BézierCE: Low-Light Image Enhancement via Zero-Reference Bézier Curve Estimation.

Due to problems such as the shooting light, viewing angle, and camera equipment, low-light images with low contrast, color distortion, high noise, and unclear details can be seen regularly in real scenes. These low-light images will not only affect our observation but will also greatly affect the performance of computer vision processing algorithms. Low-light image enhancement technology can help to improve the quality of images and make them more applicable to fields such as computer vision, machine learning, and artificial intelligence. In this paper, we propose a novel method to enhance images through Bézier curve estimation. We estimate the pixel-level Bézier curve by training a deep neural network (BCE-Net) to adjust the dynamic range of a given image. Based on the good properties of the Bézier curve, in that it is smooth, continuous, and differentiable everywhere, low-light image enhancement through Bézier curve mapping is effective. The advantages of BCE-Net's brevity and zero-reference make it generalizable to other low-light conditions. Extensive experiments show that our method outperforms existing methods both qualitatively and quantitatively.

SR-FEINR: Continuous Remote Sensing Image Super-Resolution Using Feature-Enhanced Implicit Neural Representation.

Remote sensing images often have limited resolution, which can hinder their effectiveness in various applications. Super-resolution techniques can enhance the resolution of remote sensing images, and arbitrary resolution super-resolution techniques provide additional flexibility in choosing appropriate image resolutions for different tasks. However, for subsequent processing, such as detection and classification, the resolution of the input image may vary greatly for different methods. In this paper, we propose a method for continuous remote sensing image super-resolution using feature-enhanced implicit neural representation (SR-FEINR). Continuous remote sensing image super-resolution means users can scale a low-resolution image into an image with arbitrary resolution. Our algorithm is composed of three main components: a low-resolution image feature extraction module, a positional encoding module, and a feature-enhanced multi-layer perceptron module. We are the first to apply implicit neural representation in a continuous remote sensing image super-resolution task. Through extensive experiments on two popular remote sensing image datasets, we have shown that our SR-FEINR outperforms the state-of-the-art algorithms in terms of accuracy. Our algorithm showed an average improvement of 0.05 dB over the existing method on ×30 across three datasets.

Superselective Hg(II) Removal from Water Using a Thiol-Laced MOF-Based Sponge Monolith: Performance and Mechanism.

Point-of-use (POU) devices with satisfying mercury (Hg) removal performance are urgently needed for public health and yet are scarcely reported. In this study, a thiol-laced metal-organic framework (MOF)-based sponge monolith (TLMSM) has been investigated for Hg(II) removal as the POU device for its benchmark application. The resulting TLMSM was characterized by remarkable chemical resistance, mechanical stability, and hydroscopicity (>2100 wt %). Importantly, the TLMSM has exhibited high adsorption capacity (∼954.7 mg g-1), fast kinetics (kf ∼ 1.76 × 10-5 ms-1), broad working pH range (1-10), high selectivity (Kd > 5.0 × 107 mL g-1), and excellent regeneration capability (removal efficiency >90% after 25 cycles). The high applicability of TLMSM in real-world scenarios was verified by its excellent Hg(II) removal performance in various real water matrices (e.g., surface waters and industrial effluents). Moreover, a fixed-bed column test demonstrated that ∼1485 bed volumes of the feeding streams (∼500 µg L-1) can be effectively treated with an enrichment factor of 12.6, suggesting the great potential of TLMSM as POU devices. Furthermore, the principal adsorption complexes (e.g., single-layer -S-Hg-Cl and double-layer -S-Hg-O-Hg-Cl and -S-Hg-O-Hg-OH) formed during the adsorption process under a wide range of pH were synergistically and systematically unveiled using advanced tools. Overall, this work presents an applicable approach by tailoring MOF into a sponge substrate to achieve its real application in heavy metal removal from water, especially for Hg(II).

Medium-Low Temperature Conditions Induce the Formation of Environmentally Persistent Free Radicals in Microplastics with Conjugated Aromatic-Ring Structures during Sewage Sludge Pyrolysis.

Medium-low temperature pyrolysis is an effective method of retaining active components in sludge char. However, we found that incomplete cracking reactions resulted in residues of microplastics (MPs) remaining in the char; moreover, high levels of environmentally persistent free radicals (EPFRs) were detected in these MPs. Here, we investigated the temperature-dependent variations in the char-volatile products derived from sludge and MPs under different pyrolysis scenarios using multiple in situ probe coupling techniques and electron paramagnetic resonance spectroscopy, thereby identifying the sources of EPFRs and elucidating the corresponding formation-conversion mechanisms. The temperature was the key factor in the formation of EPFRs; in particular, in the 350-450 °C range, the abundance of EPFRs increased exponentially. Reactive EPFR readily formed in MPs with conjugated aromatic-ring structures (polyethylene terephthalate and polystyrene) at a temperature above 350 °C; EPFR concentrations were 5-17 times higher than those found in other types of polymers, and these radicals exhibited half-lives of more than 90 days. The EPFR formation mechanism could be summarized as solid-solid/solid-gas interfacial interactions between the polymers and the intermediate products from sludge pyrolysis (at 160-350 °C) and the homolytic cleavage-proton transfer occurring in the polymers themselves under the dual action of thermal induction and acid sites (at 350-450 °C). Based on the understanding of the evolution of EPFRs, temperature regulation and sludge components conditioning may be effective approaches to inhibit the formation of EPFRs in MPs, constituting reliable strategies to diminish the environmental risk associated with the byproducts of sludge pyrolysis.

Low-Light Image Enhancement via Retinex-Style Decomposition of Denoised Deep Image Prior.

Low-light images are a common phenomenon when taking photos in low-light environments with inappropriate camera equipment, leading to shortcomings such as low contrast, color distortion, uneven brightness, and high loss of detail. These shortcomings are not only subjectively annoying but also affect the performance of many computer vision systems. Enhanced low-light images can be better applied to image recognition, object detection and image segmentation. This paper proposes a novel RetinexDIP method to enhance images. Noise is considered as a factor in image decomposition using deep learning generative strategies. The involvement of noise makes the image more real, weakens the coupling relationship between the three components, avoids overfitting, and improves generalization. Extensive experiments demonstrate that our method outperforms existing methods qualitatively and quantitatively.

Critical Review of Advances in Engineering Nanomaterial Adsorbents for Metal Removal and Recovery from Water: Mechanism Identification and Engineering Design.

Nanomaterial adsorbents (NAs) have shown promise to efficiently remove toxic metals from water, yet their practical use remains challenging. Limited understanding of adsorption mechanisms and scaling up evaluation are the two main obstacles. To fully realize the practical use of NAs for metal removal, we review the advanced tools and chemical principles to identify mechanisms, highlight the importance of adsorption capacity and kinetics on engineering design, and propose a systematic engineering scenario for full-scale NA implementation. Specifically, we provide in-depth insight for using density functional theory (DFT) and/or X-ray absorption fine structure (XAFS) to elucidate adsorption mechanisms in terms of active site verification and molecular interaction configuration. Furthermore, we discuss engineering issues for designing, scaling, and operating NA systems, including adsorption modeling, reactor selection, and NA regeneration, recovery, and disposal. This review also prioritizes research needs for (i) determining NA microstructure properties using DFT, XAFS, and machine learning and (ii) recovering NAs from treated water. Our critical review is expected to guide and advance the development of highly efficient NAs for engineering applications.

Metastable Facet-Controlled Cu2WS4 Single Crystals with Enhanced Adsorption Activity for Gaseous Elemental Mercury.

Purposively designing environmental advanced materials and elucidating the underlying reactivity mechanism at the atomic level allows for the further optimization of the removal performance for contaminants. Herein, using well facet-controlled I-Cu2WS4 single crystals as a model transition metal chalcogenide sorbent, we investigated the adsorption performance of the exposed facets toward gaseous elemental mercury (Hg0). We discovered that the decahedron exhibited not only facet-dependent adsorption properties for Hg0 but also recrystallization along the preferential [001] growth direction from a metastable state to the steady state. Besides, the metastable crystals with a predominant exposure of {101} facets dominated the promising adsorption efficiency (about 99% at 75 °C) while the saturated adsorption capacity was evaluated to be 2.35 mg·g-1. Subsequently, comprehensive characterizations and X-ray adsorption fine structure (XAFS), accompanied by density functional theory (DFT) calculations, revealed that it might be owing to the coordinatively unsaturated local environment of W atoms with S defects and the surface relative stability of different facets, which could be affected by the change in surface atom configuration. Hence, the new insight into the facet-dependent adsorption property of transition metal chalcogenide for Hg0 may have important implications, and the atomic-level study directly provides instructions for development and design of highly efficient functional materials.

Highly Efficient and Selective Hg(II) Removal from Water Using Multilayered Ti3C2Ox MXene via Adsorption Coupled with Catalytic Reduction Mechanism.

Mercury (Hg) removal is crucial to the safety of water resources, yet it lacks an effective removal technology, especially for emergency on-site remediation. Herein, multilayered oxygen-functionalized Ti3C2 (Ti3C2Ox) (abbreviated as M-Ti3C2) nanosheets were prepared to remove Hg(II) from water. The M-Ti3C2 has demonstrated ultrafast adsorption kinetics (the concentration decreased from 10 400 to 33 µg L-1 in 10 s), impressively high capacity (4806 mg g-1), high selectivity, and broad working pH range (3-12). The density functional theory (DFT) calculations and experimental characterizations unveil that this exceptional Hg(II) removal is owing to the distinct interaction (e.g., adsorption coupled with catalytic reduction). Specifically, Ti atoms on the {001} facets of M-Ti3C2 prefer to adsorb Hg(II) in the form of HgClOH, which subsequently undergoes homolytic cleavage to form radical species (e.g., •OH and •HgCl). Immediately, the •HgCl radicals dimerize and form crystalline Hg2Cl2 on the edges of M-Ti3C2. Up to ∼95% of dimeric Hg2Cl2 can be efficiently recovered via facile thermal treatment. Notably, owing to the adsorbed •OH and energy released during the distinct interaction, M-Ti3C2 has been oxidized to TiO2/C nanocomposites. And the TiO2/C nanocomposites have shown to have better performance on the photocatalytic degradation of organic pollutants than Degussa P25. These exceptional features coupled with mercuric recyclable nature make M-Ti3C2 an outstanding candidate for rapid/urgent Hg(II) removal and recovery.

Electrochemical Pretreatment for Sludge Sulfide Control without Chemical Dosing: A Mechanistic Study.

Sulfide is a toxic and corrosive odorant generated in various sludge treatment and disposal systems. We developed an electrochemical pretreatment (EPT) approach to eliminate sludge sulfide production without adding chemicals. Biochemical sulfide potential (BSP) test was used to evaluate the effectiveness of EPT on sludge sulfide production. The sulfide control was effective with EPT, and we determined the underlying mechanism of EPT. EPT which was operated at 12 V for 720 s eliminated 99% of dissolved sulfide and 100% of gaseous H2S(g). In comparison, the dissolved sulfide reached 104 ± 1 mg S/L in the control BSP test. A sulfur mass balance analysis in the BSP test showed that 90% of the produced sulfide was removed via metal precipitation. Metal distribution results confirmed that metals (i.e., Fe, Mn, and Ni) in the sludge became soluble after EPT and were released from their residual and organically bound fractions. EPT which was operated at 15 V solubilized around 73, 92, and 72% of Fe, Mn, and Ni, and these metals precipitated the sulfide that was produced from biological sulfate reduction. Sludge analysis revealed that EPT disintegrated sludge flocs and disrupted metal-binding functional groups. Specifically, reduction of 17% C═O functional groups in the sludge was found, which could be associated with metal release. The impact of oxidants (e.g., chlorine) generated from EPT on sulfide oxidation was minimal. The findings of this study broadened up our understanding of the electrochemical process for sulfide control during saline sludge digestion.

Deep Dehalogenation of Florfenicol Using Crystalline CoP Nanosheet Arrays on a Ti Plate via Direct Cathodic Reduction and Atomic H.

Efficient elimination of antibacterial activity of halogenated antibiotics by dehalogenation pretreatment is desired for a biochemical treatment process. In this study, crystalline cobalt phosphide nanosheet arrays on a Ti plate (C-CoP/Ti) are fabricated by a simple electrodeposition and phosphorization process. The crystalline structure greatly promotes atomic hydrogen (H*) generation. Moreover, the nanosheet arrays can provide abundant active sites and accelerate electron transfer and mass transport. As a result, the dehalogenation rate of florfenicol (FLO, an emerging organic pollutant) on C-CoP/Ti is 11.1, 2.97, and 13.6 times higher than that on amorphous CoP/Ti, Pd/Ti, and bare Ti, respectively. The C-CoP/Ti electrode achieves 97.4% dehalogenation of FLO (20 mg L-1) within 30 min at -1.2 V (vs Ag/AgCl). Nearly 100% of Cl and 20% of F are broken away within 120 min, showing the highest electrocatalytic defluorination efficiency reported so far. Both experimental results and theoretical calculations reveal that the dehalogenation of FLO on C-CoP/Ti is synergistically accomplished via direct reduction of electron transfer and indirect reduction of H*. This study develops a highly efficient non-noble metal electrode material for dehalogenation of halogenated organic compounds.

Oxidation Mechanisms of the UV/Free Chlorine Process: Kinetic Modeling and Quantitative Structure Activity Relationships.

Recently, the UV/free chlorine process has gained attention as a promising technology for destroying refractory organic contaminants in the aqueous phase. We have developed a kinetic model based on first-principles to describe the kinetics and mechanisms of the oxidation of organic contaminants in the UV/free chlorine process. Substituted benzoic acid compounds (SBACs) were chosen as the target parent contaminants. We determined the second-order rate constants between SBACs and reactive chlorine species (RCS; including [Formula: see text], [Formula: see text] and [Formula: see text]) by fitting our model to the experimental results. We then predicted the concentration profiles of SBACs under various operational conditions. We analyzed the kinetic data and predicted concentration profiles of reactive radicals ([Formula: see text] and RCS), we found that [Formula: see text] was the dominant radicals for SBACs destruction. In addition, we established quantitative structure activity relationships (QSARs) that can help predict the second-order rate constants for SBACs destruction by each type of reactive radicals using SBACs Hammett constants. Our first-principles-based kinetic model has been verified using experimental data. Our model can facilitate a design for the most cost-effective application of the UV/free chlorine process. For example, our model can determine the optimum chlorine dosage and UV light intensity that result in the lowest energy consumption.

Deactivation Mechanism of Multipoisons in Cement Furnace Flue Gas on Selective Catalytic Reduction Catalysts.

Increasing numbers of cement furnaces have applied selective catalytic reduction (SCR) units for advanced treatment of NO in the flue gas. However, the SCR catalysts may face various poisons, such as acidic, alkaline, and heavy metal species, in the fly ash. In this work, we studied the deactivation mechanisms of multipoisons (Ca, Pb, and S) on the CeO2-WO3/TiO2 catalyst, using the in situ diffuse reflectance infrared Fourier transform spectroscopy method. Calcium promoted the conversion of Ce(III) to Ce(IV) and, thus, (i) suppressed the redox cycle, (ii) decreased the NO adsorption (monodentate NO3- and bridged NO2-), and (iii) enriched the Lewis acid sites. Pb(IV) blocked Ce2(WO4)3, aggravating the electronegativity of W6+, which inhibited (i) the binding stability of tungsten and ammonia species, (ii) bridged NO3- (bonded to tungsten), and (iii) the Brønsted acid sites. The multipoisoning processes enriched O2- by repairing partial surface oxygen defects, which suppressed O22- and O-. Sulfur occupied the surface base sites and formed PbSO4 after Ce2(WO4)3 was saturated.

Tuning Pb(II) Adsorption from Aqueous Solutions on Ultrathin Iron Oxychloride (FeOCl) Nanosheets.

Structural tunability and surface functionality of layered two-dimensional (2-D) iron oxychloride (FeOCl) nanosheets are critical for attaining exceptional adsorption properties. In this study, we combine computational and experimental tools to elucidate the distinct adsorption nature of Pb(II) on 2-D FeOCl nanosheets. After finding promising Pb(II) adsorption characteristics by bulk FeOCl sheets (B-FeOCl), we applied computational quantum mechanical modeling to mechanistically explore Pb(II) adsorption on representative FeOCl facets. Results indicate that increasing the exposure of FeOCl oxygen and chlorine sites significantly enhances Pb(II) adsorption. The (110) and (010) facets of FeOCl possess distinct orientations of oxygen and chlorine, resulting in different Pb(II) adsorption energies. Consequently, the (110) facet was found to be more selective toward Pb(II) adsorption than the (010) facet. To exploit this insight, we exfoliated B-FeOCl to obtain ultrathin FeOCl nanosheets (U-FeOCl) possessing unique chlorine- and oxygen-enriched surfaces. As we surmised, U-FeOCl nanosheets achieved excellent Pb(II) adsorption capacity (709 mg g-1 or 3.24 mmol g-1). Moreover, U-FeOCl demonstrated rapid adsorption kinetics, shortening adsorption equilibration time to one-third of the time for B-FeOCl. Extensive characterization of FeOCl-Pb adsorption complexes corroborated the simulation results, illustrating that increasing the number of Pb-O and Pb-Cl interaction sites led to the improved Pb(II) adsorption capacity of U-FeOCl.

Development of a Three-Dimensional Electrochemical System Using a Blue TiO2/SnO2-Sb2O3 Anode for Treating Low-Ionic-Strength Wastewater.

Reducing energy use is crucial to commercialize electrochemical oxidation technologies. We developed a three-dimensional (3-D) electrochemical system that can significantly reduce the applied voltage and effectively degrade organic contaminants in low-ionic-strength wastewaters. The 3-D system consisted of a composite wire mesh anode (composed of blue TiO2 nanotubes covered with SnO2-Sb2O3), a proton exchange membrane, and a stainless-steel wire mesh cathode, which were compressed firmly together. For the 3-D system, we placed the anode of a 3-D electrode toward the wastewater that flowed past the anode. Both the two-dimensional (2-D) and 3-D systems had the same anode and cathode. We found that the 3-D system could reduce the applied voltage by 75.7% and reduce the electrical efficiency per log order reduction (EE/O) by 73% for 0.001 M Na2SO4. For Na2SO4 concentrations greater than 0.05 M, the 2-D system had a slightly lower EE/O. We also compared the EE/O of electrochemical advanced oxidation processes (EAOPs) with that of other advanced oxidation processes (UV/H2O2, UV/persulfate, O3/H2O2, UV/ TiO2, and UV/chlorine). We found that EAOPs have a much higher EE/O for low BA concentrations (20 mg/L) and a much lower EE/O for high BA concentrations (2000 mg/L).

Impact of Chloride Ions on UV/H2O2 and UV/Persulfate Advanced Oxidation Processes.

Chloride ion (Cl-) is one of the most common anions in the aqueous environment. A mathematical model was developed to determine and quantify the impact of Cl- on the oxidization rate of organic compounds at the beginning stage of the UV/persulfate (PS) and UV/H2O2 processes. We examined two cases for the UV/PS process: (1) when the target organic compounds react only with sulfate radicals, the ratio of the destruction rate of the target organic compound when Cl- is present to the rate when Cl- is not present (designated as rRCl-/ rR) is no larger than 1.942%; and (2) when the target organic compounds can react with sulfate radicals, hydroxyl radicals and chlorine radicals, rRCl-/ rR, can be no larger than 60%. Hence, Cl- significantly reduces the organic destruction rate in the UV/PS process. In the UV/H2O2 process, we found that Cl- has a negligible effect on the organic-contaminant oxidation rate. Our simulation results agree with the experimental results very well. Accordingly, our mathematical model is a reliable method for determining whether Cl- will adversely impact organic compounds destruction by the UV/PS and UV/H2O2 processes.

Oxidation of Microcystin-LR via Activation of Peroxymonosulfate Using Ascorbic Acid: Kinetic Modeling and Toxicity Assessment.

Advanced oxidation processes (AOPs) have been widely used for the destruction of organic contaminants in the aqueous phase. In this study, we introduce an AOP on activated peroxymonosulfate (PMS) by using ascorbic acid (H2A) to generate sulfate radicals (SO4•-). Sulfate radicals, hydroxyl radicals (HO•), and ascorbyl radicals (A•-) were found using electron spin resonance (ESR). But we found A•- is negligible in the degradation of microcystin-LR (MCLR) due to its low reactivity. We developed a first-principles kinetic model to simulate the MCLR degradation and predict the radical concentrations. The MCLR degradation rate decreased with increasing pH. The scavenging effect of natural organic matter (NOM) on SO4•- was relatively small compared to that for HO•. Considering both energy consumption and MCLR removal, the optimal H2A and PMS doses for H2A/PMS process were determined at 1.0 × 10-6 M and 1.6 × 10-5 M, respectively. In addition, we determined the toxicity using the protein phosphatase 2A (PP2A) test and the results showed that MCLR was readily detoxified and its oxidation byproducts were not hepatotoxic. Overall, our work provides a new type of AOP and a promising, efficient, and environmental-friendly method for removing microcystins in algae-laden water.

Mapping Soil Alkalinity and Salinity in Northern Songnen Plain, China with the HJ-1 Hyperspectral Imager Data and Partial Least Squares Regression.

In arid and semi-arid regions, identifying and monitoring of soil alkalinity and salinity are in urgently need for preventing land degradation and maintaining ecological balances. In this study, physicochemical, statistical, and spectral analysis revealed that potential of hydrogen (pH) and electrical conductivity (EC) characterized the saline-alkali soils and were sensitive to the visible and near infrared (VIS-NIR) wavelengths. On the basis of soil pH, EC, and spectral data, the partial least squares regression (PLSR) models for estimating soil alkalinity and salinity were constructed. The R² values for soil pH and EC models were 0.77 and 0.48, and the root mean square errors (RMSEs) were 0.95 and 17.92 dS/m, respectively. The ratios of performance to inter-quartile distance (RPIQ) for the soil pH and EC models were 3.84 and 0.14, respectively, indicating that the soil pH model performed well but the soil EC model was not considerably reliable. With the validation dataset, the RMSEs of the two models were 1.06 and 18.92 dS/m. With the PLSR models applied to hyperspectral data acquired from the hyperspectral imager (HSI) onboard the HJ-1A satellite (launched in 2008 by China), the soil alkalinity and salinity distributions were mapped in the study area, and were validated with RMSEs of 1.09 and 17.30 dS/m, respectively. These findings revealed that the hyperspectral images in the VIS-NIR wavelengths had the potential to map soil alkalinity and salinity in the Songnen Plain, China.

Population health risk via dietary exposure to trace elements (Cu, Zn, Pb, Cd, Hg, and As) in Qiqihar, Northeastern China.

The estimated daily intakes (EDIs) of six trace elements (Cu, Zn, Pb, Cd, Hg, and As) in vegetables (leafy vegetable, i.e., bok choy, fruit vegetables, i.e., cucumber and tomato, and other categories, i.e., mushroom, kidney bean, and potato), cereals (rice and wheat flour), and meats (pork, mutton, and beef) most commonly consumed by adult inhabitants of Qiqihar, Northeastern China, were determined to assess the health status of local people. The average EDIs of Cu, Zn, Pb, Cd, Hg, and As were with 20.77 µg (kg bw)-1 day-1 of Cu, 288 µg (kg bw)-1 day-1 of Zn, 2.01 µg (kg bw)-1 day-1 of Pb, 0.41 µg (kg bw)-1 day-1 of Cd, 0.01 µg (kg bw)-1 day-1 of Hg, and 0.52 µg (kg bw)-1 day-1 of As, respectively, which are below the daily allowance recommended by FAO/WHO. However, the maximum EDIs of Pb and Cd were 4.56 µg (kg bw)-1 day-1 and 1.68 µg (kg bw)-1 day-1, respectively, which are above the recommended levels [i.e., 3.58 µg (kg bw)-1 day-1 for Pb and 1.0 µg (kg bw)-1 day-1 for Cd] by FAO/WHO. This finding indicates that the potential health risk induced by daily ingestion of Pb and Cd for the local residents should receive a significant concern. Similarly, we detected elevated Pb and Cd concentrations, i.e., with average of 13.58 and 0.60 mg kg-1 dw, respectively, in the adult scalp hairs. Consumption of rice, potato, bok choy, and wheat flour contributed to 75 and 82% of Pb and Cd daily intake from foodstuffs. Nevertheless, human scalp hair is inappropriate biological material for determination of the nutritional status of trace elements in this region.