Chlorine is a crucial radionuclide that must be removed in irradiated nuclear graphite. Understanding the interaction between chlorine and graphene-based materials is essential for studying the removal process of 36Cl from irradiated nuclear graphite. In this study, first-principle density functional theory (DFT) was utilized to investigate the adsorption characteristic of chlorine on the original and reconstructed edges of graphene-based materials. Based on the calculation of adsorption energy of the structures after each step of adsorption, the most energetically favorable adsorption routes at four types of edge were determined: Along the armchair edge and reconstructed zigzag edge, the following adatoms would be adsorbed to compensate the distortion induced by the previously adsorbed atom. Meanwhile at the original zigzag edge, chlorine atoms would be adsorbed alternatively along the edge to minimize the repulsion between two adjacent chlorine atoms. The chemical nature of the bonds formed as a result of adsorption was elucidated through an examination of the density of states (DOS) for the two adsorbed chlorine atoms and the carbon atoms attached. Furthermore, to assess the relative stability of the adsorption structures, formation energy of all energetically favorable structures following adsorption was computed. Consequently, the predominant adsorption structure was identified as the reconstructed armchair edge with two chlorine atoms adsorbed. The desorption process of 36Cl2 from the predominant structure following adsorption was simulated, revealing an energy barrier of 1.14 V for desorption. Comparison with experimental results suggests that the chlorine removed from reconstructed armchair edges significantly contributes to the low-temperature removal stage of 36Cl from irradiated nuclear graphite.
Pyrolysis of methane is a carbon-economic method to obtain valuable carbon materials and COx- free H2, under the carbon peaking and carbon neutrality goals. In this work, we propose a methane pyrolysis process to produce graphite and H2 using bubble column reactor containing NiO/Al2O3 and NaCl–KCl (molten salt). The process was optimized by the different amounts of NaCl–KCl, the CH4/ Ar ratio and temperature, indicating that the CH4 conversation rate could reach 92% at 900 °C. Meanwhile, we found that the addition of molten salt could obtain pure carbon materials, even if the conversation rate of CH4 decreases. The analysis of the carbon products revealed that graphite could be obtained.
Exploring highly efficient, and low-cost oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalysts is extremely vital for the commercial application of advanced energy storage and conversion devices. Herein, a series of graphene-like C2N supported TMx@C2N, (TM = Fe, Co, Ni, and Cu, x = 1, 2) single- and dual-atom catalysts are designed. Their catalytic performance is systematically evaluated by means of spin-polarized density functional theory (DFT) computations coupled with hydrogen electrode model. Regulating metal atom and pairs can widely tune the catalytic performance. The most promising ORR/OER bifunctional activity can be realized on Cu2@ C2N with lowest overpotential of 0.46 and 0.38 V for ORR and OER, respectively. Ni2@ C2N and Ni@C2N can also exhibit good bifunctional activity through effectively balancing the adsorption strength of intermediates. The correlation of reaction overpotential with adsorption free energy is well established to track the activity and reveal the activity origin, indicating that catalytic activity is intrinsically governed by the adsorption strength of reaction intermediates. The key to achieve high catalytic activity is to effectively balance the adsorption of multiple reactive intermediates by means of the synergetic effect of suitably screened bimetal atoms. Our results also demonstrate that lattice strain can effectively regulate the adsorption free energies of reaction intermediates, regarding it as an efficient strategy to tune ORR/OER activity. This study could provide a significant guidance for the discovery and design of highly active noble-metal-free carbon-based ORR/OER catalysts.
pH plays a pivotal role in influencing various aspects of proton-coupled electron transfer (PCET) reactions in electrochemical systems. These reactions are affected by pH in terms of mass transport, electrochemical double layer (EDL) structure, and surface adsorption energy, all of which impact the overall electrochemical processes. This review article aims to provide a comprehensive understanding of the research progress made in elucidating the effects of pH on different electrochemical reactions, the hydrogen evolution reaction/hydrogen oxidation reaction (HER/HOR), oxygen reduction reaction/oxygen evolution reaction (ORR/OER), and carbon dioxide reduction reaction ( CO2RR). To embark on this endeavor, we have conducted a bibliometric analysis to clearly outline of the research trends and advancements in the field concerning the pH effects. Subsequently, we present a systematic overview of the mechanisms governing these reactions, with a special focus on pH’s influence on both the proton and electron aspects. We conclude by discussing the current challenges in this area and suggesting future research avenues that could further our understanding of pH's role in electrochemical reactions.
In this paper, iron ore tailings (IOT) were separated from the tailings field and used to prepare cement stabilized macadam (CSM) with porous basalt aggregate. First, the basic properties of the raw materials were studied. Porous basalt was replaced by IOT at ratios of 0, 20 %, 40 %, 60 %, 80 %, and 100 % as fine aggregate to prepare CSM, and the effects of different cement dosage (4 %, 5 %, 6 %) on CSM performance were also investigated. CSM’s durability and mechanical performance with ages of 7 d, 28 d, and 90 d were studied with the unconfined compression strength test, splitting tensile strength test, compressive modulus test and freeze-thaw test, respectively. The changes in Ca2+ content in CSM of different ages and different IOT ratios were analyzed by the ethylene diamine tetraacetic acid (EDTA) titration method, and the micro-morphology of CSM with different ages and different IOT replaced ratio were observed by scanning electron microscopy (SEM). It was found that with the same cement dosage, the strengths of the IOT-replaced CSM were weaker than that of the porous basalt aggregate at early stage, and the strength was highest at the replaced ratio of 60 %. With a cement dosage of 4 %, the unconfined compressive strength of CSM without IOT was increased by 6.78 % at ages from 28 d to 90 d, while the splitting tensile strength increased by 7.89 %. However, once the IOT replaced ratio reached 100 %, the values increased by about 76.24 % and 17.78 %, which was better than 0 % IOT. The CSM-IOT performed better than the porous basalt CSM at 90 d age. This means IOT can replace porous basalt fine aggregate as a pavement base.
In this study, four different samples of Se60Ge40-xBix chalcogenides glasses were synthesized by heating the melt for 18 h in vacuum Pyrex ampoules (under a 10-4 Torre vacuum), each with a different concentration (x = 0, 10, 15, and 20) of high purity starting materials. The results of direct current (DC) electrical conductivity measurements against a 1,000/T plot for all chalcogenide samples revealed two linear areas at medium and high temperatures, each with a different slope and with different activation energies (E1 and E2). In other words, these samples contain two electrical conduction mechanisms: a localized conduction at middle temperatures and extended conduction at high temperatures. The results showed the local and extended state parameters changed due to the effective partial substitution of germanium by bismuth. The density of extended states N(Eext) and localized states N(Eloc) as a function of bismuth concentration was used to gauge this effect. While the density of the localized states decreased from 1.6 × 1014 to 4.2 × 1012 (ev-1 cm-3) as the bismuth concentration increased from 0 to 15, the density of the extended states generally increased from 3.552 × 1021 to 5.86 × 1021 (ev-1 cm-3), indicating a reduction in the mullet’s randomness. This makes these alloys more widely useful in electronic applications due to the decrease in the cost of manufacturing.
CO2 photocatalytic reduction is a carbon–neutral renewable energy technology. However, this technology is restricted by the low utilization of photocatalytic electrons. Therefore, to improve the separation efficiency of photogenerated carriers and enhance the performance of CO2 photocatalytic reduction. In this paper, g-C3N4/Pd composite with Schottky junction was synthesized by using g-C3N4, a two-dimensional material with unique interfacial effect, as the substrate material in combination with the co-catalyst Pd. The composite of Pd and g-C3N4 was tested to have a strong localized surface plasmon resonance effect (LSPR), which decreased the reaction barriers and improved the electron utilization. The combination of reduced graphene oxide (rGO) created a π–π conjugation effect at the g-C3N4 interface, which shortened the electron migration path and further improved the thermal electron transfer and utilization efficiency. The results show that the g-C3N4/ rGO/Pd (CRP) exhibits the best performance for photocatalytic reduction of CO2, with the yields of 13.57 μmol g− 1 and 2.73 μmol g− 1 for CO and CH4, respectively. Using the in situ infrared test to elucidate the intermediates and the mechanism of g-C3N4/rGO/Pd (CRP) photocatalytic CO2 reduction. This paper provides a new insight into the interface design of photocatalytic materials and the application of co-catalysts.
Copper-coated carbon fibers have excellent conductivity and mechanical properties, making them a promising new lightweight functional material. One of the main challenges to their development is the poor affinity between carbon fiber and metals. This paper selects different carbon fibers for copper electroplating experiments to study the effect of carbon fiber properties on the interface bonding performance between the copper plating layer and carbon fibers. It has been found that the interfacial bonding performance between copper and carbon fiber is related to the degree of graphitization of carbon fiber. The lower the degree of graphitization of carbon fiber, the smaller the proportion of carbon atoms with sp2 hybrid structure in carbon fiber, the stronger the interfacial bonding ability between carbon fiber and copper coating. Therefore, carbon fiber with lower graphitization degree is conducive to reducing the falling off rate of copper coating and improving the quality of copper coating, and the conductivity of copper-plated carbon fibers increases with the decrease of graphitization degree of carbon fibers. The conductivity of copper-plated carbon fibers increases by more than six times when the graphitization degree of carbon fibers decreases by 23.9%. This work provides some benchmark importance for the preparation of highquality copper-plated carbon fibers.
Graphene-modified melamine sponges (RGO-MSs) were prepared, as adsorbents with photothermal conversion ability, utilizing solar energy to achieve heavy oil temperature rise, viscosity reduction, and efficient adsorption recovery of highly viscous oil. The RGO-MSs were prepared through a simple impregnation method. The photothermal performance and heavy oil adsorption performances of RGO-MSs with different densities and thicknesses were observed. It was found that as the density increases, the thermal conductivity of RGO-MS increases too, leading to the increase of the average oil absorption rate. The reduction of thickness is beneficial to improving of the adsorption rate. The prepared RGO-MS with a density of 21.5 mg/cm−3 and a height of 1 cm (RGO-MS-3-1) shows excellent mechanical properties and fatigue resistance. Cyclic adsorption–desorption of RGO-MS-3-1 was achieved through extrusion/ ethanol washing. After 10 cycles of reuse through extrusion, the adsorption capacity decreased from 52.90 to 50.02 g g− 1, with a loss of 5.4%. The material was then washed with petroleum ether and ethanol in turn. Its adsorption capacity can restored to 98.8% of the initial value, showing a promising application prospect on heavy oil leakage treatment. The easily prepared RGO-MS exhibits excellent light absorption and photothermal oil adsorption properties, providing a good solution for the problem of heavy oil leakage at sea.
A series of ZIF-67-C-IL catalysts were prepared using ZIF-67 and 1-butyl-3-methylimidazolium bis[(trifluoromethyl)sulfonyl] imide ([ BMIM]NTf2) ionic liquid as precursors. The structure of the catalysts was characterized by XRD, TEM, SEM and XPS. The catalytic performance of the catalysts for the oxygen reduction reaction (ORR) was evaluated in a three-electrode system. The results confirmed that the high-temperature treatment of the precursors resulted in the formation of N, S codoped carbon-encapsulated Co9S8 nanoparticles. To create N, S co-doped carbon coated Co9S8 nanoparticle catalysts, ionic liquids are used as sulfur and nitrogen sources. The catalytic activity of ORR can be improved using N, S co-doped carbon to prevent the aggregation of Co9S8 nanoparticles. Graphitized and N, S co-doped carbon shells are optimal for achieving high activity stability. Optimal 600-ZIF-67-C(1:1.5)-30IL catalytic activity was observed for ORR. The half-wave potential of ORR was 0.88 V vs. RHE in 0.1 mol L− 1 KOH, with a limit current density of 4.70 mA cm− 2. Similar ORR electrocatalytic activity was observed between this catalyst and commercial Pt/C (20 wt%).
This paper presents the construction and characterization of an amperometric immunosensor based on the graphene/gold nanoparticles (AuNPs/GO) nanocomposite for the detection of the bladder cancer biomarker, apolipoprotein A1 (Apo-A1). The morphological analysis of the AuNPs/GO nanocomposite demonstrated an almost spherical shape of AuNPs and the successful coverage of their surface by graphene oxide. An increased G peak and decreased D peak after the association of AuNPs with GO, implied a reduction in graphene defects. The X-ray photoelectron spectroscopy (XPS) indicated a significant decrease in the quantity of oxygen-containing functional groups in the AuNPs/GO nanocomposite, as compared to the original GO. Furthermore, the developed sensor demonstrated commendable sensitivity and selectivity, with a wide linear range for Apo-A1 detection. Importantly, the immunosensor exhibited remarkable stability over a period of 14 days, signifying its potential for practical applications.
Sulforaphane is a naturally occurring active substance found in vegetables that is known for its potential in preventing and treating cancer. This compound has demonstrated promising effects in inhibiting the growth of various types of cancer, including esophageal, lung, colon, breast, and liver cancer. However, its instability towards pH and heat limits its application in the medical and food industries. To address this challenge, novel drug delivery systems have been developed to improve the stability and efficacy of sulforaphane, making it a more suitable candidate for clinical use in cancer research. In this study, nanocomposite materials were prepared using multi-walled carbon nanotubes (MWCNTs) and chitosan (CS) as base materials, with polydopamine (PDA) acting as a bridge material. The synthesized composite materials were used as drug carriers for the release of sulforaphane. The results of the study showed that the drug loading increased with an increase in the concentration of sulforaphane, indicating that the nanocomposite materials were effective in delivering and releasing the drug. Moreover, a positive correlation was observed between the drug loading and the thickness of the PDA layer. These findings suggest that the use of MWCNTs, CS, and PDA in the development of drug delivery systems can enhance the stability and efficacy of sulforaphane, potentially leading to improved cancer treatment outcomes.
The challenge of incorporating photothermal conversion function into chitosan (CS) hybrid fibers lies in balancing functionality and mechanical properties. In this study, we successfully prepared a chitosan/graphene oxide/gelatin (CS/GA/GO) hybrid fiber using the wet spinning process, achieving improved mechanical properties and efficient photothermal conversion capabilities. When compared with pure CS fiber with a breaking strength of 1.07 cN/dtex, the breaking strength of the CS/ GA composite fiber increased by 46.73%, while the CS/GA/GO hybrid fiber showed an even greater increase of 85.98%. In addition, the introduction of gelatin (GA) led to secondary scattering of near-infrared light, enhancing the photothermal conversion efficiency. As a result, the CS/GA/GO hybrid fiber exhibited a faster temperature rise rate and higher maximum temperatures (94.3 °C, 103.0 °C, and 111.3 °C) as compared to the CS/GO hybrid fiber. The successful incorporation of GA not only improved the mechanical properties but also enhanced the photothermal performance of the hybrid fiber.
Carbon dots (CDs) are a novel type of fluorescent nanoparticles with a particle size smaller than 10 nm. They possess several advantageous properties, including excellent biocompatibility, light stability, water solubility, and low toxicity. CDs have been widely researched in recent years. As a treasure of ancient Chinese science, traditional Chinese medicine (TCM) is rich in various active ingredients and has a variety of pharmacodynamic effects, which have been used for thousands of years. TCM-CDs prepared with TCM as carbon source can create some special functions and then may play a greater medicinal value. The purpose of this review was to engage in an in-depth conversation about the use of TCM-CDs in medical therapy and bioimaging. Firstly, this study provides a comprehensive exploration of different synthesis methods for TCM-CDs, comparing their respective advantages and disadvantages. Subsequently, the intrinsic pharmacological activity of TCMCDs, encompassing antibacterial, hypoglycemic, hemostatic, anticancer, and anti-inflammatory effects, is mainly discussed, alongside their underlying mechanisms of action. Additionally, investigations into in vitro imaging of diverse cell types and the distribution and uptake of TCM-CDs under in vivo imaging guidance are presented. Finally, the significance of TCM-CD research, key challenges and issues within this field, and future directions for development are summarized and outlined.
Slipchip offers advantages such as high-throughout, low cost, and simple operation, and therefore, it is one of the technologies with the greatest potential for high-throughput, single-cell, and single-molecule analyses. Slipchip devices have achieved remarkable advances over the past decades, with its simplified molecular diagnostics gaining particular attention, especially during the COVID-19 pandemic and in various infectious diseases scenarios. Medical testing based on nucleic acid amplification in the Slipchip has become a promising alternative simple and rapid diagnostic tool in field situations. Herein, we present a comprehensive review of Slipchip device advances in molecular diagnostics, highlighting its use in digital recombinase polymerase amplification (RPA), loop-mediated isothermal amplification (LAMP), and polymerase chain reaction (PCR). Slipchip technology allows users to conduct reliable droplet transfers with high-throughput potential for single-cell and molecule analyses. This review explores the device’s versatility in miniaturized and rapid molecular diagnostics. A complete Slipchip device can be operated without special equipment or skilled handling, and provides high-throughput results in minimum settings. This review focuses on recent developments and Slipchip device challenges that need to be addressed for further advancements in microfluidics technology.
In this study, the refinement of Multiwalled Carbon Nanotubes (MWCNTs) derived from chemical vapor decomposition is investigated. An ultrasonic pretreatment method is employed to disentangle carbon and metal impurities intertwined with MWCNTs. The pretreated MWCNTs exhibit a marginal decrease in C–O/C = O content from 8.9 to 8.8%, accompanied by a 2.5% increase in sp3 carbon content, indicating a mildly destructive pretreatment approach. Subsequently, selective oxidation by CO2 and hydrochloric acid etching are utilized to selectively remove carbon impurities and residual metal, respectively. The resulting yield of intact MWCNTs is approximately 85.65 wt.%, signifying a 19.91% enhancement in the one-way yield of pristine MWCNTs. Notably, the residual metal content experiences a substantial reduction from 9.95 ± 2.42 wt.% to 1.34 ± 0.06 wt.%, representing a 15.68% increase in the removal rate. These compelling findings highlight the potential of employing a mild purification process for MWCNTs production, demonstrating promising application prospects.
In this work, the trend in the performance of carbon fiber (CF) and its composite during self-polymerization of polydopamine (PDA) at carbon fiber surface was investigated by varying the self-polymerization time of dopamine in an aqueous solution. Research has shown that the PDA coating elevated the surface roughness and polarity of the inert fiber. The tensile strength of single carbon fiber was significantly improved, especially after 9 h of polydopamine self-polymerization, increasing by 18.64% compared with that of desized carbon fiber. Moreover, the interlaminar shear strength (ILSS) of CF-PDA9-based composites was 35.06% higher than that of desized CF-based composites. This research will provide a deep insight into the thickness and activated ingredients of dopamine oxidation and self-polymerization on interfacial compatibility of carbon fiber/epoxy resin composites.
In this study, a low-cost and easily recyclable porous green adsorbent (magnetic porous loofah biochar, MPLB) was synthesized by modifying the almost zero-cost loofah biochar material with Fe3O4. The successful synthesis of the material was demonstrated by XRD, FTIR, SEM, VSM, and BET. In addition, the material exhibits outstanding magnetic separation performance (40.01 umg/g) allowing for rapid recovery within just 90 s. The adsorption process of phenol on MPLB was found to be spontaneous and endothermic. The experimental data fit exceptionally well with the pseudo-second-order kinetic model and Langmuir model (R2 > 0.99), indicating that the dominant adsorption mechanisms involved monolayer adsorption and chemisorption. These interactions were attributed to host–guest interaction, π–π conjugation, hydrogen bonding, and pore filling. The maximum adsorption capacity calculated using the Langmuir model at 298 K is 39.4 mg/g. Importantly, even after undergoing seven cycles of recycling, MPLB retained 78% of its initial adsorption capacity. In simulated experiments employing MPLB for phenol removal in actual wastewater, an impressive removal rate of 96.4% was achieved. In conclusion, MPLB exhibits significant potential as an effective adsorbent for phenol removal in wastewater.