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MXene-based photocatalytic membranes provide significant benefits for wastewater treatment by effectively combining membrane separation and photocatalytic degradation processes. MXene represents a pioneering 2D photocatalyst with a variable elemental composition, substantial surface area, abundant surface terminations, and exceptional photoelectric performance, offering significant advantages in producing high-performance photocatalytic membranes. In this review, an in-depth overview of the latest scientific progress in MXene-based photocatalytic membranes is provided. Initially, a brief introduction to the structure and photocatalytic capabilities of MXene is provided, highlighting their pivotal role in promoting the photocatalytic process. Subsequently, in pursuit of the optimal MXene-based photocatalytic membrane, critical factors such as the morphology, hydrophilicity, and stability of MXenes are meticulously taken into account. Various preparation strategies for MXene-based photocatalytic membranes, including blending, vacuum filtration, and dip coating, are also discussed. Furthermore, the application and mechanism of MXene-based photocatalytic membranes in micropollutant removal, oil-water separation, and antibacterial are examined. Lastly, the challenges in the development and practical application of MXene-based photocatalytic membranes, as well as their future research direction are delineated.
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Efficient oil-water separation has always been a research hotspot in the field of environmental studies. Employing a one-step hydrothermal approach, NiFe-layered double hydroxides (LDH) nanosheets were synthesized on nickel foam substrates. The resulting NiFe-LDH/NF membrane exhibited rejection rates exceeding 99% across six diverse oil-water mixtures, concurrently demonstrating a remarkable ultra-high flux of 1.4 × 106 L·m-2·h-1. This flux value significantly surpasses those documented in existing literature, maintaining stable performance over 1000 manual filtration cycles. These breakthroughs stem from the synergistic interplay among the three-dimensional channels of the nickel foam, the nanosheets, and the hydration layer. By leveraging the pore size of the foam to enhance the functionality of the hydration layer, the conventional trade-off between permeability and selectivity was transformed into a balanced force relationship between the hydration layer and the oil phase. The operational and failure mechanisms of the hydration layer were examined using the prepared NiFe-LDH/NF membrane, validating the correlation between oil phase viscosity and density with hydration layer rupture. Additionally, an extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory was employed to investigate changes in interaction energy, further reinforcing the study's findings. This research contributes novel insights and assistance to the comprehension and application of hydration layers in other membrane studies dedicated to oil-water separation.
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Hydrogen-bonded organic frameworks (HOFs) are a new class of crystalline porous materials that are formed through the interconnection of organic or metal-organic building units via intermolecular hydrogen bonds. The remarkable flexibility and reversibility of hydrogen bonds, coupled with the customizable nature of organic units, endow HOFs with mild synthesis conditions, high crystallinity, solvent processability, and facile self-healing and regeneration properties. Consequently, these features have garnered significant attention across various fields, particularly in the realm of membrane separation. Herein, we present an overview of the recent advances in HOF-based membranes, including their advanced fabrication strategies and fascinating applications in membrane separation. To attain the desired HOF-based membranes, careful consideration is dedicated to crucial factors such as pore size, stability, hydrophilicity/hydrophobicity, and surface charge of the HOFs. Additionally, diverse preparation methods for HOF-based membranes, including blending, in situ growth, solution-processing, and electrophoretic deposition, have been analyzed. Furthermore, applications of HOF-based membranes in gas separation, water treatment, fuel cells, and other emerging application areas are presented. Finally, the challenges and prospects of HOF-based membranes are critically pointed out.
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In the evolving landscape of water treatment, membrane technology has ascended to an instrumental role, underscored by its unmatched efficacy and ubiquity. Diverse synthesis and modification techniques are employed to fabricate state-of-the-art liquid separation membranes. Click reactions, distinguished by their rapid kinetics, minimal byproduct generation, and simple reaction condition, emerge as a potent paradigm for devising eco-functional materials. While the metal-free thiol-ene click reaction is acknowledged as a viable approach for membrane material innovation, a systematic elucidation of its applicability in liquid separation membrane development remains conspicuously absent. This review elucidates the pre-functionalization strategies of substrate materials tailored for thiol-ene reactions, notably highlighting thiolation and introducing unsaturated moieties. The consequential implications of thiol-ene reactions on membrane properties-including trade-off effect, surface wettability, and antifouling property-are discussed. The application of thiol-ene reaction in fabricating various liquid separation membranes for different water treatment processes, including wastewater treatment, oil/water separation, and ion separation, are reviewed. Finally, the prospects of thiol-ene reaction in designing novel liquid separation membrane, including pre-functionalization, products prediction, and solute-solute separation membrane, are proposed. This review endeavors to furnish invaluable insights, paving the way for expanding the horizons of thiol-ene reaction application in liquid separation membrane fabrication.
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Assembling metal-organic frameworks (MOFs) into high-performance macroscopic membranes is crucial but still challenging. MOF-containing hybrid membranes can effectively integrate the advantages of flexible guest materials and MOFs. Nevertheless, the inherent limitations in fully harnessing the distinct characteristics of MOFs persist due to the substantial guest material content necessitated in membrane fabrication. Herein, inspired by the rigid and flexible structures in biological systems, rigid MIP-202(Zr) and defective MIP-202(Zr) (D-MIP-202(Zr)) modified flexible graphene oxide (GO) sheets are synthesized in situ and then assembled into a rigid-flexible coupled MOF-based membrane. The defects in D-MIP-202(Zr) are introduced by using acetic acid as the modulation agent. The obtained GO@MIP-202(Zr) membrane possesses a hierarchical porous structure with a 99 wt% MOF proportion, which is higher than the GO@D-MIP-202(Zr) (75 wt%) membrane with a compact bulge-structured surface. The water permeability of the GO@MIP-202(Zr) membrane attains remarkedly 5762.92 L h-1 m-2 bar-1 , which is 960 and 2.6 times higher than that of the GO membrane and GO@D-MIP-202(Zr) membrane. Additionally, benefiting from the superhydrophilicity and underwater superoleophobicity, the resultant membrane not only demonstrates high rejection for oil-water emulsions but also exhibits exceptional recyclability and anti-fouling ability. These findings provide valuable insights into the assembly of MOFs into high-performance membranes.
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The photothermal process has attracted considerable attention in water treatment due to its advantages of low energy consumption and high efficiency. In this respect, photothermal materials play a crucial role in the photothermal process. Particularly, carbonaceous materials have emerged as promising candidates for this process because of exceptional photothermal performance. While previous research on carbonaceous materials has primarily focused on photothermal evaporation and sterilization, there is now a growing interest in exploring the potential of photothermal effect-assisted advanced oxidation processes (AOPs). However, the underlying mechanism of the photothermal effect assisted by carbonaceous materials remains unclear. This review aims to provide a comprehensive review of the photothermal process of carbonaceous materials in water treatment. It begins by introducing the photothermal properties of carbonaceous materials, followed by a discussion on strategies for enhancing these properties. Then, the application of carbonaceous materials-based photothermal process for water treatment is summarized. This includes both direct photothermal processes such as photothermal evaporation and sterilization, as well as indirect photothermal processes that assisted AOPs. Meanwhile, various mechanisms assisted by the photothermal effect are summarized. Finally, the challenges and opportunities of using carbonaceous materials-based photothermal processes for water treatment are proposed.
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Transition metal carbides/nitrides/carbonitrides, commonly referred to as MXenes, have gained widespread attention since their discovery in 2011 as a promising family of two-dimensional (2D) materials. Their impressive chemical, electrical, thermal, mechanical, and biological properties have fueled a surge in research focused on the synthesis and application of MXenes in various fields, including membrane-based separation. By engineering the materials and membrane structures, MXene-based membranes have demonstrated remarkable separation performance and added functionalities, such as antifouling and photocatalytic properties. In this review, we aim to have a timely and critical review of research on their fabrication strategy and performance in advanced molecular separation and ion exchange, beginning with a brief introduction of the preparation and physicochemical properties of MXenes. Finally, outlooks and future works are outlined with the aims to provide valuable insights and guidance for advancing membranes' applications in different separation domains.
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Photocatalytic membranes can effectively integrate membrane separation and photocatalytic degradation processes to provide an eco-friendly solution for efficient water purification. It is of great significance to develop highly efficient photocatalytic membranes driven by visible light to ensure the long-term stability of membrane separation systems and the maximum utilization of solar energy. Metal-organic framework (MOF) is an emerging photocatalyst with a well-defined structure and tunable chemical properties, showing a broad application prospect in the construction of high-performance photocatalytic membranes. Herein, this work provides a comprehensive review of recent advancements in MOF-based photocatalytic membranes. Initially, this work outlines the main tailoring strategies that facilitate the enhancement of the photocatalytic activity of MOF-based photocatalysts. Next, this work introduces commonly used methods for fabricating MOF-based photocatalytic membranes. Subsequently, this work discusses the application and mechanisms of MOF-based photocatalytic membranes toward organic pollutant degradation, metal ion removal, and membrane fouling mitigation. Finally, challenges in developing MOF-based photocatalytic membranes and their practical applications are presented, while also pointing out future research directions toward overcoming these existing limitations.
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Single-atom catalysts, characterized by individual metal atoms as active centers, have emerged as promising candidates owing to their remarkable catalytic efficiency, maximum atomic utilization efficiency, and robust stability. However, the limitation of single-atom catalysts lies in their inability to cater to multistep reactions using a solitary active site. Introducing an additional metal atom can amplify the number of active sites, modulate the electronic structure, bolster adsorption ability, and enable a gamut of core reactions, thus augmenting their catalytic prowess. As such, dual-atom catalysts have risen to prominence. However, a comprehensive review elucidating the realm of dual-atom catalysts in environmental remediation is currently lacking. This review endeavors to bridge this gap, starting with a discourse on immobilization techniques for dual-atom catalysts, which includes configurations such as adjacent atoms, bridged atoms, and co-facially separated atoms. The review then delves into the intrinsic activity mechanisms of these catalysts, elucidating aspects like adsorption dynamics, electronic regulation, and synergistic effects. Following this, a comprehensive summarization of dual-atom catalysts for environmental applications is provided, spanning electrocatalysis, photocatalysis, and Fenton-like reactions. Finally, the existing challenges and opportunities in the field of dual-atom catalysts are extensively discussed. This work aims to be a beacon, illuminating the path towards the evolution and adoption of dual-atom catalysts in environmental remediation.
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Molecular oxygen as a green, non-toxic, and inexpensive oxidant has displayed numerous advantages compared with other oxidants for more sustainable and environmentally benign pollutant degradation. Molecular oxygen activation stands as a groundbreaking approach in advanced oxidation processes, offering efficient environmental remediation with minimal environmental impact with the production of high-oxidation reactive oxygen species (ROS). The adaptability and energy efficiency of molecular oxygen activation significantly contribute to the progression of sustainable water remediation technologies. This review meticulously explores the principles and mechanisms of molecular oxygen activation, shedding light on the diverse ROS production pathways. Subsequently, this review comprehensively details contemporary activation approaches, including photocatalytic activation, electrocatalytic activation, piezoelectric activation, and photothermal activation, explicating their distinct activation mechanisms. Additionally, it delves into the promising applications of molecular oxygen activation in the degradation of water pollutants, primary air pollutants, and volatile organic compounds, providing an in-depth analysis of the associated degradation pathways and mechanisms. Moreover, this review also addresses the imminent challenges and emerging opportunities in environmental remediation. It is envisioned that this comprehensive analysis will spur ongoing exploration and innovation in the use of molecular oxygen activation for environmental remediation and beyond.
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Poluentes Atmosféricos , Poluentes Ambientais , Recuperação e Remediação Ambiental , Espécies Reativas de Oxigênio , Oxidantes , OxigênioRESUMO
To address current energy crises and environmental concerns, it is imperative to develop and design versatile porous materials ideal for water purification and energy storage. The advent of covalent organic frameworks (COFs), a revolutionary terrain of porous materials, is underscored by their superlative features such as divinable structure, adjustable aperture, and high specific surface area. However, issues like inferior electric conductivity, inaccessible active sites impede mass transfer and poor processability of bulky COFs restrict their wider application. As a herculean stride forward, COF/graphene hybrids amalgamate the strengths of their constituent components and have in consequence, enticed significant scientific intrigue. Herein, the current progress on the structure and properties of graphene-based materials and COFs are systematically outlined. Then, synthetic strategies for preparing COF/graphene hybrids, including one-pot synthesis, ex situ synthesis, and in situ growth, are comprehensively reviewed. Afterward, the pivotal attributes of COF/graphene hybrids are dissected in conjunction with their multifaceted applications spanning adsorption, separation, catalysis, sensing, and energy storage. Finally, this review is concluded by elucidating prevailing challenges and gesturing toward prospective strides within the realm of COF/graphene hybrids research.
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The integration of catalytic degradation and membrane separation processes not only enables continuous degradation of contaminants but also effectively alleviates inevitable membrane fouling, demonstrating fascinating practical value for efficient water purification. Such membrane-catalysis integrated system (MCIS) has attracted tremendous research interest from scientists in chemical engineering and environmental science recently. In this review, the advantages of MCIS are discussed, including the membrane structure regulation, stable catalyst loading, nano-confinement effect, and efficient natural organic matter (NOM) exclusion, highlighting the synergistic effect between membrane separation and catalytic process. Subsequently, the design considerations for the fabrication of catalytic membranes, including substrate membrane, catalytic material, and fabrication method, are comprehensively summarized. Afterward, the mechanisms and performance of MCIS based on different catalytic types, including liquid-phase oxidants/reductants involved MCIS, gas involved MCIS, photocatalysis involved MCIS, and electrocatalysis involved MCIS are reviewed in detail. Finally, the research direction and future perspectives of catalytic membranes for water purification are proposed. The current review provides an in-depth understanding of the design of catalytic membranes and facilitates their further development for practical applications in efficient water purification.
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Single-atom catalysts (SACs) for photocatalytic hydrogen peroxide (H2 O2 ) generation are researched but it is still challenging to obtain high H2 O2 yields. Herein, graphite carbon nitride (FeSA /CN) confined single Fe atoms with N/O coordination is prepared, and FeSA /CN shows high H2 O2 production via oxalic acid and O2 activation. Under visible light illumination, the concentration of H2 O2 generated by FeSA /CN can achieve 40.19 mM g-1 h-1 , which is 10.44 times higher than that of g-C3 N4 . The enhanced H2 O2 generation can be attributed to the formation of metal-organic complexes and rapid electron transfer. Moreover, the O2 activation of photocatalysts is revealed by 3,3',5,5'-tetramethylbenzidine oxidation. The results display that the O2 activation capacity of FeSA /CN is higher than that of g-C3 N4 , which facilitates the formation of H2 O2 . Finally, density functional theory calculation demonstrates that O2 is chemically adsorbed on Fe atomic sites. The adsorption energy of O2 is enhanced from -0.555 to -1.497 eV, and the bond length of OO is extended from 1.235 to 1.292 Å. These results exhibit that the confinement of single Fe atoms can promote O2 adsorption and activation. Finally, the photocatalytic mechanism is elaborated, which provides a deep understanding for SACs-catalyzed H2 O2 generation.
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Over the last decades, advanced oxidation processes (AOPs) have been widely used in surface and ground water pollution control. The heterogeneous electro-Fenton (EF) process has gained much attention due to its properties of high catalytic performance, no generation of iron sludge, and good recyclability of catalyst. As of October 2022, the cited papers and publications of EF are around 1.3 × 10-5 and 3.4 × 10-3 in web of science. Among the AOP techniques, the contaminant removal efficiencies by EF process are above 90% in most studies. Current reviews mainly focused on the mechanism of EF and few reviews comprehensively summarized heterogeneous catalysts and their applications in wastewater treatment. Thus, this review focuses on the current studies covering the period 2012-2022, and applications of heterogeneous catalysts in EF process. Two kinds of typical heterogeneous EF systems (the addition of solid catalysts and the functionalized cathode catalysts) and their applications for organic contaminants degradation in water are reviewed. In detail, solid catalysts, including iron minerals, iron oxide-based composites, and iron-free catalysts, are systematically described. Different functionalized cathode materials, containing Fe-based cathodes, carbonaceous-based cathodes, and heteroatom-doped cathodes, are also reviewed. Finally, emphasis and outlook are made on the future prospects and challenges of heterogeneous EF catalyst for wastewater treatments.
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Poluentes Químicos da Água , Água , Esgotos , Minerais , Catálise , Peróxido de Hidrogênio , Poluentes Químicos da Água/análise , OxirreduçãoRESUMO
The oily water treatment is becoming one of the hottest topics due to that increase of offshore oil transportation and the various accident oil leakages. In this study, a functional TiO2-ABS composite membrane was generated through the three-dimensional (3D) printing strategy for the first time and was conducted to simulated oily water treatment. The TiO2-ABS composite membrane demonstrated a significant promotion in hydrophilicity and oleophobicity which were evidenced by the water contact angle of 14.8° and the underwater oil contact angle of 144.7°, respectively. The optimal modified membrane had both exceedingly high flux (1.8 × 105 L m-2·h-1) and oil rejection rate (99.5%). Moreover, the results of filtration cycles of 10 days and extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory demonstrated that the modified membranes took possession of excellent stability and antifouling property. What was more, the TiO2-ABS composite membrane revealed over 99% rejection to all five types of oil/water systems. The interestingly experimental results indicated that the prepared membrane possessed a broad development trend and application prospect in the field of oily water treatment.
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Acrilonitrila , Butadienos , Estireno , Titânio , ÓleosRESUMO
Membrane-based carbon dioxide (CO2 ) capture and separation technologies have aroused great interest in industry and academia due to their great potential to combat current global warming, reduce energy consumption in chemical separation of raw materials, and achieve carbon neutrality. The emerging covalent organic frameworks (COFs) composed of organic linkers via reversible covalent bonds are a class of porous crystalline polymers with regular and extended structures. The inherent structure and customizable organic linkers give COFs high and permanent porosity, short transport channel, tunable functionality, and excellent stability, thereby enabling them rising-star alternatives for developing advanced CO2 separation membranes. Therefore, the promising research areas ranging from development of COF membranes to their separation applications have emerged. Herein, this review first introduces the main advantages of COFs as the state-of-the-art membranes in CO2 separation, including tunable pore size, modifiable surfaces property, adjustable surface charge, excellent stability. Then, the preparation approaches of COF-based membranes are systematically summarized, including in situ growth, layer-by-layer stacking, blending, and interface engineering. Subsequently, the key advances of COF-based membranes in separating various CO2 mixed gases, such as CO2 /CH4 , CO2 /H2 , CO2 /N2 , and CO2 /He, are comprehensively discussed. Finally, the current issues and further research expectations in this field are proposed.
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The greatest environmental issue of the twenty-first century is climate change. Human-caused greenhouse gas emissions are increasing the frequency of extreme weather. Carbon dioxide (CO2) accounts for 80% of human greenhouse gas emissions. However, CO2 emissions and global temperature have risen steadily from pre-industrial times. Emissions data are crucial for most carbon emission policymaking and goal-setting. Sustainable and carbon-neutral sources must be used to create green energy and fossil-based alternatives to reduce our reliance on fossil fuels. Near-real-time monitoring of carbon emissions is a critical national concern and cutting-edge science. This review article provides an overview of the many carbon accounting systems that are now in use and are based on an annual time frame. The primary emphasis of the study is on the recently created carbon emission and eliminating sources and technology, as well as the current application trends for carbon neutrality. We also propose a framework for the most advanced naturally available carbon neutral accounting sources capable of being implemented on a large scale. Forming relevant data and procedures will help the "carbon neutrality" plan decision-making process. The formation of pertinent data and methodologies will give robust database support to the decision-making process for the "carbon neutrality" plan for the globe. In conclusion, this article offers some opinions, opportunities, challenges and future perspectives related to carbon neutrality and carbon emission monitoring and eliminating resources and technologies.
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Dióxido de Carbono , Gases de Efeito Estufa , Humanos , Dióxido de Carbono/análise , Efeito Estufa , Biodiversidade , Temperatura , Tecnologia , Recursos NaturaisRESUMO
The increasingly serious pollution of antibiotics brings an enormous threat to the ecological environment and human health. Graphite phase carbon nitride (g-C3N4), as a popular photocatalytic material, is widely used in photocatalytic degradation of antibiotics in water. In order to make up for the shortage of g-C3N4 monomer, CeO2/N-doped g-C3N4 (CeNCN) composite photocatalysts co-modified with nitrogen doping and CeO2 loading were designed and synthesized with the idea of expanding visible light absorption and promoting photogenerated carrier separation. CeNCN exhibits excellent photodegradation performance, the removal rate of tetracycline reached 80.09% within 60 min, which is much higher than that of g-C3N4 (CN) and N-doped g-C3N4 (NCN); and the quasi-first-order degradation rate constant is 0.0291, which is 7.86 and 2.29 times higher than CN and NCN. Electron spin resonance and free radical trapping experiments confirmed that h+, O2- and OH are the active substances in the photocatalytic system. After 5 cycles, the degradation efficiency of tetracycline still exceeds 75%, which indicates that CeNCN has good stability. This work proves that N-doping and CeO2 loading can effectively broaden the photoresponse range of g-C3N4, facilitate the separation of photogenerated electron-hole pairs, and provide a reference for the construction of g-C3N4-based photocatalyst with high-efficiency photodegradation activity.
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Grafite , Antibacterianos , Catálise , Cério , Humanos , Luz , Nitrogênio , Compostos de Nitrogênio , TetraciclinaRESUMO
With the increasing serious water pollutions, an increasing interest has given for the nanocomposites as environmental catalysts. To date, noble metals-based nanocomposites have been extensively studied by researchers in environmental catalysis. In detail, serving as key functional parts, noble metals are usually combined with other nanomaterials for rationally designing nanocomposites, which exhibit enhanced catalytic properties in pollutants removal. Noble metals in the nanocomposites possess tailored properties, thus playing different important roles in catalytic oxidation reactions for pollutants removal. To motivate the research and elaborate the progress of noble metals, this review (i) summarizes advanced characterization techniques and rising technology of theoretical calculation for evaluating noble metal, and (ii) classifies the roles according to their disparate mechanism in different catalytic oxidation reactions. Meanwhile, the enhanced mechanism and influence factors are discussed. (iii) The conclusions, facing challenges and perspectives are proposed for further development of noble metals-based nanocomposites as environmental catalysts.
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Poluentes Ambientais , Nanoestruturas , Catálise , Metais , OxirreduçãoRESUMO
Recently, persulfate (PS) activation system has grown up as a primary branch of advanced oxidation processes, and biochar has been recognized as a potential nonmetal material in this field. However, few studies have focused on the corresponding relationship between actives sites on biochar and active species in AOPs. To pave this way, similar biochar (obtained from different pyrolysis temperature) with different functional structures were involved. In this study, biochar derived from swine bone (BBC) was applied in PS activation system to degrade acetaminophen (ACT). The results showed that both radical and non-radical pathway worked in the PS/BBCs systems, and the degradation rate (from 0.1042 to 0.4364â¯min-1) climbed with the increase of pyrolysis temperature (from 700 to 900⯰C). To probe into the corresponding relationship between functional structure and active species, the effect of pyrolysis temperature on functional structure was analyzed. It came out that 1) defects could act as active sites for various active species; 2) persistent free radicals could do favor to the generation of 1O2 and O2-; 3) hydroxyapatite in swine bone only served as hard templet for the porous structure. ACT degradation process was measured by Liquid chromatograph-mass spectrometer, and Scendesmus obliquus was applied to investigate the toxicity of PS/BBCs system. It illustrated that the existence of SO4- mainly contributed to the generation of high toxic intermediates (such as biphenyl and diphenyl ether) in the PS/BBCs system. Furthermore, the enhancement of adsorption capacity would mitigate the toxicity of PS/BBCs systems to some extent.