Lifetime Of Radicals Research Articles

Meta-substituted thienoviologen with enhanced radical stability via π-π interaction modulation for neutral aqueous organic flow batteries

The aqueous organic redox flow batteries (AORFBs) are recognized as the most promising large-scale storage technology for long-duration energy storage (LDES). Although viologen derivatives are widely used as anolyte materials for AORFBs, their practical application is strongly limited by weak conjugation and unstable radicals. Here, we present a novel thienoviologen derivative, [(NPr)2SV]Cl4, achieved utilizing a meta-substitution approach based on the pristine viologen derivatives ( [(NPr)2V]Cl4). Compared to other ortho- and para-substitution methods, this strategy features a locked plane configuration (0.14°), effectively regulating π-π interactions and suppressing reactivity between radical and oxygen, which is confirmed via X-ray single-crystal structural analyses, spectroscopy techniques, molecular dynamics simulation accompanied by linear ion trap mass spectrometry experiments. Additionally, the meta-substituted [(NPr)2SV]Cl4 significantly improves water solubility (2.39 M), enhances aromaticity, and extends radical lifetime compared with para-substituted [(NPr)2TV]Cl4. Consequently, the cycling stability of the [(NPr)2SV]Cl4-based AORFB over 2500 cycles is 4.1 times higher than that of [(NPr)2TV]Cl4. Furthermore, the 0.5 M battery delivers an impressive 99.83% capacity retention during 200 cycles and a power density of 147 mW cm-2.

Electroprecipitating the Sulfate Radical Anion Amplifies Electrochemiluminescence in Space and Time.

We have discovered a strategy to synthesize reactive radical salts, effectively bottling up radicals in space and time for future use. We apply this new principle to electrochemiluminescence (ECL) through the simultaneous electro-reduction of peroxydisulfate, S2O82-, and tris(bipyridine)ruthenium(II), [Ru(bpy)3]2+ in a water/acetonitrile mixture. The electrode generates a concentration profile exceeding the solubility of the cation and anion pair, promoting precipitation. After the application of a potential, leads are disconnected, and the crystals electrolessly chemiluminesce during dissolution and can be transported to other solutions for later chemiluminescence uses. Our method extends ECL hundreds of micrometers from the electrode surface and increases the ECL lifetime by orders of magnitude. Control experiments, including electron spin resonance, validate the crystallization of SO4•-, allowing detailed mechanistic insight. We demonstrate platform generalizability by precipitating a radical salt made of calcium and SO4•-, and we demonstrate the salt's ability to drive chemiluminescence. Our results emphasize the elegant chemical tenet that extremely reactive radicals can be bottled up as solids to be used as future reagents if precipitation occurs more quickly than the radical lifetime.

Variation in the relationship between odd isotopes of tin in mass-independent fractionation induced by the magnetic isotope effect

Experimental results are presented showing the variation in the relationship between odd isotopes of tin (Sn) in mass-independent fractionation caused by the magnetic isotope effect (MIE), which has previously only been observed for mercury. These results are consistent with the trend predicted from the difference between the magnitudes of nuclear magnetic moments of odd isotopes with a nuclear spin. However, the correlation between odd isotopes in fractionation induced by the MIE for the reaction system used in this study (solvent extraction using a crown ether) was different from that reported for the photochemical reaction of methyltin. This difference between the two reaction systems is consistent with a theoretical prediction that the correlation between odd isotopes in fractionation induced by the MIE is controlled by the relationship between the spin conversion time and radical lifetime. The characteristic changes in the correlation between odd isotopes in fractionation induced by the MIE observed for Sn in this study provide a guideline for quantitatively determining fractionation patterns caused by the MIE for elements that have multiple isotopes with a nuclear spin. These results improve our understanding of the potential impact of the MIE on mass-independent fractionation observed in natural samples, such as meteorites, and analytical artifacts of high-precision isotope analysis for heavy elements.

A Deterministic Model to Predict Tacticity Changes During Controlled Degradation of Polypropylene

Controlled degradation of polypropylene (CPP) converts high-molecular-weight (Mw) polypropylene (PP) to lower Mw PP using peroxide-induced degradation. A deterministic model is developed to predict tacticity changes in isotactic PP. The model determines instantaneous rates of defective-pentad formation and tracks accumulation of these pentads using dynamic material balances. The model relies on the assumption that lifetimes of polymeric radicals are short compared to extruder residence times. Model predictions agree with previous Monte Carlo simulations that require long simulation times. Two versions of the model are proposed: one assumes that radical migration, also called chain walking, occurs via 1–6 isomerization and one assumes 1–8 isomerization. Chain-transfer-to-polymer and chain-walking parameters are estimated using 13C NMR data obtained using initiator levels between 0.006 and 0.52 wt%. Both 1–6 and 1–8 isomerization models result in better fit to the data.

The Lifetime of Hydroxyl Radical in Realistic Fuel Cell Catalyst Layer.

The lifetime of hydroxyl radicals (⋅OH) in the fuel cell catalyst layer remains uncertain, which hampers the comprehension of radical-induced degradation mechanisms and the development of longevity strategies for proton-exchange membrane fuel cells (PEMFCs). In this study, we have precisely determined that the lifetime of ⋅OH radicals can extend up to several seconds in realistic fuel cell catalyst layers. This finding reveals that ⋅OH radicals are capable of carrying out long-range attacks spanning at least a few centimeters during PEMFCs operation. Such insights hold great potential for enhancing our understanding of radical-mediated fuel cell degradation processes and promoting the development of durable fuel cell devices.

Alkylphenols disrupt estrogen homeostasis via diradical cross-coupling reactions: A novel pathway of endocrine disruption

Estrogen, being an essential class of sex hormone, is an important target of endocrine disruption chemicals. It is well known that environmental disruptors could activate or inhibit estrogen receptors, acting as agonists or antagonists, and thus affect the circulating estrogen concentrations. Here, we report enzyme-mediated diradical cross-coupling reactions between alkylphenols (e.g., 2,4-di-tert-butylphenol [DBP], 4-nonylphenol [4-NP], and 4-tert-octylphenol [4-t-OP]) and estrogens (e.g., estradiol [E2]) that generate coupling metabolites and disrupt estrogen homeostasis. Among the phenolic xenobiotics, the screening of metabolic products revealed that alkylphenols had the highest reaction activities and generated coupling metabolites with high abundances (DBP-O-E2, 4-t-OP-O-E2, and 4-NP-O-E2). The coupling reactions were catalyzed by cytochrome P450 3A4 (CYP3A4) and verified by the detection of the coupling products in general populations. In vitro and in vivo exposures together with CYP3A4 inhibition demonstrated that cross-coupling reactions of phenols and E2 significantly reduced the normal levels of E2. We further established a unique spin-trapping-based high-throughput screening method to show the existence of diradicals in the coupling reaction. Density functional theory calculations revealed that spin aromatic delocalization was the fundamental cause of the high rebound barrier and sufficient lifetime of phenoxy radicals that enabled phenolic cross-coupling triggered by cytochrome P450. The identified mechanistic details for diradical cross-coupling reactions provide a novel pathway for phenolic chemicals to disrupt estrogen homeostasis.

Asymmetric A‐DA′D‐A′′ Molecular Configuration Type‐I Photosensitizer with Two Complementary Reactive Oxygen Species for Efficient Imaging and Photodynamic Therapy

AbstractType‐I photosensitizers (PSs) can efficiently generate reactive oxygen species (ROS) in the hypoxia condition of tumors, which show less oxygen dependence and are considered better candidates for photodynamic therapy (PDT). However, relatively few efficient type‐I organic PSs simultaneously generating two or more type‐I ROS under irradiation are reported. Herein, new alternate donor (D)‐acceptor (A) type molecules containing ladder‐type core (DA′D) fused with an electron‐deficient benzothiadiazole core are reported, which show symmetrical A‐DA′D‐A (QY1) and asymmetrical A‐DA′D‐A′′ (QY2) configurations, respectively. As these ROSs possess complementary properties of strong oxidizing ability (•OH) and long radical lifetime (O2•−), in vitro and in vivo experiments demonstrate that QY1 and QY2 show excellent PDT effects for tumor cells under normoxia or hypoxia, and can achieve remarkable tumor growth inhibition (TGI) rate of 90% for the QY2. More importantly, the generation of •OH in these PSs is revealed by experiments both in aqueous and in vitro, including the well‐known transformation of O2•− and direct electron transition from water to excited triplet PS. It thus provides a comprehensive understanding of the O2 dependence property of •OH radical and deep insights into the mechanism of type‐I PS.

Tunable Chromic Properties of Viologen-Metal Polymers Modulated by Coordination Modes for Inkless Erasable Printing.

Inkless and erasable printing (IEP) based on chromic materials holds great promise to alleviate environmental and sustainable problems. Metal-organic polymers (MOPs) are bright platforms for constructing IEP materials. However, it is still challenging to design target MOPs with excellent specific functions rationally due to the intricate component-structure-property relationships. Herein, an effective strategy was proposed for the rational design IEP-MOP materials. The stimuli-responsive viologen moiety was introduced into the construction of MOPs to give it potential chromic behaviors and two different coordination models (i.e. bilateral coordination model, M1; unilateral coordinated model, M2) based on the same viologen ligand were designed. Aided by theoretical calculations, model M1 was recommended secondarily as a more suitable system for IEP materials. Along this line, two representative viologen-ZnII MOPs 1 and 2 with models M1 and M2 were synthesized successfully. Experiments exhibit that 1 does have quicker stimuli response, stronger color contrast and longer radical lifetime compared to 2. Significantly, the obtained 1-IEP media brightly inherits the excellent chromic characteristics of 1 and the flexibility of the paper at the same time, which achieves most daily printing requirements, as well as enough resolution and durability to be used in identification by smart device.

The lifetime of polychlorophenyl radicals in methanol: A SCC–DFTB molecular dynamics study

The state of molecules of mono-, di-, and trichlorobenzenes in the gas phase and methanol solution is explored using quantum chemical molecular dynamics simulations. It is proved that saturation of chloroaryl radicals in methanol is realized using a hydrogen atom from the methyl group of solvents rather than from the hydroxyl group in most cases. No evident correlation was established between the lifetimes and other properties of radicals or their parent molecules, pointing to the importance of a solvate shell as a factor controlling the migration and diffusion of H atoms during the saturation of chloroaryl radicals.

Regulating Degradation Pathways of Polymers by Radical-Triggered Luminescence.

Understanding the radical behaviours during polymer degradation is beneficial to unveil and regulate the degradation pathways of polymers to achieve a sustainable polymer development. However, it is a long-standing challenge to study radical behaviours owing to the ultra-short lifetime of the transient radicals generated during the polymer degradation. In this contribution, we have proposed the radical-triggered luminescence to monitor the radical behaviours during polymer degradation without/with the addition of inorganic additives. It was disclosed that the pure polymers showed a single sigmoidal dynamic curve from peroxy radicals (ROO⋅) emissions, leading to the exponential proliferation for the degradation evolution. Alternatively, the degradation pathways with the addition of additives, layered double hydroxides (LDHs) with positively charged Al centers, could be modulated into a double sigmoidal dynamics, involving the main product of alkoxy radicals (RO⋅) with the activation energy of 40.2 kJ/mol and a small amount of ROO⋅ with 76.3 kJ/mol, respectively. Accordingly, the polymers with the additive-regulated pathways could exhibit prominently anti-degradation behaviours. This work is beneficial for the deep understanding of the radical mechanisms during polymer degradation, and for the rational design of anti-degradation polymers.

Regulating Degradation Pathways of Polymers by Radical‐Triggered Luminescence

AbstractUnderstanding the radical behaviours during polymer degradation is beneficial to unveil and regulate the degradation pathways of polymers to achieve a sustainable polymer development. However, it is a long‐standing challenge to study radical behaviours owing to the ultra‐short lifetime of the transient radicals generated during the polymer degradation. In this contribution, we have proposed the radical‐triggered luminescence to monitor the radical behaviours during polymer degradation without/with the addition of inorganic additives. It was disclosed that the pure polymers showed a single sigmoidal dynamic curve from peroxy radicals (ROO⋅) emissions, leading to the exponential proliferation for the degradation evolution. Alternatively, the degradation pathways with the addition of additives, layered double hydroxides (LDHs) with positively charged Al centers, could be modulated into a double sigmoidal dynamics, involving the main product of alkoxy radicals (RO⋅) with the activation energy of 40.2 kJ/mol and a small amount of ROO⋅ with 76.3 kJ/mol, respectively. Accordingly, the polymers with the additive‐regulated pathways could exhibit prominently anti‐degradation behaviours. This work is beneficial for the deep understanding of the radical mechanisms during polymer degradation, and for the rational design of anti‐degradation polymers.

Photoenzymatic Enantioselective Intermolecular Radical Hydroamination.

Since the discovery of Hofmann-Löffler-Freytag reaction more than 130 years ago, nitrogen-centered radicals have been widely studied in both structures and reactivities1-2. Nevertheless, catalytic enantioselective intermolecular radical hydroamination remains a challenge due to the existence of side reactions, short lifetime of nitrogen-centered radicals, and lack of understanding of the fundamental catalytic steps. In chemistry, nitrogen-centered radicals are produced with radical initiators, photocatalysts, or electrocatalysts. On the other hand, the generation and reaction of nitrogen-centered radicals are unknown in nature. Here we report a pure biocatalytic system by successfully repurposing an ene-reductase through directed evolution for the photoenzymatic production of nitrogen-centered radicals and enantioselective intermolecular radical hydroaminations. These reactions progress efficiently at room temperature under visible light without any external photocatalysts and exhibit excellent enantioselectivities. Detailed mechanistic study reveals that the enantioselectivity originates from the radical-addition step while the reactivity originates from the ultrafast photoinduced electron transfer (ET) from reduced flavin mononucleotide (FMNH-) to nitrogen-containing substrates.

Type-I organic photosensitizers with two complementary reactive oxygen species based on donor-acceptor (D-A) molecules

Type-I photosensitizers (PSs) are considered to be a better choice for photodynamic therapy (PDT) because they can efficiently generate reactive oxygen species (ROS) in the hypoxia condition of tumor, showing less oxygen dependence. However, there are relatively few reported highly efficient type-I organic PSs, especially those simultaneously generated two or more species of type-I ROS. Herein, based on electron-acceptor of 9,10-phenanthrenequinone (PQ), a D-A-D structural type-I PS of PPQ constructed from electron-donor of 9-phenyl-carbazole (PCZ) was firstly developed and could simultaneously produce two type-I ROS under white light irradiation. As the generated ROS of hydroxyl radical (•OH) and superoxide anion radical (O2•−) possessed complementary oxidizing ability and radical lifetime, PPQ showed excellent PDT effects for tumor cells under normoxia or hypoxia. The ability of ROS generation and PDT performance of PPQ were better than those of another PQ derivative (TPQ) constructed with common electron-donor triphenylamine (TPA). More importantly, experiments in aqueous solution and vitro both revealed that •OH generated not only from the well-known transformation of O2•− but also direct electron transition from water to triplet excited PS, which demonstrated the oxygen dependence of type-I PSs more clearly. This new type-I PS offers an opportunity to obtain deep insights of the mechanism of type-I PSs, and provides a new strategy for development of type-I PSs.

Stability and Population of Radicals in Electrical Trees in Epoxy Resins Based on Electron Paramagnetic Resonance Spectroscopy

The stability and population of radicals in aged epoxy resins with different electrical trees are investigated by electron paramagnetic resonance. Branch trees and bush trees of various sizes are produced in three types of epoxy resins which are cured by different curing agents. By examining the lifetime of radicals in three epoxies, the mobility of polymer chains is found to act as a vital factor for stability. The recombination of radicals is faster in polymers with higher mobility, leading to a shorter lifetime of radical signals. A distinguishable singlet appears in specimens without visible tree channels, proving that radicals are a precursor of electrical trees. Among spectra from a series of branch trees, two species of radicals are found to be generated successively as tree size increases. By comparing the signal intensity of branch trees and bush trees of similar sizes, bush trees show a much smaller radical population, which is attributed to relatively low electrical stress at branch tips and slow degradation of polymer chains.

A Nickel-Catalyzed Cross-Electrophile Coupling Reaction of 1,3-Dimesylates for Alkylcyclopropane Synthesis: Investigation of Stereochemical Outcomes and Radical Lifetimes.

Understanding mechanistic details of the nickel-catalyzed coupling reactions of Csp3 alcohol derivatives is key to developing selective reactions of this widely prevalent functional group. In this manuscript, we utilize a combination of experimental data and DFT studies to define the key intermediates, stereochemical outcome, and competing pathways of a nickel-catalyzed cross-electrophile coupling reaction of 1,3-dimesylates. Stereospecific formation of a 1,3-diiodide intermediate is achieved in situ by the Grignard reagent. The overall stereoablative stereochemical outcome is due to a nickel-catalyzed halogen atom abstraction with a radical rebound that is slower than epimerization of the alkyl radical. Finally, lifetimes of this alkyl radical intermediate are compared to radical clocks to enhance the understanding of the lifetime of the secondary alkyl radical.

Flower-like Nanozyme with Highly Porous Carbon Matrix Induces Robust Oxidative Storm against Drug-Resistant Cancer.

Reactive oxygen species (ROS) generators are sparking breakthroughs in sensitization and treatment of therapy-resistant tumors, yet the efficacy is drastically compromised by limited substrate concentrations, short lifetimes of free radicals, and restricted oxidative damage. Herein, a flower-like nanozyme with highly permeable leaflets accommodating catalytic metal sites was developed to address the challenges by boosting substrate and product accessibility. In the formation of a zeolite imidazole framework, cobalt ions promoted catalytic polymerization and deposition of polydopamine. The polymers acted as a stiffener for preventing framework collapse and maneuvering pore reopening during carbonization. The cobalt single-atom/cluster sites in the highly porous matrix generated peroxidase/oxidase-like activities with high catalytic efficiency (Kcat/Km) up to 6 orders of magnitude greater than that of conventional nano-/biozymes. Thereby, a robust ROS storm induced by selective catalysis led to rapid accumulation of oxidative damage and failure of antioxidant and antiapoptotic defense synchronization in drug-resistant cancer cells. By synergy of a redox homeostasis disrupter co-delivered, a significantly high antitumor efficiency was realized in vivo. This work offers a route to kinetically favorable ROS generators for advancing the treatment of therapy-resistant tumors.

Comparison of isoprene chemical mechanisms under atmospheric night-time conditions in chamber experiments: evidence of hydroperoxy aldehydes and epoxy products from NO3 oxidation

Abstract. The gas-phase reaction of isoprene with the nitrate radical (NO3) was investigated in experiments in the outdoor SAPHIR chamber under atmospherically relevant conditions specifically with respect to the chemical lifetime and fate of nitrato-organic peroxy radicals (RO2). Observations of organic products were compared to concentrations expected from different chemical mechanisms: (1) the Master Chemical Mechanism, which simplifies the NO3 isoprene chemistry by only considering one RO2 isomer; (2) the chemical mechanism derived from experiments in the Caltech chamber, which considers different RO2 isomers; and (3) the FZJ-NO3 isoprene mechanism derived from quantum chemical calculations, which in addition to the Caltech mechanism includes equilibrium reactions of RO2 isomers, unimolecular reactions of nitrate RO2 radicals and epoxidation reactions of nitrate alkoxy radicals. Measurements using mass spectrometer instruments give evidence that the new reactions pathways predicted by quantum chemical calculations play a role in the NO3 oxidation of isoprene. Hydroperoxy aldehyde (HPALD) species, which are specific to unimolecular reactions of nitrate RO2, were detected even in the presence of an OH scavenger, excluding the possibility that concurrent oxidation by hydroxyl radicals (OH) is responsible for their formation. In addition, ion signals at masses that can be attributed to epoxy compounds, which are specific to the epoxidation reaction of nitrate alkoxy radicals, were detected. Measurements of methyl vinyl ketone (MVK) and methacrolein (MACR) concentrations confirm that the decomposition of nitrate alkoxy radicals implemented in the Caltech mechanism cannot compete with the ring-closure reactions predicted by quantum chemical calculations. The validity of the FZJ-NO3 isoprene mechanism is further supported by a good agreement between measured and simulated hydroxyl radical (OH) reactivity. Nevertheless, the FZJ-NO3 isoprene mechanism needs further investigations with respect to the absolute importance of unimolecular reactions of nitrate RO2 and epoxidation reactions of nitrate alkoxy radicals. Absolute concentrations of specific organic nitrates such as nitrate hydroperoxides would be required to experimentally determine product yields and branching ratios of reactions but could not be measured in the chamber experiments due to the lack of calibration standards for these compounds. The temporal evolution of mass traces attributed to product species such as nitrate hydroperoxides, nitrate carbonyl and nitrate alcohols as well as hydroperoxy aldehydes observed by the mass spectrometer instruments demonstrates that further oxidation by the nitrate radical and ozone at atmospheric concentrations is small on the timescale of one night (12 h) for typical oxidant concentrations. However, oxidation by hydroxyl radicals present at night and potentially also produced from the decomposition of nitrate alkoxy radicals can contribute to their nocturnal chemical loss.

Ultraviolet Light-Driven gaining of hydroxyl and nitrogen oxide radicals in Plasma–Treated water

Here we numerically demonstrate that photolytic processes induced by external ultraviolet (UV) sources considerably affect the chemical properties of plasma–water systems. When describing the chemical transport between surface dielectric barrier discharge (SDBD) and deionized water, the plasma is simulated using a global model, while the gas (air) and liquid (water) regions are considered in a one-dimensional space. Our simulation involving exposure of plasma-treated water (PTW) to UV shows that long-lived species in PTW are readily photolyzed and form hydroxyl radical (OH) and nitric oxide (NO) over the entire liquid region. The total OH concentration was enhanced by 11.6 times at 100 s under exposure to a conventional UV lamp, while the total NO concentration was remarkably enhanced up to 45.8 times at 300 s. The time at which the OH concentration notably increases was advanced by more than 100 s by photolytic processes. The results directly reveal that the exposure of PTW to UV is an attractive approach to selectively releasing extra OH and NO, thereby increasing the PTW reactivity and applicability. Owing to their high reactivity and oxidizing power, the short lifetime of radicals including OH and NO in PTW, which is crucial in diverse applications, has been troublesome. In this regard, our findings will provide new guidance in utilizing PTW for various applications.

Advanced electrocatalytic redox processes for environmental remediation of halogenated organic water pollutants.

Halogenated organic compounds are widespread, and decades of heavy use have resulted in global bioaccumulation and contamination of the environment, including water sources. Here, we introduce the most common halogenated organic water pollutants, their classification by type of halogen (fluorine, chlorine, or bromine), important policies and regulations, main applications, and environmental and human health risks. Remediation techniques are outlined with particular emphasis on carbon-halogen bond strengths. Aqueous advanced redox processes are discussed, highlighting mechanistic details, including electrochemical oxidations and reductions of the water-oxygen system, and thermodynamic potentials, protonation states, and lifetimes of radicals and reactive oxygen species in aqueous electrolytes at different pH conditions. The state of the art of aqueous advanced redox processes for brominated, chlorinated, and fluorinated organic compounds is presented, along with reported mechanisms for aqueous destruction of select PFAS (per- and polyfluoroalkyl substances). Future research directions for aqueous electrocatalytic destruction of organohalogens are identified, emphasizing the crucial need for developing a quantitative mechanistic understanding of degradation pathways, the improvement of analytical detection methods for organohalogens and transient species during advanced redox processes, and the development of new catalysts and processes that are globally scalable.

Study of the radical polymerization mechanism and its application in the preparation of high-performance PMMA by reactive extrusion.

In this study, the mechanism of radical polymerization was further explored by pre-dissolving different polymers and studying the kinetics of the bulk polymerization of methyl methacrylate (MMA) under shear-free conditions. Based on the analysis of the conversion and absolute molecular weight, it was found that, contrary to the shearing effect, the inert polymer with viscosity was the key factor to preventing the mutual termination of radical active species and reducing the termination rate constant k t. Therefore, pre-dissolving the polymer could increase the polymerization rate and molecular weight of the system simultaneously, making the polymerization system enter the automatic acceleration zone faster and greatly reducing the generation of small molecular weight polymers, leading to a narrower molecular weight distribution. When the system entered the auto-acceleration zone, k t decreased rapidly and greatly and entered the second steady-state polymerization stage. Then, with the increase in the polymerization conversion, the molecular weight gradually increased, while the polymerization rate gradually decreased. In shear-free bulk polymerization systems, k t can be minimized and radical lifetimes maximized, but the polymerization system is at best a long-lived polymerization rather than a living polymerization. On this basis, by using MMA to pre-dissolve ultrahigh molecular weight PMMA and core-shell particles (CSR), the mechanical properties and heat resistance of the PMMA with pre-dissolved polymer obtained by reactive extrusion polymerization were better than for pure PMMA obtained under the same conditions. Compared with pure PMMA, the flexural strength and impact strength of PMMA with pre-dissolved CSR were up to 166.2% and 230.5%. With the same quality of CSR, the same two mechanical properties of the samples obtained by the blending method were just improved by 29.0% and 20.4%. This was closely related to the distribution of CSR in the pre-dissolved PMMA-CSR matrix with a distribution of spherical single particles 200-300 nm in diameter, which enabled PMMA-CSR to exhibit a high degree of transparency. This one-step process for realizing PMMA polymerization and high performance shows extremely high industrial application prospects.