Electroactive polylactic acid nanofiber multilayer membranes as "Green" flexible electrode for supercapacitor.

Against the backdrop of the post-COVID-19 era, the demand for masks has become increasingly steady, discarded masks have brought about new environmental problems due to the lack of effective means of disposal as well as recycling mechanisms. To solve this problem, we make secondary use of discarded polylactic acid (PLA) masks. The nanofiber multilayer membranes PLA/PDA/GO/PPy were synthesized by layer-by-layer self-assembly for flexible supercapacitors (SCs). The multiple coating on PLA significantly increases the capacitive performance. Optimization of the PLA/PDA/GO/PPy demonstrates capacitance up to 1331 mF cm-2. Symmetric aqueous SCs using PLA/PDA/GO/PPy electrodes show higher energy density than other literature-reported SCs based on nanofiber multilayer membranes. In addition, we also explored the effects of discarded PLA/PDA/GO/PPy on the growth of ryegrass and canola in the soil. The exceptional combination of remarkable electrochemical properties and excellent environmental friendliness makes the PLA membrane promising for supercapacitors.

Molecular insights into linkages among free-floating macrophyte-derived organic matter, the fate of antibiotic residues, and antibiotic resistance genes.

Macrophyte rhizospheric dissolved organic matter (ROM) served as widespread abiotic components in aquatic ecosystems, and its effects on antibiotic residues and antibiotic resistance genes (ARGs) could not be ignored. However, specific influencing mechanisms for ROM on the fate of antibiotic residues and expression of ARGs still remained unclear. Herein, laboratory hydroponic experiments for water lettuce (Pistia stratiotes) were carried out to explore mutual interactions among ROM, sulfamethoxazole (SMX), bacterial community, and ARGs expression. Results showed ROM directly affect SMX concentrations through the binding process, while CO and N-H groups were main binding sites for ROM. Dynamic changes of ROM molecular composition diversified the DOM pool due to microbe-mediated oxidoreduction, with enrichment of heteroatoms (N, S, P) and decreased aromaticity. Microbial community analysis showed SMX pressure significantly stimulated the succession of bacterial structure in both bulk water and rhizospheric biofilms. Furthermore, network analysis further confirmed ROM bio-labile compositions as energy sources and electron shuttles directly influenced microbial structure, thereby facilitating proliferation of antibiotic resistant bacteria (Methylotenera, Sphingobium, Az spirillum) and ARGs (sul1, sul2, intl1). This investigation will provide scientific supports for the control of antibiotic residues and corresponding ARGs in aquatic ecosystems.

Antibiotic resistance in soil-plant systems: A review of the source, dissemination, influence factors, and potential exposure risks.

As an emerging environmental contaminant, the widespread of antibiotic resistance has caused a series of environmental issues and human health concerns. A load of antibiotic residues induced by agricultural practices have exerted selective pressure to bacterial communities in the soil-plant system, which facilitated the occurrence and dissemination of antibiotic resistance genes (ARGs) through horizontal gene transfer. As a result, the enrichment of ARGs within crops at harvest under the influence of food ingestion could lead to critical concerns of public health. In this review, the prevalence and dissemination of antibiotic resistance in the soil-plant system are highlighted. Moreover, different underlying mechanisms and detection methods for ARGs transfer between the soil environment and plant compartments are summarized and discussed. On the other hand, a wide range of influencing factors for the transfer and distribution of antibiotic resistance within the soil-plant system are also presented and discussed. In response to exposure of antibiotic residues and resistomes, corresponding hazard identification assessments have been summarized, which could provide beneficial guides of the toxicological tolerance for the general population. Finally, further research priorities for detection and management ARGs spread are also suggested.

Nitrogen-doped nanocarbon derived from candle soot for persulfate activation on sulfamethoxazole removal: Performance and mechanism.

Recently, carbon materials have attracted much attention in activating persulfate (PS) for the removal of organic pollutants. Seeking a greener, lower-cost, and higher-performance carbon material has become an important aspect of research. In this study, candle soot was innovatively used as a nanocarbon material, and its performance for PS activation was improved by simple ammonium ferric citrate modification. The optimal catalytic performance was achieved using 0.15 g/L modified candle soot (AS) and only 0.1 mM PS, with sulfamethoxazole (SMX) removal efficiency up to 95.5% within 120 min. Quenching tests, together with electron paramagnetic resonance measurements, showed that O2- and 1O2 were the main reactive species for SMX degradation. Meanwhile, electron transfer pathway was also occurred. Various characterization results showed that graphitic N and carbonyl group were the main active sites for PS activation. Moreover, AS/PS system exhibited high catalytic activity and stability for SMX degradation over a wide initial pH range (3∼9), or even in the presence of Cl-, H2PO4- and NO3-. This work not only taps the potential of candle soot as an environmental functional material, but also showcases the roadmap for the discovery, design, and resource utilization of other waste carbon materials in wastewater treatment.

Application of sludge biochar nanomaterials in Fenton-like processes: Degradation of organic pollutants, sediment remediation, sludge dewatering.

In today's society, wastewater sludge has become solid waste, and the preparation of wastewater sludge into sludge biochar nanomaterials (SBCs) for resource utilization has become a promising method. SBCs have advantages over other biomasses, including their complex composition, wide range of raw materials, and especially the presence of various transition metals with catalytic properties. Heterogeneous Fenton processes using SBCs as catalyst carriers have shown great potential in the removal of pollutants. In this review, the synthesis methods of SBCs are reviewed and the effects of different synthesis methods on their physicochemical properties are discussed. Furthermore, the successful applications of raw SBCs, metal-modified SBCs, and Fenton sludge-SBCs in organic pollutant degradation, sediment remediation, and sludge dewatering are reviewed. The mechanisms occurring with different metals as active sites are explored, and the review shows that the degradation efficiency and stability of SBCs are very satisfactory. We also provide an outlook on the future development of SBCs. We hope that this review will help readers gain a clearer and deeper understanding of SBCs and promote the development of SBCs.

From residue to resource: new insights into the synthesis of functionalized lignin micro/nanospheres by self-assembly technology for waste resource utilization.

Among the most abundant biopolymers in the biosphere, lignin is a renewable aromatic compound that represents an untapped opportunity to create new biological products. However, the complex interlacing structures of cellulose, hemicellulose and lignin, as well as the unique properties of lignin, limit the utilization of value-added lignin. Lignin-based nanomaterials open the door for lignin applications in environmental pollutant remediation, biofuel production, biomedicine, and other fields. Herein, we present various factors influencing the formation of micro-nanospheres by self-assembly techniques through a review of previous literature, and emphasize the simple and green synthesis of lignin micro/nanospheres (LMNPs) under non-modified conditions. More importantly, we discuss the mechanism of the formation of nanospheres. Considering the heterogeneity of lignin and the polarity of different solvents, we propose that self-assembly techniques should focus more on the influence brought by lignin itself or the solvent, so that the external conditions can be controlled to prepare LMNPs, which can be used in specific fields. A brief overview of the contribution of lignin-based nanomaterials in various fields is also presented. This review could provide insight for the development of lignin-based nanomaterials.

Metallic Co and crystalline Co-Mo oxides supported on graphite felt for bifunctional electrocatalytic hydrogen evolution and urea oxidation.

Oxygen evolution reaction (OER) and urea oxidation reaction (UOR) play important roles in the field of hydrogen energy preparation and pollution treatment. In this work, by merging bimetallic Co-Mo oxides with metallic Co on the graphite felt (GF), we effectively manufacture a 3D bifunctional and highly efficient electrocatalyst (CoMoO@Co/GF) with multi-site functionality for the simultaneous reduction of water and the oxidation of urea in an alkaline medium. The presence of metallic Co causes Co-Mo oxides to evolve from amorphous to crystalline structures. The coupling interface produced between metallic Co and Co-Mo oxides is proven to facilitate electron transport in addition to extensively accessible and highly electroactive Co-Mo oxide nanoflower architecture. The experimental results reveal that the overpotentials for OER and UOR in the CoMoO@Co/GF electrode require only 269 and 115 mV to obtain a current density of 10 mA cm-2, respectively. Furthermore, with the aid of urea, the overpotential for HER at the current density of 10 mA cm-2 is lowered to 155 mV. Most notably, the constructed CoMoO@Co/GF-based electrolytic cell only requires a 1.5 V dry battery to achieve effective H2 evolution and noteworthy stability, outperforming the commercial catalyst-based device and many previous results. The combination of experiments and theoretical calculations further clarifies the active sites in the catalyst. What's more, the pathway of electron transfer in the catalytic process is defined.

Uniform polypyrrole electrodeposition triggered by phytic acid-guided interface engineering for high energy density flexible supercapacitor.

Unevenly distributed polypyrrole (PPy) films/coatings with extensive "dead volumes" via electrodeposition have emerged as a main challenge for high energy density flexible supercapacitor. In this work, we have fabricated a phytic acid-guided graphite carbon felt/polypyrrole (GF@PA@PPy) 3D porous composite with less "dead volumes" via electrodeposition. After the activation of phytic acid (PA), the quantity and content of defects and oxygen-containing groups on the surface of carbon felt (GF) have increased. First, these functional groups improve the hydrophilicity of the surface of GF, resulting in the preferential uniform distribution of pyrrole monomer (Py). While significantly, the synergistic effects between the defects and oxygen-containing groups boost the attraction of pyrrole ring, and thus promotes the formation of perfect PPy films with less "dead volume" on GF. Finally, the supercapacitor assembled from the GF@PA@PPy-40 displays a high areal energy density of 0.0732 mWh cm-2, exceeding the previously reported PPy-based electrodes values. The deeper understanding of the role for the defects and oxygen-containing groups in the synthesis of PPy/carbon materials offers a new strategy to construct advanced PPy-based supercapacitors.

Hierarchical urchin-like amorphous carbon with Co-adding anchored on nickel foam: A free-standing electrode for advanced asymmetrical supercapacitors and adsorbed Pb (II).

The booming development of carbon materials is of great value for diverse applications, owing to their superior electron conductivity, unique structures, and excellent cycle lifetime. This study presents two hierarchically structured amorphous carbon materials for asymmetric supercapacitor (ASC) device: i) the MOFs-derived urchin-like amorphous carbon anchored on nickel foam (UAC@NF) as positive electrode; ii) high temperature activated graphite carbon felt (GF500) as negative electrode. This ASC device achieves a higher energy density of 0.036 mWh cm-3 at a power density of 0.984 mW cm-3 and demonstrates better cycling performance with 91.4% capacitance retention after 10,000 cycles, compared with the other carbon-based supercapacitor. In addition, the UAC@NF after 10,000 cycles displays much better adsorption performance for Pb (II) compared with the unused UAC@NF. We have demonstrated the relationship between carbon materials' structure and performance by combining experiment and theoretical calculation. Predominantly, our work can provide a new direction for the common development of amorphous carbon materials in the field of energy and environment.

Jointed Synchronous Photocatalytic Oxidation and Chromate Reduction Enabled by the Defect Distribution upon BiVO4: Mechanism Insight and Toxicity Assessment.

Exploring active and ecological materials for the restoration of complex pollution system is highly desired. This study presents a facile defect-tailoring strategy for combined pollutants purification with BiVO4 photocatalysis in which the jointed synchronous reaction of oxidation and reduction is integrated instead of the sequential reaction in two individual systems. XPS and EPR reveal that BiVO4 with a suitable oxygen vacancies (OVs) concentration and distribution exhibits superior photocatalytic activity under the coexistence of TC-HCl and Cr(VI) with Cr(VI) reduction efficiency increased by 71 times compared with the individual Cr(VI) system along with TC-HCl removal efficiency comparable to a single TC-HCl system. The mechanism of synchronous redox reactions mediated by surface OVs is revealed by comprehensive characterization together with reaction kinetic analysis, and the electronic band structure adjustment induced by the OVs variation is confirmed. Active species identification tests and intermediate product analysis confirm that singlet oxygen (1O2) accounts for the selective oxidation of TC-HCl, while electrons dominate the reduction of Cr(VI), under a coexistent environment. The influence of water quality parameters (e.g., pH, cations, anions, and organic substances) on the photocatalytic activity is investigated considering the complexity of the real aquatic environment. Importantly, toxicity assessment with Gram-negative strain E. coli as a model bacterium validates that the toxicity of the intermediates can be reduced to low or even ultralow levels. This work is dedicated to the mechanistic study of defect photocatalysis over BiVO4 and provides a jointed synchronous reaction system for combined pollutant purification.

Constructing ultrathin FeS/FeOxH@Fe nano-sheets for highly efficient oxygen evolution reaction.

Exploring earth-abundant catalysts with ultra-high activity and durability are the decisive challenges for oxygen evolution reaction. This work prepared the FeS/FeOxH@Fe nanosheets as the efficient and stable electrocatalysts of oxygen evolution reaction (OER) through a simple one-step co-deposition method. The FeS/FeOxH@Fe exhibited small overpotentials of 245, 376 and 482 mV at the current density of 10, 500 and 1000 mA cm-2 without iR-compensations in 1.0 M KOH solution, respectively. Constructing amorphous structure and the interface between amorphous and crystal can obviously improve the conductivity of FeOxH, which is beneficial to the improvement of catalytic performance. This work may provide an effective and controlled strategy to design highly active OER catalysts with an interface structure between amorphous and crystal by a well-designed co-deposition.

Oxygen vacancy-rich doped CDs@graphite felt-600 heterostructures for high-performance supercapacitor electrodes.

Carbon dots (CDs) have attracted much attention owing to their distinctive 0D chemical structure, ultra-small size, and intrinsic surface/edge defects, and have been widely used in many kinds of research fields. In this work, a facile method to synthesize an oxygen vacancy-rich doped CDs@graphite felt-600 heterostructure with outstanding electrochemical properties is presented. The electron spin resonance (ESR) provides clear evidence for the existence of abundant oxygen vacancies in the CDs@graphite felt-600 heterostructure. The as-synthesized CDs@graphite felt-600 shows superior areal specific capacitance (5.99 F cm-2), due to abundant oxygen vacancies and extensive surface/edge defects in the heterostructure. In addition, a home-made coin cell supercapacitor (SC) with CDs@graphite felt-600 as the electrode delivers a large areal energy density of 20.7 µW h cm-2 at a power density of 150.0 µW cm-2. To determine the charge storage mechanism at the interface of CDs@graphite felt-600, the binding energies between the CDs and graphite felt are calculated by density functional theory (DFT).

Carbon Dots-Decorated Carbon-Based Metal-Free Catalysts for Electrochemical Energy Storage.

In the past ten years, carbon dots-decorated, carbon-based, metal-free catalysts (CDs-C-MFCs) have become the fastest-growing branch in the metal-free materials for energy storage field. However, the further development of CDs-C-MFCs needs to clear up the electronic transmission mechanism rather than primarily relying on trial-and-error approaches. This review presents systematically and comprehensively for the first time the latest advances of CDs-C-MFCs in supercapacitors and metal-air batteries. The structure-performance relationship of these materials is carefully discussed. It is indicated that carbon dots (CDs) can act as the electron-rich regions in CDs-C-MFCs owing to their unique properties, such as quantum confinement effects, abundant defects, countless functional groups, etc. More importantly, specific doping can effectively modify the charge/spin distribution and then facilitate electron transfer. In addition, present challenges and future prospects of the CDs-C-MFCs are also given.

Synthesis of high-performance sodium carboxymethyl cellulose-based adsorbent for effective removal of methylene blue and Pb (II).

In this work, a biobased adsorbent (CMC-PAMA) consisting of sodium carboxymethyl cellulose, polyacrylic acid and polyacrylamide was prepared by a simple thermal crosslinking method for the removal of methylene blue (MB) and Pb (II) from aqueous solutions. The CMC-PAMA showed excellent static adsorption capacities for MB and Pb (II) of 1611.44 mg·g-1 840.11 mg·g-1, respectively, indicating its excellent performance on dyes dynamic removal. The adsorption performance of the as-prepared CMC-PAMA could be fitted well with pseudo-second-order and Langmuir isothermal model. The adsorption mechanism between CMC-PAMA and Pb (II) was confirmed by FT-IR, XPS and ion-exchange behavior. Interestingly, CMC-PAMA showed high efficiency for separation of MB/methyl orange (MO) mixtures, low equilibrium swelling ratio (0.52 g·g-1) in distilled water, good stability and reusability. With those combined advantages, CMC-PAMA could find potential application in wastewater treatment.