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The complete removal of tetracycline residuals under visible light still is a challenging task because of their robust ring structure. To tackle this issue, we explore a novel Bi2O3-sensitized TiO2 visible-light photocatalyst by combining p-n heterojunction with hollow structure. The hollow TiO2/Bi2O3 photocatalyst manifests excellent photocatalytic performance and recyclability toward the complete degradation (100%) of antibiotics under visible light (λ > 420 nm) because of the synergistic effect of p-n heterojunction and hollow structure, successfully overcoming the challenge of the incomplete removal of antibiotics over almost all of the reported visible-light photocatalysts. selleck Additionally, the effects of inorganic ions, pH value, water matrix, and outdoor light on the degradation of tetracyclines were investigated with many details. Notably, the degradation pathways and mechanism of tetracycline were revealed according to trapping experiments, HPLC-MS, and photoelectrochemical characterizations. Therefore, this work provides a new insight into developing visible-light photocatalysts with excellent photocatalytic performances for the complete removal of other refractory contaminants.Most proteins in the α-macroglobulin (αM) superfamily contain reactive thiol esters that are required for their biological function. Here, we have characterized the human α2-macroglobulin (A2M) and complement component C3 mutants A2M Q975C and C3 Q1013C, which replace the CGEQ thiol ester motifs of the original proteins with the disulfide-forming sequence CGEC. Mass spectrometry showed that the intended disulfide was formed in both proteins. The correct folding and native conformation of A2M Q975C were shown by its assembly to a tetramer, an initially slow electrophoretic mobility with a demonstrable conformational collapse induced by proteolysis, functional protease trapping, and conformation-dependent interactions with low-density lipoprotein receptor-related protein 1. However, A2M Q975C had a decreased capacity to inhibit trypsin and was more susceptible to cleavage by trypsin or thermolysin when compared to wild-type A2M. C3 Q1013C also folded correctly and was initially in a native conformation, as demonstrated by its cation exchange elution profile, electrophoretic mobility, and interaction with complement factor B, although it assumed a conformation that was distinct from native C3, C3b, or C3(H2O) when cleaved by trypsin. These results demonstrate that disulfides can substitute thiol esters and maintain the native conformations of A2M and C3. Additionally, they indicate that proteolysis is not the sole factor in the conformational changes of A2M and C3 and that thiol ester lysis also plays a role.Sensitivity and linearity are two key parameters of flexible strain sensors. Although the introduction of microstructures (e.g., channel crack inspired by the geometry of the spider's slit organ) can effectively improve the sensitivity, the sudden breakage of the conductive path in turn leads to poor linearity. In practical applications, in order to achieve precise detection of subtle strains, high sensitivity and high linearity are required simultaneously. Here, we report a strain sensor design strategy based on the ductile fragmentation of functionalized graphene multilayers (FGMs) in which the conductive path is gradually broken to ensure high sensitivity while greatly improving the linear response of the sensor. The presence of oxygen-containing functional groups plays a key role in the deformation and fracture behaviors of the sensitive layer. High sensitivity (gauge factor ∼ 200) and high linearity (adjusted R-square ∼ 0.99936) have been achieved simultaneously in the strain range of 0-2.5%. In addition, the sensor also shows an ultralow detection limit (ε less then 0.001%), an ultrafast response (response time ∼ 50 μs), good stability, and good patterning capability compatible with complex curved surface manufacturing. These outstanding performances allow the FGM-based strain sensors to accurately distinguish the sound amplitude and frequency, highlighting the sensor's potential as smart devices for human voice detection. Such sensors have potential applications in the fields of smart skin, wearable electronics, robotics, and so on.Roxarsone (ROX) is widely used in animal farms, thereby producing organoarsenic-bearing manure/wastewater. ROX cannot be completely degraded and nor can its arsenical metabolites be effectively immobilized during anaerobic digestion, potentially causing arsenic contamination upon discharge to the environment. Herein, we designed and tested a sulfate-mediated bioelectrochemical system (BES) to enhance ROX degradation and in situ immobilization of the released inorganic arsenic. Using our BES (0.5 V voltage and 350 μM sulfate), ROX and its metabolite, 4-hydroxy-3-amino-phenylarsonic acid (HAPA), were completely degraded within 13-22 days. In contrast, the degradation efficiency of ROX and HAPA was less then 85% during 32-day anaerobic digestion. In a sulfate-mediated BES, 75.0-83.2% of the total arsenic was immobilized in the sludge, significantly more compared to the anaerobic digestion (34.1-57.3%). Our results demonstrate that the combination of sulfate amendment and voltage application exerted a synergetic effect on enhancing HAPA degradation and sulfide-driven arsenic precipitation. This finding was further verified using real swine wastewater. A double-cell BES experiment indicated that As(V) and sulfate were transported from the anode to the cathode chamber and coprecipitated as crystalline alacranite in the cathode chamber. These findings suggest that the sulfate-mediated BES is a promising technique for enhanced arsenic decontamination of organoarsenic-bearing manure/wastewater.Manipulating the dynamics of dark excited states (DESs), such as higher excited singlet or excited triplet states with no or small radiative decay, are of both fundamental and practical interests, an important application being photoactivated diagnosis and therapy (phototheranostics), which include photoacoustic (PA) imaging, photodynamic therapy (PDT), and photothermal therapy (PTT). However, the current understanding of DESs in organic structures is rather limited, thus making any rational manipulation of DES in organic materials very challenging.A DES decays primarily by radiationless transition through two pathways (i) singlet-to-triplet intersystem crossing (ISC) and (ii) internal conversion (IC) relaxation. The deactivation of a DES via ISC can generate cytotoxic reactive oxygen species (ROS) for PDT, while IC could convert photons into heat for PA imaging and PTT. In this Account, we highlight our research on developing a fundamental understanding of structure-property relationships for manipulation ofn for cumulative multiphoton absorption, thus greatly increasing the strength of the PA signal for nonlinear PA imaging, and (2) shown by an example of an organic molecule, BODIPY, nanoscale charge-transfer state mediated strong IC in aggregate nanoparticles resulting in exceptionally high photothermal conversion efficiency of 61% for both PA and PTT. Some in vivo results of the phototheranostic studies using BODIPY are presented, providing an elegant example of nanoscale manipulation of the excited state dynamics.This Account concludes with a summary and discussion of future perspectives. We hope this Account will deepen the understanding of molecular and nanoscale control of excited state dynamics in organic materials, hopefully enticing a broad range of scientists within different disciplinary areas.Heart failure is the terminal stage of many cardiovascular diseases and is considered to be closely related to oxidative stress. Early understanding of pathogenesis can greatly improve the treatment and reduce the mortality of heart disease. In this work, based on the analysis of coumarin derivates by theoretical calculations, we designed and synthesized a fluorescent probe BCO with a large Stokes shift (107 nm) and excellent selectivity toward H2O2 in a living system. The distribution of H2O2 in the heart and thoracic aorta tissues was imaged with the aid of the probe BCO, which demonstrated that the cellular H2O2 level is upregulated in heart failure. This work provides a useful tool, BCO, for the evaluation of cellular oxidative stress and to further understand the pathophysiology process of heart disease.The human body emits a wide range of chemicals, including CO2 and isoprene. To examine the impact of cognitive tasks on human emission rates of CO2 and isoprene, we conducted an across-subject, counterbalanced study in a controlled chamber involving 16 adults. The chamber replicated an office environment. In groups of four, participants engaged in 30 min each of cognitive tasks (stressed activity) and watching nature documentaries (relaxed activity). Measured biomarkers indicated higher stress levels were achieved during the stressed activity. Per-person CO2 emission rates were greater for stressed than relaxed activity (30.3 ± 2.1 vs 27.0 ± 1.7 g/h/p, p = 0.0044, mean ± standard deviation). Isoprene emission rates were also elevated under stressed versus relaxed activity (154 ± 25 μg/h/p vs 116 ± 20 μg/h/p, p = 0.041). The chamber temperature was held constant at 26.2 ± 0.49 °C; incidental variation in temperature did not explain the variance in emission rates. Isoprene emission rates increased linearly with salivary α-amylase levels (r2 = 0.6, p = 0.02). These results imply the possibility of considering cognitive tasks when determining building ventilation rates. They also present the possibility of monitoring indicators of cognitive tasks of occupants through measurement of air quality.Escherichia coli Nissle 1917 (EcN) is a probiotic bacterium, commonly employed to treat certain gastrointestinal disorders. It is fast emerging as an important target for the development of therapeutic engineered bacteria, benefiting from the wealth of knowledge of E. coli biology and ease of manipulation. Bacterial synthetic biology projects commonly utilize engineered plasmid vectors, which are simple to engineer and can reliably achieve high levels of protein expression. However, plasmids typically require antibiotics for maintenance, and the administration of an antibiotic is often incompatible with in vivo experimentation or treatment. EcN natively contains plasmids pMUT1 and pMUT2, which have no known function but are stable within the bacteria. Here, we describe the development of the pMUT plasmids into a robust platform for engineering EcN for in vivo experimentation, alongside a CRISPR-Cas9 system to remove the native plasmids. We systematically engineered both pMUT plasmids to contain selection markers, fluorescent markers, temperature sensitive expression, and curli secretion systems to export a customizable functional material into the extracellular space. We then demonstrate that the engineered plasmids were maintained in bacteria as the engineered bacteria pass through the mouse GI tract without selection, and that the secretion system remains functional, exporting functionalized curli proteins into the gut. Our plasmid system presents a platform for the rapid development of therapeutic EcN bacteria.
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