In this study, a sulfur–phosphorus co-doped nanocarbon (SPC) catalyst was synthesized using a straightforward one-step colloidal carbonization method and demonstrated high performance in the metal-free direct oxidation of alcohols to aldehydes. This metal-free SPC catalyst showed exceptional efficiency, achieving a conversion rate of 90% for benzyl alcohol and a selectivity of 94% toward benzaldehyde within only 1 h at 130°C. Moreover, it displays exceptional cycle stability and a high turnover frequency (17.1 × 10–3 mol g–1 h–1). Theoretical analysis suggested that the catalyst’s superior performance is attributed to the presence of unsaturated edge defects and S–P– moieties, which increase the density of states at the Fermi level, lower the band gap energy, and promote electron localization. Additionally, the doping introduces cooperative co-active S–P–C sites, facilitating a synergistic multisite catalytic effect that lowers the energy barriers. These findings represent a significant advancement in the field of metal-free direct alcohol oxidation.
High-temperature energy storage performance of dielectric capacitors is crucial for the next generation of power electronic devices. However, conduction losses rise sharply at elevated temperature, limiting the application of energy storage capacitors. Here, the mica films magnetron sputtered by different insulating layers are specifically investigated, which exhibit the excellent high-temperature energy storage performance. The experimental results revealed that the PbZrO3/Al2O3/PbZrO3 (PZO/AO/PZO) interface insulating layers can effectively reduce the high-temperature leakage current and conduction loss of the composite films. Consequently, the ultrahigh energy storage density (Wrec) and charge–discharge efficiency (η) can be achieved simultaneously in the flexible mica-based composite films. Especially, PZO/AO/PZO/mica/PZO/AO/PZO (PAPMPAP) films possess excellent Wrec of 27.5 J/cm3 and η of 87.8% at 200°C, which are significantly better than currently reported high-temperature capacitive energy storage dielectric materials. Together with outstanding power density and electrical cycling stability, the flexible films in this work have great application potential in high-temperature energy storage capacitors. Moreover, the magnetron sputtering technology can deposit large-area nanoscale insulating layers on the surface of capacitor films, which can provide technical support for the industrial production of capacitors.
Single-atom catalysts (SACs) have rapidly become a hot topic in photocatalytic research due to their unique physical and chemical properties, high activity, and high selectivity. Among many semiconductor carriers, the special structure of carbon nitride (C3N4) perfectly meets the substrate requirements for stabilizing SACs; they can also compensate for the photocatalytic defects of C3N4 materials by modifying energy bands and electronic structures. Therefore, developing advanced C3N4-based SACs is of great significance. In this review, we focus on elucidating efficient preparation strategies and the burgeoning photocatalytic applications of C3N4-based SACs. We also outline prospective strategies for enhancing the performance of SACs and C3N4-based SACs in the future. A comprehensive array of methodologies is presented for identifying and characterizing C3N4-based SACs. This includes an exploration of potential atomic catalytic mechanisms through the simulation and regulation of atomic catalytic behaviors and the synergistic effects of single or multiple sites. Subsequently, a forward-looking perspective is adopted to contemplate the future prospects and challenges associated with C3N4-based SACs. This encompasses considerations, such as atomic loading, regulatory design, and the integration of machine learning techniques. It is anticipated that this review will stimulate novel insights into the synthesis of high-load and durable SACs, thereby providing theoretical groundwork for scalable and controllable applications in the field.
Developing an efficient freshwater and electricity co-generation device (FECGD) can solve the shortage of freshwater and electricity. However, the poor salt resistance and refrigeration properties of the materials for FECGD put big challenges in the efficient and stable operation of these devices. To address these issues, we propose the covalent organic framework (COF) confined co-polymerization strategy to prepare COF-modified acrylamide cationic hydrogels (ACH-COF), where hydrogen bonding interlocking between negatively charged polymer chains and COF pores can form a salt resistant hydrogel for stabilizing tunable passive interfacial cooling (TPIC). The FECPDs based on the TPIC and salt resistance of ACH-COF display a maximum output power density of 2.28 W m–2, which is 4.3 times higher than that of a commercial thermoelectric generator under one solar radiation. The production rate of freshwater can reach 2.74 kg m–2 h–1. Our results suggest that the high efficiency and scalability of the FECGD can hold the promise of alleviating freshwater and power shortages.
Increasing climate-related extreme weather events and conflicts hinder safe water sanitation for vulnerable populations. In developing areas, centralized water systems are impractical due to high costs and poor infrastructure. Thus, technologies utilizing renewable energy like solar and mechanical energy for water treatment hold promise. It is critical to develop photocatalysts and piezoelectric/triboelectric catalysts that capture solar energy as well as mechanical energy to generate disinfectants to maximize energy utilization. The latest advancements in principles, materials, and processes utilizing solar and mechanical energy for water disinfection are highlighted in this review. First, we elucidate both direct and indirect mechanisms of sunlight-mediated water disinfection, discuss the evolution of photocatalysts from simple UV absorption to visible-light utilization, and even near-infrared light exploitation to enhance solar spectrum utilization efficiency. Furthermore, we delve into the fundamental principles of piezoelectricity and triboelectricity relying on mechanical energy conversion as well as summarize the development of piezo/triboelectric catalysts from being driven by high-frequency energy to utilizing low-frequency mechanical energy from the environment. Finally, challenges and directions for efficient systems are outlined to inspire rational design strategies and accelerate the production of superior catalytic systems applicable across a broad range.
The rapid evolution of electric vehicles (EVs) highlights the critical role of battery technology in promoting sustainable transportation. This review offers a comprehensive introduction to the diverse landscape of batteries for EVs. In particular, it examines the impressive array of available battery technologies, focusing on the predominance of lithium-based batteries, such as lithium-ion and lithium-metal variants. Additionally, it explores battery technologies beyond lithium (“post-lithium”), including aluminum, sodium, and magnesium batteries. The potential of solid-state batteries is also discussed, along with the current status of various battery types in EV applications. The review further addresses end-of-life treatment strategies for EV batteries, including reuse, remanufacturing, and recycling, which are essential for mitigating the environmental impact of batteries and ensuring sustainable lifecycle management. Finally, market perspectives and potential future research directions for battery technologies in EVs are also discussed.
Sepsis is responsible for approximately 5.3 million deaths globally each year. Here, we constructed hierarchical chitin microspheres loaded with MOF-919 (Ch/metal–organic frameworks [MOFs]) for the rapid and efficient removal of lipopolysaccharide (LPS) in complex blood environments. Furthermore, abundant active sites on MOF-919(Sc) also enable a record-high adsorption capacity of 9.56 mg/g in biomass-based adsorbents due to the coordination interactions between endotoxin and MOF-919(Sc). The LPS level of sepsis rabbits was less than 2 EU/mL (clearance rate >95%) after 90-min hemoperfusion, showing no adverse effect on the rabbit organs. Additionally, compared to the commonly used LPS scrubber Toraymyxin (polymethyl methacrylate), the chitin adsorbent is significantly more cost-effective and environmentally friendly. The preparation strategy for hierarchical porous microspheres offers notable advantages in designability, recyclability, and renewability, providing a new approach to sepsis treatment and promising prospects for the biomedical application of sustainable biomass materials.
In the past decade, molybdenum ditelluride (MoTe2) has received significant attention from the scientific community due to its structural features and unique properties originate from them. In the current review, the properties, various preparation approaches, and versatile applications of MoTe2 are presented. The review provides a brief update on the state of our fundamental understanding of MoTe2 material and also discusses the issues that need to be resolved. To introduce MoTe2, we briefly summarize its structural, optoelectronic, magnetic, and mechanical properties in the beginning. Then, different preparation methods of MoTe2, such as exfoliation, laser treatment, deposition, hydrothermal, microwave, and molecular beam epitaxy, are included. The excellent electrical conductivity, strong optical activity, tunable bandgap, high sensitivity, and impressive stability make it an ideal contender for different applications, including energy storage, catalysis, sensors, solar cells, photodetectors, and transistors. The performance of MoTe2 in these applications is systematically introduced along with mechanistic insights. At the end of the article, the challenges and possible future directions are highlighted to further modify MoTe2 material for the numerous functionalities. Therefore, the availability of different phases and layer structures implies a potential for MoTe2 to lead an era of two-dimensional materials that began from the exfoliation of graphene.
The utilization of single atoms (SAs) as trifunctional electrocatalyst for nitrogen reduction, oxygen reduction, and oxygen evolution reactions (NRR, ORR, and OER) is still a formidable challenge. Herein, we devise one-pot synthesized palladium SAs stabilized on nitrogen-doped carbon palladium SA electrocatalyst (Pd-SA/NC) as efficient trifunctional electrocatalyst for NRR, ORR, and OER. Pd-SA/NC performs a robust catalytic activity toward NRR with faradaic efficiency of 22.5% at –0.25 V versus reversible hydrogen electrode (RHE), and the relative Pd utilization efficiency is enhanced by 17-fold than Pd-NP/NC. In addition, the half-wave potential reaches 0.876 V versus RHE, amounting to a 58-time higher mass activity than commercial Pt/C. Moreover, the overpotential at 10 mA cm–2 is as low as 287 mV for Pd-SA/NC, outperforming the commercial IrO2 by 360 times in turnover frequency at 1.6 V versus RHE. Accordingly, the assembled rechargeable zinc-air battery (ZAB) achieves a maximum power density of 170 mW cm–2, boosted by 2.3 times than Pt/C–IrO2. Two constructed ZABs efficiently power the NRR-OER system to electrochemically generate ammonia implying its superior trifunctionality.
The manipulation of hydrogen bonding within protic ionic liquids is conducive to conquering the robust hydrogen bonding interactions in cellulose for its effective dissolution, but it is a great challenge to establish the delicate balance of hydrogen bonding network between solvent and cellulose. Herein, we proposed the concept of “hydrogen bond producers” for urea molecules in 1,1,3,3-tetramethylguanidinium methoxyacetate acid ([TMGH][MAA]) to enhance the dissolution of cellulose. The optimization of physicochemical properties for [TMGH][MAA] solvent as a function of urea concentration revealed a remarkable increase in cellulose solubility from 13% to 17% (w/w) by adding only 0.25 wt% urea, highlighting the efficiency of [TMGH][MAA] as a powerful solvent for the dissolution of cellulose. The experimental and simulation results verified that the significant improvement on dissolution of cellulose was attributed to the hydrogen bonding interaction of urea molecules with ion pairs and part of free ions, reducing the interference with the active ions bonded to cellulose. Furthermore, the considerable enhancement on comprehensive properties of regenerated cellulose films demonstrated the effectiveness of [TMGH][MAA]/urea solvent. The concept of “hydrogen bond producers” presented here opens a new avenue for significantly enhancing the dissolution of natural cellulose, promoting the sustainable development in large-scale processing of cellulose.