Latest ArticlesEnvironmental endocrine disruptors, represented by bisphenol A (BPA), have been widely detected in the environment, bringing potential health risks to human beings. Nitrogen-containing biocarbon catalyst can activate peroxymonosulfate (PMS) to degrade BPA in water, but its active sites remain opaque. Herein, in this work, nitrogen-containing biochar, i.e., CNedge, enriched with graphitic-N defects at the edges was prepared by one-pot co-pyrolysis of chitosan and potassium carbonate. The results showed that the CNedge/PMS system can effectively degrade 98% of BPA (50 mg/L). The electron transfer based non-radical oxidation mechanism was responsible for BPA degradation. Edge graphitic-N doping endows biochar with strong electron transfer ability. The catalyst had good recovery and reuse performance. This catalytic oxidation was also feasible for other refractory pollutants removal and worked well for treating practical wastewater. This work may provide valuable information in unraveling the N doping configuration-activity relationship during activating PMS by biochar.
Tryptophan (Trp) is an essential amino acid that plays a critical role in human physiology. The increasing demand for Trp has created a highly promising market, underscoring the urgent necessity for the development of efficient strategies for the simultaneous detection and uptake of tryptophan. Herein, we report an expanded "Texas-sized" molecular box (An-TxSB), which incorporates luminescent anthracene bridging subunits and molecular recognition motifs. This luminescent molecular box demonstrates exceptional sensitivity to Trp in water, permitting its precise quantification with a notably low limit of detection (LOD) of 0.42 µmol/L. Moreover, An-TxSB facilitates the proficient uptake of Trp from simulated water samples, thereby revealing an impressive Trp adsorption capacity of up to 226.0 µmol/g.
In this study, a series of arylene-bridged bis(benzimidazolium)triflates 1–62+·2[OTf–] were synthesized by grafting different π-linkers with benzimidazolium scaffolds. Among them, compound 12+·2[OTf–] with anthracene as the linker exhibited remarkable electron transfer capabilities across four distinct redox states. The inclusion of an anthracene unit as the π-linker contributes to its exceptional redox and optoelectronic characteristics. Consequently, 12+·2[OTf–] was successfully utilized as both an electrochromic molecule in an ECD under applied voltage for the first time, and a highly efficient photocatalyst for the formation of carbon–phosphorus bonds via visible-light-induced cross-dehydrogenative coupling reactions.
Compared to organic thin films, organic single crystals offer significant potential in organic phototransistors (OPTs) due to their enhanced charge transport, large surface area, and defect-free nature. However, the development of n-type semiconductors has lagged behind p-type semiconductors. To enhance semiconductor device performance, a doping process can be employed, which typically involves the introduction of charged impurities into the crystalline semiconducting material. Its aim is to reduce the Ohmic losses, increase carrier density, improve transport capabilities, and facilitate effective carrier injection, ultimately enhancing the electrical properties of the material. Traditional doping processes, however, often pose a risk of damaging the structure of single crystals. In this study, we have synthesized novel cyano-substituted chiral perylene diimides, which self-assemble into two-dimensional single crystals that can be used for n-type semiconductor devices. We have employed a surface doping strategy using diethylamine vapor without disrupting the crystal structure. The fabricated devices exhibit significantly higher charge transport properties after doping, achieving a maximum electron mobility of 0.14 cm2 V−1 s−1, representing an improvement of over threefold. Furthermore, the optoelectronic performance of the doped devices has significantly improved, with the external quantum efficiency increased by over 9 times and the significantly improved response time. These results suggest that our surface doping technology is a promising way for enhancing the performance of 2D organic single-crystal OPTs.
Organic electrode materials (OEMs) have attracted substantial attention for aqueous zinc-ion batteries (AZIBs) due to their advantages in relieving resource and environmental anxiety. However, the potential of OEMs is plagued by their low achievable capacity and high solubility. Here, we have proposed a new concept of "co-coordination force" and designed a rigid-flexible coupling crystalline polymer that can overcome the abovementioned limitations. The obtained crystalline polymer (BQSPNs) with multiredox centres makes the BQSPNs exist intermolecular hydrogen bonds (HB) among -C=O, -C=N, and -NH and consequently exhibits transverse two-dimensional arrays and longitudinal π-π stacking structure. Additionally, in-situ FTIR, Raman, variable temperature FTIR spectra, and 2D nuclear overhauser effect spectroscopy (NOESY) well capture the existence and evolution process of HB during the electrochemistry reaction process of BQSPNs, uncovering the effect of HB in stabilizing the structure and promoting the reaction kinetics. As a result, the BQSPNs with rationally designed "co-coordination force" deliver a high capacity of 459.6 mAh/g and a stable cycling lifetime for more than 100,000 cycles at 10 A/g in AZIBs. Our results disclose the HB effect and provide a brand-new strategy for high-performance OEMs design.
Stimuli-triggered release and alleviating resistance of iridium(Ⅲ)-based drugs at tumor sites remains challengeable for clinical hepatoma therapy. Herein, a doxorubicin@iridium-transferrin (DOX@Ir-TF) nanovesicle was synthesized by carboxylated-transferrin (TF) and doxorubicin-loaded amphiphilic iridium-amino with quaternary ammonium (QA) groups and disulfide bonds. The QA groups enhanced photophysical properties and broadened production capacity of photoinduced-reactive oxygen species (ROS), while the disulfide-bridged bonds regulated oxidative stress levels through reacting with glutathione (GSH); simultaneously, modification of TF improved recognition and endocytosis of the nanovesicle for tumor cells. Based on in-vitro results, a controlled-release behavior of DOX upon a dual-responsiveness of GSH and near-infrared ray (NIR) irradiation was presented, along with high-efficiency generation of ROS. After an intravenous injection, the nanovesicle was targeted at tumor sites, realizing TF-navigated photoacoustic imaging guidance and synergistic chemotherapy-photodynamic therapy under NIR/GSH stimulations. Overall, newly-synthesized DOX@Ir-TF nanovesicle provided a potential in subcutaneous hepatocellular carcinoma therapy due to integrations of targeting delivery, dual-stimuli responsive release, synergistic therapy strategy, and real-time monitoring.
Covalently bonded bridging between different semiconductors is a remarkable approach to improve the transfer of charge carriers at interfaces. In this study, we designed a ternary heterojunction (MBG) combining of molybdenum diselenide (MoSe2), black phosphorus nanosheets (Bpn) and graphitic carbon nitride (GCN). Among this MBG of MoSe2/Bpn/GCN, (ⅰ) the covalently bonded bridging effect between Bpn/GCN facilitates directional charge carrier transfer, meanwhile (ⅱ) a Z-scheme heterojunction is formed between MoSe2/GCN to enhance the separation of photogenerated carriers. Furthermore, (ⅲ) this composite exhibits an increased absorption for visible light. Using this MBG, photocatalytic degradation of over 98% of moxifloxacin is achieved within 20 min, with O2•− confirmed as the primary photocatalytic active species. These findings provide novel insights into the construction of efficient heterojunction by covalently bonded bridging.
Maximizing solar energy utilization is a persistent challenge in photo catalysis, which determines sustainable solar-driven photocatalytic process. Photo thermal-coupled photo catalysis is considered as a promising solution to tackle the issues of sustainable energy scarcity and environmental pollution by harvesting the full-spectrum solar energy. Herein, a highly efficient photo thermal-accelerated photo catalysis system is elaborately established, in which the assembled carbonized stick/Nb2C MXene evaporator can heat water into vapor and the integrated g-C3N4 photocatalyst further enables high-efficiency photocatalytic hydrogen production. The designed hyperboloid wood-based architecture possesses a multiphase interface of water steam/catalyst/hydrogen to reduce the transport resistance of hydrogen gas in liquid and ultimately maximize the output of hydrogen energy. Consequently, this coupled photothermal-photocatalytic system achieves a stable solar evaporation rate of 2.16 kg m-1 h-1 under one sun irradiation and highly efficient hydrogen-evolving rate of 3096 µmol g-1 h-1. This work paves a way to explore the improvement of photocatalytic hydrogen production by synergic photothermal effect for potential applications in renewable solar energy utilization and hydrogen production.
Water contamination by tetracycline (TC) has emerged as an environmental concern owing to its widespread use and antibiotic resistance. Application of peracetic acid (PAA) in the water and wastewater treatment has recently been proposed and demonstrated to be effective for TC abatement, yet the underlying reaction kinetics between the PAA and TC are not yet clear. To explore the reaction kinetics, the effect of solution pH on TC abatement by PAA is studied and the species-specific rate constants are calculated. The ability to donate and accept electrons for different species of TC and PAA is evaluated via density functional theory (DFT) calculations. The pH-dependent apparent second-order rate constants of TC abatement by PAA exhibits the parabolic shape with the maximum at pH 8.5 (9.75 L mol−1 s−1). This phenomenon is closely related to the speciation of TC and PAA, in which the reaction between PAAH and TTC2− possesses the highest species-specific rate constants according to the kinetic simulation. Further DFT calculations suggest that the HOMO of TTCH+, TTC, TTC−, TTC2− and the LUMO of PAAH and PAA− are –6.40, –6.26, –5.10, –4.94 eV and –0.24, 0.60 eV, respectively. According to the DFT calculations, deprotonation of TC and PAA leads to an increase of the HOMO value of TC and the LUMO value of PAA. Furthermore, the HOMOTC–LUMOPAA values is in good agreement with the trend of species-specific rate constants, which can be used to evaluate the reactivity between PAA and TC with different species. This study provides the kinetic data and theoretical basis for the reaction of PAA and TC, which is critical for the application of PAA in the treatment of water and wastewater.
In recent years, FeCl3-photocatalyzed direct C–H/Si–H bond functionalization reactions have attracted huge attention. In those transformations, chlorine radical (Cl•) could be generated from FeCl3 via a ligand-to-metal charge transfer (LMCT)/homolysis process under light irradiation. The resulting chlorine radical subsequently acts as a hydrogen atom transfer (HAT) agent to abstract the hydrogen atom of aliphatic C–H, O–H, or Si–H bonds to give the corresponding C/Si/O-centered radicals for various organic transformations. In this review, we summarized the recent advances in the application of FeCl3 as a HAT photocatalyst for the C/Si–H functionalization to construct C–C, C–N, C–Si, C–S, C–B, and C-P bonds.
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