotechnology, Nano), and the production of materials (materials science, Mat) are essential elements. In order to explain the contribution of Chem, Nano, and Mat to nanoarchitectonics, this review article is described according to two major sections, Chem & Nano and Nano to Mat. In Chem & Nano section, the integration of chemistry and nanotechnology is overviewed, and the next section, Nano to Mat, illustrates how molecules and nanomaterials are architecturally transformed into functional materials. These include supramolecular polymers and functional metal‐organic frameworks, which have attracted widespread attention, as well as emerging areas such as organic reactions by nanotechnology, chemical synthesis in nanospace, and material creation by dynamic motions at interfaces. It is emphasized that Chem+Nano+Mat is essential for nanoarchitectonics. [ABSTRACT FROM AUTHOR]

Transition metal dichalcogenides (TMDC) exhibit highly superior electrical properties and are typically obtained through mechanical exfoliation. This method has significant limitations, however, such as patterning issues and non‐uniformity, which hinder their application in integrated circuits as transistors and array pixel displays. To overcome these challenges, various large‐scale deposition methods have been developed. In this review, we introduce five major methods for TMDC deposition: chemical vapor deposition, physical vapor deposition, atomic layer deposition, pulsed laser deposition, and ink‐jet printing. An overview of each method is provided in the following order: surface analysis, electrical characteristics, and limitations of each method are discussed. Furthermore, we present three key strategies for an advanced device fabrication using the discussed deposition methods. By implementing these strategies, we can accelerate the development of highly crystalline and scalable TMDC thin films, which are essential for producing advanced electronic devices with improved performance. Owing to recent technological advancements, TMDC devices have the potential to become the leading material for next‐generation semiconductor devices. These devices can be specifically designed and optimized for innovative applications. [ABSTRACT FROM AUTHOR]

Engineered nitric oxide-releasing supramolecular nanostructures (SNFs-NO) enhance antimicrobial photodynamic therapy (APDT) against Gram-positive methicillin-resistant Staphylococcus aureus (MRSA) and Gram-negative Escherichia coli (E. coli). This is achieved by disrupting cell membranes and inhibiting respiratory activities through the generation of reactive oxygen species (ROS) in the cellular system. [Display omitted] Light‐controlled therapies offer a promising strategy to prevent and suppress infections caused by numerous bacterial pathogens. Excitation of exogenously supplied photosensitizers (PS) at specific wavelengths elicits levels of reactive oxygen intermediates toxic to bacteria. Porphyrin-based supramolecular nanostructure frameworks (SNF) are effective PS with unique physicochemical properties that have led to their widespread use in photomedicine. Herein, we developed a nitric oxide (NO) releasing, biocompatible, and stable porphyrin-based SNF (SNF-NO), which was achieved through a confined noncovalent self-assembly process based on π–π stacking. Characterization of the SNFs via scanning electron microscopy (SEM) and transmission electron microscopy (TEM) analysis showed the formation of three-dimensional, well-defined octahedral structures. These SNF-NO were shown to exhibit a red shift due to the noncovalent self-assembly of porphyrins, which also show extended light absorption to broadly cover the entire visible light spectrum to enhance photodynamic therapy (PDT). Under visible light irradiation (46 J cm−2), the SNF generates high yields of singlet oxygen (1O 2) radicals, hydroxyl radicals (HO), superoxide radicals (O 2 ), and peroxynitrite (ONOO−) radicals that have shown potential to enhance antimicrobial photodynamic therapy (APDT) against Gram-positive methicillin-resistant Staphylococcus aureus (MRSA) and Gram-negative Escherichia coli (E. coli). The resulting SNFs also exhibit significant biofilm dispersion and a decrease in biomass production. The combination of robust photosensitizer SNFs with nitric oxide-releasing capabilities is dynamic in its ability to target pathogenic infections while remaining nontoxic to mammalian cells. The engineered SNFs have enormous potential for treating and managing microbial infections. [ABSTRACT FROM AUTHOR]

The development of nanotechnology has made it possible to evaluate properties and functions at the nano-level. In order to fulfill this as material chemistry, it is necessary to develop a concept that integrates nanotechnology with existing fields such as supramolecular chemistry. This role is assigned to nanoarchitectonics, which is considered as a post-nanotechnology concept. In this paper, several recent examples related to nanoarchitectonics especially at interfaces are reviewed and discussed. In addition to nontechnology-driven organic reaction at solid surfaces, various nano-films preparation though techniques such as Langmuir-Blodgett (LB) method and layer-by-layer (LbL) assembly were discussed as nanoarchitectonics approaches to create functional materials such as two-dimensional nanocarbons and electroactive ultrathin films at interfaces. [ABSTRACT FROM AUTHOR]

Few‐layered graphitic carbon nitride (g‐C3N4) has been considered a popular base for constructing composite materials in photocatalytic CO2 reduction and H2 generation applications, particularly for constructing g‐C3N4 based composites based on the idea of nanoarchitectonics. The photocatalytic activity of these constructed g‐C3N4 composites relies on the composition, morphology, microstructure of the material. This review aims to focus on the summary of latest progress in the development of few‐layered g‐C3N4 nanosheets based noble metal clusters/nanoparticles and other semiconductor nanomaterials modified composite materials constructed using the technology of nanoarchitectonics for photocatalytic H2 generation and CO2 reduction. This review covers a brief introduction of the enhanced photogenerated carrier separation and transfer as well as extended light absorption of superior thin g‐C3N4 nanosheets based photocatalysts; discussions on the mechanism of g‐C3N4 based photocatalyst involved photocatalytic H2O splitting and CO2 reduction system; the latest progress in the study of nanoarchitectonics of a variety of g‐C3N4 based heterostructures including type II, Z‐scheme, S‐scheme, and Schottky junction. Major challenges on nanoarchitectonics of superior thin g‐C3N4 based heterostructures, as well as the recommendations for future studies of these materials to attain higher efficiency in photocatalytic H2 generation and CO2 reduction, are also concluded. [ABSTRACT FROM AUTHOR]

Nanoarchitectonics has emerged as a post-nanotechnology concept. As one of the applications of nanoarchitectonics, this review paper discusses the control of stem cell fate and function as an important issue. For hybrid nanoarchitectonics involving living cells, it is crucial to understand how biomaterials and their nanoarchitected structures regulate behaviours and fates of stem cells. In this review, biomaterials for the regulation of stem cell fate are firstly discussed. Besides multipotent differentiation, immunomodulation is an important biological function of mesenchymal stem cells (MSCs). MSCs can modulate immune cells to treat multiple immune- and inflammation-mediated diseases. The following sections summarize the recent advances of the regulation of the immunomodulatory functions of MSCs by biophysical signals. In the third part, we discussed how biomaterials direct the self-organization of pluripotent stem cells for organoid. Bioactive materials are constructed which mimic the biophysical cues of in vivo microenvironment such as elasticity, viscoelasticity, biodegradation, fluidity, topography, cell geometry, and etc. Stem cells interpret these biophysical cues by different cytoskeletal forces. The different cytoskeletal forces lead to substantial transcription and protein expression, which affect stem cell fate and function. Regulations of stem cells could not be utilized only for tissue repair and regenerative medicine but also potentially for production of advanced materials systems. Materials nanoarchitectonics with integration of stem cells and related biological substances would have high impacts in science and technology of advanced materials.

Electro-catalytic activity of Pt in the oxygen reduction reaction (ORR) depends strongly on its morphology. For an understanding of how morphology affects the catalytic properties of Pt, the investigation of Pt materials having well-defined morphologies is required. However, the challenges remain in rational and facile synthesis of Pt particles with tuneable well-defined morphology. A promising approach for the controlled synthesis of Pt particles is ‘self-assembly of building blocks’. Here, we report a unique synthesis method to control Pt morphology by using a self-assembly route, where nanoflower, nanowire, nanosheet and nanotube morphologies of Pt particles have been produced in a controlled manner. In the growth mechanism, Pt nanoparticles (5–11 nm) are rapidly prepared by using NaBH4 as a reductant, followed by their agglomeration promoted by adding 1,2-ethylenediamine. The morphology of the resulting Pt particles can be easily controlled by tuning hydrophobic/hydrophilic interactions by the addition of isopropanol and H2O. Of the Pt particles prepared using this method, Pt nanotubes show the highest ORR catalytic activity in an acid electrolyte with an onset potential of 1.02 V vs. RHE.

This review is dedicated to various functional nanoarchitectonic nanocomposites based on molecular octahedral metal atom clusters (Nb6, Mo6, Ta6, W6, Re6). Powder and film nanocomposites with two-dimensional, one-dimensional and zero-dimensional morphologies are presented, as well as film matrices from organic polymers to inorganic layered oxides. The high potential and synergetic effects of these nanocomposites for biotechnology applications, photovoltaic, solar control, catalytic, photonic and sensor applications are demonstrated. This review also provides a basic level of understanding how nanocomposites are characterized and processed using different techniques and methods. The main objective of this review would be to provide guiding significance for the design of new high-performance nanocomposites based on transition metal atom clusters.

Micro- and nanopatterning of metal oxide materials is an important process to develop electronic or optoelectronic devices. ZnO is a material of choice for its semiconducting and photoluminescence properties. In the frame of the nanoarchitectonics concept, we have developed and investigated a new process that relies on direct writing laser patterning in the Deep-UV (DUV) range to prepare photoluminescent microstructures of ZnO at room temperature, under air. This process is based on a synthesis of colloidal ZnO nanocrystals (NCs) with a careful choice of the ligands on the surface to obtain an optimal (i) stability of the colloids, (ii) redissolution of the non-insolated parts and (iii) cross-linking of the DUV-insolated parts. The mechanisms of photocrosslinking are studied by different spectroscopic methods. This room temperature process preserves the photoluminescence properties of the NCs and the wavelength used in DUV allows to reach a sub-micrometer resolution, which opens new perspectives for the integration of microstructures on flexible substrates for optoelectronic applications.

Like the proposal of nanotechnology by Richard Feynman, the nanoarchitectonics concept was initially proposed by Masakazu Aono. The nanoarchitectonics strategy conceptually fuses nanotechnology with other research fields including organic chemistry, supramolecular chemistry, micro/nanofabrication, materials science, and bio-related sciences, and aims to produce functional materials from nanoscale components. In this review article, bio-interactive nanoarchitectonics and two-dimensional materials and environments are discussed as a selected topic. The account gives general examples of nanoarchitectonics of two-dimensional materials for energy storage, catalysis, and biomedical applications, followed by explanations of bio-related applications with two-dimensional materials such as two-dimensional biomimetic nanosheets, fullerene nanosheets, and two-dimensional assemblies of one-dimensional fullerene nanowhiskers (FNWs). The discussion on bio-interactive nanoarchitectonics in two-dimensional environments further extends to liquid–liquid interfaces such as fluorocarbon–medium interfaces and viscous liquid interfaces as new frontiers of two-dimensional environments for bio-related applications. Controlling differentiation of stem cells at fluidic liquid interfaces is also discussed. Finally, a conclusive section briefly summarizes features of bio-interactive nanoarchitectonics with two-dimensional materials and environments and discusses possible future perspectives.

The consumption of energy is an important resource that cannot be ignored in modern society. Non-renewable forms of energy, such as coal, natural gas, and oil, have always been important strategic resources and are always facing a crisis of shortage. Therefore, there is an urgent need for green renewable forms of energy. As an emerging green energy source, the moist-electric generator (MEG) has been studied in recent years and may become an energy source that can be utilized in daily life. Along with the advancement of technological means, nanoarchitectonics play an important role in MEG devices. This review aims to provide a comprehensive summary of the fundamentals of the MEG from the perspective of different material classifications and to provide guidance for future work in the field of MEGs. The effects of various parameters and structural designs on the output power, recent important literature and works, the mechanism of liquid–solid interactions at the nanoscale, and the application status and further potential of MEG devices are discussed in this review. It is expected that this review may provide valuable knowledge for future MEG research.