Synergistic activation of persulfate by Fe-based perovskite photocatalysis for alkali lignin degradation in pulp and paper wastewater.

A synergistic photocatalytic system based on Fe-based perovskite with persulfate was constructed for alkali lignin (AL) degradation in pulp and paper wastewater. The degradation performance and mechanism on AL were carried out under ambient temperature and pressure, accompanied by visible light irradiation. The results showed that the synergistic photocatalytic system exhibited much better performance on AL degradation than the single catalytic system. The degradation efficiency reached 73.5% under the optimal conditions and was constant at around 65% over the pH range from 2 to 8. A significant escalation of the AL degradation was observed at pH 10, reaching 80.1%. The photogenerated holes, 1O2 and SO4-·, generated by the system were involved in the degradation, and the holes played a dominant role. During the degradation process, the efficient promotion of cleavage events in lignin methoxy, ß-O-4 bond, and benzene ring was observed. Consequently, the depolymerization process led to the generation of high-value compounds, namely p-hydroxybenzaldehyde and vanillin. Remarkably, the yields of the high-value compounds in the synergistic photocatalytic system were five times larger than those in the control. This study offered a viable method to activate persulfate for alkali lignin degradation and to achieve a mutually beneficial strategy for wastewater treatment and recycling.

Efficient degradation and mineralization of polyethylene terephthalate microplastics by the synergy of sulfate and hydroxyl radicals in a heterogeneous electro-Fenton-activated persulfate oxidation system.

The presence of polyethylene terephthalate (PET) microplastics (MPs) in waters has posed considerable threats to the environment and humans. In this work, a heterogeneous electro-Fenton-activated persulfate oxidation system with the FeS2-modified carbon felt as the cathode (abbreviated as EF-SR) was proposed for the efficient degradation of PET MPs. The results showed that i) the EF-SR system removed 91.3 ± 0.9 % of 100 mg/L PET after 12 h at the expense of trace loss (< 0.07 %) of [Fe] and that ii) dissolved organics and nanoplastics were first formed and accumulated and then quickly consumed in the EF-SR system. In addition to the destruction of the surface morphology, considerable changes in the surface structure of PET were noted after EF-SR treatment. On top of the emergence of the O-H bond, the ratio of C-O/C=O to C-C increased from 0.25 to 0.35, proving the rupture of the backbone of PET and the formation of oxygen-containing groups on the PET surface. With the verified involvement and contributions of SO4•- and •OH, three possible paths were proposed to describe the degradation of PET towards complete mineralization through chain cleavage and oxidation in the EF-SR system.

Performance and mechanistic studies of rapid atenolol degradation through peroxymonosulfate activation by V, Co, and bamboo carbon catalyst.

Developing the Co-based catalysts with high reactivity for the sulfate radical (SO4-·)-based advanced oxidation processes (SR-AOPs) has been attracting numerous attentions. To improve the peroxymonosulfate (PMS) activation process, a novel Co-based catalyst simultaneously modified by bamboo carbon (BC) and vanadium (V@CoO-BC) was fabricated through a simple solvothermal method. The atenolol (ATL) degradation experiments in V@CoO-BC/PMS system showed that the obtained V@CoO-BC exhibited much higher performance on PMS activation than pure CoO, and the V@CoO-BC/PMS system could fully degrade ATL within 5 min via the destruction of both radicals (SO4-· and O2-··) and non-radicals (1O2). The quenching experiments and electrochemical tests revealed that the enhancing mechanism of bamboo carbon and V modification involved four aspects: (i) promoting the PMS and Co ion adsorption on the surface of V@CoO-BC; (ii) enhancing the electron transfer efficiency between V@CoO-BC and PMS; (iii) activating PMS with V3+ species; (iv) accelerating the circulation of Co2+ and Co3+, leading to the enhanced yield of reactive oxygen species (ROS). Furthermore, the V@CoO-BC/PMS system also exhibited satisfactory stability under broad pH (3-9) and good efficiency in the presence of co-existing components (HCO3-, NO3-, Cl-, and HA) in water. This study provides new insights to designing high-performance, environment-friendly bimetal catalysts and some basis for the remediation of antibiotic contaminants with SR-AOPs.

Porous covalent organic framework nanofibrous membrane for excellent enrichment and ultra-high sensitivity detection of trace organochlorine pesticides in water.

Developing adsorbents with high performance and long service life for effective extracting the trace organochlorine pesticides (OCPs) from real water is attracting numerous attentions. Herein, a self-standing covalent organic framework (COF-TpPa) membrane with fiber morphology was successfully synthesized by using electrospun nanofiber membranes as template and employed as solid-phase microextraction (SPME) coating for ultra-high sensitivity extraction and analysis of trace OCPs in water. The as-synthesized COF-TpPa membrane exhibited a high specific surface area (800.83 m2 g-1), stable nanofibrous structure, and excellent chemical and thermal stability. Based on the COF-TpPa membrane, a new SPME analytical method in conjunction with gas chromatography-mass spectrometry (GC-MS) was established. This proposed method possessed favorable linearity in concentration of 0.05-2000 ng L-1, high sensitivity with enrichment factors ranging from 2175 to 5846, low limits of detection (0.001-0.150 ng L-1), satisfactory precision (RSD < 10 %), and excellent repeatability (>150 cycles), which was better than most of the reported works. Additionally, the density functional theory (DFT) calculations and XPS results demonstrated that the outstanding enrichment performance of the COF-TpPa membrane was owing to synergistic effect of π-π stacking effects, high specific surface area and hydrogen bonding. This work will expect to extend the applications of COF membrane to captures trace organic pollutants in complex environmental water, as well as offer a multiscale interpretation for the design of effective adsorbents.

Protein extraction from chlorella pyrenoidosa microalgae: Green methodologies, functional assessment, and waste stream valorization for bioenergy production.

C. pyrenoidosa, a species of microalgae, has been recognized as a viable protein source for human consumption. The primary challenges in this context are the development of an efficient extraction process and the valorization of the resultant waste streams. This study, situated within the paradigm of circular economy, presents an innovative extraction approach that achieved a protein extraction efficiency of 62 %. The extracted protein exhibited remarkable oil-water emulsifying performances, such as uniform morphology with high creaming stability, suggesting a sustainable alternative to conventional emulsifiers. Additionally, hydrothermal liquefaction technique was employed for converting the residual biomass and waste solution from the extraction process into biocrude. A biocrude yield exceeding 40 wt%, characterized by a carbon content of 73 % and a higher heating value of 36 MJ/kg, were obtained. These findings demonstrate the promising potential of microalgae biorefinery, which is significant for paving toward circular economy and zero-waste society.

Gold Nanoparticles Bioproduced in Cyanobacteria in the Initial Phase Opened an Avenue for the Discovery of Corresponding Cerium Nanoparticles.

The production of isolated metallic nanoparticles with multifunctionalized properties, such as size and shape, is crucial for biomedical, photocatalytic, and energy storage or remediation applications. This study investigates the initial particle formations of gold nanoparticles (AuNPs) bioproduced in the cyanobacteria Anabaena sp. using high-resolution transmission electron microscopy images for digital image analysis. The developed method enabled the discovery of cerium nanoparticles (CeNPs), which were biosynthesized in the cyanobacteria Calothrix desertica. The particle size distributions for AuNPs and CeNPs were analyzed. After 10 h, the average equivalent circular diameter for AuNPs was 4.8 nm, while for CeNPs, it was approximately 5.2 nm after 25 h. The initial shape of AuNPs was sub-round to round, while the shape of CeNPs was more roundish due to their amorphous structure and formation restricted to heterocysts. The local PSDs indicate that the maturation of AuNPs begins in the middle of vegetative cells and near the cell membrane, compared to the other regions of the cell.

Enhanced lactic acid production from household food waste under hyperthermophilic conditions: Mechanisms and regulation.

An annual production of about 500 million tons of household food waste (HFW) has been documented, resulting in significant implications for human health and the environment in the absence of appropriate treatment. The anaerobic fermentation of HFW in an open system offers the potential to recover high value-added products, lactic acid (LA), thereby simultaneously addressing waste treatment and enhancing resource recovery efficiency. Most of LA fermentation studies have been conducted under mesophilic and thermophilic conditions, with limited research on the production of LA through anaerobic fermentation under hyperthermophilic conditions. This study aimed to produce LA through anaerobic fermentation from HFW under hyperthermophilic conditions (70 ± 1 °C), while varying pH values (5.0 ± 0.1, 7.0 ± 0.1, and 9.0 ± 0.1), and compare the results with LA production under mesophilic (35 ± 1 °C) and thermophilic (52 ± 1 °C) conditions. The findings of this study indicated that the combination of hyperthermophilic conditions and a neutral pH (pH7_70) yielded the highest concentration of LA, measuring at 17.75 ± 1.51 g/L. The mechanism underlying the high yield of LA at 70 °C was elucidated through the combined analysis of organics dissolution, enzymes activities, and 16S rRNA microbiome sequencing.

Efficient dispersive solid phase extraction of trace nitrophenol pollutants in water with triazine porous organic polymer modified nanofiber membrane.

Detecting trace endocrine disruptors in water is crucial for evaluating the water quality. In this work, a innovative modified polyacrylonitrile@cyanuric chloride-triphenylphosphine nanofiber membrane (PAN@CC-TPS) was prepared by in situ growing triazine porous organic polymers on the polyacrylonitrile (PAN) nanofibers, and used in the dispersive solid phase extraction (DSPE) to enrich trace nitrobenzene phenols (NPs) in water. The resluted PAN@CC-TPS nanofiber membrane consisted of numerous PAN nanofibers cover with CC-TPS solid spheres (∼2.50 µm) and owned abundant functional groups, excellent enrichment performance and good stability. In addition, the method based on PAN@CC-TPS displayed outstanding capacity in detecting the trace nitrobenzene phenols, with 0.50-1.00 µg/L of the quantification, 0.10-0.80 µg/L of the detection limit, 85.35-113.55 % of the recovery efficiency, and 98.08-103.02 of the enrichment factor, which was comparable to most materials. Meanwhile, when PAN@CC-TPS was adopted in the real water samples (sea water and river water), the high enrichment factors and recovery percentages strongly confirmed the feasibility of PAN@CC-TPS for enriching and detecting the trace NPs. Besides, the related mechanism of extracting NPs on PAN@CC-TPS mainly involved the synergistic effect of hydrogen bonding, π-π stacking and hydrophobic effect.

Insights into Enhanced Peroxydisulfate Activation with B and Fe Co-Doped Biochar from Bark for the Rapid Degradation of Guaiacol.

A boron and iron co-doped biochar (B-Fe/biochar) from Masson pine bark was fabricated and used to activate peroxydisulfate (PDS) for the degradation of guaiacol (GL). The roles of the dopants and the contribution of the radical and non-radical oxidations were investigated. The results showed that the doping of boron and iron significantly improved the catalytic activity of the biochar catalyst with a GL removal efficiency of 98.30% within 30 min. The degradation of the GL mainly occurred through the generation of hydroxyl radicals (·OHs) and electron transfer on the biochar surface, and a non-radical degradation pathway dominated by direct electron transfer was proposed. Recycling the B-Fe/biochar showed low metal leaching from the catalyst and satisfactory long-term stability and reusability, providing potential insights into the use of metal and non-metal co-doped biochar catalysts for PDS activation.

Insights to PFOS elimination with peroxydisulfate activation mediated by boron modified Fe/C catalysts: Enhancing mechanism of boron and PFOS degradation pathway.

In this study, the boron-doped iron-carbon composite (Fe@B/C-2) was prepared via a simple solvothermal and secondary calcination process by using iron metal-organic frameworks (Fe-MOFs) as precursor. The obtained Fe@B/C-2 possessed abundant active sites and low iron ion leaching, and exhibited excellent performance on peroxydisulfate (PDS) activation for efficient PFOS (10 mg/L) degradation (94 %) in 60 min, with 0.2 g/L of catalyst dosage, 1.0 g/L of PDS dosage and at 5.0 of initial pH. The radical scavenging and electron paramagnetic resonance (EPR) tests demonstrated that SO4·- and ·OH were the primary active species during PFOS elimination. Under the attack of these species, PFOS was first transformed into PFOA, followed by a sequential defluorination process, and lastly mineralized into CO2 and F-. Notably, DFT results revealed that Fe species, -BC3/-BC2O structures on the carbon matrix performed crucial roles in PDS activation. The extraordinary catalytic activity of Fe@B/C-2 was attributable to the synergistic effects of Fe nanoparticles and the B-doped on carbon matrix. The doped B not only could activate the inert carbon skeleton and provided more catalytic centers, but also could accelerate the electron transfer efficiency, leading to a boost in PDS decomposition.

Rapid PFOS mineralization with peroxydisulfate activation process mediated by N modified Fe-based catalyst.

As the cheap and efficient catalysts, the iron-based catalysts have been considered as one of the most promising catalysts for peroxydisulfate (PDS) activation and the development of high-performance iron-based catalysts are attracting growing attentions. In this work, a magnetic Fe-based catalysts (Fe/NC-1000) was obtained by using Fe modified ZIF-8 as the precursor and used to activate the PDS for the degradation of perfluorooctane sulphonate (PFOS). Morphology and structure analysis showed that the resulted Fe/NC-1000 catalyst was displayed porous spheres (40-60 nm) and mainly composed of Fe0, FeNx and carbon. When Fe/NC-1000 was employed to activate the PDS (0.1 g/L of catalyst dosage, 0.5 g/L of PDS dosage and at initial pH of 4.6), the Fe/NC-1000/PDS system exhibited excellent efficiency (97.9 ± 0.1) % for PFOS (10 mg/L) degradation within 30 min. The quenching tests and EPR results revealed that the Fe/NC-1000/PDS system degraded PFOS primarily through singlet oxygen (1O2) evolution and electron-transfer process. Besides, based on the degradation byproducts determined by LC-MS-MS, the PFOS first occurred de-sulfonation to form PFOA, and then the resulted PFOA underwent stepwise defluorination in the Fe/NC-1000/PDS system. Density Functional Theory (DFT) calculations and electrochemistry tests strongly confirmed that Fe/NC-1000 exhibited high electron transfer efficiency, resulting in promoted performance on activating PDS. Importantly, the results of Ecological Structure-Activity Relationship (ECOSAR) analysis showed that the intermediates were lowly toxic during the PFOS degradation, manifesting a green process for PFOS removal. This study would provide more understandings for the persulfate activation process mediated by Fe-based catalysts for Perfluorinated alkyl substances (PFAS) elimination.

A biomass fiber adsorbent grafted with phosphate/amidoxime for efficient extraction of uranium from seawater by synergistic effect.

There are approximately 4 billion tons of uranium in the ocean, which is unmatched by the surface. Nevertheless, it's very challenging to extract uranium from the ocean due to the exceedingly low concentration of uranium in the ocean (about 3.3 µg L-1) as well as high salinity level. Current methods are often limited by selectivity, sustainability, economics, etc. Herein, phosphoric acid group and amidoxime group were grafted to skin collagen fibers through " initiated access" to design a new uranium extraction material, abbreviated as CGPA. Through laboratory simulation experiments, it is concluded that the maximum adsorption capacity of CGPA for uranium reaches 263.86 mg g-1. It has high adsorption, selectivity, and reusability for uranium. In the actual seawater extraction experiment, CGPA obtained 29.64 µg of uranium after extracting 10.0 L of seawater, and the extraction rate was 90.1%. The adsorbent has excellent effects in kinetics, selectivity, extraction capacity, renewability, etc. In the extraction of uranium from seawater, and is an economically feasible and industrially expandable adsorbent.

Fabrication of covalent organic frameworks modified nanofibrous membrane for efficiently enriching and detecting the trace polychlorinated biphenyls in water.

Enriching and detecting the trace pollutants in actual matrices are critical to evaluating the water quality. Herein, a novel nanofibrous membrane, named PAN-SiO2@TpPa, was prepared by in situ growing ß-ketoenamine-linked covalent organic frameworks (COF-TpPa) on the aminated polyacrylonitrile (PAN) nanofibers, and adopted for enriching the trace polychlorinated biphenyls (PCBs) in various natural water body (river, lake and sea water) through the solid-phase micro-extraction (SPME) process. The resulted nanofibrous membrane owned abundant functional groups (-NH-, -OH and aromatic groups), outstandingly thermal and chemical stability, and excellent ability in extracting PCBs congeners. Based on the SPME process, the PCBs congeners could be quantitatively analyzed by the traditional gas chromatography (GC) method, with the satisfactory linear relationship (R2>0.99), low detection limit (LODs, 0.1∼5 ng L-1), high enrichment factors (EFs, 2714∼3949) and multiple recycling (>150 runs). Meanwhile, when PAN-SiO2@TpPa was adopted in the real water samples, the low matrix effects on the enrichment of PCBs at both 5 and 50 ng L-1 over PAN-SiO2@TpPa membrane firmly revealed the feasibility of enriching the trace PCBs in real water. Besides, the related mechanism of extracting PCBs on PAN-SiO2@TpPa mainly involved the synergistic effect of hydrophobic effect, π-π stacking and hydrogen bonding.

Ultra-efficient adsorption of diclofenac sodium on fish-scale biochar functionalized with H3PO4 via synergistic mechanisms.

Developing safe and efficient diclofenac sodium (DS) removal technology has become a critical issue. This study synthesized the fish-scale biochar by co-pyrolysis of fish scale and phosphoric acid (H3PO4). In addition to increasing the specific surface area and pore volume of fish-scale biochar, H3PO4 assisted in the formation of Graphitic N and sp2 C, as well as reacting with C═O groups to form a significant number of phosphorus-containing groups. All these functional groups could act as major active sites for DS adsorption. Adsorption data could well fit pseudo-second-order and Langmuir models. The maximum adsorption capacity of FSB600-15 for DS was 967.1 mg g-1, which was much better than that reported in the literature. Under the synergistic effect of various mechanisms (pore-filling effect, electrostatic attraction, H-bonding, π-π, and n-π electron donor-acceptor interactions), the DS ultra-efficient adsorption on FSB600-15 was realized. Meanwhile, the DS adsorption by FSB600-15 was an endothermic, spontaneous, and entropy-increasing process. Furthermore, the DS adsorption capacity was more than 426.5 mg g-1 in the actual water, which was sufficient for practical applications.

Effectively remove printing ink from plastic surface over quaternary ammonium-modified waste cooking oil.

The printing ink on the plastic surface will greatly reduce the quality of recycled plastic products. In this work, quaternary ammonium-modified waste cooking oil (WCOEQ) was fabricated using waste cooking oil, epichlorohydrin, and trimethylamine aqueous solution as raw materials, through ring-opening esterification and quaternary amination reaction. The synthesis conditions of WCOEQ were optimised, and the structure and properties of WCOEQ were characterised by Fourier transform infrared spectroscopy, zeta potential, and 1H NMR. Furthermore, WCOEQ had excellent emulsifying performance, low kraft point, low critical micelle concentration value, good foaming, and stability, which could effectively reduce the surface tension of water, showing application potential in the field of plastic deinking. Importantly, compared with the waste cooking oil without deinking effect, the WCOEQ had an excellent deinking performance on the ink on the plastic surface, and the deinking efficiency could be improved by increasing the concentration of the deinking agent, the deinking temperature, and prolonging the pre-soaking and stirring time. The results of atomic force microscope, energy-dispersive spectroscopy, optical photos, and Leica microscope showed that the roughness changed significantly and the ink molecules were gradually peeling off. This work highlighted the potential of quaternary ammonium-modified waste cooking oil for excellent removal of printing inks on the plastic surface.

Example of removing printing ink from plastic surface using quaternary ammonium-modified waste cooking oil.

The printing ink on the plastic surface greatly reduces the quality of recycled plastic products. In this work, quaternary ammonium-modified waste cooking oil (WCOQE) was fabricated, using waste cooking oil, epichlorohydrin and trimethylamine aqueous solution as raw materials, by ring-opening esterification and quaternary amination reaction. The synthesis conditions of WCOQE were optimized, and the structure and properties of WCOQE were characterized by FTIR, zeta potential and 1H NMR. Furthermore, WCOQE had excellent emulsifying performance, low kraft point, low CMC value, good foaming and stability, which could effectively reduce the surface tension of water, showing application potential in the field of plastic deinking. Importantly, compared with the waste cooking oil without deinking effect, the WCOQE had an excellent deinking performance on the ink on plastic surface, and the deinking efficiency could be improved by increasing the concentration of deinking agent, the deinking temperature, and prolonging the pre-soaking and stirring time. The results of AFM, EDS, optical photos and Leica microscope showed that the roughness changed significantly, and the ink molecules were gradually peeling off. This work highlighted the excellent potential of quaternary ammonium-modified waste cooking oil for the removal of printing inks on the plastic surface.

Catalytic reforming of polyethylene pyrolysis vapors to naphtha range hydrocarbons with low aromatic content over a high silica ZSM-5 zeolite.

In this study, the microwave-assisted pyrolysis coupled with ex-situ catalytic reforming of polyethylene for naphtha range hydrocarbons, with low aromatic content, was investigated. Experimental results revealed that ZSM-5 zeolites with low SiO2/Al2O3 ratios led to high aromatic selectivity, while an extremely high SiO2/Al2O3 ratio significantly reduced the aromatic selectivity. The high selectivity of C5-C12 hydrocarbons (98.9 %) with low selectivity of C5-C12 aromatics (28.5 %) was obtained over a high silica ZSM-5 zeolite at a pyrolysis temperature of 500 °C, catalytic cracking temperature of 460 °C, and a weight hourly space velocity of 7 h-1. The liquid oil produced was mainly composed of C5-C12 olefins that can be easily converted into paraffin-rich naphtha by hydrogenation or hydrogen transfer reactions as the feedstock for new plastic manufacturing. 8 cycles of regeneration-reaction cycles were carried out successfully with little change on the product distribution, showing the great potential for continuous production of low-aromatic liquid oil. Catalyst characterization showed that the catalyst deactivation was primarily caused by coke deposition (approximately 16.0 wt%) on the surface of the catalysts, and oxidative regeneration was able to recover most of the pore structure and acidity of the zeolite by effectively removing coke. This study provides a better understanding for the plastic-to-naphtha process and even for scale-up studies.

High-resolution particle size and shape analysis of the first Samarium nanoparticles biosynthesized from aqueous solutions via cyanobacteria Anabaena cylindrica.

Samarium (Sm) is one of the most sought-after rare earth metals. Price trends and dwindling resources are making recovery increasingly attractive. In this context, the use of cyanobacteria is highly promising. For Sm it was unclear whether Anabaena cylindrica produces particles through metabolically active Sm3+ uptake. High-resolution (HR) imaging now clearly demonstrates microbe generated biosynthesis of Sm nano-sized particles (Sm NPs) in vivo. Furthermore, a simple method to determine particle size and shape with high accuracy is presented. Digital image analysis with ImageJ of HR-TEMs is used to characterize Sm NPs revealing a nearly uniform local size distribution. Assuming round particles, the overall average area size is 135.5 nm2, resp. 11.9 nm diameter. In HR, where different cell sections of the same cell are averaged, the mean particle is smaller, 76.7 nm2 resp. 8.9 nm diameter. The reciprocal aspect ratio is 0.63. The Feret major axis ratio is calculated as shape factor, with 35% of the particles between 1.2 and 1.4. A roundness classification shows that 38% of particles are fairly round and 41% are very round. Consequently, A. cylindrica represents a suitable microorganism for possible Sm recovery and biosynthesis of roundish nano-sized particles.

Lightweight, amphipathic and fire-resistant prGO/MXene spherical beads for rapid elimination of hazardous chemicals.

Frequent leaks of hazardous chemicals have a huge impact on human lives, property and the ecological environment. Therefore, the three-dimensional functional porous materials with high absorption efficiency and special wettability for the disposal of hazardous chemical spills is an urgent demand. In this work, a series of spherical beads consisting of partially reduced graphene oxide (prGO) and MXene (Ti3C2Tx) nanosheets were constructed by hydrogen bond induced self-assembly along with freeze-drying and thermal treatment. The lightweight and amphipathic prGO/MXene spherical beads (prGMSBDs) had millimeter-level size, spherical morphology and highly porous internal structure, which were especially suitable for eliminating hazardous chemicals. Because of their excellent thermal stability and fire retardance, the prGMSBDs could be used to absorb flammable organic liquids, reducing the fire risk of the flammable hazardous chemical spills. Indeed, the prGMSBDs exhibited outstanding absorption performances for various hazardous chemicals, including organic solvents and water-based concentrated acid and alkali. Moreover, the prGMSBDs showed relatively stable absorption performance after five absorption-drying cycles. Due to meeting the requirements of both amphipathic characteristic and flame retardancy, the prGMSBDs reported in this work may offer a promising strategy for rapidly cleaning up various hazardous chemicals and open a feasible route to protecting the combustible hazardous chemical spills from fire.

Constructing segregated polystyrene composites for excellent fire resistance and electromagnetic wave shielding.

Electroconductive polystyrene (PS) composites with ideal flame-retardant properties are considered as potential electromagnetic interference (EMI) shielding materials. In this work, PS/silicon wrapped ammonium polyphosphate/multi-wall carbon nanotubes (PS/SiAPP/MWCNT) composites with segregated structure were synthesized via the methods of balling mill and hot-pressing. The obtained results revealed that the SiAPP and MWCNT were successfully introduced onto PS spheres and showed uniform distribution on the PS surface. The thermogravimetric analysis showed that PS/SiAPP/MWCNT containing 7 wt% MWCNT exhibited excellent thermal stability. Furthermore, the results of cone calorimeter test indicated that the heat release rate and total heat release of the PS/SiAPP/MWCNT containing a loading of 7 wt% MWCNT were reduced by 60.5% and 33.9%, respectively. In addition, the EMI shielding performance could reach 11 dB. Above results implied that the synergistic effect between the MWCNT and SiAPP effectively enhanced the flame retardant performance of the PS by promoting the generation of dense and continuous char layer to protect the PS from burning. The multiple reflection and adsorption are responsible for improved EMI shielding effectiveness. Therefore, segregated PS/SiAPP/MWCNT hybrid is an up-and-coming candidate for satisfactory EMI shielding materials with exceptional fire retardancy for electronic devices.