Latest ArticlesOrganic radical as a powerful tool has been extensively applied in synthetic chemistry. However, harnessing radical-mediated noncovalent interactions to fabricate soft materials remains elusive. Here we report a new category of supramolecular hydrogel system held by multiple radical-radical (polyradical) interactions, and its photosensitive cross-linking structure. A simple polyacrylamide with triarylamine (TAA) pendants is designed as the precursor. The TAA units in polymer can be converted into active TAA•+ radical cations with light and further associate each other via TAA•+‒TAA•+ stacking interactions to form stable supramolecular network. Temporal control of the light irradiation dictates the degree of radical stacks, thus regulating the mechanical performance of the resulting hydrogel materials on-demand. Moreover, the reversible collapse of this hydrogels can be promoted by adding radical scavenger or exerting reduction voltage.
Synthetic antigen-encoding mRNA plays an increasingly significant role in tumor vaccine technology owing to its antigen-specific immune-activation. However, its immune efficacy is challenged by inferior delivery efficiency and demand for suitable adjuvants. Here, we develop a novel mRNA nanovaccine based on a multifunctional nanocapsule, which is a dual-adjuvant formulation composed of cytosine-phosphate-guanine motifs loaded tetrahedral framework nucleic acid (CpG-tFNA) and an immunopeptide murine β-defensin 2 (mDF2β). This mRNA nanovaccine successfully achieves intracellular delivery, antigen expression and presentation of dendritic cells, and proliferation of antigen-specific T cells. In a tumor prophylactic vaccination model, it exerts an excellent inhibitory effect on lymphoma occurrence through cellular immunity. This mRNA nanovaccine has promising prophylactic applications in tumors and many other diseases.
Production of value-added chemicals and fuels from biomass via electrochemical methods has been of emerging interest in light of the increasing environmental, economic, and political challenges. Paired electrolysis, with anodic oxidation and cathodic reduction reactions pairing in a single electrochemical cell, offers an effective way to produce desired products in both electrodes, thus achieving complete electron economy. In this work, an efficient 5-hydroxymethylfurfural (HMF) paired electrolysis system is developed over a self-supported ultrathin Co3O4 nanoarray electrocatalyst for simultaneous production of value-added 2, 5-dihydroxymethylfuran (DHMF) and 2, 5-furandicarboxylic acid (FDCA). The as-designed paired electrolysis cell achieves a high HMF conversion and DHMF/FDCA selectivity at both anode and cathode without external hydrogen and oxygen input. A near-quantitative yield (95.7%) of FDCA and 78.8% yield of DHMF can be achieved in the paired electrolysis system, with a total Faradaic efficiency of 127%. This work will open up new opportunities in designing efficient electrochemical devices to simultaneously produce building-block chemicals from biomass-derived molecules in both anode and cathode.
The development of low-cost and high-performance ZnO Schottky photodetectors (PDs) has drawn intensive attention, but still a challenge due to their poor conductivity and low light utilization efficiency. Here, we introduce Ti3C2TX into ZnO films to fabricate Schottky UV PDs via facile spin-coated method. The fabricated ZnO/Ti3C2TX/ZnO compound film shows outstanding performance on photocurrent, responsivity, noise equivalent power (NEP), normalized detection rate (D*), and linear dynamic region (LDR), compared with the original ZnO device. The photocurrent is significantly increased by 466%, and the responsivity is improved by one order of magnitude. In addition, it exhibits relatively low NEP (5.99 × 10−11 W), strong D* (2.53 × 109 Jones), and high LDR (28 dB). The superior performance is ascribed to the enhanced conductivity and light absorption of ZnO film after introduction of Ti3C2TX modification layer, leading to simultaneously faster electron transfer, lower the radiation recombination of electron and holes on the ZnO/Ti3C2TX/ZnO compound film. This work provides a facile way to develop low-cost and high-performance ZnO Schottky PDs.
A huge amount of waste printed circuit boards (WPCBs) was produced while the electronic manufacturing industry developed rapidly. WPCBs mainly consist of organic compounds, which makes it possible to prepare them into porous carbon as valuable adsorbent. However, WPCBs are also rich in valuable metals. Cu makes up the most of these metals. It is worth studying whether the residual metal will affect the application of carbon materials. In this study, the porous active carbon (AC) was prepared from WPCBs as an adsorbent. Sulfadiazine (SD), a widely detected antibiotic contaminant, was used as a target pollutant. Nitric acid (HNO3) was used to modify AC (AC-HNO3) to remove the residual Cu. The experiment results showed that the adsorption kinetics of SD by AC (k = 0.0025) and AC-HNO3 (k = 0.0029) can be described better using a pseudo-second-order kinetic equation. The adsorption isotherms of AC and AC-HNO3 on SD could be fitted by the Langmuir model. AC had a larger adsorption capacity than AC-HNO3. Density functional theory (DFT) calculation results suggested that the −OH group and Cu on the surface of AC could be the adsorption sites and promote the SD adsorption. This work provides practical methods to recycle WPCBs into wealth and realized waste control by waste.
The binding interactions between 4-aminopyridine (4-AP) and a series of cucurbit[n]urils (Q[5], Q[6], TMeQ[6], Q[7], Q[8]) have been studied using 1H NMR spectroscopy, UV–vis absorption spectroscopy, isothermal titration calorimetry (ITC) and X-ray crystallography. The data indicates that the Q[5]@4-AP complex exhibits exo binding, which is not observed in the other four host-guest complexes. Furthermore, X-ray crystallography clearly reveals how the Q[n]s bind with 4-AP to form complexes, for example Q[5] forms an outer-surface complex, whilst Q[6], TMeQ[6] and Q[7] formed 1:1 host and guest type complexes, and Q[8] formed a stable 1:2 ternary complex due to its large cavity, which can accommodate two 4-AP molecules.
Ultra-long room temperature phosphorescence (URTP) has been increasingly recognized in pure organic luminophor in recent years. Through a simpler molecular design and charge separation-recombination pathway, organic luminophor can achieve even better URTP properties. In this work, we achieved URTP in a system of host-guest doped benzophenone derivatives whose phosphorescence is visible to the naked eye. The differences in the wavelength lifetimes of luminescent emission correspond to different photophysical mechanisms. Through a combination of theoretical calculations and experiments, the host acts as a powerful substrate that restricts the motion of the guest and inhibits the non-radiative transitions of the guest, accompanied by a charge transfer separation-recombination process between the host and the guest, resulting in an URTP phenomenon. Transient absorption results demonstrate the existence of a charge-separated state. The design strategy via charge separation is generic and easy to implement, providing a direction for the future design of doped URTP.
MIL-88A(Fe)@sponge (MS) was synthesized by a dip-coating method, which displayed efficient photocatalytic Cr(Ⅵ) reduction efficiency under both low power LED UV light and real solar light irradiation. It was observed that MS (0.2 g/L) could remove 100% Cr(Ⅵ) (10 mg/L) by adding 0.4 mmol/L tartaric acid (TA) without adjusting pH (pH 5.05) within 6.0 min and 3.0 min under UV light and real solar light irradiation, respectively. Besides, the photo-induced e− and radicals (O2•− and CO2•−) were found to play the momentous roles in the MS/TA/UVL/Cr(Ⅵ) system by the scavenger experiments and electron spin resonance (ESR) tests. MS was also filled into a fixed-bed reactor to test the possibility of long-term Cr(Ⅵ) reduction operation in TA/UVL system. As expected, the results revealed that MS could still maintain 100% activity up to 60 h. These results demonstrated that MIL-88A(Fe) might be the potentially efficient catalyst for large-scale wastewater treatment in the near future.
Herein, a bidirectional polarization strategy is proposed for hosting efficient and durable lithium-sulfur battery (Li-S) electrochemistry. By co-doping electronegative N and electropositive B in graphene matrix (BNrGO), the bidirectional electron redistribution enables a higher polysulfide affinity over its mono-doped counterparts, contributing to strong sulfur immobilization and fast conversion kinetics. As a result, BNrGO as the cathode host matrix realizes excellent cycling stability over 1000 cycles with a minimum capacity fading of 0.027% per cycle, and superb rate capability up to 10 C. Meanwhile, decent areal capacity (6.46 mAh/cm2) and cyclability (300 cycles) are also achievable under high sulfur loading and limited electrolyte. This work provides instructive insights into the interaction between doping engineering and sulfur electrochemistry for pursuing superior Li-S batteries.
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