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Organic piezoelectric nanogenerators (PENGs) are attractive in harvesting mechanical energy for various self-powering systems. However, their practical applications are severely restricted by their low output open circuit voltage. To address this issue, herein, we prepared two two-dimensional (2D) covalent organic frameworks (COFs, CityU-13 and CityU-14), functionalized with fluorinated alkyl chains for PENGs. The piezoelectricity of both COFs was evidenced by switchable polarization, characteristic butterfly amplitude loops, phase hysteresis loops, conspicuous surface potentials and high piezoelectric coefficient value (d33). The PENGs fabricated with COFs displayed highest output open circuit voltages (60 V for CityU-13 and 50 V for CityU-14) and delivered satisfactory short circuit current with an excellent stability of over 600 seconds. The superior open circuit voltages of CityU-13 and CityU-14 rank in top 1 and 2 among all reported organic materials-based PENGs.
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Antibiotics are refractory degradable organic pollutants that present a significant hazard to water environments. In this work, a ternary composite (KB/BMO-GO) comprising of graphene oxide (GO), Bi2MoO6 (BMO), and a cross-linked benzene polymer (KB) was synthesized and applied to promote the synergistic adsorption-photocatalytic degradation of the refractory pollutant, oxytetracycline (OTC). The inclusion of GO and KB in the composite enhanced the OTC adsorption performance of the catalysts, and the construction of Z-scheme heterojunction promoted the photogenerated charge separation efficiency and broadened the range of light absorption, thereby enhancing the photocatalytic performance. Moreover, we compared the performance of catalysts loaded with different mass ratios of KB (x% KB/BMO-GO). Among them, the 15 % KB/BMO-GO catalyst sample had the best OTC degradation performance. Specifically, 15 % KB/BMO-GO could adsorb 69.7 % of OTC in 30 min, reaching an OTC degradation rate of 93.3 % under visible light irradiation. h+ and 1O2 are the main active substances in the photocatalytic process. In addition, the catalysts are acid-alkali and salt-resistant, as well as good reusability. This study provides a valuable reference for the preparation of highly efficient photocatalysts for synergistic adsorption-photodegradation processes.
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Photocatalysis is a green and environmentally friendly method for degrading dangerous and nonbiodegradable pollutants. In this study, a sequence of metal-free triazine-based electronic donor-acceptor (D-A) conjugated polymers Tr-X (X = Th, BT, BTh) were prepared by D-A configuration regulation between triazine (Tr) and monomers containing N and S, such as thiophene (Th), bithiophene (BTh) and benzothiadiazole (BT) units, for the photocatalytic degradation of bisphenol A (BPA) and benzene contaminants in water under visible light. Among these, Tr-BTh exhibited complete photocatalytic degradation owing to its excellent D-A configuration. Moreover, the N and S atoms, which are rich in triazine and thiophene units, serve as highly dispersed reactive sites. The separation and transfer of photogenerated carriers can be further improved by expanding the light-absorption range of polymers. In addition, the polymers showed good adsorption for BPA and other aromatic organic pollutants through π-π interaction and surface hydrogen bonding, which provides a facile strategy for efficient polymer-based photocatalysts for water purification.
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Endothelial repair is essential for restoring tissue fluid homeostasis following lung injury. R-spondin3 (RSPO3), a secreted protein mainly produced by endothelial cells (ECs), has shown its protective effect on endothelium. However, the specific mechanisms remain unknown. To explore whether and how RSPO3 regulates endothelial regeneration after inflammatory vascular injury, the role of RSPO3 in sepsis-induced pulmonary endothelial injury was investigated in EC-specific RSPO3 knockdown, inducible EC-specific RSPO3 deletion mice, EC-specific RSPO3 overexpression mice, systemic RSPO3-administration mice, in isolated mouse lung vascular endothelial cells (MLVECs), and in plasma from septic patients. Here we show that plasma RSPO3 levels are decreased in septic patients and correlated with endothelial injury markers and PaO2/FiO2 index. Both pulmonary EC-specific knockdown of RSPO3 and inducible EC-specific RSPO3 deletion inhibit pulmonary ECs proliferation and exacerbate ECs injury, whereas intra-pulmonary EC-specific RSPO3 overexpression promotes endothelial recovery and attenuates ECs injury during endotoxemia. We show that RSPO3 mediates pulmonary endothelial regeneration by a LGR4-dependent manner. Except for ß-catenin, integrin-linked kinase (ILK)/Akt is also identified as a novel downstream effector of RSPO3/LGR4 signaling. These results conclude that EC-derived RSPO3 mediates pulmonary endothelial regeneration by LGR4-dependent activation of ß-catenin and ILK signaling pathways after inflammatory vascular injury.
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Células Endoteliais , Pulmão , Proteínas Serina-Treonina Quinases , Receptores Acoplados a Proteínas G , Regeneração , Transdução de Sinais , Trombospondinas , beta Catenina , Animais , Trombospondinas/metabolismo , Trombospondinas/genética , Proteínas Serina-Treonina Quinases/metabolismo , Proteínas Serina-Treonina Quinases/genética , Camundongos , Humanos , Receptores Acoplados a Proteínas G/metabolismo , Receptores Acoplados a Proteínas G/genética , beta Catenina/metabolismo , beta Catenina/genética , Células Endoteliais/metabolismo , Pulmão/patologia , Pulmão/metabolismo , Lesões do Sistema Vascular/metabolismo , Lesões do Sistema Vascular/genética , Lesões do Sistema Vascular/patologia , Proliferação de Células , Masculino , Sepse/metabolismo , Inflamação/metabolismo , Inflamação/patologiaRESUMO
Herein, self-assembled monolayers (SAMs) are constructed on the surface of Ti3C2 MXene to improve its environmental stability and piezocatalytic activity. Ti3C2/SAMs-X (X = H, Cl, and NH2) was prepared to enhance the piezocatalytic degradation of bisphenol A (BPA) and hydrogen production. Surface-treated Ti3C2 exhibits different lattice parameters and symmetry, thus leading to an increased polarization. The presence of polar functional groups in SAMs remarkably increases the surface potential of Ti3C2, thereby promoting the migration of piezoelectric electrons. Ti3C2/SAMs-NH2 exhibits the highest piezocatalytic performance, thus improving BPA removal and H2 generation by 7 and 1.8 times, respectively. In addition, Ti3C2/SAMs-NH2 remained stable under 100% relative humidity for 15 days. Therefore, it provides a facile strategy for modulating piezocatalytic properties through interfacial self-assembly-induced lattice distortion.
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Producing sulfur from a sulfide oxidation reaction (SOR)-based technique using sulfide aqueous solution has attracted considerable attention due to its ecofriendliness. This study demonstrates that NiS-doped cobalt sulfide NiS-CoS-supported NiCo alloy foam can deliver the SOR with superior electrocatalytic activity and robust stability compared to reported non-noble metal-based catalysts. Only 0.34 V vs RHE is required to drive a current density of 100 mA cm-2 for the SOR. According to the experiment, the catalyst exhibits a unique sulfurophobicity feature because of the weak interaction between sulfur and the transition metal sulfide (low affinity for elemental sulfur), preventing electrode corrosion during the SOR process. More impressively, the chain-growth mechanism of the SOR from short- to long-chain polysulfides was revealed by combining electrochemical and spectroscopic in situ methods, such as in situ ultraviolet-visible and Raman. It is also demonstrated that electrons can transfer straight from the sulfion (S2-) to the active site on the anode surface during the low-energy-consumption SOR process. This work provides new insight into simultaneous energy-saving hydrogen production and high-value-added S recovery from sulfide-containing wastewater.
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AIM: Exercise training exerts protective effects against sepsis-associated multiple organ dysfunction. This study aimed to investigate whether aerobic exercise protected against sepsis-associated acute kidney injury (AKI) via modulating R-spondin 3 (RSPO3) expression. METHODS: To investigate the effects of aerobic exercise on lipopolysaccharide (LPS)-induced AKI, LPS (20 mg/kg) was intraperitoneally injected after six weeks of treadmill training. To investigate the role of RSPO3 in LPS-induced AKI, wild-type (WT) or inducible endothelial cell-specific RSPO3 knockout (RSPO3EC-/- ) mice were intraperitoneally injected with 12 mg/kg LPS. RSPO3 was intraperitoneally injected 30 min before LPS treatment. RESULTS: Aerobic exercise-trained mice were more resistant to LPS-induced body weight loss and hypothermia and had a significant higher survival rate than sedentary mice exposed to LPS. Exercise training restored the LPS-induced decreases in serum and renal RSPO3 levels. Exercise or RSPO3 attenuated, whereas inducible endothelial cell-specific RSPO3 knockout exacerbated LPS-induced renal glycocalyx loss, endothelial hyperpermeability, inflammation, and AKI. Bioinformatics analysis results revealed significant increases in the expression of matrix metalloproteinases (MMPs) in kidney tissues of mice exposed to sepsis or endotoxaemia, which was validated in renal tissue from LPS-exposed mice and LPS-treated human microvascular endothelial cells (HMVECs). Both RSPO3 and MMPs inhibitor restored LPS-induced downregulation of tight junction protein, adherens junction protein, and glycocalyx components, thus ameliorating LPS-induced endothelial leakage. Exercise or RSPO3 reversed LPS-induced upregulation of MMPs in renal tissues. CONCLUSION: Increased renal expression of RSPO3 contributes to aerobic exercise-induced protection against LPS-induced renal endothelial hyperpermeability and AKI by suppressing MMPs-mediated disruption of glycocalyx and tight and adherens junctions.
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Injúria Renal Aguda , Animais , Humanos , Camundongos , Injúria Renal Aguda/prevenção & controle , Injúria Renal Aguda/metabolismo , Células Endoteliais/metabolismo , Lipopolissacarídeos/farmacologia , Metaloproteinases da Matriz/metabolismo , Metaloproteinases da Matriz/farmacologia , Camundongos Endogâmicos C57BL , Sepse/complicações , Sepse/metabolismoRESUMO
Dysregulation of vitamin D receptor (VDR) is implicated in chronic obstructive pulmonary disease. However, whether VDR dysregulation contributes to the development of pulmonary fibrosis remains largely unknown. Analysis of bulk and single-cell RNA profiling datasets revealed VDR upregulation in lung fibroblasts from patients with pulmonary fibrosis or fibrotic mice, which was validated in lung fibroblasts from bleomycin-exposed mice and bleomycin-treated fibroblasts. Stable VDR knockdown promoted, whereas the VDR agonist paricalcitol suppressed lung fibroblast proliferation and activation. Gene set enrichment analysis (GSEA) showed that the JAK/STAT pathway and unfolded protein response (UPR), a process related to endoplasmic reticulum (ER) stress, were enriched in lung fibroblasts of fibrotic lungs. Stable VDR knockdown stimulated, but paricalcitol suppressed ER stress and JAK1/STAT3 activation in lung fibroblasts. The STAT3 inhibitor blocked bleomycin- or stable VDR knockdown-induced ER stress. Paricalcitol inhibited the bleomycin-induced enrichment of STAT3 to the ATF6 promoter, thereby suppressing ATF6 expression in fibroblasts. Paricalcitol or intrapulmonary VDR overexpression inactivated JAK1/STAT3 and suppressed ER stress in bleomycin-treated mice, thus resulting in the inhibition of fibroblast proliferation and activation. Collectively, this study suggests that fibroblast VDR upregulation may be a self-protective response to limit fibroblast proliferation and activation during pulmonary fibrosis by suppressing the JAK1/STAT3/ER stress pathway.
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Converting CO2 into high-value C2 chemicals such as acetate with high selectivity and efficiency is a critical issue in renewable energy storage. Herein, for the first time we present a vibration-driven piezocatalysis with tin(II) monosulfide (SnS) nanobelts for conversion of CO2 to acetate with 100 % selectivity, and the highest production rate (2.21â mM h-1 ) compared with reported catalysts. Mechanism analysis reveal that the polarized charges triggered by periodic mechanical vibration promote the adsorption and activation of CO2 . The electron transfer can be facilitated due to built-in electric field, decreased band gap and work function of SnS under stress. Remarkably, reduced distance between active sites leads to charge enrichment on Sn sites, promoting the C-C coupling, reducing the energy barriers of the rate determining step. It puts forward a bran-new strategy for converting CO2 into high-value C2 products with efficient, low-cost and environment-friendly piezocatalysis utilizing mechanical energy.
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The production of hydrogen peroxide (H2O2) from oxygen and water is an attractive route for converting solar energy into chemical energy. In order to achieve high solar-to-H2O2 conversion efficiency, floral inorganic/organic (CdS/TpBpy) composite with strong oxygen absorption and S-scheme heterojunction was synthesized by simple solvothermal-hydrothermal methods. The unique flower-like structure increased the active sites and oxygen absorption. The existence of S-scheme heterojuntion facilitated the charge transfer across the built-in electric field. Without sacrificial reagents or stabilizers, the optimal CdS/TpBpy had a higher H2O2 production (3600 µmol g-1 h-1), which was 2.4 and 25.6 times than those of TpBpy and CdS, respectively. Meanwhile, CdS/TpBpy inhibited the H2O2 decomposition, thus increasing the overall output. Furthermore, a series of experiments and calculations were carried out to verify the photocatalytic mechanism. This work demonstrates a modification method to improve the photocatalytic activity of hybrid composites, and shows potential applications in energy conversion.
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Although many superwetting materials have been designed for the treatment of oil-containing wastewater, separation strategies for oil-in-water systems containing bacteria have rarely been reported. Herein, poly(vinylidene difluoride)- and poly(lactic acid)-blended fibrous membranes loaded with silver and copper oxide nanoparticles were successfully prepared by a two-step method of electrostatic spinning and liquid-phase synthesis. The product membrane showed excellent super-oleophilic properties in air and hydrophobicity under oil. It could separate water-in-oil emulsion systems containing surfactants with an efficiency above 90%. More importantly, the nanoparticle-loaded fibers were characterized by material degradability and slowly released ions. The fibers exhibited excellent antibacterial activities against both gram-positive and -negative bacteria. This work provides a feasible strategy for water-in-oil emulsion separation and bacterial treatment of wastewater.
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Urea degradation is one of the most crucial links in the natural nitrogen cycle. Exploring the real active species in the urea electro-oxidation process is of great significance for understanding the urea electro-oxidation mechanism and designing catalysts. A highly active and stable Prussian blue analogue catalyst (PBA@NiFe/NF) loaded on nickel foam was synthesized for electro-oxidation of urea. In situ Raman spectra revealed that Ni in PBA@NiFe/NF was able to maintain a stable divalent nickel (Ni(II)) state for up to 3.5 h during the initial urea oxidation process, which is rarely reported in previous research studies. In addition, with the participation of iron, the Ni-Fe bimetallic center significantly improves the electro-oxidation of urea. Our work provides a new idea for prolonging the Ni(II) activity in electrocatalytic oxidation of urea.
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In this study, a 3D thornball-like hierarchical ß-In2S3, displaying extremely rapid photodegradation of cationic dyes, was synthesized by a facile method. The formation of a uniform thornball-like structure depended on the microwave reaction method and citric acid as the pH regulator. The size of In2S3 was easily adjusted by changing the microwave irradiation time from 5 min to 15 min. The morphology, structure, composition, energy level, charge separation, and surface properties of different-sized In2S3 were characterized. The results showed that In2S3 synthesized in 10 min (In2S3-10) displayed optimal interface property for the electron-hole separation, maximum hydrophilia with most surface negative charges for the surface adsorption, contributing to the complete photodegradation of rhodamine B (RhB) in just 25 minutes of visible light illumination. The photodegradation path of RhB was speculated with four possible paths, including the processes of de-ethylation, open-ring of xanthene, and rupture of carbon-carbon bonds up to the decomposition into small molecules. Finally, the reusability of In2S3-10 was tested, obtaining nearly 96% photodegradation efficiency after sequential 5 cycles.
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A long-standing challenge in pneumonia diagnosis is recognizing the pathological lung texture, especially the ground-glass appearance pathological texture. One main difficulty lies in precisely extracting and recognizing the pathological features. The patients, especially those with mild symptoms, show very little difference in lung texture, neither conventional computer vision methods nor convolutional neural networks perform well on pneumonia diagnosis based on chest X-ray (CXR) images. In the meanwhile, the Coronavirus Disease 2019 (COVID-19) pandemic continues wreaking havoc around the world, where quick and accurate diagnosis backed by CXR images is in high demand. Rather than simply recognizing the patterns, extracting feature maps from the original CXR image is what we need in the classification process. Thus, we propose a Vision Transformer (VIT)-based model called PneuNet to make an accurate diagnosis backed by channel-based attention through X-ray images of the lung, where multi-head attention is applied on channel patches rather than feature patches. The techniques presented in this paper are oriented toward the medical application of deep neural networks and VIT. Extensive experiment results show that our method can reach 94.96% accuracy in the three-categories classification problem on the test set, which outperforms previous deep learning models.
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COVID-19 , Aprendizado Profundo , Pneumonia , Humanos , COVID-19/diagnóstico por imagem , Raios X , SARS-CoV-2 , Algoritmos , Pneumonia/diagnóstico por imagem , Teste para COVID-19RESUMO
Light-driven reaction of oxygen and water to hydrogen peroxide (H2O2) is an environmental protection method, which can convert solar energy into green products. In this work, perylene-3, 4, 9, 10-tetracarboxylic diimide (PDINH) could be recrystallized in situ on the surface of porous carbon nitride (PCN), to obtain an all-organic S-scheme heterojunction (PDINH/PCN). The design of the hierarchical porous photocatalyst improved the mass transfer, enhanced the light absorption and increased specific surface area. Moreover, the construction of the S-scheme heterojunction at the interface of PDINH and PCN exhibited suitable band, which facilitated the separation and transfer of carriers. The H2O2 production rate was up to 922.4 µmol g-1h-1, which was 2.6 and 53.3 times higher than that of PCN and PDINH. Therefore, the all-organic S-scheme heterojunction provides an insight for improving the photocatalytic H2O2 production.
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Developing of fast and efficient adsorbents for removal of low concentration refractory organics in water is significant. Herein, a novel calix[4]arene-based porous organic polymer CaPy is constructed through Sonogashira-Hagihara cross-coupling polycondensation. The strong polar sulfonate is further anchored onto the polymer skeleton of CaPy and three sulfonate-modified anionic polymers CaPy-S1, CaPy-S2, and CaPy-S3 were obtained and fully characterized. The adsorption isotherms showed that the maximum adsorption capacities of CaPy, CaPy-S1, CaPy-S2, and CaPy-S3 toward methylene blue (MB) were 270, 1454, 558 and 1381 mg g-1, whereas those for Rhodamine B (RhB) were 183, 2653, 1132, and 1796 mg g-1, respectively. The maximum adsorption capacity toward RhB was the highest reported vale among the currently used synthetic adsorbents. In addition, the pseudo-second-order rate constants of CaPy, CaPy-S1, CaPy-S2, and CaPy-S3 toward MB were 0.00572, 0.488, 2.24, and 0.192 g mg-1 min-1, respectively, and those toward RhB were 0.000234, 0.138, 0.0819, and 0.203 g mg-1 min-1, respectively. The pseudo-second-order rate constant of CaPy-S2 toward MB was 2.24 g mg-1 min-1 indicating one of the highest adsorption speeds. The activation energy of CaPy-S1 for RhB and MB were 121 and 109 kJ mol-1, respectively, demonstrating that the adsorption of both dyes on CaPy-S1 was chemisorption process. Further, the obtained values of Gibbs free energy were negative, revealing that the adsorption process was spontaneous. This work provides an effective approach for improving adsorption performance via post-modification.
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Calixarenos , Poluentes Químicos da Água , Purificação da Água , Adsorção , Alcanossulfonatos , Cátions , Corantes , Azul de Metileno , Polímeros , Porosidade , Eletricidade Estática , Água , Poluentes Químicos da Água/análiseRESUMO
An optimized oxygen activity of catalysts can facilitate oxidation of volatile organic compounds. This work shows the first construction of Ce-Co oxide thin-walled nanoboxes. Bulk-phase lattice oxygen is activated by metal-metal interactions. The subsequent uniform dispersion of low loaded Pt nanoparticles further enhances the surface-adsorbed oxygen content, and creates an oxygen-rich reaction interface. Competitive adsorption of water vapor was also inhibited, and complete catalytic oxidation of toluene was achieved at low temperature (T90 =140 °C). A diffuse reflectance infrared Fourier-transform spectroscopy probe was used to investigate the adsorption-catalytic process and the possible synergistic catalytic mechanism (Langmuir-Hinshelwood and Mars-van Krevelen). This work provides a strategy for improving the catalyt Crystal structure ic oxidation performance of nanocatalysts for volatile organic compounds by increasing the catalytic oxygen activity.
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Diarylselenides are a representative class of molecules in organoselenium compounds. We herein report a Rh-catalyzed direct diarylation of selenium with benzamide derivatives. The use of elemental selenium as the Se source is intriguing in terms of atom economy, cost, stability, and handling. A series of diarylselenides with amide moieties were readily accessible through directed C-H activation. The intermediacy of electrophilic Se(IV) species was indicated by control experiments.
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Electrocatalyzed urea-assisted wastewater splitting is a promising approach for sustainable hydrogen production. However, the lack of cost-efficient electrocatalysts hinders its practical application. Herein, bimetal phosphide (NiCoPx) nanowire arrays decorated with ultrathin NiFeCo metal-organic framework (NiFeCo-MOF) nanosheets on porous nickel foam (NF) were designed for urea-assisted wastewater splitting. The core-shell NiCoPx@NiFeCo-MOF hybrids were prepared via successive hydrothermal, gas-phase phosphorization and hydrothermal strategies. Encouragingly, the novel NiCoPx@NiFeCo-MOF/NF electrode served as an excellent bifunctional electrocatalyst for both the cathodic hydrogen evolution reaction (HER) and the anodic urea oxidation reaction (UOR) in urea-assisted water splitting, which merely required an overpotential of 44 mV to deliver a current density of 10 mA cm-2 for HER and a voltage of 1.37 V to deliver a current density of 100 mA cm-2 for UOR in 1.0 M KOH + 0.5 M urea. Benefiting from the highly exposed electroactive sites in exquisite three-dimensional (3D) hierarchical structure, multicomponent synergistic effect, accelerated electron transfer, easy electrolyte access and diffusion of released gas bubbles, the as-fabricated NiCoPx@NiFeCo-MOF/NF exhibited outstanding electrocatalytic performance. The mechanism of water splitting was elucidated by density functional theory calculations. Interestingly, NiFeCo-MOF possessed optimized COO* adsorption ability on Ni sites that were beneficial to UOR intermediates. More significantly, this work paves the way for the design and fabrication of bifunctional electrocatalysts for urea-containing wastewater treatment and sustainable hydrogen production.
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Low mass-transfer efficiency and reaction-driving force make it difficult to realize thorough purification in traditional low-concentration pollutant treatments. Herein, we propose an "adsorption/catalysis in situ" perylene based bifunctional micelle for efficient, accurate and rapid adsorption and catalytic degradation of low-concentration bisphenol A (BPA). They show super-fast (within 10â s), high capacity (448â mg g-1 ) and selectivity for BPA adsorption, due to π-π, hydrophobic interactions and hydrogen bonding. The BPA degradation efficiency improves by up to 8â times after forming micelles compared with simple perylene nanorods, which is primarily due to the superior mass-transfer from adsorption. Moreover, self-assembly can optimize the stacking of the perylene moieties and facilitate charge transfer in micelle, and the regular π-π stacking of inside perylene units enhances the response to visible light, resulting in high catalytic capacity and good cycling stability.