Unveiling the Dynamic Electrocatalytic Activity of Online Synthesized Bimetallic Nanocatalysts via Electrochemiluminescence Microscopy.

Effective bimetallic nanoelectrocatalysis demands precise control of composition, structure, and understanding catalytic mechanisms. To address these challenges, we employ a two-in-one approach, integrating online synthesis with real-time imaging of bimetallic Au@Metal core-shell nanoparticles (Au@M NPs) via electrochemiluminescence microscopy (ECLM). Within 120 s, online electrodeposition and in situ catalytic activity screening alternate. ECLM captures transient faradaic processes during potential switches, visualizes electrochemical processes in real-time, and tracks catalytic activity dynamics at the single-particle level. Analysis using ECL photon flux density eliminates size effects and yields quantitative electrocatalytic activity results. Notably, a nonlinear activity trend corresponding to the shell metal to Au surface atomic ratio is discerned, quantifying the optimal surface component ratio of Au@M NPs. This approach offers a comprehensive understanding of catalytic behavior during the deposition process with high spatiotemporal resolution, which is crucial for tailoring efficient bimetallic nanocatalysts for diverse applications.

Photoinduced Electrogenerated Chemiluminescence Imaging of Plasmonic Photoelectrochemistry at Single Nanocatalysts.

In this study, we proposed a novel imaging technique, photoinduced electrogenerated chemiluminescence microscopy (PECLM), to monitor redox reactions driven by hot carriers on single gold nanoparticles (AuNPs) on TiO2. Under laser irradiation, plasmon-generated hot carriers were separated by an electric field, leaving hot holes on the surface of AuNPs to drive ECL reactions. PECL intensity was highly sensitive to the number of hot carriers. Through quantitative image analysis, we found that PECL density on individual AuNPs decreased significantly with an increase in particle diameter, indicating that particle size has a significant impact on photoelectrochemical conversion efficiency. For the first time, we verified the feasibility of PECLM in mapping the catalytic activity of single photocatalysts. PECLM opens a new prospect for the in situ imaging of photocatalysis in a high-throughput way, which not only facilitates the optimization of plasmonic photocatalysts but also contributes to the dynamic study of photocatalytic processes on micro/nanointerfaces.

Electrogenerated Chemiluminescence Imaging of Single-Atom Nanocatalysts.

Single-atom catalysts (SACs), distinguished by their maximum atom efficiency and precise control over the coordination and electronic properties of individual atoms, show great promise in electrocatalysis. Gaining a comprehensive understanding of the electrochemical performance of SACs requires the screening of electron transfer process at micro/nano scale. This research pioneers the use of electrogenerated chemiluminescence microscopy (ECLM) to observe the electrocatalytic reactions at individual SACs. It boasts sensitivity at the single photon level and temporal resolution down to 100 ms, enabling real-time capture of the electrochemical behavior of individual SACs during potential sweeping. Leveraging the direct correlation between ECL emission and heterogeneous electron transfer processes, we introduced photon flux density for quantitative analysis, unveiling the electrocatalytic efficiency of individual SACs. This approach systematically reveals the relationship between SACs based on different metal atoms and their peroxidase (POD)-like activity. The outcomes contribute to a fundamental understanding of SACs and pave the way for designing SACs with diverse technological and industrial applications.

Cascade Reaction Regulated Electrochemiluminescence via Dual-Atomic-Site Catalysts.

Single-atom catalysts (SACs), a novel kind of electrocatalysts with full metal utilization, have been developed as unique signal amplifiers in several sensing platforms. Herein, based on theoretical prediction of the oxygen reduction reaction (ORR) mechanism on different atom sites, we constructed dual-atomic-site catalysts (DACs), Fe/Mn-N-C, to catalyze luminol-dissolved oxygen electrochemiluminescence (ECL). Computational simulation indicated that the weak adsorption of OH* on a single Fe site was overcome by introducing Mn as the secondary metallic active site, resulting in a synergic dual-site cascade mechanism. The superior catalytic activity of Fe/Mn-N-C DACs for the ORR was proven by the highly efficient cathodic luminol ECL, surpassing the performance of single-site catalysts (SACs), Fe-N-C and Mn-N-C. Furthermore, the ECL system, enhanced by a cascade reaction, exhibited remarkable sensitivity to ascorbic acid, with a detection limit of 0.02 nM. This research opens up opportunities for enhancing both the ECL efficiency and sensing performance by employing a rational atomic-scale design for DACs.

Malaria epidemiological characteristics and control in Guangzhou, China, 1950-2022.

BACKGROUND: Malaria was once widespread in Guangzhou, China. However, a series of control measures have succeeded in eliminating local malaria infections. Based on the analysis of the characteristics of malaria epidemics in Guangzhou, China, from 1950 to 2022, the changes and effectiveness of malaria control strategies and surveillance management in Guangzhou from 1950 to 2022 are described. METHODS: Data on malaria prevention and treatment in Guangzhou from 1950 to 2022 were collected, and descriptive epidemiological methods were used to analyse the prevalence of malaria, preventive and control measures taken, and the effectiveness of prevention and treatment in different periods. Data on malaria cases were obtained from the Guangzhou Centre for Disease Control and Prevention (CDC) and the China Communicable Disease Reporting System. RESULTS: The development of the malaria control system in Guangzhou has gone through four periods: 1. High malaria prevalence (1950-1979), 2. Intensive prevention and control stage (1980-2000), 3. Consolidating gains in malaria control (2001-2008), and 4. Preventing reestablishment of transmission (2009-2022). During Period 1, only medical institutions at all levels and the local CDCs, the Guangzhou CDC participated in the malaria prevention and control system, establishing a three-tier health system on malaria prevention and control. During Period 2, other types of organizations, including the agricultural sector, schools and village committees, the construction department and street committee, are involved in the malaria control system. During Period 3, more and more organizations are joining forces to prevent and control malaria. A well-established multisectoral malaria control mechanism and an improved post-elimination surveillance management system are in place. Between 1950 and 2022, a total of 420,670 cases of malaria were reported. During Period 1, there was an epidemic of malaria in the early 1950s, with an annual incidence rate of more than 10,000/100,000, including a high rate of 2887.98/100,000 in 1954. In Period 2 malaria was gradually brought under control, with the average annual malaria incidence rate dropping to 3.14/100,000. During Period 3, the incidence rate was kept below 1/100,000, and by 2009 local malaria infections were eliminated. CONCLUSION: For decades, Guangzhou has adopted different malaria control strategies and measures at different epidemic stages. Increased collaboration among civil organizations in Guangzhou in malaria control has led to a significant decline in the number of malaria cases and the elimination of indigenous malaria infections by 2009.The experience of Guangzhou can guide the development of malaria control strategies in other cities experiencing similar malaria epidemics.

Sacral dural arteriovenous fistula supplied by bilateral lateral sacral arteries: case report and literature review.

Sacral dural arteriovenous fistulas (DAVFs) with bilateral arterial supplies are extremely rare. To date, only two cases with arterial supply from bilateral lateral sacral arteries (LSAs) were reported. We report a rare case of sacral DAVF with arterial supply from bilateral LSAs. A 56-year-old man presented with a 2-month history of progressive weakness and numbness in his lower extremities, along with urinary incontinence. Spinal magnetic resonance imaging (MRI) showed extensive edema of the spinal cord, vascular flow voids, and intraparenchymal enhancement. Spinal angiography revealed a spinal DAVF at the level of S1 supplied by bilateral LSAs and drained ascending into the perimedullary venous plexus. The fistula was successfully treated with endovascular embolization. Sacral DAVFs present various diagnostic and treatment difficulties because of the complex angioarchitecture. Successful management of these lesions requires a profound understanding of the variable patterns of arterial supply in this region.

Stability analysis and optimal control of a fractional-order generalized SEIR model for the COVID-19 pandemic.

In view of the spread of corona virus disease 2019 (COVID-19), this paper proposes a fractional-order generalized SEIR model. The non-negativity of the solution of the model is discussed. Based on the established threshold R0, the existence of the disease-free equilibrium and endemic equilibrium is analyzed. Then, sufficient conditions are established to ensure the local asymptotic stability of the equilibria. The parameters of the model are identified based on the statistical data of COVID-19 cases. Furthermore, the validity of the model for describing the COVID-19 outbreak is verified. Meanwhile, the accuracy of the relevant theoretical results are also verified. Considering the relevant strategies of COVID-19 prevention and control, the fractional optimal control problem (FOCP) is proposed. Numerical schemes for Riemann-Liouville (R-L) fractional-order adjoint system with transversal conditions is presented. Based on the relevant statistical data, the corresponding FOCP is numerically solved, and the control effect of the COVID-19 outbreak under the optimal control strategy is discussed.

Stability analysis of a nonlocal SIHRDP epidemic model with memory effects.

The prediction and control of COVID-19 is critical for ending this pandemic. In this paper, a nonlocal SIHRDP (S-susceptible class, I-infective class (infected but not hospitalized), H-hospitalized class, R-recovered class, D-death class and P-isolated class) epidemic model with long memory is proposed to describe the multi-wave peaks for the spread of COVID-19. Based on the basic reproduction number R 0 , which is completely controlled by fractional order, the stability of the proposed system is studied. Furthermore, the numerical simulation is conducted to gauge the performance of the proposed model. The results on Hunan, China, reveal that R 0 < 1 suggests that the disease-free equilibrium point is globally asymptotically stable. Likewise, the situation of the multi-peak case in China is presented, and it is clear that the nonlocal epidemic system has a superior fitting effect than the classical model. Finally an adaptive impulsive vaccination is introduced based on the proposed system. Then employing the real data of France, India, the USA and Argentina, parameters identification and short-term forecasts are carried out to verify the effectiveness of the proposed model in describing the case of multiple peaks. Moreover, the implementation of vaccine control is expected once the hospitalized population exceeds 20 % of the total population. Numerical results of France, Indian, the USA and Argentina shed light on the varied effect of vaccine control in different countries. According to the vaccine control imposed on France, no obvious effect is observed even consider reducing human contact. As for India, although there will be a temporary increase in hospitalized admissions after execution of vaccination control, COVID-19 will eventually disappear. Results on the USA have seen most significant effect of vaccine control, the number of hospitalized individuals drops off and the disease is eventually eradicated. In contrast to the USA, vaccine control in Argentina has also been very effective, but COVID-19 cannot be completely eradicated.

Single Cell Imaging of Electrochemiluminescence-Driven Photodynamic Therapy.

We report a photodynamic therapy driven by electrochemiluminescence (ECL). The luminescence generated by Ru(bpy)32+ and co-reactant tripropylamine (TPA) pair acts as both optical readout for ECL imaging, and light source for the excitation of photosensitizer to produce reactive oxygen species (ROS) in photodynamic therapy (PDT) system. The ECL-driven PDT (ECL-PDT) relies on the effective energy transfer from ECL emission to photosensitizer chlorin e6 (Ce6), which sensitizes the surrounding O2 into ROS. The dynamic process of gradual morphological changes, the variation of cell-matrix adhesions, as well as the increase of cell membrane permeability in the process of ECL-PDT were monitored under ECL microscopy (ECLM) with good spatiotemporal resolution. Combining real-time imaging with ECL-PDT, this new strategy provides not only new insights into dynamic cellular processes, but also promising potential of ECL in clinical applications.

Sewage as a Possible Transmission Vehicle During a Coronavirus Disease 2019 Outbreak in a Densely Populated Community: Guangzhou, China, April 2020.

BACKGROUND: Sewage transmission of SARS-CoV-2 has never been demonstrated. During a COVID-19 outbreak in Guangzhou, China in April 2020, we investigated the mode of transmission. METHODS: We collected clinical and environmental samples from quarantined residents and their environment for RT-PCR testing and genome sequencing. A case was a resident with a positive RT-PCR test regardless of symptoms. We conducted a retrospective cohort study of all residents of cases' buildings to identify risk factors. RESULTS: We found 8 cases (onset: 5-21 April). During incubation period, cases 1 and 2 frequented market T where a COVID-19 outbreak was ongoing; cases 3-8 never visited market T, lived in separate buildings and never interacted with cases 1 and 2. Working as a janitor or wastepicker (RR = 13; 95% CIexact, 2.3-180), not changing to clean shoes (RR = 7.4; 95% CIexact, 1.8-34) and handling dirty shoes by hand (RR = 6.3; 95% CIexact, 1.4-30) after returning home were significant risk factors. RT-PCR detected SARS-CoV-2 in 19% of 63 samples from sewage puddles or pipes, and 24% of 50 environmental samples from cases' apartments. Viruses from the squat toilet and shoe-bottom dirt inside the apartment of cases 1 and 2 were homologous with those from cases 3-8 and the sewage. Sewage from the apartment of cases 1 and 2 leaked out of a cracked pipe onto streets. Rainfall after the onset of cases 1 and 2 flooded the streets. CONCLUSIONS: SARS-CoV-2 might spread by sewage, highlighting the importance of sewage management during outbreaks.

Super-Resolution Electrogenerated Chemiluminescence Microscopy for Single-Nanocatalyst Imaging.

Electrogenerated chemiluminescence microscopy (ECLM) provides a real-time imaging approach to visualize the surface-dependent catalytic activity of nanocatalysts, which helps to rationalize the design of catalysts. In this study, we first propose super-resolution ECLM that could measure the facet- and site-specific activities of a single nanoparticle with nanometer resolution. The stochastic nature of the ECL emission makes the generation of photons obey Poisson statistics, which fits the requirement of super-resolution radial fluctuation (SRRF). By processing an SRRF algorithm, the spatial resolution of ECL images achieved ca. 100 nm, providing more abundant details on electrocatalytic reactivities at the subparticle level. Beyond conventional wide-field ECL imaging, super-resolution ECLM provided the spatial distribution of catalytic activities at a Au nanorod and nanoplate with scales of a few hundred nanometers. It helped uncover the facet- and defect-dependent surface activity, as well as the dynamic fluctuation of reactivity patterns on single nanoparticles. The super-resolution ECLM provides high spatiotemporal resolution, which shows great potential in the field of catalysis, biological imaging, and single-entity analysis.

Alkaline Phosphatase-Triggered Etching of Au@FeOOH Nanoparticles for Enzyme Level Assay under Dark-Field Microscopy.

In clinical diagnosis, the level of biological enzymes in serum has been generally regarded as markers of human diseases. In this work, a kind of simple and sensitive plasmonic probe (indicated as Au@FeOOH) has been synthesized with the guidance of plasmonic imaging and subsequently developed for the alkaline phosphatase (ALP) level detection under dark-field microscopy (DFM). As a kind of hydrolysis enzyme, ALP can promote the hydrolysis of l-ascorbic acid 2-phosphate to ascorbic acid (AA). AA further acts as a strong reduction reagent for the decomposition of the FeOOH shell, which results in a blue shift of localized surface plasmon resonance spectra and an obvious color change under DFM. RGB analyses show that using a ΔR/G value instead of scattering wavelength or R/G value as the analytical signal, the deviation attributed to the size distribution of the initial Au NPs is greatly suppressed, and a linear range from 0.2 to 6.0 U/L (R2 = 0.99) and a limit of detection of 0.06 U/L are acquired with various concentrations of ALP during the detection. Besides, this approach exhibits excellent selectivity in complex biological serum samples, which is expected to be applied for the early diagnosis of clinical diseases by monitoring various biomarkers in the future.

Secondary Transmission of Coronavirus Disease from Presymptomatic Persons, China.

We explored the secondary attack rate in different types of contact with persons presymptomatic for coronavirus disease (COVID-19). Close contacts who lived with or had frequent contact with an index case-patient had a higher risk for COVID-19. Our findings provide population-based evidence for transmission from persons with presymptomatic COVID-19 infections.

COVID-19 Outbreak Associated with Air Conditioning in Restaurant, Guangzhou, China, 2020.

During January 26-February 10, 2020, an outbreak of 2019 novel coronavirus disease in an air-conditioned restaurant in Guangzhou, China, involved 3 family clusters. The airflow direction was consistent with droplet transmission. To prevent the spread of the virus in restaurants, we recommend increasing the distance between tables and improving ventilation.

Real-Time Tracking the Electrochemical Synthesis of Au@Metal Core-Shell Nanoparticles toward Photo Enhanced Methanol Oxidation.

Single particle plasmon scattering can provide real-time imaging information on the synthesis of nanomaterials. Here, an electrochemical deposition strategy is reported to synthesize plasmonic Au@Metal core-shell nanoparticles (Au@M NPs), which exhibit localized surface plasmon resonance (LSPR) properties. Because of the excellent catalytic activity of the methanol oxidation reaction (MOR), Pt, Pd, and Rh were reduced on the surface of Au NPs to form monometallic and bimetallic shells. Under dark field microscopy (DFM), the scattering changes could be utilized to track the surface nucleation and bulk deposition process. The synthesized Au@M NPs, which combined the plasmonic and electrocatalytic features, showed greatly enhanced activity for MOR. Under LSPR excitation, the electroxidation process toward MOR was accelerated and increased approximately linearly with increased illumination intensity, which could be mostly attributed to the generation of energetic charge carriers. This strategy of real-time plasmonic tracking electrochemical deposition at the single particle level is facile and universal, which could be extended to the precise synthesis of other plasmonic core-shell nanomaterials and the investigation of the pathway of plasmon accelerated chemical conversion.

Forecast analysis of the epidemics trend of COVID-19 in the USA by a generalized fractional-order SEIR model.

In this paper, a generalized fractional-order SEIR model is proposed, denoted by SEIQRP model, which divided the population into susceptible, exposed, infectious, quarantined, recovered and insusceptible individuals and has a basic guiding significance for the prediction of the possible outbreak of infectious diseases like the coronavirus disease in 2019 (COVID-19) and other insect diseases in the future. Firstly, some qualitative properties of the model are analyzed. The basic reproduction number R 0 is derived. When R 0 < 1 , the disease-free equilibrium point is unique and locally asymptotically stable. When R 0 > 1 , the endemic equilibrium point is also unique. Furthermore, some conditions are established to ensure the local asymptotic stability of disease-free and endemic equilibrium points. The trend of COVID-19 spread in the USA is predicted. Considering the influence of the individual behavior and government mitigation measurement, a modified SEIQRP model is proposed, defined as SEIQRPD model, which is divided the population into susceptible, exposed, infectious, quarantined, recovered, insusceptible and dead individuals. According to the real data of the USA, it is found that our improved model has a better prediction ability for the epidemic trend in the next two weeks. Hence, the epidemic trend of the USA in the next two weeks is investigated, and the peak of isolated cases is predicted. The modified SEIQRP model successfully capture the development process of COVID-19, which provides an important reference for understanding the trend of the outbreak.

A fractional-order SEIHDR model for COVID-19 with inter-city networked coupling effects.

In the end of 2019, a new type of coronavirus first appeared in Wuhan. Through the real-data of COVID-19 from January 23 to March 18, 2020, this paper proposes a fractional SEIHDR model based on the coupling effect of inter-city networks. At the same time, the proposed model considers the mortality rates (exposure, infection and hospitalization) and the infectivity of individuals during the incubation period. By applying the least squares method and prediction-correction method, the proposed system is fitted and predicted based on the real-data from January 23 to March 18 - m where m represents predict days. Compared with the integer system, the non-network fractional model has been verified and can better fit the data of Beijing, Shanghai, Wuhan and Huanggang. Compared with the no-network case, results show that the proposed system with inter-city network may not be able to better describe the spread of disease in China due to the lock and isolation measures, but this may have a significant impact on countries that has no closure measures. Meanwhile, the proposed model is more suitable for the data of Japan, the USA from January 22 and February 1 to April 16 and Italy from February 24 to March 31. Then, the proposed fractional model can also predict the peak of diagnosis. Furthermore, the existence, uniqueness and boundedness of a nonnegative solution are considered in the proposed system. Afterward, the disease-free equilibrium point is locally asymptotically stable when the basic reproduction number R 0 ≤ 1 , which provide a theoretical basis for the future control of COVID-19.

Metallic Inverse Opals: An Electrochemiluminescence enhanced Substrate for Sensitive Bioanalysis.

Here, we proposed a novel local surface plasmon resonance (LSPR) enhanced ECL strategy based on the metallic inverse opals and Ru(bpy)32+-doped silica nanoparticles (RuSi NPs). Gold inverse opals (GIOs), as a plasmonic array, could interact with the ECL of RuSi NPs and excite the electromagnetic (EM) field at the gold surface. The triggered EM field could enhance the ECL emission of RuSi NPs. We compared the electrochemical and ECL performances of RuSi NPs modified on the gold electrodes with different surface morphologies and found that the ECL emission of RuSi NPs patterned at the inner surface of GIOs exhibited the highest intensity. The finite-difference time-domain (FDTD) simulations indicated that the EM field was related to the surface morphology of the metallic nanostructure, and the highest EM field was observed at the inner surface of the GIOs. Because of the superior ECL performances, the inner surfaces of GIOs were developed for nucleic acid detection with a detection limit of 3.3 fM (S/N = 3), which shows great promise for bioanalysis.

An Efficient Electrochemiluminescence Enhancement Strategy on Bipolar Electrode for Bioanalysis.

This paper develops an efficient electrochemiluminescence (ECL) enhancement strategy on closed bipolar electrode for the detection of prostate specific antigen (PSA). We first synthesized a cyclometalated iridium(III) complex (pq)2Irbza with high ECL efficiency and used as ECL emitter in the anodic cell of BPE. While we introduced a Pt-tipped Au NRs and constructed a sandwich immune structure at the cathodic pole of BPE. Combined the signal amplification strategies of enzyme catalysis and the synergistic catalytic effect of bimetallic structure for the reduction of H2O2, the attached Pt-tipped Au NRs-GOx-Ab2 nanocomplex as both recognition probes and signal amplification units could mediate the ECL signals of (pq)2Irbza/tripropylamine (TPrA) on the anodes of BPE through faradaic reaction due to the charge neutrality of BPE. Therefore, a highly sensitive BPE-ECL sensor for detection of PSA with a detection limit of 0.72 pg/mL and a linear range from 1.0 pg/mL to 10 ng/mL was obtained. This work is expected to broaden the application of iridium complex and bimetallic nanocatalyst in biological detection and could be utilized to detect many other biological molecules.

Extinction Analysis of Stochastic Predator-Prey System with Stage Structure and Crowley-Martin Functional Response.

In this paper, we researched some dynamical behaviors of a stochastic predator-prey system, which is considered under the combination of Crowley-Martin functional response and stage structure. First, we obtained the existence and uniqueness of the global positive solution of the system. Then, we studied the stochastically ultimate boundedness of the solution. Furthermore, we established two sufficient conditions, which are separately given to ensure the stochastic extinction of the prey and predator populations. In the end, we carried out the numerical simulations to explain some cases.