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Showing papers in "Nature Nanotechnology in 2021"


Journal ArticleDOI
TL;DR: In this paper, the authors discuss the biological role of extracellular vesicles and how they can be applied as drug carriers, focusing on the current state of their manufacturing and existing challenges.
Abstract: Extracellular-vesicle-based cell-to-cell communication is conserved across all kingdoms of life. There is compelling evidence that extracellular vesicles are involved in major (patho)physiological processes, including cellular homoeostasis, infection propagation, cancer development and cardiovascular diseases. Various studies suggest that extracellular vesicles have several advantages over conventional synthetic carriers, opening new frontiers for modern drug delivery. Despite extensive research, clinical translation of extracellular-vesicle-based therapies remains challenging. Here, we discuss the uniqueness of extracellular vesicles along with critical design and development steps required to utilize their full potential as drug carriers, including loading methods, in-depth characterization and large-scale manufacturing. We compare the prospects of extracellular vesicles with those of the well established liposomes and provide guidelines to direct the process of developing vesicle-based drug delivery systems. In this Review the authors discuss the biological role of extracellular vesicles and how they can be applied as drug carriers, focusing on the current state of their manufacturing and existing challenges.

481 citations


Journal ArticleDOI
TL;DR: In this paper, an anode-free aqueous zinc battery with an alkylammonium salt additive has been developed, which enables the formation of a robust, Zn2+conducting and waterproof SEI.
Abstract: Metallic zinc is an ideal anode due to its high theoretical capacity (820 mAh g−1), low redox potential (−0.762 V versus the standard hydrogen electrode), high abundance and low toxicity. When used in aqueous electrolyte, it also brings intrinsic safety, but suffers from severe irreversibility. This is best exemplified by low coulombic efficiency, dendrite growth and water consumption. This is thought to be due to severe hydrogen evolution during zinc plating and stripping, hitherto making the in-situ formation of a solid–electrolyte interphase (SEI) impossible. Here, we report an aqueous zinc battery in which a dilute and acidic aqueous electrolyte with an alkylammonium salt additive assists the formation of a robust, Zn2+-conducting and waterproof SEI. The presence of this SEI enables excellent performance: dendrite-free zinc plating/stripping at 99.9% coulombic efficiency in a Ti||Zn asymmetric cell for 1,000 cycles; steady charge–discharge in a Zn||Zn symmetric cell for 6,000 cycles (6,000 h); and high energy densities (136 Wh kg−1 in a Zn||VOPO4 full battery with 88.7% retention for >6,000 cycles, 325 Wh kg−1 in a Zn||O2 full battery for >300 cycles and 218 Wh kg−1 in a Zn||MnO2 full battery with 88.5% retention for 1,000 cycles) using limited zinc. The SEI-forming electrolyte also allows the reversible operation of an anode-free pouch cell of Ti||ZnxVOPO4 at 100% depth of discharge for 100 cycles, thus establishing aqueous zinc batteries as viable cell systems for practical applications. A solid–electrolyte interphase that is permeable to Zn(ii) ions but waterproof is formed using an aqueous electrolyte composition. Cycling performances in an anode-free aqueous pouch cell show promise for intrinsically safe energy storage applications.

360 citations


Journal ArticleDOI
TL;DR: In this article, the authors review four platform technologies that have enabled the clinical translation of nucleic acid therapeutics: antisense oligonucleotides, ligand-modified small interfering RNA conjugates, lipid nanoparticles and adeno-associated virus vectors.
Abstract: The increasing number of approved nucleic acid therapeutics demonstrates the potential to treat diseases by targeting their genetic blueprints in vivo. Conventional treatments generally induce therapeutic effects that are transient because they target proteins rather than underlying causes. In contrast, nucleic acid therapeutics can achieve long-lasting or even curative effects via gene inhibition, addition, replacement or editing. Their clinical translation, however, depends on delivery technologies that improve stability, facilitate internalization and increase target affinity. Here, we review four platform technologies that have enabled the clinical translation of nucleic acid therapeutics: antisense oligonucleotides, ligand-modified small interfering RNA conjugates, lipid nanoparticles and adeno-associated virus vectors. For each platform, we discuss the current state-of-the-art clinical approaches, explain the rationale behind its development, highlight technological aspects that facilitated clinical translation and provide an example of a clinically relevant genetic drug. In addition, we discuss how these technologies enable the development of cutting-edge genetic drugs, such as tissue-specific nucleic acid bioconjugates, messenger RNA and gene-editing therapeutics.

344 citations


Journal ArticleDOI
TL;DR: The cathode is composed of uniformly embedded ZnS nanoparticles and Co–N–C single-atom catalyst to form double-end binding sites inside a highly oriented macroporous host, which can effectively immobilize and catalytically convert polysulfide intermediates during cycling, thus eliminating the shuttle effect and lithium metal corrosion.
Abstract: Lithium–sulfur batteries are attractive alternatives to lithium-ion batteries because of their high theoretical specific energy and natural abundance of sulfur. However, the practical specific energy and cycle life of Li–S pouch cells are significantly limited by the use of thin sulfur electrodes, flooded electrolytes and Li metal degradation. Here we propose a cathode design concept to achieve good Li–S pouch cell performances. The cathode is composed of uniformly embedded ZnS nanoparticles and Co–N–C single-atom catalyst to form double-end binding sites inside a highly oriented macroporous host, which can effectively immobilize and catalytically convert polysulfide intermediates during cycling, thus eliminating the shuttle effect and lithium metal corrosion. The ordered macropores enhance ionic transport under high sulfur loading by forming sufficient triple-phase boundaries between catalyst, conductive support and electrolyte. This design prevents the formation of inactive sulfur (dead sulfur). Our cathode structure shows improved performances in a pouch cell configuration under high sulfur loading and lean electrolyte operation. A 1-A-h-level pouch cell with only 100% lithium excess can deliver a cell specific energy of >300 W h kg−1 with a Coulombic efficiency >95% for 80 cycles. The shuttling effect in Li–S batteries can be drastically suppressed by using a single-atom Co catalyst and polar ZnS nanoparticles embedded in a macroporous conductive matrix as a cathode. Using this strategy, Li–S pouch cells show stable cycling and high energy performances.

326 citations


Journal ArticleDOI
TL;DR: In this article, the authors summarize the latest insights into cellular uptake mechanisms and pathways and highlight limitations of current systems to study endocytosis, particularly problems with non-specific inhibitors.
Abstract: Endocytosis is a critical step in the process by which many therapeutic nanomedicines reach their intracellular targets. Our understanding of cellular uptake mechanisms has developed substantially in the past five years. However, these advances in cell biology have not fully translated to the nanoscience and therapeutics literature. Misconceptions surrounding the role of different endocytic pathways and how to study these pathways are hindering progress in developing improved nanoparticle therapies. Here, we summarize the latest insights into cellular uptake mechanisms and pathways. We highlight limitations of current systems to study endocytosis, particularly problems with non-specific inhibitors. We also summarize alternative genetic approaches to robustly probe these pathways and discuss the need to understand how cells endocytose particles in vivo. We hope that this critical assessment of the current methods used in studying nanoparticle uptake will guide future studies at the interface of cell biology and nanomedicine.

303 citations


Journal ArticleDOI
TL;DR: It is demonstrated that a hierarchically designed polymer nanofibre-based film, produced by a scalable electrostatic spinning process, enables selective mid-infrared emission, effective sunlight reflection and therefore excellent all-day radiative cooling performance.
Abstract: Traditional cooling systems consume tremendous amounts of energy and thus aggravate the greenhouse effect1,2. Passive radiative cooling, dissipating an object’s heat through an atmospheric transparency window (8–13 μm) to outer space without any energy consumption, has attracted much attention3–9. The unique feature of radiative cooling lies in the high emissivity in the atmospheric transparency window through which heat can be dissipated to the universe. Therefore, for achieving high cooling performance, the design and fabrication of selective emitters, with emission strongly dominant in the transparency window, is of essential importance, as such spectral selection suppresses parasitic absorption from the surrounding thermal radiation. Recently, various materials and structures with tailored spectrum responses have been investigated to achieve the effect of daytime radiative cooling6–8,10–15. However, most of the radiative cooling materials reported possess broad-band absorption/emission covering the whole mid-infrared wavelength11–15. Here we demonstrate that a hierarchically designed polymer nanofibre-based film, produced by a scalable electrostatic spinning process, enables selective mid-infrared emission, effective sunlight reflection and therefore excellent all-day radiative cooling performance. Specifically, the C–O–C (1,260–1,110 cm−1) and C–OH (1,239–1,030 cm−1) bonding endows the selective emissivity of 78% in 8–13 μm wavelength range, and the design of nanofibres with a controlled diameter allows for a high reflectivity of 96.3% in 0.3–2.5 μm wavelength range. As a result, we observe ~3 °C cooling improvement of this selective thermal emitter as compared to that of a non-selective emitter at night, and 5 °C sub-ambient cooling under sunlight. The impact of this hierarchically designed selective thermal emitter on alleviating global warming and temperature regulating an Earth-like planet is also analysed, with a significant advantage demonstrated. With its excellent cooling performance and a scalable process, this hierarchically designed selective thermal emitter opens a new pathway towards large-scale applications of all-day radiative cooling materials. A hierarchically designed polymer nanofibre-based film produced by a scalable electrospinning process enables selective mid-infrared emission and effective sunlight reflection, and thus realizes an excellent all-day radiative cooling performance.

302 citations


Journal ArticleDOI
Kensaku Kodama1, Tomoyuki Nagai1, Akira Kuwaki1, Ryosuke Jinnouchi1, Yu Morimoto1 
TL;DR: In this paper, the development history of Pt-based nanocatalysts and recent analytical studies are summarized to identify the origin of these technical issues, and promising strategies for overcoming those issues are also discussed.
Abstract: The past 30 years have seen progress in the development of Pt-based nanocatalysts for the oxygen reduction reaction, and some are now in production on a commercial basis and used for polymer electrolyte fuel cells (PEFCs) for automotives and other applications. Further improvements in catalytic activity are required for wider uptake of PEFCs, however. In laboratories, researchers have developed various catalysts that have much higher activities than commercial ones, and these state-of-the-art catalysts have potential to improve energy conversion efficiencies and reduce the usage of platinum in PEFCs. There are several technical issues that must be solved before they can be applied in fuel cell vehicles, which require a high power density and practical durability, as well as high efficiency. In this Review, the development history of Pt-based nanocatalysts and recent analytical studies are summarized to identify the origin of these technical issues. Promising strategies for overcoming those issues are also discussed. This Review summarizes the development history of Pt-based nanocatalysts and recent analytical studies to identify the technical issues in the automobile application, proposing promising strategies for overcoming the trade-offs among the efficiency,power density, and durability of polymer electrolyte fuel cells.

286 citations


Journal ArticleDOI
TL;DR: In this paper, the authors distinguished nanoplastics from microplastics with respect to their transport properties, interactions with light and natural colloids, a high fraction of particle molecules on the surface, bioavailability and diffusion times for the release of plastic additives.
Abstract: Increasing concern and research on the subject of plastic pollution has engaged the community of scientists working on the environmental health and safety of nanomaterials. While many of the methods developed in nano environment, health and safety work have general applicability to the study of particulate plastics, the nanometric size range has important consequences for both the analytical challenges of studying nanoscale plastics and the environmental implications of these incidental nanomaterials. Related to their size, nanoplastics are distinguished from microplastics with respect to their transport properties, interactions with light and natural colloids, a high fraction of particle molecules on the surface, bioavailability and diffusion times for the release of plastic additives. Moreover, they are distinguished from engineered nanomaterials because of their high particle heterogeneity and their potential for rapid further fragmentation in the environment. These characteristics impact environmental fate, potential effects on biota and human health, sampling and analysis. Like microplastics, incidentally produced nanoplastics exhibit a diversity of compositions and morphologies and a heterogeneity that is typically absent from engineered nanomaterials. Therefore, nanoscale plastics must be considered as distinct from both microplastics and engineered nanomaterials.

250 citations


Journal ArticleDOI
TL;DR: X-ray activated, lanthanide-based nanoparticles with a tunable emission in the biologically relevant NIR-II spectral region, which allows high-contrast, multimodal in vivo deep-tissue organ imaging.
Abstract: Persistent luminescence is not affected by background autofluorescence, and thus holds the promise of high-contrast bioimaging. However, at present, persistent luminescent materials for in vivo imaging are mainly bulk crystals characterized by a non-uniform size and morphology, inaccessible core-shell structures and short emission wavelengths. Here we report a series of X-ray-activated, lanthanide-doped nanoparticles with an extended emission lifetime in the second near-infrared window (NIR-II, 1,000-1,700 nm). Core-shell engineering enables a tunable NIR-II persistent luminescence, which outperforms NIR-II fluorescence in signal-to-noise ratios and the accuracy of in vivo multiplexed encoding and multilevel encryption, as well as in resolving mouse abdominal vessels, tumours and ureters in deep tissue (~2-4 mm), with up to fourfold higher signal-to-noise ratios and a threefold greater sharpness. These rationally designed nanoparticles also allow the high-contrast multiplexed imaging of viscera and multimodal NIR-II persistent luminescence-magnetic resonance-positron emission tomography imaging of murine tumours.

236 citations


Journal ArticleDOI
TL;DR: In this article, the authors presented a highly stable and ultrapermeable zeolitic imidazolate framework-8 (ZIF-8)-nanocrystal-hybridized GOm that is prepared by ice templating and subsequent in situ crystallization of ZIF-eight at the nanosheet edges.
Abstract: The robustness of carbon nanomaterials and their potential for ultrahigh permeability has drawn substantial interest for separation processes. However, graphene oxide membranes (GOms) have demonstrated limited viability due to instabilities in their microstructure that lead to failure under cross-flow conditions and applied hydraulic pressure. Here we present a highly stable and ultrapermeable zeolitic imidazolate framework-8 (ZIF-8)-nanocrystal-hybridized GOm that is prepared by ice templating and subsequent in situ crystallization of ZIF-8 at the nanosheet edges. The selective growth of ZIF-8 in the microporous defects enlarges the interlayer spacings while also imparting mechanical integrity to the laminate framework, thus producing a stable microstructure capable of maintaining a water permeability of 60 l m−2 h−1 bar−1 (30-fold higher than GOm) for 180 h. Furthermore, the mitigation of microporous defects via ZIF-8 growth increased the permselectivity of methyl blue molecules sixfold. Low-field nuclear magnetic resonance was employed to characterize the porous structure of our membranes and confirm the tailored growth of ZIF-8. Our technique for tuning the membrane microstructure opens opportunities for developing next-generation nanofiltration membranes. Highly stable and ultrapermeable membranes can be fabricated by the hybridization of zeolitic imidazolate framework-8 and graphene oxide.

220 citations


Journal ArticleDOI
TL;DR: In this paper, a large-scale, electrically reconfigurable non-volatile active metasurface platform based on optical phase change materials (PCMs) is presented.
Abstract: Active metasurfaces promise reconfigurable optics with drastically improved compactness, ruggedness, manufacturability and functionality compared to their traditional bulk counterparts. Optical phase-change materials (PCMs) offer an appealing material solution for active metasurface devices with their large index contrast and non-volatile switching characteristics. Here we report a large-scale, electrically reconfigurable non-volatile metasurface platform based on optical PCMs. The optical PCM alloy used in the devices, Ge2Sb2Se4Te (GSST), uniquely combines giant non-volatile index modulation capability, broadband low optical loss and a large reversible switching volume, enabling notably enhanced light–matter interactions within the active optical PCM medium. Capitalizing on these favourable attributes, we demonstrated quasi-continuously tuneable active metasurfaces with record half-octave spectral tuning range and large optical contrast of over 400%. We further prototyped a polarization-insensitive phase-gradient metasurface to realize dynamic optical beam steering. An electrically reconfigurable optical metasurface using a Ge2Sb2Se4Te phase change material shows half an octave spectral tuning and promising performances for optical beam steering applications.

Journal ArticleDOI
TL;DR: An all-solid-state, electrically tunable and reflective metasurface array that can generate a specific phase or a continuous sweep between 0 and 360° at an estimated rate of 5.4 MHz while independently adjusting the amplitude.
Abstract: Spatial light modulators are essential optical elements in applications that require the ability to regulate the amplitude, phase and polarization of light, such as digital holography, optical communications and biomedical imaging. With the push towards miniaturization of optical components, static metasurfaces are used as competent alternatives. These evolved to active metasurfaces in which light-wavefront manipulation can be done in a time-dependent fashion. The active metasurfaces reported so far, however, still show incomplete phase modulation (below 360°). Here we present an all-solid-state, electrically tunable and reflective metasurface array that can generate a specific phase or a continuous sweep between 0 and 360° at an estimated rate of 5.4 MHz while independently adjusting the amplitude. The metasurface features 550 individually addressable nanoresonators in a 250 × 250 μm2 area with no micromechanical elements or liquid crystals. A key feature of our design is the presence of two independent control parameters (top and bottom gate voltages) in each nanoresonator, which are used to adjust the real and imaginary parts of the reflection coefficient independently. To demonstrate this array’s use in light detection and ranging, we performed a three-dimensional depth scan of an emulated street scene that consisted of a model car and a human figure up to a distance of 4.7 m. By controlling two voltage gates separately from one another, a spatial light modulator has been made that can continuously vary the phase of 360 degrees while independently adjusting the amplitude.

Journal ArticleDOI
TL;DR: In this article, the authors demonstrate the epitaxial growth of 2'inch (50'mm) monolayer molybdenum disulfide (MoS2) single crystals on a C-plane sapphire.
Abstract: Two-dimensional (2D) semiconductors, in particular transition metal dichalcogenides (TMDCs), have attracted great interest in extending Moore’s law beyond silicon1–3. However, despite extensive efforts4–25, the growth of wafer-scale TMDC single crystals on scalable and industry-compatible substrates has not been well demonstrated. Here we demonstrate the epitaxial growth of 2 inch (~50 mm) monolayer molybdenum disulfide (MoS2) single crystals on a C-plane sapphire. We designed the miscut orientation towards the A axis (C/A) of sapphire, which is perpendicular to the standard substrates. Although the change of miscut orientation does not affect the epitaxial relationship, the resulting step edges break the degeneracy of nucleation energy for the antiparallel MoS2 domains and lead to more than a 99% unidirectional alignment. A set of microscopies, spectroscopies and electrical measurements consistently showed that the MoS2 is single crystalline and has an excellent wafer-scale uniformity. We fabricated field-effect transistors and obtained a mobility of 102.6 cm2 V−1 s−1 and a saturation current of 450 μA μm–1, which are among the highest for monolayer MoS2. A statistical analysis of 160 field-effect transistors over a centimetre scale showed a >94% device yield and a 15% variation in mobility. We further demonstrated the single-crystalline MoSe2 on C/A sapphire. Our method offers a general and scalable route to produce TMDC single crystals towards future electronics. Unidirectional alignment of MoS2 domains during epitaxial growth on C/A sapphire enables the realization of large-area MoS2 single crystals.

Journal ArticleDOI
TL;DR: In this article, the key advances in nanocatalysts that have led to the impressive electrochemical conversion of CO2 to useful products and provides benchmarks that others can use to compare their results.
Abstract: Electrochemical conversion of CO2 to useful products at temperatures below 100 °C is nearing the commercial scale. Pilot units for CO2 conversion to CO are already being tested. Units to convert CO2 to formic acid are projected to reach pilot scale in the next year. Further, several investigators are starting to observe industrially relevant rates of the electrochemical conversion of CO2 to ethanol and ethylene, with the hydrogen needed coming from water. In each case, Faradaic efficiencies of 80% or more and current densities above 200 mA cm−2 can be reproducibly achieved. Here we describe the key advances in nanocatalysts that lead to the impressive performance, indicate where additional work is needed and provide benchmarks that others can use to compare their results. This Perspective describes the key advances in nanocatalysts that have led to the impressive electrochemical conversion of CO2 to useful products and provides benchmarks that others can use to compare their results.

Journal ArticleDOI
TL;DR: In this article, the authors place nanoplastics in the context of global plastic pollution by assessing its sources and risks, and by assessing commonalities nanoparticles may share with other nanosized objects in environmental systems, such as engineered nanomaterials and natural colloids.
Abstract: Numerous studies have made the ubiquitous presence of plastic in the environment undeniable, and thus it no longer comes as a surprise when scientists measure the accumulation of macroplastic litter and microplastic fragments in both urban and remote sites. Nanoplastics have recently emerged in the discussions of scientists, regulators and the public, as the weathering of macroplastics may lead to a substantial burden of nanoplastics in various ecosystems. While nanoplastics particles themselves have not (yet) been extensively measured in the environment, there is increased concern that this size fraction of plastic may be more extensively distributed and hazardous that larger-sized particles. This assessment may emanate from an unease with the term 'nano', which may elicit a negative response over uncertainties of the pervasiveness of nanoplastics specifically, or from the lessons learned by many years of intensive environmental health and safety research of engineered nanomaterials. Ultimately, the different physical and chemical characteristics of the different size classes of plastic pollution (macroplastics, microplastics and nanoplastics) will result in divergent fate and hazards. As nanoscientists specializing in understanding the fate, transport and interactions of nanoparticles in human and environmental systems, in this Perspective, we try to place nanoplastics in the context of global plastic pollution by assessing its sources and risks, and by assessing commonalities nanoplastics may share with other nanosized objects in environmental systems, such as engineered nanomaterials and natural colloids.

Posted ContentDOI
TL;DR: In this paper, a general approach combining wet-chemistry impregnation and two-step annealing is devised for the scalable synthesis of a library of ultra-high-density single-atom catalysts with drastically enhanced reactivity.
Abstract: The stabilization of transition metals as isolated centres with high areal density on suitably tailored carriers is crucial for maximizing the industrial potential of single-atom heterogeneous catalysts. However, achieving single-atom dispersions at metal contents above 2 wt% remains challenging. Here we introduce a versatile approach combining impregnation and two-step annealing to synthesize ultra-high-density single-atom catalysts with metal contents up to 23 wt% for 15 metals on chemically distinct carriers. Translation to a standardized, automated protocol demonstrates the robustness of our method and provides a path to explore virtually unlimited libraries of mono- or multimetallic catalysts. At the molecular level, characterization of the synthesis mechanism through experiments and simulations shows that controlling the bonding of metal precursors with the carrier via stepwise ligand removal prevents their thermally induced aggregation into nanoparticles. The drastically enhanced reactivity with increasing metal content exemplifies the need to optimize the surface metal density for a given application. Moreover, the loading-dependent site-specific activity observed in three distinct catalytic systems reflects the well-known complexity in heterogeneous catalyst design, which now can be tackled with a library of single-atom catalysts with widely tunable metal loadings. A general versatile approach combining wet-chemistry impregnation and two-step annealing is devised for the scalable synthesis of a library of ultra-high-density single-atom catalysts with drastically enhanced reactivity.

Journal ArticleDOI
TL;DR: In this paper, the authors provide an overview of recent progress in 2D spintronics and opto-spintronics using van der Waals heterostructures and highlight the unique spin-related phenomena arising from spin-orbit and magnetic proximity effects.
Abstract: The large variety of 2D materials and their co-integration in van der Waals heterostructures enable innovative device engineering. In addition, their atomically thin nature promotes the design of artificial materials by proximity effects that originate from short-range interactions. Such a designer approach is particularly compelling for spintronics, which typically harnesses functionalities from thin layers of magnetic and non-magnetic materials and the interfaces between them. Here we provide an overview of recent progress in 2D spintronics and opto-spintronics using van der Waals heterostructures. After an introduction to the forefront of spin transport research, we highlight the unique spin-related phenomena arising from spin–orbit and magnetic proximity effects. We further describe the ability to create multifunctional hybrid heterostructures based on van der Waals materials, combining spin, valley and excitonic degrees of freedom. We end with an outlook on perspectives and challenges for the design and production of ultracompact all-2D spin devices and their potential applications in conventional and quantum technologies. The preparation of a diverse set of 2D materials and their co-integration in van der Waals heterostructures enable innovative material design and device engineering. This Review summarizes recent advances in 2D spintronics and opto-spintronics, the underlying physical concepts and future perspectives of the field.

Journal ArticleDOI
TL;DR: This Review summarizes how distinct approaches to nanostructural engineering enhance features that determine the selectivity and stability of catalysts and highlights breakthroughs towards their commercialization.
Abstract: Nanostructured materials of diverse architecture are ubiquitous in industrial catalysis. They offer exciting prospects to tackle various sustainability challenges faced by society. Since the introduction of the concept a century ago, researchers aspire to control the chemical identity, local environment and electronic properties of active sites on catalytic surfaces to optimize their reactivity in given applications. Nowadays, numerous strategies exist to tailor these characteristics with varying levels of atomic precision. Making headway relies upon the existence of analytical approaches able to resolve relevant structural features and remains challenging due to the inherent complexity even of the simplest heterogeneous catalysts, and to dynamic effects often occurring under reaction conditions. Computational methods play a complementary and ever-increasing role in pushing forward the design. Here, we examine how nanoscale engineering can enhance the selectivity and stability of catalysts. We highlight breakthroughs towards their commercialization and identify directions to guide future research and innovation. This Review summarizes how distinct approaches to nanostructural engineering enhance features that determine the selectivity and stability of catalysts.

Journal ArticleDOI
TL;DR: In this article, light-sensitive iron oxide nanoparticles embedded in biocompatible electrospun nanofibres induce membrane permeabilization by photothermal effects without direct cellular contact with the nanoparticles.
Abstract: Nanoparticle-sensitized photoporation is an upcoming approach for the intracellular delivery of biologics, combining high efficiency and throughput with excellent cell viability. However, as it relies on close contact between nanoparticles and cells, its translation towards clinical applications is hampered by safety and regulatory concerns. Here we show that light-sensitive iron oxide nanoparticles embedded in biocompatible electrospun nanofibres induce membrane permeabilization by photothermal effects without direct cellular contact with the nanoparticles. The photothermal nanofibres have been successfully used to deliver effector molecules, including CRISPR-Cas9 ribonucleoprotein complexes and short interfering RNA, to adherent and suspension cells, including embryonic stem cells and hard-to-transfect T cells, without affecting cell proliferation or phenotype. In vivo experiments furthermore demonstrated successful tumour regression in mice treated with chimeric antibody receptor T cells in which the expression of programmed cell death protein 1 (PD1) is downregulated after nanofibre photoporation with short interfering RNA to PD1. In conclusion, cell membrane permeabilization with photothermal nanofibres is a promising concept towards the safe and more efficient production of engineered cells for therapeutic applications, including stem cell or adoptive T cell therapy.

Journal ArticleDOI
TL;DR: In this article, a prototype of cancer metalloimmunotherapy using cyclic dinucleotide (CDN) stimulator of interferon genes (STING) agonists and Mn2+ was demonstrated.
Abstract: Nutritional metal ions play critical roles in many important immune processes. Hence, the effective modulation of metal ions may open up new forms of immunotherapy, termed as metalloimmunotherapy. Here, we demonstrate a prototype of cancer metalloimmunotherapy using cyclic dinucleotide (CDN) stimulator of interferon genes (STING) agonists and Mn2+. We screened various metal ions and discovered specific metal ions augmented STING agonist activity, wherein Mn2+ promoted a 12- to 77-fold potentiation effect across the prevalent human STING haplotypes. Notably, Mn2+ coordinated with CDN STING agonists to self-assemble into a nanoparticle (CDN–Mn2+ particle, CMP) that effectively delivered STING agonists to immune cells. The CMP, administered either by local intratumoural or systemic intravenous injection, initiated robust anti-tumour immunity, achieving remarkable therapeutic efficacy with minute doses of STING agonists in multiple murine tumour models. Overall, the CMP offers a new platform for local and systemic cancer treatments, and this work underscores the great potential of coordination nanomedicine for metalloimmunotherapy. The stimulation of interferon genes (STING) pathway with STING agonists such as cyclic dinucleotides (CDNs) has emerged as a promising immunotherapeutic approach. Here, the authors show that Mn2+ can amplify the STING-promoted anti-tumour immune response in challenging murine tumour models by coordinating with CDNs and self-assembling into nanoparticles that can be delivered locally and systemically.

Journal ArticleDOI
TL;DR: In this paper, the authors proposed a phase-change antenna and metasurface that offers strong, reversible, non-volatile, multi-phase switching and spectral tuning of light scattering in the visible and near-infrared spectral ranges.
Abstract: The success of semiconductor electronics is built on the creation of compact, low-power switching elements that offer routing, logic and memory functions. The availability of nanoscale optical switches could have a similarly transformative impact on the development of dynamic and programmable metasurfaces, optical neural networks and quantum information processing. Phase-change materials are uniquely suited to enable their creation as they offer high-speed electrical switching between amorphous and crystalline states with notably different optical properties. Their high refractive index has already been harnessed to fashion them into compact optical antennas. Here, we take the next important step, by showing electrically-switchable phase-change antennas and metasurfaces that offer strong, reversible, non-volatile, multi-phase switching and spectral tuning of light scattering in the visible and near-infrared spectral ranges. Their successful implementation relies on a careful joint thermal and optical optimization of the antenna elements that comprise a silver strip that simultaneously serves as a plasmonic resonator and a miniature heating stage. Our metasurface affords electrical modulation of the reflectance by more than fourfold at 755 nm. A metasurface comprising electrically controlled heating units and a phase-change material offer non-volatile and reversible modulation of reflectance by more than fourfold.

Journal ArticleDOI
TL;DR: In this article, the potential applications of nanotechnology-based treatments for infectious diseases, with a specific focus on the progress and challenges in developing nanomedicines against HIV, tuberculosis and malaria.
Abstract: Infectious diseases are a major driver of morbidity and mortality globally. Treatment of malaria, tuberculosis and human immunodeficiency virus infection are particularly challenging, as indicated by the ongoing transmission and high mortality associated with these diseases. The formulation of new and existing drugs in nano-sized carriers promises to overcome several challenges associated with the treatment of these diseases, including low on-target bioavailability, sub-therapeutic drug accumulation in microbial sanctuaries and reservoirs, and low patient adherence due to drug-related toxicities and extended therapeutic regimens. Further, nanocarriers can be used for formulating vaccines, which represent a major weapon in our fight against infectious diseases. Here we review the current burden of infectious diseases with a focus on major drivers of morbidity and mortality. We then highlight how nanotechnology could aid in improving existing treatment modalities. We summarize our progress so far and outline potential future directions to maximize the impact of nanotechnology on the global population. This Review outlines the potential applications of nanotechnology-based treatments for infectious diseases, with a specific focus on the progress and challenges in developing nanomedicines against HIV, tuberculosis and malaria.

Journal ArticleDOI
TL;DR: In this article, an overview of nanomaterials that have been used to overcome clinical barriers to T-cell-based immunotherapies and provide an outlook of this emerging field at the interface of cancer immunotherapy and Nanomaterial design.
Abstract: T-cell-based immunotherapies hold promise for the treatment of many types of cancer, with three approved products for B-cell malignancies and a large pipeline of treatments in clinical trials. However, there are several challenges to their broad implementation. These include insufficient expansion of adoptively transferred T cells, inefficient trafficking of T cells into solid tumours, decreased T-cell activity due to a hostile tumour microenvironment and the loss of target antigen expression. Together, these factors restrict the number of therapeutically active T cells engaging with tumours. Nanomaterials are uniquely suited to overcome these challenges, as they can be rationally designed to enhance T-cell expansion, navigate complex physical barriers and modulate tumour microenvironments. Here, we present an overview of nanomaterials that have been used to overcome clinical barriers to T-cell-based immunotherapies and provide our outlook of this emerging field at the interface of cancer immunotherapy and nanomaterial design. This Review discusses the progress and the remaining challenges for the clinical application of nanomaterial-based T-cell immunotherapies.

Journal ArticleDOI
TL;DR: In this article, the authors examine how novel nanophotonic platforms could overcome the hardware restrictions of existing LiDAR technologies and present the device specifications required by the industrial sector.
Abstract: Light detection and ranging (LiDAR) technology, a laser-based imaging technique for accurate distance measurement, is considered one of the most crucial sensor technologies for autonomous vehicles, artificially intelligent robots and unmanned aerial vehicle reconnaissance. Until recently, LiDAR has relied on light sources and detectors mounted on multiple mechanically rotating optical transmitters and receivers to cover an entire scene. Such an architecture gives rise to limitations in terms of the imaging frame rate and resolution. In this Review, we examine how novel nanophotonic platforms could overcome the hardware restrictions of existing LiDAR technologies. After briefly introducing the basic principles of LiDAR, we present the device specifications required by the industrial sector. We then review a variety of LiDAR-relevant nanophotonic approaches such as integrated photonic circuits, optical phased antenna arrays and flat optical devices based on metasurfaces. The latter have already demonstrated exceptional functional beam manipulation properties, such as active beam deflection, point-cloud generation and device integration using scalable manufacturing methods, and are expected to disrupt modern optical technologies. In the outlook, we address the upcoming physics and engineering challenges that must be overcome from the viewpoint of incorporating nanophotonic technologies into commercially viable, fast, ultrathin and lightweight LiDAR systems.

Journal ArticleDOI
TL;DR: It is shown that SiO 2 NPs, as well as soluble Si(OH) 4, can induce systemic acquired resistance in a dose-dependent manner, which involves the defence hormone salicylic acid, and specifically designed silica nanoparticles have the potential to serve as an inexpensive, highly efficient, safe and tracelessly degradable alternative for pesticides.
Abstract: In plants, pathogen attack can induce an immune response known as systemic acquired resistance that protects against a broad spectrum of pathogens. In the search for safer agrochemicals, silica nanoparticles (SiO2 NPs; food additive E551) have recently been proposed as a new tool. However, initial results are controversial, and the molecular mechanisms of SiO2 NP-induced disease resistance are unknown. Here we show that SiO2 NPs, as well as soluble Si(OH)4, can induce systemic acquired resistance in a dose-dependent manner, which involves the defence hormone salicylic acid. Nanoparticle uptake and action occurred exclusively through the stomata (leaf pores facilitating gas exchange) and involved extracellular adsorption in the air spaces in the spongy mesophyll of the leaf. In contrast to the treatment with SiO2 NPs, the induction of systemic acquired resistance by Si(OH)4 was problematic since high Si(OH)4 concentrations caused stress. We conclude that SiO2 NPs have the potential to serve as an inexpensive, highly efficient, safe and sustainable alternative for plant disease protection. New mechanistic insights into nanoparticle–plant interactions show that specifically designed silica nanoparticles have the potential to serve as an inexpensive, highly efficient, safe and tracelessly degradable alternative for pesticides.

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TL;DR: This Review will discuss aspects along with recent nanomaterial advances towards vaccines against infectious disease, with a particular emphasis on HIV/AIDS, malaria and tuberculosis, which are not yet treatable with vaccination.
Abstract: Despite the overwhelming success of vaccines in preventing infectious diseases, there remain numerous globally devastating diseases without fully protective vaccines, particularly human immunodeficiency virus (HIV), malaria and tuberculosis. Nanotechnology approaches are being developed both to design new vaccines against these diseases as well as to facilitate their global implementation. The reasons why a given pathogen may present difficulties for vaccine design are unique and tied to the co-evolutionary history of the pathogen and humans, but there are common challenges that nanotechnology is beginning to help address. In each case, a successful vaccine will need to raise immune responses that differ from the immune responses raised by normal infection. Nanomaterials, with their defined compositions, commonly modular construction, and length scales allowing the engagement of key immune pathways, collectively facilitate the iterative design process necessary to identify such protective immune responses and achieve them reliably. Nanomaterials also provide strategies for engineering the trafficking and delivery of vaccine components to key immune cells and lymphoid tissues, and they can be highly multivalent, improving their engagement with the immune system. This Review will discuss these aspects along with recent nanomaterial advances towards vaccines against infectious disease, with a particular emphasis on HIV/AIDS, malaria and tuberculosis. Several globally significant infectious diseases are not yet treatable with vaccination; nanomaterials are being investigated to provide new strategies for vaccine development.

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TL;DR: In this article, the authors used synchrotron-based X-ray diffraction and pair distribution function analysis to identify and differentiate two elusive components, LiH and LiF, in the SEI of lithium metal anodes.
Abstract: A comprehensive understanding of the solid–electrolyte interphase (SEI) composition is crucial to developing high-energy batteries based on lithium metal anodes. A particularly contentious issue concerns the presence of LiH in the SEI. Here we report on the use of synchrotron-based X-ray diffraction and pair distribution function analysis to identify and differentiate two elusive components, LiH and LiF, in the SEI of lithium metal anodes. LiH is identified as a component of the SEI in high abundance, and the possibility of its misidentification as LiF in the literature is discussed. LiF in the SEI is found to have different structural features from LiF in the bulk phase, including a larger lattice parameter and a smaller grain size (<3 nm). These characteristics favour Li+ transport and explain why an ionic insulator, like LiF, has been found to be a favoured component for the SEI. Finally, pair distribution function analysis reveals key amorphous components in the SEI. X-ray diffraction and Rietveld refinement analysis confirm the presence of LiH in the solid–electrolyte interphase of lithium metal anodes.

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TL;DR: These powerful tools reveal that the curvature of the cobalt oxide layers occurring near the surface dictates the structural stability of the material at high potentials and, in turn, the electrochemical performances of curved layered cathode materials.
Abstract: Layered lithium cobalt oxide (LiCoO2, LCO) is the most successful commercial cathode material in lithium-ion batteries. However, its notable structural instability at potentials higher than 4.35 V (versus Li/Li+) constitutes the major barrier to accessing its theoretical capacity of 274 mAh g−1. Although a few high-voltage LCO (H-LCO) materials have been discovered and commercialized, the structural origin of their stability has remained difficult to identify. Here, using a three-dimensional continuous rotation electron diffraction method assisted by auxiliary high-resolution transmission electron microscopy, we investigate the structural differences at the atomistic level between two commercial LCO materials: a normal LCO (N-LCO) and a H-LCO. These powerful tools reveal that the curvature of the cobalt oxide layers occurring near the surface dictates the structural stability of the material at high potentials and, in turn, the electrochemical performances. Backed up by theoretical calculations, this atomistic understanding of the structure–performance relationship for layered LCO materials provides useful guidelines for future design of new cathode materials with superior structural stability at high voltages. A three-dimensional continuous rotation electron diffraction method allows atomistic characterization of the chemistry of curved layered cathode materials.

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TL;DR: In this paper, a heterogeneous moisture-enabled electric generator (HMEG) based on a bilayer of polyelectrolyte films was developed, and a sequentially aligned stacking strategy was created for large-scale integration of HMEG units, to offer a voltage of more than 1,000
Abstract: Environmentally adaptive power generation is attractive for the development of next-generation energy sources. Here we develop a heterogeneous moisture-enabled electric generator (HMEG) based on a bilayer of polyelectrolyte films. Through the spontaneous adsorption of water molecules in air and induced diffusion of oppositely charged ions, one single HMEG unit can produce a high voltage of ~0.95 V at low (25%) relative humidity (RH), and even jump to 1.38 V at 85% RH. A sequentially aligned stacking strategy is created for large-scale integration of HMEG units, to offer a voltage of more than 1,000 V under ambient conditions (25% RH, 25 °C). Using origami assembly, a small section of folded HMEGs renders an output of up to 43 V cm−3. Such integration devices supply sufficient power to illuminate a lamp bulb of 10 W, to drive a dynamic electronic ink screen and to control the gate voltage for a self-powered field effect transistor. A power generator exhibits enhanced output due to a dual-charge-carrier design. The voltage produced is constant yet competitive even under low relative humidity.

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TL;DR: In this article, the authors describe the transport, transformation and bioavailability of MoS2 nanomaterials through a combination of in vivo experiments and molecular dynamics simulations, and show that after intravenous injection molybdenum is significantly enriched in liver sinusoid and splenic red pulp.
Abstract: Many nanoscale biomaterials fail to reach the clinical trial stage due to a poor understanding of the fundamental principles of their in vivo behaviour. Here we describe the transport, transformation and bioavailability of MoS2 nanomaterials through a combination of in vivo experiments and molecular dynamics simulations. We show that after intravenous injection molybdenum is significantly enriched in liver sinusoid and splenic red pulp. This biodistribution is mediated by protein coronas that spontaneously form in the blood, principally with apolipoprotein E. The biotransformation of MoS2 leads to incorporation of molybdenum into molybdenum enzymes, which increases their specific activities in the liver, affecting its metabolism. Our findings reveal that nanomaterials undergo a protein corona-bridged transport–transformation–bioavailability chain in vivo, and suggest that nanomaterials consisting of essential trace elements may be converted into active biological molecules that organisms can exploit. Our results also indicate that the long-term biotransformation of nanomaterials may have an impact on liver metabolism. Understanding the in vivo biotransformation of nanomaterials used for biomedical applications might shed light on their long-term effects and safety. Here the authors show that molybdenum derived from nanomaterials is mainly transported in the liver, in a corona-mediated process, and is incorporated in molybdoenzymes, with an effect on liver metabolism.