MnFe2O4/MoS2 catalyst used for ozonation: optimization and mechanism analysis of phenolic wastewater treatment.

The performance of catalytic ability of MFe2O4/MoS2 in the ozonation process was investigated in this work. The synthesized MnFe2O4/MoS2 was optimize prepared and then characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, X-ray photo-electron spectroscopy, and magnetic saturation strength. The results showed that when Cphenol = 200 mg/L, initial pH = 9.0, Q = 0.10 L/min, and CMnFe2O4/MoS2 = 0.10 g/L, MnFe2O4/MoS2 addition improved the degradation efficiency of phenol by 20.0%. The effects of pH, catalyst dosage, and inorganic ions on the phenol removal by the MnFe2O4/MoS2 catalytic ozonation were investigated. Five cycle experiments proved that MnFe2O4/MoS2 had good recyclability and stability. MnFe2O4/MoS2 also showed good catalytic performance in the treatment of coal chemical wastewater pesticide wastewater. The MnFe2O4 doped with MoS2 could provide abundant surface active sites for ozone and promote the stable cycle of Mn2+/Mn3+and Fe2+/Fe3+, thus generating large amounts of •OH and improving the degradation of phenol by ozonation. The MnFe2O4/MoS2/ozonation treatment system provides a technical reference and theoretical basis for industrial wastewater treatment.

Subtle tuning of nanodefects actuates highly efficient electrocatalytic oxidation.

Achieving controllable fine-tuning of defects in catalysts at the atomic level has become a zealous pursuit in catalysis-related fields. However, the generation of defects is quite random, and their flexible manipulation lacks theoretical basis. Herein, we present a facile and highly controllable thermal tuning strategy that enables fine control of nanodefects via subtle manipulation of atomic/lattice arrangements in electrocatalysts. Such thermal tuning endows common carbon materials with record high efficiency in electrocatalytic degradation of pollutants. Systematic characterization and calculations demonstrate that an optimal thermal tuning can bring about enhanced electrocatalytic efficiency by manipulating the N-centered annulation-volatilization reactions and C-based sp3/sp2 configuration alteration. Benefiting from this tuning strategy, the optimized electrocatalytic anodic membrane successfully achieves >99% pollutant (propranolol) degradation during a flow-through (~2.5 s for contact time), high-flux (424.5 L m-2 h-1), and long-term (>720 min) electrocatalytic filtration test at a very low energy consumption (0.029 ± 0.010 kWh m-3 order-1). Our findings highlight a controllable preparation approach of catalysts while also elucidating the molecular level mechanisms involved.

Insights into thermal hydrolysis pretreatment temperature for enhancing volatile fatty acids production from sludge fermentation: Performance and mechanism.

To reveal the impact of thermal hydrolysis pretreatment (THP) temperature on the unclear mechanisms of volatile fatty acids (VFAs) production, four groups were established with different temperatures (100, 120, 140 and 160 °C), and high throughput sequencing technology was utilized. The results indicated that the optimal VFAs production occurred at 140 °C. Moreover, as the THP temperature increased, the proportion of acetic acid also increased, accounting for 10.8% to 26.7% of the VFAs, compared to only 4.9% in the control group. Mechanism investigations revealed that THP facilitated the hydrolysis and release of biodegradable organic matter. Moreover, the abundance of VFAs production and hydrolytic microorganisms and related metabolic functional genes expression were evidently improved by THP. Overall, this study deepens the understanding of the mechanisms through which different THP temperatures stimulate the production of VFAs through acidogenic fermentation, providing technical support for future THP application in sludge treatment.

High-density dispersion of CuNx sites for H2O2 activation toward enhanced Photo-Fenton performance in antibiotic contaminant degradation.

In this study, a copper-based catalyst (CuCN) with CuNx active sites highly dispersed in a porous carbon nitride matrix was synthesized and applied to a heterogeneous photo-assisted Photo-Fenton (PF) system to degrade tetracycline (TET). The results showed that the CuCN/PF system degraded up to 93.6% of TET within 60 min for ultrapure water matrix under the best experimental conditions, and more than 70% of TET for both river and lake water matrix. Toxicological tests suggested that the environmental risk caused by TET can be effectively inhibited by the CuCN/PF system. The good visible-light response and charge transport abilities of CuCN catalyst were identified in photoelectrochemical experiments. Free radical scavenging experiments and electron paramagnetic resonance (EPR) spectroscopy indicated that the active species in the degradation process were·OH, h+,·O2- and 1O2. Density functional theory (DFT) calculations revealed the positive effect of CuNx sites in CuCN on the formation of hydroxyl radicals by activating H2O2. This work will provide a new insight for the development of high-efficiency heterogeneous catalysts in wastewater environmental remediation.

Novel conditioner for efficient dewaterability and modification of oily sludge with high water content.

The oily sludge with high water content (OS) was dewatered, modified, and converted into solid fuel by a novel chemical conditioner (OSO-101). The effect of OSO-101 dosage on the dewaterability of OS was studied, showing that OSO-101 dosage of 15% (wt.) could achieve the best dewaterability efficiency of OS (98.18%). Meanwhile, compared with some conventional conditioners, OSO-101 developed by our team was more effective in improving OS dewaterability efficiency. And OSO-101 may have free radical reaction, polar reaction, and redox reaction with petroleum hydrocarbons in OS, thereby polymerizing and forming condensed solid structures. The calorific value change of OS after conditioning, heavy metal content, and dioxin content of fly ash leached from incinerated product were measured for resource analysis and environmental assessment. Results showed that the resultant OS fuel blocks had extremely low content of heavy metals, dioxins, and other toxic and hazardous substances leached from fly ash. And this process did not require secondary treatment and fully met environmental protection emission standards. Additionally, OSO-101 had certain economic rationality and could effectively recover the calorific value contained in OS. This research is expected to provide new insights for efficient dewaterability and modification of OS, as well as subsequent resource utilization and harmless treatment, bringing potential environmental and economic benefits.

High-efficiency removal of tetracycline by carbon-bridge-doped g-C3N4/Fe3O4 magnetic heterogeneous catalyst through photo-Fenton process.

Carbon-bridge-modified malonamide (MLD)/g-C3N4 (CN) was prepared by copolymerization of MLD with urea and melamine and loaded with Fe3O4 for the high-efficiency removal of tetracycline (TC) in water under photo-Fenton. The prepared catalysts were characterized by SEM, TEM, N2 adsorption-desorption analysis, XPS, XRD, and FTIR, which proved that the modification method successfully introduced the C bridge into the carbon nitride molecular system and increased the structural defects of the catalyst. The Carbon-bridge-modified MLD/CN/Fe3O4 also had good visible-light response and charge-separation and transport abilities in the photoelectrochemical test. Degradation results showed that the photo-Fenton degradation of TC reached 95.8%, and the mineralization rate was 55.7% within 80 min at 80 mM H2O2 dosage, 0.5 g/L catalyst dosage, and near-neutral pH by 0.8MLD/CN/Fe3O4. Moreover, the oxidation products and mineralization pathways of TC were explored by LC-MS. Toxicity analysis indicated low environmental threat of the intermediates in TC mineralization. EPR analysis and H2O2 decomposition efficiency analyses showed an improvement in the H2O2 decomposition performance of 0.8MLD/CN/Fe3O4. This work could provide a valuable insight for the application of heterogeneous photo-Fenton technology in wastewater treatment.

Effective and simultaneous removal of organic/inorganic arsenic using polymer-based hydrated iron oxide adsorbent: Capacity evaluation and mechanism.

In this study, resin-based hydrated iron oxide (HFOR) composites were prepared and used as a functional adsorbent for the simultaneous removal of p-Arsanilic acid (p-ASA) and arsenate (As (V)). The effects of solution pH and coexisting substances on the adsorption of different arsenic species were also investigated. Results showed that the coexisting substances slightly affected the adsorption process of two arsenic species. Analysis of the adsorption behavior, isotherm equilibrium, and adsorption kinetics, as well as that results of the X-ray photoelectron spectroscopy, zeta potential, and other analytical methods revealed that the satisfactory adsorption performance of HFOR can be attributed to the electrostatic interactions induced by the positively charged groups and the coordination of the hydrated iron oxide nanoparticles, which exhibited excellent specific adsorption for both arsenic species. Moreover, HFOR showed high acid and alkali resistance and reusability, as well as a constant co-removal performance for different arsenic species in five consecutive operating cycles (55 mg As/g of As(V) and 18 mg/g of p-ASA). Results of continuous running fixed-bed column experiments confirmed that HFOR enabled excellent simultaneous adsorption for p-ASA and As(V).

Enhanced removal of tris(2-chloroethyl) phosphate using a resin-based nanocomposite hydrated iron oxide through a Fenton-like process: Capacity evaluation and pathways.

The effective removal of organophosphorus compounds (OPs) effectively from water environment remains an important but challenging task. In this study, a resin-based nanocomposite of hydrated iron oxide (HD1) was used as Fenton-like catalyst for effectively catalyzing the decomposition of hydrogen peroxide to degrade tris(2-chloroethyl) phosphate (TCEP). The results showed that HD1 was successfully prepared, which had great versatility, catalytic performance and adsorption capacity. Besides, HD1/H2O2 was capable of degrading TCEP completely with less than 0.2 mg/L of inorganic phosphorus (IP) in the effluent at the initial TCEP of 38 mg/L, pH = 4, H2O2 dosage of 20 mM, and the Kobs could result in about 1.0530 min-1 under identical conditions. More attractively, inorganic ions (i.e., Cl-, CO32-, SO42-, NO3-, HCO3-, Ca2+, and Mg2+) exhibited moderate effect on TCEP degradation. The negative effect of natural organic matters (NOM) (i.e., HA) on the degradation of TCEP was responsible for competition for the active oxygen species. Combined with electron paramagnetic resonance (EPR) spectra, X-ray photoelectron spectroscopy (XPS) and other analytical methods and radical quenching experiments, the possible removal process of TCEP was discussed, including two processes of oxidative degradation and immobilization of IP. Besides, hydroxyl radicals (•OH) was the key active species that contributed to TCEP degradation through hydroxylation-oxidation and C-O bond cracking, and specificity adsorption of HFO on IP was revealed. Furthermore, the results showed that HD1 had desirable acid and alkali resistance. In the continuous running fixed bed column experiment, HD1 showed a satisfactory performance in cycle operations. This work proposed a new enhanced process for removing TCEP in water environment by HD1/H2O2, and the multi-functional material, HD1 was promising in treatment of water containing organic phosphorus pollutants. This will be believed that this study will provide new ideas and new materials for the treatment of organic phosphorus-based organic pollutants, and lay the foundation for further deepening and expanding the application of adsorption resins in the field of water pollution control.

Efficient removal of Cu(II) organic complexes by polymer-supported, nanosized, and hydrated Fe(III) oxides through a Fenton-like process.

In this study, a polymer-supported, nanosized, and hydrated Fe(III) oxide (HFOD) was developed as a Fenton-like catalyst for the efficient removal of metal complexes in water. HFOD was prepared through the irreversible impregnation of hydrated iron(III) oxide (HFO) nanoparticles into cation exchange resin and characterized through X-ray photoelectron spectroscopy (XPS) and ion chromatography. The mechanism of Cu(II) ion removal and the degradation pathway of Cu(II)-citrate were analyzed through UV-vis spectrophotometry (UV) and liquid chromatography-mass spectrometry (LC-MS). The optimal removal rate of Cu(II) and TOC by a Fenton-like reaction at pH 4 and 40 mM H2O2 reached 81.6 % and 75.6 %, respectively. The removal efficiency of Cu(II)-citrate was remarkably affected with the addition of humic acid. However, the addition of competitive ions did not significantly reduce the removal rate of Cu(II)-citrate, thereby proving that the Fenton-like reaction by HFOD had a certain salt tolerance. Simultaneously, hydroxyl radical (•OH) was verified as the main free radical for Cu(II)-citrate degradation in a Fenton-like reaction, and citrate degradation was a process decarboxylation. HFOD recycling experiments and stability experiments showed that HFOD had high stability with good acid/alkali resistance and showed remarkable potential in the practical application of fixed-bed as catalysts for Fenton-like reactions.

Effective treatment of residue of acrylic acid production using a fluid-bed/fixed-bed system with low energy consumption.

In order to effectively deal with large amounts of complex organic pollutants in the harmful distillation residues with low energy consumption, a novel two-stage fluid-bed/fixed-bed system was designed to catalyze oxidation of acrylic acid production residue. The effects of fluid-bed temperature, gaseous hourly space velocity (GHSV), and oxygen excess rate on the purification of acrylic acid production residue in the two-stage fluid-bed/fixed-bed system were studied to prove the feasibility of the method. The chemical oxygen demand (COD) of the discharged liquid was <100 mg/L, and the volatile organic compounds (VOCs) of the discharged gas amounted to <10 mg/m3 with a fluid-bed temperature of 380°C, emulsified residue's GHSV of 0.28 L/(kgcat ·hr), and O2 excessive rate of more than 4.32. The result of techno-economics indicates the feasibility of the long-term operation of process. Results further illustrate the advantages of the proposed two-stage fluid-bed/fixed-bed system, which can treat acrylic acid production residue with high efficiency (COD < 100 mg/L, VOCs < 10 mg/m3 ) and low energy consumption (~24,856 kw·hr/ton) in the chemical industry. PRACTITIONER POINTS: A novel two-stage fluid-bed/fixed-bed system was developed for acrylic acid production residue treatment. No extra energy was required at low temperature in the two-stage fluid-bed/fixed-bed system. Purification of residue could be finished at low temperature by the catalytic pyrolysis and catalytic oxidation process. The two-stage system did not produce toxic gases and particulate matters.