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The development of alternative alloy catalysts with high activity, surpassing platinum group metals, for the oxygen reduction reaction (ORR) is urgently needed in the field of electrocatalysis. The Ag-based single-atom alloy (AgSAA) cluster has been proposed as a promising catalyst for the ORR; however, enhancing its activity under operational conditions remains challenging due to limited insights into its actual active site. Here, we demonstrate that the operando formation of the MO x (OH) y complex serves as the key active site for catalyzing the ORR over AgSAA cluster catalysts, as revealed through comprehensive neural network potential molecular dynamics simulations combined with first-principles calculations. The volcano plot of the ORR over the MO x (OH) y complex addresses the gaps inherent in traditional metallic alloy models for pure AgSAA cluster catalysts in ORR catalysis. The appropriate orbital hybridization between OH and the dopant metal in the MO x (OH) y complexes indicated that the Ag54Co1, Ag54Pd1, and Ag54Au1 clusters are optimal AgSAA catalysts for the ORR. Our work underscores the significance of theoretical modeling considering the reaction atmosphere in uncovering the true active site for the ORR, which can be extended to other reaction systems for rational catalyst design.
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Background: A newly introduced obesity-related index, the weight-adjusted-waist index (WWI), emerges as a promising predictor of cardiovascular disease (CVD). Given the known synergistic effects of hypertension and obstructive sleep apnea (OSA) on cardiovascular risk, we aimed to explore the relationship between the WWI and CVD risk specifically within this high-risk cohort. Methods: A total of 2265 participants with hypertension and OSA were included in the study. Multivariate Cox regression analysis was used to calculate hazard ratios (HRs) and 95% confidence intervals (CIs) for CVD events. The restricted cubic spline (RCS) was used to further evaluate the nonlinear dose-response relationship. Results: During a median follow-up period of 6.8 years, 324 participants experienced a CVD event. Multivariate Cox regression analysis revealed that compared to the reference group, the HRs for the second, third, and fourth groups were 1.12 (95% CI, 0.79-1.59), 1.35 (95% CI, 0.96-1.89), and 1.58 (95% CI, 1.13-2.22), respectively. Moreover, RCS analysis illustrated a clear J-shaped relationship between the WWI and CVD risk, particularly notable when WWI exceeded 11.5 cm/âkg, signifying a significant increase in CVD risk. Conclusion: There was a J-shaped relationship between WWI and CVD in hypertensive patients with OSA, especially when the WWI was greater than 11.5 cm/âkg, the risk of CVD was significantly increased.
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Apple (Malus domestica Borkh.) is among the most widely planted and economically valuable horticultural crops globally. Over time, the apple fruit's cut surface undergoes browning, and the degree of browning varies among different apple varieties. Browning not only affects the appearance of fruits but also adversely affects their taste and flavor. In the present study, we observed browning in different apple varieties over time and analyzed the expression of genes in the polyphenol oxidase gene family. The results indicated a strong correlation between the browning degree of the fruit and the relative expression of the polyphenol oxidase gene MdPPO2. With the MdPPO2 promoter as bait, the basic leucine zipper (bZIP) transcription factor MdbZIP44 was identified using the yeast single-hybrid screening method. Further investigation revealed that the overexpression of MdbZIP44 in 'Orin' callus could enhance the expression of MdPPO2 and promote browning of the callus. However, knocking out MdbZIP44 resulted in a callus with no apparent browning phenotype. In addition, our results confirmed the interaction between MdbZIP44 and MdbZIP11. In conclusion, the results indicated that MdbZIP44 can induce apple fruit browning by activating the MdPPO2 promoter. The results provide a theoretical basis for further clarifying the browning mechanism of apple fruit.
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Frutas , Malus , Proteínas de Plantas , Regiones Promotoras Genéticas , Malus/genética , Malus/metabolismo , Regiones Promotoras Genéticas/genética , Proteínas de Plantas/genética , Proteínas de Plantas/metabolismo , Frutas/genética , Frutas/metabolismo , Regulación de la Expresión Génica de las Plantas , Catecol Oxidasa/metabolismo , Catecol Oxidasa/genética , Factores de Transcripción/metabolismo , Factores de Transcripción/genética , Factores de Transcripción con Cremalleras de Leucina de Carácter Básico/metabolismo , Factores de Transcripción con Cremalleras de Leucina de Carácter Básico/genéticaRESUMEN
In the evolving field of food safety, rapid and precise detection of antibiotic residues is crucial. This study aimed to tackle this challenge by integrating advanced inkjet printing technology with sophisticated microfluidic paper-based analytical devices (µPADs). The µPAD design utilized "green" quantum dots synthesized via an eco-friendly hydrothermal method using green white mulberry leaves as the carbon source, serving as the key fluorescent detection material. The action mechanism involved a photoinduced electron transfer system using red carbon dots (CDs) as electron donors and blue CDs combined with two-dimensional layered molybdenum disulfide (MoS2) nanosheets as electron acceptors. This system could quickly detect antibiotics within 10 min in pork and water samples, demonstrating high sensitivity and recovery rates: 6.5 pmol/L at 99.75%-110% for sulfadimethoxine, 3.3 pmol/L at 99%-105% for sulfamethoxazole, and 8.5 pmol/L at 98.5%-105% for tetracycline. It achieved a relative standard deviation under 5%, ensuring reliability and reproducibility. The fabricated sensor offered a promising application for the rapid and efficient on-site detection of antibiotic residues in food.
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Antibacterianos , Carbono , Contaminación de Alimentos , Puntos Cuánticos , Carbono/química , Antibacterianos/análisis , Puntos Cuánticos/química , Animales , Porcinos , Contaminación de Alimentos/análisis , Fluorescencia , Residuos de Medicamentos/análisis , Reproducibilidad de los Resultados , Dispositivos Laboratorio en un Chip , Espectrometría de Fluorescencia/métodos , Agua , Morus/químicaRESUMEN
Radiation-tolerance and repairable flexible transistors and integrated circuits (ICs) with low power consumption have become hot topics due to their wide applications in outer space, nuclear power plants, and X-ray imaging. Here, we designed and developed novel flexible semiconducting single-walled carbon nanotube (sc-SWCNT) thin-film transistors (TFTs) and ICs. Sc-SWCNT solid-electrolyte-gate dielectric (SEGD) TFTs showcase symmetric ambipolar characteristics with flat-band voltages (VFB) of â¼0 V, high ION/IOFF ratios (>105), and the recorded irradiation resistance (up to 22 Mrad). Moreover, flexible sc-SWCNT ICs, including CMOS-like inverters and NAND and NOR logic gates, have excellent operating characteristics with low power consumption (≤8.4 pW) and excellent irradiation resistance. Significantly, sc-SWCNT SEGD TFTs and ICs after radiation with a total irradiation dose (TID) ≥ 11 Mrad can be repaired after thermal heating at 100 °C. These outstanding characteristics are attributed to the designed device structures and key core materials including SEGD and sc-SWCNT.
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Rechargeable lithium-ion batteries are integral to contemporary energy storage, yet current anode material systems struggle to meet the increasing demand for extended range capabilities. This work introduces a novel composite anode material composed of one-dimensional 2H-phase tin disulfide (SnS2) nanoribbons enclosed within cavities of single-walled carbon nanotubes (SnS2@SWCNTs), achieved through precise atomic engineering. Employing aberration-corrected transmission electron microscopy, we precisely elucidated the crystal structure of SnS2 within the confines of the SWCNTs. This deliberate design effectively addresses the inherent limitations of SnS2 as a lithium-ion anode material, including its low electrical conductivity, considerable volume expansion effects, and unstable solid electrolyte interface membrane. Testing confirmed that SnS2 transforms into the Li5Sn2 alloy phase after full lithiation and back to SnS2 after delithiation, showing excellent reversibility. The composite also benefits from edge effects, improving lithium storage through stronger binding and lower migration barriers, which were supported by calculations. This pioneering work advances high-performance anode materials for applications.
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The development of neuromorphic optoelectronic systems opens up the possibility of the next generation of artificial vision. In this work, the novel broadband (from 365 to 940 nm) and multilevel storage optoelectronic synaptic thin-film transistor (TFT) arrays are reported using the photosensitive conjugated polymer (poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(bithiophene)], F8T2) sorted semiconducting single-walled carbon nanotubes (sc-SWCNTs) as channel materials. The broadband synaptic responses are inherited to absorption from both photosensitive F8T2 and sorted sc-SWCNTs, and the excellent optoelectronic synaptic behaviors with 200 linearly increasing conductance states and long retention time > 103 s are attributed to the superior charge trapping at the AlOx dielectric layer grown by atomic layer deposition. Furthermore, the synaptic TFTs can achieve IOn/IOff ratios up to 106 and optoelectronic synaptic plasticity with the low power consumption (59 aJ per single pulse), which can simulate not only basic biological synaptic functions but also optical write and electrical erase, multilevel storage, and image recognition. Further, a novel Spiking Neural Network algorithm based on hardware characteristics is designed for the recognition task of Caltech 101 dataset and multiple features of the images are successfully extracted with higher accuracy (97.92%) of the recognition task from the multi-frequency curves of the optoelectronic synaptic devices.
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To simulate biological visual systems and surpass their functions and performance, it is essential to develop high-performance optoelectronic neuromorphic electronics with broadband response, low power consumption, and fast response speed. Among these, optoelectronic synaptic transistors have emerged as promising candidates for constructing neuromorphic visual systems. In this work, flexible printed broadband (from 275 to 1050 nm) optoelectronic carbon nanotube synaptic transistors with good stability, high response speed (3.14 ms), and low-power consumption (as low as 0.1 fJ per event with the 1050 nm pulse illumination) using PbS quantum dots (QDs) modified semiconducting single-walled carbon nanotubes (sc-SWCNTs) as active layers are developed. In response to optical pulses within the ultraviolet to near-infrared wavelength range, the optoelectronic neuromorphic devices exhibit excitatory postsynaptic current, paired-pulse facilitation, and a transition from short-term plasticity to long-term plasticity, and other optical synaptic behaviors. Furthermore, a simplified neural morphology visual array is developed to simulate integrated functions such as image perception, memory, and preprocessing. More importantly, it can also emulate other complicated bionic functions, such as the infrared perception of salmon eyes and the warning behavior of reindeer in different environments. This work holds immense significance in advancing the development of artificial neural visual systems.
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Continuum manipulators can improve spatial adaptability and operational flexibility in constrained environments by endowing them with contraction and extension capabilities. There are currently desired requirements to quantify the shape of an extensible continuum manipulator for strengthening its obstacle avoidance capability and end-effector position accuracy. To address these issues, this study proposes a methodology of using silicone rubber strain sensors (SRSS) to estimate the shape of an extensible continuum manipulator. The way is to measure the strain at specific locations on the deformable body of the manipulator, and then reconstruct the shape by integrating the information from all sensors. The slender sensors are fabricated by a rolling process that transforms planar silicone rubber sensors into cylindrical structures. The proprioceptive model relationship between the strain of the sensor and the deformation of the manipulator is established with considering the phenomenon of torsion of the manipulator caused by compression. The physically extensible continuum manipulator equipped with three driving tendons and nine SRSS was designed. Comprehensive evaluations of various motion trajectories indicate that this method can accurately reconstruct the shape of the manipulator, especially under end-effector loads. The experimental results demonstrate that the mean (maximum) absolute position error of the endpoint is 1.61% (3.45%) of the manipulator length.
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The development of large-scale integration of optoelectronic neuromorphic devices with ultralow power consumption and broadband responses is essential for high-performance bionics vision systems. In this work, we developed a strategy to construct large-scale (40 × 30) enhancement-mode carbon nanotube optoelectronic synaptic transistors with ultralow power consumption (33.9 aJ per pulse) and broadband responses (from 365 to 620 nm) using low-work function yttrium (Y)-gate electrodes and the mixture of eco-friendly photosensitive Ag2S quantum dots (QDs) and ionic liquids (ILs)-cross-linking-poly(4-vinylphenol) (PVP) (ILs-c-PVP) as the dielectric layers. Solution-processable carbon nanotube thin-film transistors (TFTs) showed enhancement-mode characteristics with the wide and controllable threshold voltage window (-1 Vâ¼0 V) owing to use of the low-work-function Y-gate electrodes. It is noted that carbon nanotube optoelectronic synaptic transistors exhibited high on/off ratios (>106), small hysteresis and low operating voltage (≤2 V), and enhancement mode even under the illumination of ultraviolet (UV, 365 nm), blue (450 nm), and green (550 nm) to red (620 nm) pulse lights when introducing eco-friendly Ag2S QDs in dielectric layers, demonstrating that they have the strong fault-tolerant ability for the threshold voltage drifts caused by various manufacturing scenarios. Furthermore, some important bionic functions including a high paired pulse facilitation index (PPF index, up to 290%), learning and memory function with the long duration (200 s), and rapid recovery (2 s). Pavlov's dog experiment (retention time up to 20 min) and visual memory forgetting experiments (the duration of high current for 180 s) are also demonstrated. Significantly, the optoelectronic synaptic transistors can be used to simulate the adaptive process of vision in varying light conditions, and we demonstrated the dynamic transition of light adaptation to dark adaptation based on light-induced conditional behavior. This work undoubtedly provides valuable insights for the future development of artificial vision systems.
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The advent of flexible single-walled carbon nanotube thin-film transistors (SWCNT-TFTs) has transformed electronics, providing significant benefits like low operating voltage, reduced power consumption, cost-effectiveness, and improved signal amplification. This study focuses on leveraging these attributes to develop a novel flexible high-sensitivity and energy-efficient chloride ion sensors based on printed flexible SWCNT-TFTs utilizing polymers-sorted semiconducting SWCNTs (sc-SWCNTs) as the active layers and ion liquids-poly(4-vinylphenol as dielectric layers along with the evaporated deposition of aluminum electrodes and printed silver electrodes as the gate and source-drain electrodes, respectively. The sensors exhibit several operational advantages, including low voltage requirements (≤1 V), rapid response speed (5.32 s), significant signal amplification (Up to 702.6 %), low power consumption (0.31 µJ at 1 mmol chloride ion), good repeatability, high sensitivity for both low and high concentrations of chloride ion (up to 100 mmol/L) and excellent mechanical flexibility (No obvious changes after bending for 10,000 times with a 5 mm radius). The detection mechanism of chloride ions was analyzed using X-ray Photoelectron Spectroscopy (XPS). It was found that chloride ions react with silver nanoparticles (AgNPs) to form silver chloride (AgCl) on printed electrodes, impeding carrier transport and reducing the currents in SWCNT TFTs. Importantly, our sensors' compatibility with smart devices allows for real-time monitoring of chloride ion levels in human sweat, offering significant potential for daily health monitoring.
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The performance of a chemical reaction is critically dependent on the electronic and/or geometric structures of a material in heterogeneous catalysis. Over the past century, the Sabatier principle has already provided a conceptual framework for optimal catalyst design by adjusting the electronic structure of the catalytic material via a change in composition. Beyond composition, it is essential to recognize that the geometric atomic structures of a catalyst, encompassing terraces, edges, steps, kinks, and corners, have a substantial impact on the activity and selectivity of a chemical reaction. Crystal-phase engineering has the capacity to bring about substantial alterations in the electronic and geometric configurations of a catalyst, enabling control over coordination numbers, morphological features, and the arrangement of surface atoms. Modulating the crystallographic phase is therefore an important strategy for improving the stability, activity, and selectivity of catalytic materials. Nonetheless, a complete understanding of how the performance depends on the crystal phase of a catalyst remains elusive, primarily due to the absence of a molecular-level view of active sites across various crystal phases. In this review, we primarily focus on assessing the dependence of catalytic performance on crystal phases to elucidate the challenges and complexities inherent in heterogeneous catalysis, ultimately aiming for improved catalyst design.
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Hypertensive patients with snoring and elevated plasma homocysteine levels are common. When these factors are combined, the risk of coronary heart disease (CHD) is high. Herein, we developed and validated an easy-to-use nomogram to predict high-risk CHD in snoring hypertensive patients with elevated plasma homocysteine.Snoring patients (n = 1,962) with hyperhomocysteinemia and hypertension were divided into training (n = 1,373, 70%) and validation (n = 589, 30%) sets. We extracted CHD predictors using multivariate Cox regression analysis, then constructed a nomogram model. Internal validation using 1,000 bootstrap resampling was performed to assess the consistency and discrimination of the predictive model using the area under the receiver operating characteristic curve (AUC) and calibration plots.We constructed a nomogram model with the extracted predictors, including age, waist-height ratio, smoking, and low-density lipoprotein cholesterol levels. The AUCs of the training and validation cohorts at 80 months were 0.735 (95% CI: 0.678-0.792) and 0.646 (95% CI: 0.547-0.746), respectively. The consistency between the observed CHD survival and the probability of CHD survival in the training and validation sets was acceptable based on the calibration plots. A total of more than 151 points in the nomogram can be used in the identification of high-risk patients for CHD among snoring hypertensive patients with elevated plasma homocysteine.We developed a CHD risk prediction model for snoring hypertension patients with hyperhomocysteinemia. Our findings provide a useful clinical tool for the rapid identification of high-risk CHD at an early stage.
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Enfermedad Coronaria , Hiperhomocisteinemia , Hipertensión , Humanos , Hiperhomocisteinemia/complicaciones , Hiperhomocisteinemia/diagnóstico , Hiperhomocisteinemia/epidemiología , Ronquido/epidemiología , Enfermedad Coronaria/complicaciones , Enfermedad Coronaria/diagnóstico , Enfermedad Coronaria/epidemiología , Hipertensión/complicaciones , Hipertensión/epidemiología , Homocisteína , NomogramasRESUMEN
Flavonoids, such as anthocyanins and proanthocyanidins (PAs), play essential roles in plant growth, development, and stress response. Red-fleshed apples represent a valuable germplasm resource with high flavonoid content. Understanding and enriching the regulatory network controlling flavonoid synthesis in red-fleshed apples holds significant importance for cultivating high-quality fruits. In this study, we successfully isolated an NAC transcription factor, MdNAC14-Like, which exhibited a significant negative correlation with the content of anthocyanin. Transient injection of apple fruit and stable expression of callus confirmed that MdNAC14-Like acts as an inhibitor of anthocyanin synthesis. Through yeast monohybrid, electrophoretic mobility shift, and luciferase reporter assays, we demonstrated the ability of MdNAC14-Like to bind to the promoters of MdMYB9, MdMYB10, and MdUFGT, thus inhibiting their transcriptional activity and subsequently suppressing anthocyanin synthesis. Furthermore, our investigation revealed that MdNAC14-Like interacts with MdMYB12, enhancing the transcriptional activation of MdMYB12 on the downstream structural gene MdLAR, thereby promoting PA synthesis. This comprehensive functional characterization of MdNAC14-Like provides valuable insights into the intricate regulatory network governing anthocyanin and PA synthesis in apple.
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Malus , Proantocianidinas , Malus/genética , Malus/metabolismo , Antocianinas/metabolismo , Proantocianidinas/metabolismo , Regulación de la Expresión Génica de las Plantas , Proteínas de Plantas/genética , Proteínas de Plantas/metabolismo , Flavonoides/metabolismoRESUMEN
OBJECTIVE: To investigate the clinical efficacy of three-dimensional (3D) printing-assisted shaping titanium cage combined with Masquelet technology in the treatment of calcaneal infectious defects. METHODS: A retrospective analysis was performed of the data from nine patients with chronic calcaneal infection defects treated with distal gastronal flap coverage and one patient with free anterolateral thigh flap coverage, also using a 3D printing-assisted shaping titanium cage combined with both mask technology and rib autografting from January 2017 to January 2019. There were seven males and three females, with a mean age of 37 years (range, 17-52 years). The injury mechanism of the 10 patients included four motor vehicle incidents, four high fall injuries, and two rolling compactions. All patients were treated by twoâstage procedures. The first stage included debridement, polymethyl methacrylate (PMMA) filling, and regional flap coverage. The soft tissue defect of the 10 cases included 80 cm2 in four cases and 56 cm2, 40 cm2, and 15 cm2 in each of two cases. The bone defect was 24 cm3 and 18 cm3 in each of four cases and 3 cm3 in two cases. The second stage was the mask technology of 3D printing-assisted shaping titanium cage combined with rib autografting. Time of bone union, calcaneus morphology, implant position, and the Maryland and AOFAS hind foot scores were recorded to evaluate the clinical outcome. RESULTS: All 10 patients were followed up for a mean of 18.5 months (range, 12-30 months). Infection occurred in two patients 2 months after the first stage operation and were successfully treated by debridement and PMMA replacement. The incision of the other eight cases all healed successfully. Cultures from the 10 cases included five cases of methicillin-resistant Staphylococcus aureus, three cases of S. aureus, and one case each of Escherichia coli and Pseudomonas aeruginosa. All 10 patients exhibited calcaneus bone union after the second stage operation. The mean time for bone union was 4.32 (range, 3-8) months. Bone trabeculae were observed in a CT scan 13 (range, 10-22) months post-operation. The mean Maryland score at 12 months post-operation was 92 (range, 86-98) and the mean AOFAS ankle hind foot score was 89.8 (range, 83-100). CONCLUSION: Three-dimensional printing-assisted shaping titanium cages and Masquelet technology may be effective methods for the treatment of infectious calcaneal defects.
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Calcáneo , Staphylococcus aureus Resistente a Meticilina , Osteomielitis , Femenino , Masculino , Humanos , Adulto , Titanio , Polimetil Metacrilato , Estudios Retrospectivos , Staphylococcus aureus , Osteomielitis/diagnóstico por imagen , Osteomielitis/cirugía , Impresión Tridimensional , Calcáneo/diagnóstico por imagen , Calcáneo/cirugíaRESUMEN
OBJECTIVE: To explore asurgical methods for replantation of severed finger. METHODS: From January 2018 to November 2022, 8 amputated-finger patients were performed surgical reconstructions by using polyfoliate free flaps with the first dorsal metatarsal artery, including 7 males and 1 female, aged from 20 to 55 years old, and defect areas ranged from (1.0 to 2.0) cm×(3.0 to 4.5) cm. Finger pulp sensation, shape and other relevant parameters were assessed following the upper extremity functional evaluation standard, which was put forward by Hand Surgery Branch of Chinese Medical Association. And maryland foot functional score was used to evaluate foot function. RESULTS: Amputated fingers and flaps of all the 8 patients were survived. All patients were followed up for 4 to 20 months, their finger color and temperature tured to normal, with good wear-resistance and cold-resistance. According to Hand Surgery Branch of Chinese Medical Association, functional score ranged 61 to 92;4 patients got excellent result and 4 good. Maryland foot functional score ranged from 93 to 100;and 8 patients got excellent result. CONCLUSION: It is feasible to repair severed fingers with soft tissue defects using polyfoliate free flaps that driven by the flippers of the first and second toes of the foot. This method ccould bridge blood vessels, increase soft tissue volume of the injured finger, and avoid finger shortening, with high patient satisfaction.
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Pie , Procedimientos de Cirugía Plástica , Masculino , Humanos , Femenino , Adulto Joven , Adulto , Persona de Mediana Edad , Pie/cirugía , Extremidad Inferior , Colgajos Quirúrgicos , Dedos del PieRESUMEN
A universal roll-to-roll (R2R) printing approach was developed to construct large area (8 cm × 14 cm) semiconducting single-walled carbon nanotube (sc-SWCNT) thin films on flexible substrates (such as polyethylene terephthalate (PET), paper, and Al foils) at a printing speed of 8 m min-1 using highly concentrated sc-SWCNT inks and crosslinked poly-4-vinylphenol (c-PVP) as the adhesion layer. Bottom-gated and top-gated flexible printed p-type TFTs based on R2R printed sc-SWCNT thin films exhibited good electrical properties with a carrier mobility of â¼11.9 cm2 V-1 s-1, Ion/Ioff ratios of â¼106, small hysteresis, and a subthreshold swing (SS) of 70-80 mV dec-1 at low gate operating voltages (±1 V), and excellent mechanical flexibility. Furthermore, the flexible printed complementary metal oxide semiconductor (CMOS) inverters demonstrated rail-to-rail voltage output characteristics under an operating voltage as low as VDD = -0.2 V, a voltage gain of 10.8 at VDD = -0.8 V, and power consumption as low as 0.056 nW at VDD = -0.2 V. To the best of our knowledge, the electrical properties of the printed SWCNT TFTs (such as Ion/Ioff ratio, mobility, operating voltage, and mechanical flexibility) and printed CMOS inverters based on the R2R printed sc-SWCNT active layer in this work are excellent compared to those of R2R printed SWCNT TFTs reported in the literature. Consequently, the universal R2R printing method reported in this work could promote the development of fully printed low-cost, large-area, high-output, and flexible carbon-based electronics.