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1.
Proc Natl Acad Sci U S A ; 118(9)2021 03 02.
Artigo em Inglês | MEDLINE | ID: mdl-33619098

RESUMO

Acetogenic bacteria use cellular redox energy to convert CO2 to acetate using the Wood-Ljungdahl (WL) pathway. Such redox energy can be derived from electrons generated from H2 as well as from inorganic materials, such as photoresponsive semiconductors. We have developed a nanoparticle-microbe hybrid system in which chemically synthesized cadmium sulfide nanoparticles (CdS-NPs) are displayed on the cell surface of the industrial acetogen Clostridium autoethanogenum The hybrid system converts CO2 into acetate without the need for additional energy sources, such as H2, and uses only light-induced electrons from CdS-NPs. To elucidate the underlying mechanism by which C. autoethanogenum uses electrons generated from external energy sources to reduce CO2, we performed transcriptional analysis. Our results indicate that genes encoding the metal ion or flavin-binding proteins were highly up-regulated under CdS-driven autotrophic conditions along with the activation of genes associated with the WL pathway and energy conservation system. Furthermore, the addition of these cofactors increased the CO2 fixation rate under light-exposure conditions. Our results demonstrate the potential to improve the efficiency of artificial photosynthesis systems based on acetogenic bacteria integrated with photoresponsive nanoparticles.


Assuntos
Acetatos/química , Proteínas de Bactérias/metabolismo , Compostos de Cádmio/química , Dióxido de Carbono/química , Clostridium/metabolismo , Elétrons , Nanopartículas/química , Sulfetos/química , Acetatos/metabolismo , Processos Autotróficos , Proteínas de Bactérias/química , Proteínas de Bactérias/genética , Compostos de Cádmio/metabolismo , Dióxido de Carbono/metabolismo , Clostridium/genética , Clostridium/efeitos da radiação , Coenzimas/química , Coenzimas/metabolismo , Dinitrocresóis/química , Dinitrocresóis/metabolismo , Metabolismo Energético/genética , Regulação Bacteriana da Expressão Gênica , Luz , NAD/química , NAD/metabolismo , NADP/química , NADP/metabolismo , Nanopartículas/metabolismo , Fotossíntese/genética , Sulfetos/metabolismo , Transcrição Gênica
2.
Proc Natl Acad Sci U S A ; 117(13): 7516-7523, 2020 03 31.
Artigo em Inglês | MEDLINE | ID: mdl-32170009

RESUMO

Among CO2-fixing metabolic pathways in nature, the linear Wood-Ljungdahl pathway (WLP) in phylogenetically diverse acetate-forming acetogens comprises the most energetically efficient pathway, requires the least number of reactions, and converts CO2 to formate and then into acetyl-CoA. Despite two genes encoding glycine synthase being well-conserved in WLP gene clusters, the functional role of glycine synthase under autotrophic growth conditions has remained uncertain. Here, using the reconstructed genome-scale metabolic model iSL771 based on the completed genome sequence, transcriptomics, 13C isotope-based metabolite-tracing experiments, biochemical assays, and heterologous expression of the pathway in another acetogen, we discovered that the WLP and the glycine synthase pathway are functionally interconnected to fix CO2, subsequently converting CO2 into acetyl-CoA, acetyl-phosphate, and serine. Moreover, the functional cooperation of the pathways enhances CO2 consumption and cellular growth rates via bypassing reducing power required reactions for cellular metabolism during autotrophic growth of acetogens.


Assuntos
Aminoácido Oxirredutases/metabolismo , Aminometiltransferase/metabolismo , Processos Autotróficos/fisiologia , Complexos Multienzimáticos/metabolismo , Acetilcoenzima A/metabolismo , Aminoácido Oxirredutases/genética , Aminometiltransferase/genética , Proteínas de Bactérias/metabolismo , Ciclo do Carbono , Dióxido de Carbono/metabolismo , Monóxido de Carbono/metabolismo , Clostridium/metabolismo , Redes e Vias Metabólicas , Complexos Multienzimáticos/genética , Família Multigênica , Óxido Nítrico Sintase/genética , Óxido Nítrico Sintase/metabolismo
3.
RNA ; 24(12): 1839-1855, 2018 12.
Artigo em Inglês | MEDLINE | ID: mdl-30249742

RESUMO

Acetogens synthesize acetyl-CoA via CO2 or CO fixation, producing organic compounds. Despite their ecological and industrial importance, their transcriptional and post-transcriptional regulation has not been systematically studied. With completion of the genome sequence of Acetobacterium bakii (4.28-Mb), we measured changes in the transcriptome of this psychrotolerant acetogen in response to temperature variations under autotrophic and heterotrophic growth conditions. Unexpectedly, acetogenesis genes were highly up-regulated at low temperatures under heterotrophic, as well as autotrophic, growth conditions. To mechanistically understand the transcriptional regulation of acetogenesis genes via changes in RNA secondary structures of 5'-untranslated regions (5'-UTR), the primary transcriptome was experimentally determined, and 1379 transcription start sites (TSS) and 1100 5'-UTR were found. Interestingly, acetogenesis genes contained longer 5'-UTR with lower RNA-folding free energy than other genes, revealing that the 5'-UTRs control the RNA abundance of the acetogenesis genes under low temperature conditions. Our findings suggest that post-transcriptional regulation via RNA conformational changes of 5'-UTRs is necessary for cold-adaptive acetogenesis.


Assuntos
Acetobacterium/fisiologia , Adaptação Fisiológica/genética , Conformação de Ácido Nucleico , Transcriptoma/genética , Regiões 5' não Traduzidas/genética , Acetobacterium/genética , Temperatura Baixa , Regulação da Expressão Gênica/genética , Genoma Bacteriano/genética , Genoma Bacteriano/fisiologia , Análise de Sequência de DNA
4.
BMC Genomics ; 19(1): 837, 2018 Nov 23.
Artigo em Inglês | MEDLINE | ID: mdl-30470174

RESUMO

BACKGROUND: Acetogenic bacteria constitute promising biocatalysts for the conversion of CO2/H2 or synthesis gas (H2/CO/CO2) into biofuels and value-added biochemicals. These microorganisms are naturally capable of autotrophic growth via unique acetogenesis metabolism. Despite their biosynthetic potential for commercial applications, a systemic understanding of the transcriptional and translational regulation of the acetogenesis metabolism remains unclear. RESULTS: By integrating genome-scale transcriptomic and translatomic data, we explored the regulatory logic of the acetogenesis to convert CO2 into biomass and metabolites in Eubacterium limosum. The results indicate that majority of genes associated with autotrophic growth including the Wood-Ljungdahl pathway, the reduction of electron carriers, the energy conservation system, and gluconeogenesis were transcriptionally upregulated. The translation efficiency of genes in cellular respiration and electron bifurcation was also highly enhanced. In contrast, the transcriptionally abundant genes involved in the carbonyl branch of the Wood-Ljungdahl pathway, as well as the ion-translocating complex and ATP synthase complex in the energy conservation system, showed decreased translation efficiency. The translation efficiencies of genes were regulated by 5'UTR secondary structure under the autotrophic growth condition. CONCLUSIONS: The results illustrated that the acetogenic bacteria reallocate protein synthesis, focusing more on the translation of genes for the generation of reduced electron carriers via electron bifurcation, rather than on those for carbon metabolism under autotrophic growth.


Assuntos
Acetatos/metabolismo , Proteínas de Bactérias/genética , Eubacterium/crescimento & desenvolvimento , Fermentação , Regulação Bacteriana da Expressão Gênica , Processos Autotróficos , Biocombustíveis , Ciclo do Carbono , Metabolismo Energético , Eubacterium/genética , Eubacterium/metabolismo , Gases/análise , Genoma Bacteriano , Transcriptoma
5.
Nano Lett ; 13(9): 4362-8, 2013 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-23919596

RESUMO

An electroassisted method is developed to transfer silicon (Si) wire arrays from the Si wafers on which they are grown to other substrates while maintaining their original properties and vertical alignment. First, electroassisted etching is used to form a sacrificial porous Si layer underneath the Si wires. Second, the porous Si layer is separated from the Si wafer by electropolishing, enabling the separation and transfer of the Si wires. The method is further expanded to develop a current-induced metal-assisted chemical etching technique for the facile and rapid synthesis of Si nanowires with axially modulated porosity.


Assuntos
Nanotecnologia , Nanofios/química , Silício/química , Cristalização , Eletrônica , Porosidade , Propriedades de Superfície
6.
Nat Commun ; 15(1): 4443, 2024 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-38789512

RESUMO

Transparent radiative cooling holds the promise to efficiently manage thermal conditions in various electronic devices without additional energy consumption. Radiative cooling cover windows designed for foldable and flexible displays could enhance cooling capacities in the ubiquitous deployment of flexible electronics in outdoor environments. However, previous demonstrations have not met the optical, mechanical, and moisture-impermeable criteria for such cover windows. Herein, we report transparent radiative cooling metamaterials with a thickness of 50 microns as a cover window of foldable and flexible displays by rational design and synthesis of embedding optically-modulating microstructures in clear polyimide. The resulting outcome not only includes excellent light emission in the atmospheric window under the secured optical transparency but also provides enhanced mechanical and moisture-impermeable properties to surpass the demands of target applications. Our metamaterials not only substantially mitigate the temperature rise in heat-generating devices exposed to solar irradiance but also enhance the thermal management of devices in dark conditions. The light output performance of light-emitting diodes in displays on which the metamaterials are deployed is greatly enhanced by suppressing the performance deterioration associated with thermalization.

7.
ACS Sens ; 9(2): 662-673, 2024 02 23.
Artigo em Inglês | MEDLINE | ID: mdl-38300847

RESUMO

Self-healing hydrogels are in high demand for wearable sensing applications due to their remarkable deformability, high ionic and electrical conductivity, self-adhesiveness to human skin, as well as resilience to both mechanical and electrical damage. However, these hydrogels face challenges such as delayed healing times and unavoidable electrical hysteresis, which limit their practical effectiveness. Here, we introduce a self-healing hydrogel that exhibits exceptionally rapid healing with a recovery time of less than 0.12 s and an ultralow electrical hysteresis of less than 0.64% under cyclic strains of up to 500%. This hydrogel strikes an ideal balance, without notable trade-offs, between properties such as softness, deformability, ionic and electrical conductivity, self-adhesiveness, response and recovery times, durability, overshoot behavior, and resistance to nonaxial deformations such as twisting, bending, and pressing. Owing to this unique combination of features, the hydrogel is highly suitable for long-term, durable use in wearable sensing applications, including monitoring body movements and electrophysiological activities on the skin.


Assuntos
Hidrogéis , Dispositivos Eletrônicos Vestíveis , Humanos , Eletricidade , Condutividade Elétrica , Movimento
8.
PNAS Nexus ; 3(5): pgae156, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38715730

RESUMO

The increasing need for precise dietary monitoring across various health scenarios has led to innovations in wearable sensing technologies. However, continuously tracking food and fluid intake during daily activities can be complex. In this study, we present a machine-learning-powered smart neckband that features wireless connectivity and a comfortable, foldable design. Initially considered beneficial for managing conditions such as diabetes and obesity by facilitating dietary control, the device's utility extends beyond these applications. It has proved to be valuable for sports enthusiasts, individuals focused on diet control, and general health monitoring. Its wireless connectivity, ergonomic design, and advanced classification capabilities offer a promising solution for overcoming the limitations of traditional dietary tracking methods, highlighting its potential in personalized healthcare and wellness strategies.

9.
ACS Appl Mater Interfaces ; 16(20): 26613-26623, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38728055

RESUMO

Strain gauges, particularly for wearable sensing applications, require a high degree of stretchability, softness, sensitivity, selectivity, and linearity. They must also steer clear of challenges such as mechanical and electrical hysteresis, overshoot behavior, and slow response/recovery times. However, current strain gauges face challenges in satisfying all of these requirements at once due to the inevitable trade-offs between these properties. Here, we present an innovative method for creating strain gauges from spongy Ag foam through a steam-etching process. This method simplifies the traditional, more complex, and costly manufacturing techniques, presenting an eco-friendly alternative. Uniquely, the strain gauges crafted from this method achieve an unparalleled gauge factor greater than 8 × 103 at strains exceeding 100%, successfully meeting all required attributes without notable trade-offs. Our work includes systematic investigations that reveal the intricate structure-property-performance relationship of the spongy Ag foam with practical demonstrations in areas such as human motion monitoring and human-robot interaction. These breakthroughs pave the way for highly sensitive and selective strain gauges, showing immediate applicability across a wide range of wearable sensing applications.

10.
Proc Natl Acad Sci U S A ; 107(22): 9950-5, 2010 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-20479263

RESUMO

The fabrication of nanowire (NW) devices on diverse substrates is necessary for applications such as flexible electronics, conformable sensors, and transparent solar cells. Although NWs have been fabricated on plastic and glass by lithographic methods, the choice of device substrates is severely limited by the lithographic process temperature and substrate properties. Here we report three new transfer-printing methods for fabricating NW devices on diverse substrates including polydimethylsiloxane, Petri dishes, Kapton tapes, thermal release tapes, and many types of adhesive tapes. These transfer-printing methods rely on the differences in adhesion to transfer NWs, metal films, and devices from weakly adhesive donor substrates to more strongly adhesive receiver substrates. Electrical characterization of fabricated NW devices shows that reliable ohmic contacts are formed between NWs and electrodes. Moreover, we demonstrated that Si NW devices fabricated by the transfer-printing methods are robust piezoresistive stress sensors and temperature sensors with reliable performance.

11.
Nano Lett ; 12(6): 3339-43, 2012 Jun 13.
Artigo em Inglês | MEDLINE | ID: mdl-22594496

RESUMO

Vertical silicon nanowire (SiNW) array devices directly connected on both sides to metallic contacts were fabricated on various non-Si-based substrates (e.g., glass, plastics, and metal foils) in order to fully exploit the nanomaterial properties for final applications. The devices were realized with uniform length Ag-assisted electroless etched SiNW arrays that were detached from their fabrication substrate, typically Si wafers, reattached to arbitrary substrates, and formed with metallic contacts on both sides of the NW array. Electrical characterization of the SiNW array devices exhibits good current-voltage characteristics consistent with the SiNW morphology.


Assuntos
Cristalização/métodos , Eletrônica/instrumentação , Nanotubos/química , Nanotubos/ultraestrutura , Silício/química , Elasticidade , Condutividade Elétrica , Substâncias Macromoleculares/química , Teste de Materiais , Conformação Molecular , Tamanho da Partícula , Propriedades de Superfície
12.
Nano Lett ; 12(12): 6485-91, 2012 Dec 12.
Artigo em Inglês | MEDLINE | ID: mdl-23167740

RESUMO

Polycrystalline Si (poly-Si) thin-film, due to its low Si consumption, low substrate cost, and good stability, is an attractive candidate for cost-effective solar cells, but the as-deposited poly-Si typically has a columnar structure with grain boundaries in between, severely limiting the efficiency of the poly-Si. Here, we report a micropillar poly-Si solar cell that utilizes the columnar structure of the as-deposited poly-Si grains. We first formed submicrometer diameter poly-Si pillars, smaller than the initial grain sizes, and used these pillars as the seeds for the subsequent epitaxial growth of Si, which effectively reduces grain boundary density in the final poly-Si crystal. In addition, the vertically aligned micropillar arrays form radial p-n junctions that further mitigate the grain boundary recombination losses by improving the light absorption and charge-carrier collection efficiencies. Consequently, the maximum efficiency of micropillar poly-Si thin-film solar cells is 6.4%, that is, ∼1.5 times higher than that of the planar cells.


Assuntos
Fontes de Energia Elétrica , Silício/química , Desenho de Equipamento , Nanoestruturas/química , Energia Solar
13.
ACS Nano ; 17(24): 25014-25026, 2023 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-38059775

RESUMO

Vertically ordered Si needles are of particular interest for long-term intracellular recording owing to their capacity to infiltrate living cells with negligible damage and minimal toxicity. Such intracellular recordings could greatly benefit from simultaneous live cell imaging without disrupting their culture, contributing to an in-depth understanding of cellular function and activity. However, the use of standard live imaging techniques, such as inverted and confocal microscopy, is currently impeded by the opacity of Si wafers, typically employed for fabricating vertical Si needles. Here, we introduce a transparent intracellular sensing platform that combines vertical Si needles with a percolated network of Au-Ag nanowires on a transparent elastomeric substrate. This sensing platform meets all prerequisites for simultaneous intracellular recording and imaging, including electrochemical impedance, optical transparency, mechanical compliance, and cell viability. Proof-of-concept demonstrations of this sensing platform include monitoring electrical potentials in cardiomyocyte cells and in three-dimensionally engineered cardiovascular tissue, all while conducting live imaging with inverted and confocal microscopes. This sensing platform holds wide-ranging potential applications for intracellular research across various disciplines such as neuroscience, cardiology, muscle physiology, and drug screening.


Assuntos
Microscopia , Nanofios , Sobrevivência Celular , Miócitos Cardíacos , Agulhas
14.
ACS Nano ; 17(22): 22733-22743, 2023 Nov 28.
Artigo em Inglês | MEDLINE | ID: mdl-37933955

RESUMO

E-textiles, also known as electronic textiles, seamlessly merge wearable technology with fabrics, offering comfort and unobtrusiveness and establishing a crucial role in health monitoring systems. In this field, the integration of custom sensor designs with conductive polymers into various fabric types, especially in large areas, has presented significant challenges. Here, we present an innovative additive patterning method that utilizes a dual-regime spray system, eliminating the need for masks and allowing for the programmable inscription of sensor arrays onto consumer textiles. Unlike traditional spray techniques, this approach enables in situ, on-the-fly polymerization of conductive polymers, enabling intricate designs with submillimeter resolution across fabric areas spanning several meters. Moreover, it addresses the nozzle clogging issues commonly encountered in such applications. The resulting e-textiles preserve essential fabric characteristics such as breathability, wearability, and washability while delivering exceptional sensing performance. A comprehensive investigation, combining experimental, computational, and theoretical approaches, was conducted to examine the critical factors influencing the operation of the dual-regime spraying system and its role in e-textile fabrication. These findings provide a flexible solution for producing e-textiles on consumer fabric items and hold significant implications for a diverse range of wearable sensing applications.

15.
Nano Lett ; 11(8): 3435-9, 2011 Aug 10.
Artigo em Inglês | MEDLINE | ID: mdl-21696196

RESUMO

We report a simple, versatile, and wafer-scale water-assisted transfer printing method (WTP) that enables the transfer of nanowire devices onto diverse nonconventional substrates that were not easily accessible before, such as paper, plastics, tapes, glass, polydimethylsiloxane (PDMS), aluminum foil, and ultrathin polymer substrates. The WTP method relies on the phenomenon of water penetrating into the interface between Ni and SiO(2). The transfer yield is nearly 100%, and the transferred devices, including NW resistors, diodes, and field effect transistors, maintain their original geometries and electronic properties with high fidelity.

16.
Nano Lett ; 11(3): 1300-5, 2011 Mar 09.
Artigo em Inglês | MEDLINE | ID: mdl-21322602

RESUMO

Vertical transfer of silicon nanowire (SiNW) arrays with uniform length onto adhesive substrates was realized by the assistance of creating a horizontal crack throughout SiNWs. The crack is formed by adding a water soaking step between consecutive Ag-assisted electroless etching processes of Si. The crack formation is related to the delamination, redistribution, and reattachment of the Ag film during the water soaking and subsequent wet etching steps. Moreover, the crack facilitates embedding SiNWs inside polymers.

17.
Nano Lett ; 11(7): 2704-8, 2011 Jul 13.
Artigo em Inglês | MEDLINE | ID: mdl-21609002

RESUMO

We report an efficient hybrid Si microwire (radial junction) and planar solar cell with a maximum efficiency of 11.0% under AM 1.5G illumination. The maximum efficiency of the hybrid cell is improved from 7.2% to 11.0% by passivating the top surface and p-n junction with thin a-SiN:H and intrinsic poly-Si films, respectively, and is higher than that of planar cells of the identical layers due to increased light absorption and improved charge-carrier collections in both wires and planar components.


Assuntos
Fontes de Energia Elétrica , Silício/química , Energia Solar , Nanotecnologia , Tamanho da Partícula , Propriedades de Superfície
18.
Nano Lett ; 11(11): 4978-84, 2011 Nov 09.
Artigo em Inglês | MEDLINE | ID: mdl-21999403

RESUMO

We report a hierarchically branched TiO(2) nanorod structure that serves as a model architecture for efficient photoelectrochemical devices as it simultaneously offers a large contact area with the electrolyte, excellent light-trapping characteristics, and a highly conductive pathway for charge carrier collection. Under Xenon lamp illumination (UV spectrum matched to AM 1.5G, 88 mW/cm(2) total power density), the branched TiO(2) nanorod array produces a photocurrent density of 0.83 mA/cm(2) at 0.8 V versus reversible hydrogen electrode (RHE). The incident photon-to-current conversion efficiency reaches 67% at 380 nm with an applied bias of 0.6 V versus RHE, nearly two times higher than the bare nanorods without branches. The branches improve efficiency by means of (i) improved charge separation and transport within the branches due to their small diameters, and (ii) a 4-fold increase in surface area which facilitates the hole transfer at the TiO(2)/electrolyte interface.


Assuntos
Hidrogênio/química , Nanoestruturas/química , Nanoestruturas/efeitos da radiação , Titânio/química , Titânio/efeitos da radiação , Campos Eletromagnéticos , Hidrogênio/isolamento & purificação , Luz , Teste de Materiais , Nanoestruturas/ultraestrutura
19.
Sci Adv ; 8(13): eabn1772, 2022 04.
Artigo em Inglês | MEDLINE | ID: mdl-35353558

RESUMO

Ocular drug delivery remains a grand challenge due to the complex structure of the eye. Here, we introduce a unique platform of ocular drug delivery through the integration of silicon nanoneedles with a tear-soluble contact lens. The silicon nanoneedles can penetrate into the cornea in a minimally invasive manner and then undergo gradual degradation over the course of months, enabling painless and long-term sustained delivery of ocular drugs. The tear-soluble contact lens can fit a variety of corneal sizes and then quickly dissolve in tear fluid within a minute, enabling an initial burst release of anti-inflammatory drugs. We demonstrated the utility of this platform in effectively treating a chronic ocular disease, such as corneal neovascularization, in a rabbit model without showing a notable side effect over current standard therapies. This platform could also be useful in treating other chronic ocular diseases.


Assuntos
Lentes de Contato , Silício , Animais , Córnea , Sistemas de Liberação de Medicamentos , Coelhos , Silício/análise , Lágrimas/química
20.
Nano Lett ; 10(12): 5116-22, 2010 Dec 08.
Artigo em Inglês | MEDLINE | ID: mdl-21043492

RESUMO

We demonstrate orientation-controlled alignment of axially modulated pn SiNWs by applying dc electric fields across metal electrodes. The as-aligned pn SiNWs exhibit rectifying behaviors with a 97.7% yield, and about 35% of them exhibit no hysteresis in their current-voltage curves that can be directly used to construct AND/OR logic gates. Moreover, the as-aligned pn SiNWs can be packaged either with polydimethylsiloxane or additional metal layer to protect and even improve the quality of these NW diodes.

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