Pt-O-Ce interaction enhanced by Al substitution to promote the acetone degradation through accelerating the breaking of CC bond in acetic acid intermediate.

The reaction rate of volatile organic compounds (VOCs) oxidation is controlled by the rate-limiting step in the total reaction process. This study proposes a novel strategy, by which the rate-limiting step of acetone oxidation is accelerated by enhanced chemical bond interaction with more electrons transfer through Al-substituted CeO2 loaded Pt (Pt/Al-CeO2). Results indicate that the rate-limiting step in the process of acetone oxidation is the decomposition of acetic acid. Al substitution enhances the Pt-O-Ce interaction that transfers more electrons from Pt/Al-CeO2 to acetic acid, promoting the breaking of its CC bond with a lower free energy barrier. Attributing to these, the reaction rate of Pt/Al-CeO2 is 13 times as high as that of Pt/CeO2 and its TOFPt value is 11 times as high as that of Pt/CeO2 at 150 °C. Moreover, the CO2 selectivity of Pt/Al-CeO2 also increases by 22 %. This work establishes the relationship between Pt-O-Ce interaction and acetone oxidation that provides novel perspectives on the development of efficient materials for VOCs oxidation.

Innervation of nociceptor neurons in the spleen promotes germinal center responses and humoral immunity.

Peripheral sensory neurons widely innervate various tissues to continuously monitor and respond to environmental stimuli. Whether peripheral sensory neurons innervate the spleen and modulate splenic immune response remains poorly defined. Here, we demonstrate that nociceptive sensory nerve fibers extensively innervate the spleen along blood vessels and reach B cell zones. The spleen-innervating nociceptors predominantly originate from left T8-T13 dorsal root ganglia (DRGs), promoting the splenic germinal center (GC) response and humoral immunity. Nociceptors can be activated by antigen-induced accumulation of splenic prostaglandin E2 (PGE2) and then release calcitonin gene-related peptide (CGRP), which further promotes the splenic GC response at the early stage. Mechanistically, CGRP directly acts on B cells through its receptor CALCRL-RAMP1 via the cyclic AMP (cAMP) signaling pathway. Activating nociceptors by ingesting capsaicin enhances the splenic GC response and anti-influenza immunity. Collectively, our study establishes a specific DRG-spleen sensory neural connection that promotes humoral immunity, suggesting a promising approach for improving host defense by targeting the nociceptive nervous system.

Acetone Efficient Degradation under Simulated Humid Conditions by Mn-O-Pt Interaction Taming-Triggered Water Dissociation Intensification.

As a generally existing component in industrial streams, H2O usually inhibits the catalytic degradation efficiency of volatile organic compounds (VOCs) greatly. Here, we propose a novel strategy that accelerates the H2O dissociation and facilitates positive feedbacks during VOC oxidation by fabricating citric acid (CA)-assisted Pt(K)-Mn2O3/SiO2 (Pt-Mn/KS-xCA). Results reveal that the complexation of carboxyl groups of citric acid with Mn cations leads to the formation of small Mn2O3 (4.1 ± 0.2 nm) and further enhances the Mn-O-Pt interaction (strengthened by the Si-O-Mn interaction), which can transfer more electrons from Pt-Mn/KS-6CA to H2O, thus facilitating its breaking of covalent bonds. It subsequently produces abundant surface hydroxyl groups, improving the adsorption and activation abilities of acetone reactant and ethanol intermediate. Attributing to these, the acetone turnover frequency value of Pt-Mn/KS-6CA is 1.8 times higher than that of Pt-Mn/KS at 160 °C, and this multiple changes to 6.3 times in the presence of H2O. Remarkably, acetone conversion over Pt-Mn/KS-6CA increases by up to 14% in the presence of H2O; but it decreases by up to 26% for Pt-Mn/KS due to its weak dissociation ability and high adsorption capacity toward H2O. This work sheds new insights into the design of highly efficient catalytic materials for VOC degradation under humid conditions.

Characterization of atmospheric mercury from mercury-added product manufacturing using passive air samplers.

Although alternatives to mercury (Hg) are available in most products and industrial activities, Hg continues to be an ingredient in some products, including fluorescent lamps and electrical and electronic equipment (EEE). In this work, low-cost passive air samplers (PASs) were used to investigate the atmospheric Hg pollution in Zhongshan, a large industrial city and major hub of mercury-added product manufacturing in South China. The GEM concentrations in the atmosphere were measured for two weeks during the summer of 2019 at a total of 144 sites across Zhongshan. Comparison with the results of active sampling confirmed that the PASs yielded accurate and reliable gaseous elemental mercury (GEM) concentrations and were thus well-suited for multi-site field monitoring. The mean GEM concentrations in the areas with mercury-added product manufacturing activities (5.1 ± 0.4 ng m-3) were significantly higher than those in other parts of Zhongshan (1.5 ± 0.4 ng m-3), indicating that local releases, rather than regional transport, were responsible for the atmospheric Hg pollution. Elevated GEM concentrations (up to 11.4 ng m-3) were found in the vicinity of fluorescent lamp and EEE factories and workshops, indicating significant Hg vapor emissions, presumably from the outdated production technologies and non-standard operation by under-trained workers. The Hg emissions from mercury-added product manufacturing were estimated to be 0.06 and 7.8 t yr-1 for Zhongshan and China, respectively, based on the scales of fluorescent lamp and EEE production. The non-carcinogenic health risk of Zhongshan residents from inhalation and ingestion was judged acceptable, whereby the inhalation exposure in Hg-polluted areas exceeded that of dietary ingestion. These findings demonstrate that mercury-added product manufacturing still contributes notably to anthropogenic gaseous Hg releases in the industrial areas with intense mercury-added product manufacturing activities.

Accelerating the Low-Temperature Catalytic Oxidation of Acetone over Al-Substituted Mn-Al Oxides by Rate-Limiting Step Modulation.

In order to enhance the catalytic activity and improve the stability of Mn-Al oxides in acetone oxidation, it is interesting to have found that modulating and accelerating the rate-limiting step by Al substitution rather than just mixing of Mn and Al is crucial for hydrocarbon efficient catalytic destruction. Here, a series of Mn-Al oxides with different Al substitution ratios were prepared by a scalable and facile hydrothermal-redox strategy. The reaction rate, selectivity, and stability of the representative α-MnO2 catalyst in acetone oxidation can be remarkably promoted by simple replacing of the partial framework Mn with Al, which changes the rate-limiting step from acetic acid dissociation to ethanol decomposition accelerated by H2O molecules. Among them, MnAl0.5 displays the best catalytic performance with 90% of acetone converted at just 165 °C and a remarkable CO2 yield. DFT results suggest that the py and px orbitals of the O element take part in the formation of the carbonyl group when the intermediate of removing H* from ethanol reacts with the hydroxyl group of H2O. The dxz orbital of Mn with p-electron of Al plays a vital role in the rate-limiting step. The work provides new insights into engineering catalysts for industrial VOC efficient and economical mineralization.

A New Fusion Fault Diagnosis Method for Fiber Optic Gyroscopes.

The fiber optic gyroscope (FOG) is a high precision inertial navigation device, and it is necessary to ensure its reliability for effective use. However, the extracted fault features are easily distorted due to the interference of vibrations when the FOG is in operation. In order to minimize the influence of vibrations to the greatest extent, a fusion diagnosis method was proposed in this paper. It extracted features from fault data with Fast Fourier Transform (FFT) and wavelet packet decomposition (WPD), and built a strong diagnostic classifier with a sparse auto encoder (SAE) and a neural network (NN). Then, a fusion neural network model was established based on the diagnostic output probabilities of the two primary classifiers, which improved the diagnostic accuracy and the anti-vibration capability. Then, five fault types of the FOG under random vibration conditions were established. Fault data sets were collected and generated for experimental comparison with other methods. The results showed that the proposed fusion fault diagnosis method could perform effective and robust fault diagnosis for the FOG under vibration conditions with a high diagnostic accuracy.

Promotional effects of calcination temperature and H2O on the catalytic activity of Al-substituted MnAlO catalysts for low-temperature acetone oxidation.

In order to enhance the role of Al in the materials, Al-substituted MnAlO catalysts were synthesized via the hydrothermal-redox method at different calcination temperatures for acetone oxidation. There were Al-substituted α-MnO2 and amorphous aluminum oxide existed with homogeneous dispersion of elements in the catalysts. The surface property, reaction rate, CO2 yield and water resistance of MnAlO catalysts were greatly affected by calcination temperatures. MnAlO-450 catalyst exhibited the best catalytic performance (acetone conversion of 90% at 165 °C) with CO2 yield higher than 99.7%, which was mainly related to the weaker Mn-O bond strength, lower temperature reducibility and abundant Lewis acid sites. The acetone conversion of MnAlO-450 increased by as much as 16% in the presence of 1 vol% H2O compared to that in the absence of H2O at T50 (the temperature for 50% conversion of acetone). The acceleration consumption of ethanol as the main by-product by H2O improved the catalytic performance. This work would shed light on the Al substitution based catalysts for OVOC oxidation with highly efficient and water resistance.

Effects of pulsed ultrasound treatment on the physicochemical and textural properties of chicken myofibrillar protein gel.

This study explored the effects of varying the time of pulsed ultrasound (PUS) treatment on the physicochemical and textural properties of chicken myofibrillar protein (CMP) gel. The solubility rapidly increased at ≤ 6 min and then steadily decreased, while the particle size showed the opposite trend. At longer PUS treatment times, the total sulfhydryl（-SH）and reactive SH content of CMP gel all decreased. The absolute value of the zeta potential and surface hydrophobicity at 6 min were higher. The most hydrogen bonds were formed. G' and G″ were also optimal, indicating that a more viscoelastic gel was formed. Meanwhile, the textural properties (including hardness and springiness) were significantly improved by PUS. These findings show that PUS significantly affected the physicochemical and textural properties of CMP gel, and at 6 min, the best gel hardness and springiness were achieved.

An Integrated Compensation Method for the Force Disturbance of a Six-Axis Force Sensor in Complex Manufacturing Scenarios.

As one of the key components for active compliance control and human-robot collaboration, a six-axis force sensor is often used for a robot to obtain contact forces. However, a significant problem is the distortion between the contact forces and the data conveyed by the six-axis force sensor because of its zero drift, system error, and gravity of robot end-effector. To eliminate the above disturbances, an integrated compensation method is proposed, which uses a deep learning network and the least squares method to realize the zero-point prediction and tool load identification, respectively. After that, the proposed method can automatically complete compensation for the six-axis force sensor in complex manufacturing scenarios. Additionally, the experimental results demonstrate that the proposed method can provide effective and robust compensation for force disturbance and achieve high measurement accuracy.

BKM120 sensitizes BRCA-proficient triple negative breast cancer cells to olaparib through regulating FOXM1 and Exo1 expression.

Poly (ADP-ribose) polymerase (PARP) inhibitors offer a significant clinical benefit for triple-negative breast cancers (TNBCs) with BRCA1/2 mutation. However, the narrow clinical indication limits the development of PARP inhibitors. Phosphoinositide 3-kinase (PI3K) inhibition sensitizes BRCA-proficient TNBC to PARP inhibition, which broadens the indication of PARP inhibitors. Previously researches have reported that PI3K inhibition induced the defect of homologous recombination (HR) mediated repair by downregulating the expression of BRCA1/2 and Rad51. However, the mechanism for their synergistic effects in the treatment of TNBC is still unclear. Herein, we focused on DNA damage, DNA single-strand breaks (SSBs) repair and DNA double-strand breaks (DSBs) repair three aspects to investigate the mechanism of dual PI3K and PARP inhibition in DNA damage response. We found that dual PI3K and PARP inhibition with BKM120 and olaparib significantly reduced the proliferation of BRCA-proficient TNBC cell lines MDA-MB-231 and MDA231-LM2. BKM120 increased cellular ROS to cause DNA oxidative damage. Olaparib resulted in concomitant gain of PARP1, forkhead box M1 (FOXM1) and Exonuclease 1 (Exo1) while inhibited the activity of PARP. BKM120 downregulated the expression of PARP1 and PARP2 to assist olaparib in blocking PARP mediated repair of DNA SSBs. Meanwhile, BKM120 inhibited the expression of BRAC1/2 and Rad51/52 to block HR mediated repair through the PI3K/Akt/NFκB/c-Myc signaling pathway and PI3K/Akt/ FOXM1/Exo1 signaling pathway. BKM120 induced HR deficiency expanded the application of olaparib to HR proficient TNBCs. Our findings proved that PI3K inhibition impaired the repair of both DNA SSBs and DNA DSBs. FOXM1 and Exo1 are novel therapeutic targets that serves important roles in DNA damage response.

Efficient catalytic degradation of toluene at a readily prepared Mn-Cu catalyst: Catalytic performance and reaction pathway.

Fabricating of economical transitional metal oxide-based materials with satisfied low-temperature catalytic performance and application perspective is still a challenge in deep degradation of VOCs. Here, Mn-Cu bimetallic oxides were facilely prepared by one-step hydrothermal-redox method, which displayed much higher catalytic activity in toluene oxidation than those synthesized by hydrolysis-driven redox-precipitation or co-precipitation approach. It is shown that the lattice defect and oxygen vacancy concentration over prepared materials can be tuned by controlling Cu/Mn molar ratio. Amongst, spinel structured MnCu0.5 exhibited the highest catalytic activity, superior durability and water resistance in toluene total oxidation owing to abundant surface adsorbed oxygen species, excellent low-temperature reducibility, and high amounts of Cu+ and Mn3+. In detail, the reaction rate of MnCu0.5 was over 9.0 times higher than that of MnCu0.75, MnCu0.75-P and MnCu0.75-H2O2 at relative low temperature of 210 °C. The cyclic redox process with easier oxygen species mobility played a key role in the catalytic oxidation of toluene. Typical reaction intermediates as benzyl alcohol, benzaldehyde, benzene, phenol, and benzoquinone could be detected by PTR-MS, which further decomposed to acetone, ethanol, ketone, acetic acid, methanol, formaldehyde and acetaldehyde species by ring opening before total mineralization.

Atmospheric mercury pollution caused by fluorescent lamp manufacturing and the associated human health risk in a large industrial and commercial city.

Although already eliminated in most industrial processes, mercury, as an essential ingredient in all energy-efficient lighting technologies, is still used in fluorescent lamp manufacturing. This study was conducted to investigate the atmospheric pollution caused by fluorescent lamp production and assess the associated public health risk in a large industrial and commercial city of south China, Zhongshan, which is a major production hub of lighting products. Concentrations of total gaseous mercury (TGM) in the atmosphere were measured over a total of 342 sites in the industrial, commercial, and residential areas. The average levels of TGM in the industrial, commercial, and residential areas prior to the landing of a typhoon were 12 ± 11, 3.6 ± 2.1, and 2.7 ± 1.3 ng⋅m-3, respectively. TGM concentrations in the industrial areas exhibited significant diurnal variation, with levels in the working hours being much higher than those in the non-working hours, which indicates that the high atmospheric mercury concentrations were contributed by local emissions, instead of regional transport. Most fluorescent lamp manufacturing activities in the city were shut down during a typhoon event, which resulted in a significant reduction in the average TGM level (down to 1.6 ± 1.8 ng⋅m-3) and rendered the difference in the average TGM levels in the industrial areas no longer significant between the working and non-working hours. Elevated TGM levels (up to 49 ng⋅m-3) were found near clusters of small-scale fluorescent lamp workshops in both industrial and commercial areas, which is indicative of significant emissions of mercury vapor resulting from obsolete equipment and production technologies. No significant non-carcinogenic risk was found for the general residents in the sampling area over the study period, while the risk for the workers in the fluorescent lamp manufacturing facilities and workshops could be higher. These findings indicate that fluorescent lamp manufacturing in the developing countries is a major source of atmospheric mercury.

Development of a photoelectric phase-locked loop model to better synchronize frequency combs and microwaves.

The high phase coherence between ultralow-noise microwaves and ultrahigh-stable optical frequency combs (OFCs) is of both scientific and technological relevance for telecommunication, timekeeping, astronomy, and metrology. Here, a photoelectric phase-locked loop (PLL) model with ultralow phase noise based on the optical-microwave phase detector technique has been proposed and experimentally demonstrated. A detailed mathematical model for tight, real-time phase synchronization of OFCs and microwaves is developed to investigate the feasibility and analyze the characteristics of the phase-coherent system. We fabricate a compact PLL circuit with a proportional-integral-derivative regulator for the synchronization of an OFC to a microwave reference. Once synchronized, the long-term stability of the OFC agrees to 2.4×10-14 at a 1000 s averaging time, which is enhanced by more than 4 orders of magnitude. Besides, the OFC almost acquires the same frequency stability as the microwave source. The ability to better phase synchronize OFCs and microwaves enables a wide range of applications beyond the laboratory.