Ambient Synthesis of Porphyrin-Based Fe-Covalent Organic Frameworks for Efficient Infected Skin Wound Healing.

Reactive oxygen species (ROS) have emerged as a promising treatment option for antibacterial and biofilm eradication. However, their therapeutic efficacy is significantly hampered by the unique microenvironments of diabetic wounds. In this study, we designed and synthesized porphyrin-based Fe covalent organic frameworks (Fe-COF) through a Schiff base condensation reaction. Subsequently, Fe-COF were encapsulated with hyaluronic acid (HA) through electrostatic adsorption, resulting in a novel formulation named HA-Fe-COF for diabetic wound healing. HA-Fe-COF were engineered to respond to hyaluronidase in the infected wound, leading to the controlled release of Fe-COF. Those released Fe-COF served a dual role as photosensitizers, generating singlet oxygen and localized heating when exposed to dual light sources. Additionally, they acted as peroxidase-like nanozymes, facilitating the production of ROS through enzymatic reactions. This innovative approach enabled a synergistic therapeutic effect combining photodynamic, photothermal, and chemodynamic modalities. Furthermore, the sustained release of HA from HA-Fe-COF promoted angiogenesis, collagen deposition, and re-epithelialization during the diabetic wound healing process. This "all-in-one" strategy offers a novel approach for the development of antimicrobial and biofilm eradication strategies that minimize damage to healthy tissues in vivo.

Grappling with the trade-offs of carbon emission trading and green certificate: Achieving carbon neutrality in China.

Although our knowledge of national carbon emission trading system and green certificate trading system are powerful incentive instruments that can deliver on increasingly ambitious climate targets in China, there remains an uncertainty of systems' structural reforms. This study builds on and extends a well-established dynamic computable general equilibrium (CGE) model to incorporate carbon trading system and green certificate trading system into the modeling framework, simulating a diverse of system development pathways further allows an exploration of the many possible policy effect. Then, using total factor productivity as a comprehensive indicator to asses policy effectiveness, the evolutionary trend of comprehensive effects under different paths are separately evaluated to discover the reforms' optimal range. Our work offers main results: First, these instruments provide a price signal. The introduction of a carbon allowance auction drive up carbon prices, while the implementation of a green certificate punishment and the expansion of the trading scope promote an increase in green certificate prices. Second, all policy scenarios that help reduce carbon emission intensity and optimize the power supply structure. However, in achieving the net-zero goal, the green certificate policy incurs more economic costs than the carbon trading policy. Indeed, the combination of multiple policy tools alleviates the decline of social welfare levels. Third, synergism design among policy tools: the focus should be on carbon trading policy from 2021 to 2030, green certificate trading policy from 2030 to 2050, and strengthened policy from 2050 to 2060. Reform measures within policies may need to be introduced in a timely manner. This study offers specific insights and tailored policy proposals to support policymakers in balancing environmental goals with economic and social needs in light of the aforementioned findings.

Reactive Oxygen-Correlated Photothermal Imaging of Smart COF Nanoreactors for Monitoring Chemodynamic Sterilization and Promoting Wound Healing.

Chemodynamic therapy (CDT) has emerged as a promising approach for treating infected diabetic wounds, while reliable imaging technology for simultaneous monitoring of ROS and therapeutic processes is still a formidable challenge. Herein, smart covalent organic framework (COF) nanoreactors (COF NRs) are constructed by hyaluronic acid (HA) packaged glucose oxidase (GOx) covalently linked Fe-COF for diabetic wound healing. Upon the breakdown of the HA protective layer, GOx consumes glucose to produce gluconic acid and hydrogen peroxide (H2 O2 ), resulting in decreased local pH and H2 O2 supplementation. Density functional theory (DFT) calculations show that Fe-COF has high catalytic activity towards H2 O2 , leading to in situ generation of hydroxyl radicals (·OH) for sterilization, and the localized downregulation of glucose effectively improved the microenvironment of diabetic wounds. Meanwhile, based on the near-infrared photothermal imaging of oxidized 3,3',5,5'-tetramethylbenzidine (oxTMB), the authors showed that TMB can be applied for the point-of-care testing of ·OH and glucose, and assessing the sterilization progress in vivo. More significantly, the facile photothermal signaling strategy can be extended to monitor various ROS-mediated therapeutic systems, enabling accurate prediction of treatment outcomes.

Multimodal neuroimaging data from a 5-week heart rate variability biofeedback randomized clinical trial.

We present data from the Heart Rate Variability and Emotion Regulation (HRV-ER) randomized clinical trial testing effects of HRV biofeedback. Younger (N = 121) and older (N = 72) participants completed baseline magnetic resonance imaging (MRI) including T1-weighted, resting and emotion regulation task functional MRI (fMRI), pulsed continuous arterial spin labeling (PCASL), and proton magnetic resonance spectroscopy (1H MRS). During fMRI scans, physiological measures (blood pressure, pulse, respiration, and end-tidal CO2) were continuously acquired. Participants were randomized to either increase heart rate oscillations or decrease heart rate oscillations during daily sessions. After 5 weeks of HRV biofeedback, they repeated the baseline measurements in addition to new measures (ultimatum game fMRI, training mimicking during blood oxygen level dependent (BOLD) and PCASL fMRI). Participants also wore a wristband sensor to estimate sleep time. Psychological assessment comprised three cognitive tests and ten questionnaires related to emotional well-being. A subset (N = 104) provided plasma samples pre- and post-intervention that were assayed for amyloid and tau. Data is publicly available via the OpenNeuro data sharing platform.

Protocol for optical detection of iodide ions in aqueous environments using a zirconium(IV)-enhanced strategy.

Detection of radioactive iodide ions (I-) is important for protecting human beings from the hazards of radioactive pollution. Herein, we present a protocol for detecting I- using a zirconium(IV)-enhanced strategy. We describe steps for optimizing the I- detection approach, establishing standard curves, and finally applying the approach. The use of zirconium(IV) greatly improves the detection performance and endows this approach with an ultralow detection limit of 0.176 nM together with wide applicability in various aqueous environments. For complete details on the use and execution of this protocol, please refer to Feng et al. (2022).1.

Ultrafast extraction of uranium from seawater using photosensitized biohybrid system with bioinspired cascaded strategy.

The highly effective utilization of uranium resources in global seawater is a viable method to satisfy the rising demands for fueling nuclear energy industry. Herein, inspired by the multi-mechanisms of the marine bacteria for uranium immobilization, CdS nanoparticles are deposited on the cell of marine bacterial strain Bacillus velezensis UUS-1 to create a photosensitized biohybrid system UUS-1/CdS. This system achieves high uranium extraction efficiency using a cascaded strategy, where the bacterial cells guarantee high extraction selectivity and the photosensitive CdS nanoparticles realize cascading photoreduction of high soluble U(VI) to low soluble U(IV) to enhance extraction capacity. As one of the fastest-acting adsorbents in natural seawater, a high extraction capacity for uranium of 7.03 mg g-1 is achieved with an ultrafast extraction speed of 4.69 mg g-1 d-1. The cascaded strategy promisingly improves uranium extraction performance and pioneers a new direction for the design of adsorbents to extract uranium from seawater.

Transcriptional Inhibition of AGPAT2 Induces Abnormal Lipid Metabolism and Oxidative Stress in the Liver of Nile Tilapia Oreochromis niloticus.

The enzyme 1-acylglycerol-3-phosphate O-acyltransferase 2 (AGPAT2) is an intermediate enzyme in triglyceride synthesis. The aim was to study the regulatory mechanism of AGPAT2 on Nile tilapia, Oreochromis niloticus. In this study, antisense RNA technology was used to knock-down AGPAT2 in Nile tilapia. Compared with the control groups (transfected with ultrapure water or the blank expression vector), the AGPAT2 knock-down group showed a significantly higher weight gain rate, special growth rate, visceral somatic index, and hepatopancreas somatic index; and significantly increased the total cholesterol, triglycerides, glucose, low-density lipoprotein cholesterol, and insulin levels in serum. In addition, the contents of total cholesterol and triglycerides and the abundance of superoxide dismutase, catalase, and glutathione peroxidase in the liver significantly increased, while the malondialdehyde content significantly decreased. The liver cells became severely vacuolated and accumulated lipids in the AGPAT2 knock-down group. Comparative transcriptome analyses (AGPAT2 knock-down vs. control group) revealed 1789 differentially expressed genes (DEGs), including 472 upregulated genes and 1313 downregulated genes in the AGPAT2 knock-down group. Functional analysis showed that the main pathway of differentially expressed genes enrichment was lipid metabolism and oxidative stress, such as steroid biosynthesis, unsaturated fatty acid biosynthesis, the PPAR signaling pathway, and the P53 pathway. We used qRT-PCR to verify the mRNA expression changes of 13 downstream differential genes in related signaling pathways. These findings demonstrate that knock-down of AGPAT2 in tilapia leads to abnormal lipid metabolism and oxidative stress.

Fabrication of Ru/WO3-W2N/N-doped carbon sheets for hydrogen evolution reaction.

Recent experimental analysis indicates WO3-based nanostructures exhibit poor hydrogen evolution reactivity, particularly in alkaline medium, arising from the low electron transfer rate. It is imperative to tune the composition and structure of WO3 to boost the cleavage of H-OH bond. Here, we construct Ru/WO3-W2N/N-doped carbon sheets (Ru/WO3-W2N/NC) using m-WO3 nanosheets as precursors with the aid of RuCl3, Tris (hydroxymethyl) aminomethane, and dopamine. Structural investigation reveals the formation of N-doped carbon sheets, Ru nanoparticles, and WO3-W2N. As a result, hydrogen evolution reactivity is greatly improved on Ru/WO3-W2N/N-doped carbon sheets with 64 mV at 10 mA/cm2 in 1 mol/L (M) KOH, outperforming most of WO3-based electrocatalysts in previous literatures. Meanwhile, it facilitates the generation of H2 in 0.5 M H2SO4 with the excellent activity of 110 mV at 10 mA/cm2. Our work provides an efficient strategy to tailor the electronic structure of WO3 to catalyze acidic and alkaline hydrogen evolution reaction.

Effects of a Randomised Trial of 5-Week Heart Rate Variability Biofeedback Intervention on Cognitive Function: Possible Benefits for Inhibitory Control.

Previous research suggests that higher heart rate variability (HRV) is associated with better cognitive function. However, since most previous findings on the relationship between HRV and cognitive function were correlational in nature, it is unclear whether individual differences in HRV play a causal role in cognitive performance. To investigate whether there are causal relationships, we used a simple breathing manipulation that increases HRV through a 5-week HRV biofeedback intervention and examined whether this manipulation improves cognitive performance in younger and older adults (N = 165). The 5-week HRV biofeedback intervention did not significantly improve inhibitory control, working memory and processing speed across age groups. However, improvement in the Flanker score (a measure of inhibition) was associated with the amplitude of heart rate oscillations during practice sessions in the younger and older intervention groups. Our results suggest that daily practice to increase heart rate oscillations may improve inhibitory control, but future studies using longer intervention periods are warranted to replicate the present finding.

Increasing coordination and responsivity of emotion-related brain regions with a heart rate variability biofeedback randomized trial.

Heart rate variability is a robust biomarker of emotional well-being, consistent with the shared brain networks regulating emotion regulation and heart rate. While high heart rate oscillatory activity clearly indicates healthy regulatory brain systems, can increasing this oscillatory activity also enhance brain function? To test this possibility, we randomly assigned 106 young adult participants to one of two 5-week interventions involving daily biofeedback that either increased heart rate oscillations (Osc+ condition) or had little effect on heart rate oscillations (Osc- condition) and examined effects on brain activity during rest and during regulating emotion. While there were no significant changes in the right amygdala-medial prefrontal cortex (MPFC) functional connectivity (our primary outcome), the Osc+ intervention increased left amygdala-MPFC functional connectivity and functional connectivity in emotion-related resting-state networks during rest. It also increased down-regulation of activity in somatosensory brain regions during an emotion regulation task. The Osc- intervention did not have these effects. In this healthy cohort, the two conditions did not differentially affect anxiety, depression, or mood. These findings indicate that modulating heart rate oscillatory activity changes emotion network coordination in the brain.

TILES-2019: A longitudinal physiologic and behavioral data set of medical residents in an intensive care unit.

The TILES-2019 data set consists of behavioral and physiological data gathered from 57 medical residents (i.e., trainees) working in an intensive care unit (ICU) in the United States. The data set allows for the exploration of longitudinal changes in well-being, teamwork, and job performance in a demanding environment, as residents worked in the ICU for three weeks. Residents wore a Fitbit, a Bluetooth-based proximity sensor, and an audio-feature recorder. They completed daily surveys and interviews at the beginning and end of their rotation. In addition, we collected data from environmental sensors (i.e., Internet-of-Things Bluetooth data hubs) and obtained hospital records (e.g., patient census) and residents' job evaluations. This data set may be may be of interest to researchers interested in workplace stress, group dynamics, social support, the physical and psychological effects of witnessing patient deaths, predicting survey data from sensors, and privacy-aware and privacy-preserving machine learning. Notably, a small subset of the data was collected during the first wave of the COVID-19 pandemic.

Ambient synthesis of metal-covalent organic frameworks with Fe-iminopyridine linkages.

Highly crystalline Fe-COFs were constructed from the building blocks carrying pyridyl-aldehyde and triamine moieties in the presence of Fe(OTf)2 and acetic acid under ambient conditions via a subcomponent assembly strategy. The spectral results prove the coordination of atomically distributed Fe(II) ions with the nitrogen species of covalently formed iminopyridine linkages.

Metal-Phenolic Network-Functionalized Magnetic Nanoparticles for Enzyme Immobilization.

Metal-phenolic network (MPN) coating is an emerging class of surface functionalization method and has attracted ever-growing interest in areas of bioengineering and biotechnology. Although various applications for MPN coatings, including drug delivery, cytoprotection, and antimicrobial surfaces, have been studied in the form of films and capsules, their interaction with enzyme molecules and the subsequent influence of biocatalytic properties are poorly understood. Herein, MPN coatings composed of different types of metal ions (CuII, FeIII, ZnII, MnII, AuIV) coordinated with tannic acid (TA) were fabricated on Fe3O4 nanoparticles as a facile nanoplatform for immobilizing alcohol dehydrogenase (ADH). The results show that the different polarization capacities of metal ions (i.e., Lewis acids) could affect the hydrophilicity and hydrophobicity of the coordinated MPN coatings, while the enzyme immobilization rate, biocatalytic activity, and stability are in turn influenced by the surface properties of the MPN coatings. Among the different metal ions, the Fe3O4-TA-ZnII showed the highest enzyme immobilizing efficiency (91.53%) and catalytic activity (60.45 U/mg ADH). Besides, the enzyme re-usability and tolerance to extreme conditions were both enhanced after immobilization. These results highlight an advanced strategy for the interfacial construction of hybrid heterogeneous biocatalytic systems with potential use in biomedical applications.

How does the design of personal carbon trading system affect willingness to participate under carbon neutrality goal?-evidence from a choice experiment.

In order to achieve the emission peak and carbon neutrality ("30·60" goals), personal carbon trading may be included in China's carbon trading market in the future, based on the corporate-level carbon trading that is already in place. It will be an effective solution to reduce carbon emissions from the consumption side and can be used as a supplement to the corporate carbon trading mechanism and carbon tax. This study constructs a personal carbon trading system based on the fundamental realities of China, which includes four attributes: carbon quota acquisition, trading partner selection, low-carbon behavior offset mechanism, and value preservation mode. Through questionnaire survey and choice experiment, the logit model is used to analyze the influence of the four attributes upon the individual willingness to participate in personal carbon trading and the heterogeneity of the public on personal carbon trading in the context of carbon neutrality policy. The study found that the influence of the attributes on the willingness to participate was ranked as follows: carbon quota acquisition > value preservation mode > low-carbon behavior offset mechanism > trading partner selection. The level of knowledge about carbon neutrality and salary will have a significant positive impact on the attribute-level preference of personal carbon trading. Finally, suggestions are made for designing, applying, and promoting personal carbon trading mechanisms to improve the public's willingness to participate in personal carbon trading and perfect the construction of carbon trading systems at the consumption side. The take-home message of the study is that a well-established personal carbon trading mechanism is an effective solution for reducing greenhouse gas emissions.

Testing environmental Kuznets curve hypothesis: considering the impact of Sino-US trade on three main industries in China.

To achieve carbon neutrality and carbon reduction goals, China needs to consider industrial structure and trade. This study aims to test the validity of environmental Kuznets curve (EKC) hypothesis at the industry level in China and study the different impact of Sino-US trade in intermediate goods and trade in final goods on China's environment. To do so, we used the annual data of China's 25 sectors in 1990-2015 and classified 25 sectors into three main industries. Based on the Stochastic Impacts by Regression on Population, Affluence and Technology framework, we investigated the validity of EKC hypothesis and the driving factors of greenhouse gas (GHG) emissions. The results show that (1) EKC hypothesis is verified for the country and the tertiary industry. (2) Compared with the primary industry and the secondary industry, the economic growth of the tertiary industry brings less GHG emissions. (3) Intermediate goods exported to all sectors in the USA will increase GHG emissions in the country and the three main industries, but final goods exported to consumers in the USA will reduce GHG emissions except the tertiary industry. From our results, the EKC hypothesis is a suitable model for environmental policy in tertiary industry, but it does not apply to the primary industry and the secondary industry. Environmental policy in the primary industry and the secondary industry needs to focus on reducing energy intensity. In the case of exports to the USA, intermediate goods pollute the environment, while final improve the environment. Thus, China needs to increase controls on exports of intermediate goods with low added value and high pollution and gradually shift to the production of environmentally friendly final goods.

Halogen hydrogen-bonded organic framework (XHOF) constructed by singlet open-shell diradical for efficient photoreduction of U(VI).

Synthesis of framework materials possessing specific spatial structures or containing functional ligands has attracted tremendous attention. Herein, a halogen hydrogen-bonded organic framework (XHOF) is fabricated by using Cl- ions as central connection nodes to connect organic ligands, 7,7,8,8-tetraaminoquinodimethane (TAQ), by forming a Cl-···H3 hydrogen bond structure. Unlike metallic node-linked MOFs, covalent bond-linked COFs, and intermolecular hydrogen bond-linked HOFs, XHOFs represent a different kind of crystalline framework. The electron-withdrawing effect of Cl- combined with the electron-rich property of the organic ligand TAQ strengthens the hydrogen bonds and endows XHOF-TAQ with high stability. Due to the production of excited electrons by TAQ under light irradiation, XHOF-TAQ can efficiently catalyze the reduction of soluble U(VI) to insoluble U(IV) with a capacity of 1708 mg-U g-1-material. This study fabricates a material for uranium immobilization for the sustainability of the environment and opens up a new direction for synthesizing crystalline framework materials.

Tuning Photoexcited Charge Transfer in Imine-Linked Two-Dimensional Covalent Organic Frameworks.

The generation of a long-lived charge-separated state in versatile π-conjugated two-dimensional covalent organic frameworks (2D COFs), a process essential to extending their great potentials in advanced semiconducting applications, is yet fully elucidated. Herein, we report a systematic investigation of the photophysical properties of three highly crystalline imine-linked 2D COFs using steady-state and transient absorption spectroscopy accompanied by time-dependent density functional theory (TDDFT) calculations. The different electron affinity between 5,5',5″-(1,3,5-benzenetriyl)tris(2-pyridinecarboxaldehyde) (BTPA) and three tunable electron-donating/accepting triamine monomers dominated the formation of the excited-state, charge-transfer direction, and lifetime. A prominent charge transfer from electron-rich 4,4',4″-triaminotriphenylamine (TAPA) to BTPA in COFTAPA-BTPA led to the long-lived charge-separated state, which was attributed to a greater degree of delocalization compared to the two other COFs. These results provide fundamental insight into the importance of structure-property correlation for designing advanced photoactive 2D COF materials with the efficient charge transfer and long-lived charge-separated state.

Amidoxime Group-Anchored Single Cobalt Atoms for Anti-Biofouling during Uranium Extraction from Seawater.

Marine biofouling is one of the most significant challenges hindering practical uranium extraction from seawater. Single atoms have been widely used in catalytic applications because of their remarkable redox property, implying that the single atom is highly capable of catalyzing the generation of reactive oxygen species (ROS) and acts as an anti-biofouling substance for controlling biofouling. In this study, the Co single atom loaded polyacrylamidoxime (PAO) material, PAO-Co, is fabricated based on the binding ability of the amidoxime group to uranyl and cobalt ions. Nitrogen and oxygen atoms from the amidoxime group stabilize the Co single atom. The fabricated PAO-Co exhibits a broad range of antimicrobial activity against diverse marine microorganisms by producing ROS, with an inhibition rate up to 93.4%. The present study is the first to apply the single atom for controlling biofouling. The adsorbent achieves an ultrahigh uranium adsorption capacity of 9.7 mg g-1 in biofouling-containing natural seawater, which decreased only by 11% compared with that in biofouling-removed natural seawater. These findings indicate that applying single atoms would be a promising strategy for designing biofouling-resistant adsorbents for uranium extraction from seawater.