Phosphorus/nitrogen co-doped and bimetallic MOF-derived cathode for all-solid-state rechargeable zinc–air batteries

With the merits of high safety and energy density, all-solid-state zinc–air batteries possess potential applications in flexible and wearable electronic devices. Especially, the air cathodes with bifunctional catalytic activity, i.e. oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) have been received enormous attention. In this work, we provide a novel phosphorus/nitrogen co-doped and bimetallic metal–organic framework (MOF)-derived cathode configurated with phosphorus-doped bimetallic FeNi alloys and a nitrogen-doped porous carbon layer loaded on graphene (P–FeNi/NC@G). The P–FeNi/NC@G electrode exhibits a superior OER activity with an overpotential of 310 mV at 10 mA cm⁻² and an ORR performance with a half-wave potential of 0.81 V. With P–FeNi/NC@G as the air cathode, the integrated all-solid-state rechargeable zinc–air battery presents a high open-circuit voltage of 1.53 V, a high peak power density of 159 mW cm⁻², a small charge–discharge voltage gap of 0.73 V at 5 mA cm⁻², as well as excellent long-term stability up to 144 cycles. This work not only expands the air cathode materials database but also develops a new co-doped synthesis method that can be utilized to fabricate a cathode with promoted catalytic efficiency, resulting in improved performance for an all-solid-state zinc–air battery.

The bimetallic FeNi-MOFs are employed to fabricate P–FeNi and N–carbon co-doped bifunctional catalyst. Due to the enhanced catalytic performance, the peak power density of all-solid-state zinc–air battery is 159 mW cm⁻².     

The effect of surfactants on hydrate particle agglomeration in liquid hydrocarbon continuous systems: a molecular dynamics simulation study

Anti-agglomerants (AAs), both natural and commercial, are currently being considered for gas hydrate risk management of petroleum pipelines in offshore operations. However, the molecular mechanisms of the interaction between the AAs and gas hydrate surfaces and the prevention of hydrate agglomeration remain critical and complex questions that need to be addressed to advance this technology. Here, we use molecular dynamics (MD) simulations to investigate the effect of model surfactant molecules (polynuclear aromatic carboxylic acids) on the agglomeration behaviour of gas hydrate particles and disruption of the capillary liquid bridge between hydrate particles. The results show that the anti-agglomeration pathway can be divided into two processes: the spontaneous adsorption effect of surfactant molecules onto the hydrate surface and the weakening effect of the intensity of the liquid bridge between attracted hydrate particles. The MD simulation results also indicate that the anti-agglomeration effectiveness of surfactants is determined by the intrinsic nature of their molecular functional groups. Additionally, we find that surfactant molecules can affect hydrate growth, which decreases hydrate particle size and correspondingly lower the risk of hydrate agglomeration. This study provides molecular-level insights into the anti-agglomeration mechanism of surfactant molecules, which can aid in the ultimate application of natural or commercial AAs with optimal anti-agglomeration properties.

Schematic of anti-agglomeration effect of surfactants promoting gas hydrate particle dispersion.     

Controllable stripping of radiolabeled group in vivo to optimize nuclear imaging via NO-responsive bioorthogonal cleavage reaction

A novel “turn-off” strategy for controllable radionuclide clearance is established. 1,4-dihydropyridine (DHP) is used as a conditional linker to connect a radioisotope labeled moiety and nano-agent. A highly specific, sensitive and effective C–C bond cleavage of DHP happens in vivo when treated with nitric oxide which is provided by glyceryl trinitrate (GTN). The radioactive cut-off part from the nanoparticle is observed to be cleared quickly by microSPECT-CT. 3–5 times decreases of radioactivity in the blood, kidneys, intestine, heart and lungs are observed after GTN treatment in a biodistribution assay. The radioactivity redistribution indicates that the radioactive leaving part is indeed cut off and the radionuclide metabolism accelerated. Organ level internal dose assessment reveals the GTN treated groups carry only ½ the radiation dose of the control group. Collectively, a feasible pathway for controllable radionuclide clearance is for the first time provided for high contrast and low radiation nuclear imaging.

A novel “turn-off” strategy was developed for controllable radionuclide clearance in organisms.

Radiolabeled compounds with biological activity, or radiotracers, have been widely used for nuclear imaging and radiation therapy. Compared with other imaging modalities, a unique problem in radiotracer-based imaging is that the radioactivity cannot be simply “turned off”. As a result, it is impossible to carry out multi-scans of the same organ with different tracers in a short period. For instance, there are three kinds of marker receptors (ER, PR, HER2) expressed in breast cancer. Different type of breast cancer expresses a different combination of these three. Therefore, three kinds of radiotracers that aim to bind the corresponding receptors will be used to distinguish individual breast cancer phenotype. The uptake of a second tracer can''t be quantified accurately before the radioactivity of the first tracer decayed to background level, which may need one or two days depending on the half-life of radionuclide. So, it''s necessary to develop a strategy to “quench” the radioactivity. Furthermore, nonspecific binding is inevitable, and the “noise” or “background” from non-specific binding of radiotracers to non-target proteins cannot be easily differentiated from the specific binding component.Therefore, it''s meaningful to develop a kind of reaction that could strip the radiation by control. To achieve this goal, the metabolism of the radioactive part should be accelerated. The biorthogonal cleavage reaction would perfectly meet the needs, if (1) cleavable reactions could happen by the control in vivo; (2) the cut-off part has a relatively fast metabolism; (3) radionuclide is linked on the cut-off part.¹ One of the key issues that bio-orthogonal reactions resolve is to bind two components into one, and make the different metabolic rate of different components synchronized.² As the reaction in the opposite direction of bio-orthogonal reaction, the bio-orthogonal cleavage reaction can extinguish the radiation by diversifying the metabolism of radionuclides and the slow metabolic targeting components.Dihydropyridine (DHP) and its cleavage-triggering partner nitric oxide (NO) can perfectly meet the three conditions. NO, a hydrophobic signal molecule, could spread without any transmembrane transporter, which means NO could spread quickly and spend little energy.^3–5 Many kinds of NO donor drugs are commercially available, such as glyceryl trinitrate (GTN), sodium nitroprusside, etc. In our previous work,⁶ it was demonstrated that the physiological concentration of NO is high enough to cleave the C–C bond of DHP. Furthermore, NO donor drugs could offer a circumstance with higher NO concentration than normal physiological concentration. Therefore, it is possible for the reaction between DHP and NO from donor drugs to occur in vivo. Herein, a NO-triggerred “turn-off” system to extinguish the radiation by cleaving the radionuclides from nanoparticles is present. Benzyl group substituted 1,4-dihydropyridine can be cleaved through controlled NO stimulation by intraperitoneal injection of GTN.Nanoparticles as the major kind of theranostic agents have been developed quickly over these years.^7–11 During the process of synthesis, nanoparticles with similar shape, scale and dispersion properties would be obtained by manipulating conditions precisely. Therefore, the metabolism of nanoparticles in the living body is more predictable than diverse small molecules. Especially, radionuclides labeled nanoparticles not only play roles in diagnosis but also work well on tumor therapy. Enhanced permeability and retention (EPR) effect make nanoparticles wonderful radiotherapy reagents.^12–15 However, nanoparticles mean to be easily captured by the mononuclear phagocyte system (MPS), which makes the nanoparticles mostly enriched in liver besides in tumor.^16–20 Furthermore, metabolism of nanoparticles are quite slow than most of the small molecules, which means the radionuclides labeled on nanoparticles have similar slow metabolism to their carriers. Unnecessarily loaded radiation from the nanoparticles will also harm normal liver cells where the nanoparticles accumulate heavily.     

Changes in thyroid hormone levels and related gene expressions in embryo–larval zebrafish exposed to binary combinations of bifenthrin and acetochlor

Ecotoxicology - Bifenthrin (BF) and acetochlor (AT) are widely used as an insecticide and herbicide, respectively, which are introduced to the aquatic environment as a natural result. Although the...