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REACTIVE & FUNCTIONAL POLYMERS · 2025 · IF 5.1

Effects of flame-retardant nanocomposite combined with warm mix asphalt techniques on molecular conversion and fire safety

Lu He,Qing-Qing Bi,Yue Ma,De-Yi Wang

The combination of flame retardant with warm mix asphalt (WMA) technology in asphalt pavements has become an important strategy for improving safety, conserving energy, and safeguarding the environment, especially in tunnel applications. This study explored the incorporation of flame-retardant nanocomposite and three distinct types of WMA additives into asphalt to investigate the mechanisms underlying the modification process and fire safety. Additionally, warm-mix asphalt samples without flame retardant were analyzed as control specimens for comparative analysis. The WMA additives notably enhanced the dispersion of flame-retardant nanocomposite and facilitated the conversion of medium and large molecules within the asphalt matrix. The combination of the organic WMA additive and flame-retardant nanocomposite provided superior flame retardancy and smoke suppression properties compared to asphalt that contained only flame retardant. The peak heat release rate and peak smoke production rate were significantly reduced by 45.5 % and 45.7 %, respectively. The detailed analysis indicated that the flame-retardant mechanism primarily resulted from the char layers reinforced by the continuous crystal grid structures in the asphalt, alongside the inert gases released by the flame-retardant nanocomposite. These results underscore the potential and significance of flame-retardant warm-mix asphalt for engineering applications.

CAS / MDL: 102-54-5
研究领域: 土木工程 · 材料科学 · 消防安全
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WATER RESEARCH · 2021 · IF 11.236

Unravelling molecular transformation of dissolved effluent organic matter in UV/H2O2, UV/persulfate, and UV/chlorine processes based on FT-ICR-MS analysis

Bingliang Zhang,Xuening Wang,Zhuoyao Fang,Shu Wang,Chao Shan,Si Wei,Bingcai Pan

ABSTRACT Ultraviolet-based advanced oxidation processes (UV-AOPs) are very promising in advanced treatment of municipal secondary effluents. However, the transformation of dissolved effluent organic matter (dEfOM) in advanced treatment of real wastewater, particularly at molecular level, remains unclear. In this study, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) coupled with multiple statistical analysis were performed to better understand the transformation of dEfOM in UV/H 2 O 2 , UV/persulfate (UV/PS), and UV/chlorine treatments. An obvious increase in oxygen content of dEfOM was observed after every UV-AOPs treatment, and the detailed oxygenation processes were further uncovered by mass difference analysis based on 24 types of typical reactions. Generally, UV/H 2 O 2 process was subjected to the most oxygenation reactions with the typical tri-hydroxylation one (+3O), whereas di-hydroxylation reaction (+H 2 O 2 ) was dominant in UV/PS and UV/chlorine processes. Additionally, the three UV-AOPs shared the majority of precursors, and more proportions of unique products were identified for each process. The precursors with lower H/C and higher aromaticity were readily degraded by UV/chlorine over UV/H 2 O 2 and UV/PS, with the products featuring lower molecular weight. Moreover, dEfOM of high aromaticity tended to produce chlorinated byproducts through addition reactions in chlorination and UV/chlorine processes. Among these UV-AOPs, the highest reduction of both acute toxicity and specific UV absorbance at 254 nm (SUVA 254 ) was observed for UV/chlorine, implying the potential for UV/chlorine process in advanced treatment of wastewater. In addition, acute toxicity was highly correlated with SUVA 254 and CHOS compounds. This study is believed to help better understand the different fates of dEfOM in real wastewater during UV-AOPs treatment.

研究领域: 环境科学 · 废水处理
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FUEL · 2025 · IF 7.5

Molecular conversion of polypropylene pyrolysis revealed by Ag+ complexation ESI Orbitrap MS

Yan Zhang,Yaqi Wang,Zhengyu Chen,Quan Shi,Linzhou Zhang

Pyrolysis has emerged as a key approach for converting plastic waste into valuable resources. However, this process is an extremely complex reaction system, and the molecular conversion behavior and pathways have not been fully understood. This study systematically investigated the thermal pyrolysis of polypropylene (PP) over a temperature range of 420–500 °C, and the composition of PP pyrolysis oils was analyzed using Ag + complexation electrospray ionization high-resolution Orbitrap mass spectrometry. The results indicate that the pyrolysis oils are primarily composed of mono-olefins and diolefins at lower temperature and pressure, with a three-carbon repeating unit. Secondary reactions intensified at elevated temperatures and pressure, progressively converting heavy olefins to polycyclic aromatics. The results of mass spectrometry analysis were compared with gas chromatography showing significant advantages, and were in good agreement with the molecular structure information provided by nuclear magnetic resonance hydrogen spectroscopy and Fourier transform infrared spectroscopy. Furthermore, the PP pyrolysis pathways at varying temperatures were proposed showing the full pathway of cracking and aromatization.

研究领域: 环境科学 · 化学工程 · 分析化学
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Journal of Materials Chemistry A · 2025 · IF 9.5

A design strategy of high-activity swarm mobile nanocatalysts for hydrogenolysis of complex N-benzyl compounds via anchoring–confinement synergy

Junjie Wang,Yuanyuan Ma,Jianwei Song,Chuanyou Xiao,He Huang,Chenghui Sun,Siping Pang

Ultrasmall metal nanoparticles are used as active sites in numerous heterogeneous catalysts. However, the metal sites in these catalysts are typically considered to be static, which limits the transformation of complex organic molecules with special multidimensional spatial structures that are distant from these sites. This study proposes and verifies a swarm mobile catalyst design strategy based on the synergistic induction of the “anchoring–confinement effect”. Enhanced catalytic efficiency is achieved by increasing the collision frequency between active sites and reactants. Specifically, the ultrasmall Pd(OH)2 nanoparticles (approximately 1.85 nm), formed under the synergistic effect, are rapidly transformed into mobile Pd species that participate in the reaction. The special support with hierarchical macro–meso–micropores effectively enhances the mass transfer process. The catalyst demonstrates the highest activity in the hydrogenation debenzylation of hexabenzylhexaazaisowurtzitane (HBIW), achieving a high turnover number (TON) of 161.4 and a product yield of 91.4%, with the amount of Pd used in the catalyst being only 0.85 wt‰ of HBIW at near-room temperature. The successful implementation of this strategy offers a new concept for the design and synthesis of efficient heterogeneous catalysts.

研究领域: 催化化学 · 纳米材料科学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2021 · IF 7.963

Effect of bromide on molecular transformation of dissolved effluent organic matter during ozonation, UV/H2O2, UV/persulfate, and UV/chlorine treatments

Bingliang Zhang,Zhuoyao Fang,Shu Wang,Xifeng Shi,Bo Guo,Jie Gao,Dandan Wang,Wansong Zong

Ozonation and ultraviolet-based advanced oxidation processes (UV-AOPs) play important roles in advanced treatment of municipal wastewater for water reuse . Bromide is widely present in wastewater at different concentration levels (ranging from μg/L to mg/L). However, the effect of bromide on molecular transformation of dissolved effluent organic matter (dEfOM) in real wastewater during ozonation and UV-AOPs treatments still remains unclear. Herein, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) was utilized to characterize the overall molecular transformation of dEfOM and the formation of unknown halogenated byproducts (X-BPs) in ozonation, UV/H 2 O 2 , UV/persulfate (UV/PS), and UV/chlorine (UV/Cl) processes in the presence of additional bromide. Compared with the same oxidation processes without additional bromide, the degree of dEfOM oxygenation had some extent decrement with the effect of bromide. A slightly increment of the number of unknown brominated byproducts (Br-BPs) was observed during ozonation, UV/H 2 O 2 , and UV/PS treatments in the presence of additional bromide, and the largest increment of these compounds was found in UV/Cl process. A total of 82 chlorinated byproducts (Cl-BPs) and 183 Br-BPs were detected in all oxidation processes with the effect of bromide, and the number of Br-BPs was significantly higher than that of Cl-BPs. Based on mass difference analysis, 69 pairs of possible precursors/Br-BPs were identified. In addition, the additional bromide did not remarkably increase the concentrations of trihalomethanes (THMs) and haloacetic acids (HAAs) in ozonation, UV/H 2 O 2 , and UV/PS treatments, while the production of THMs and HAAs significantly decreased by 68.06% and 54.55%, respectively, during UV/Cl treatment. The calculated cytotoxicity increased to some extent for each treatment, especially for UV/Cl treatment, and the compound with largest contribution to cytotoxicity was monobromoacetic acid. This study provides new insights into the formation and transformation of X-BPs during advanced treatment of real wastewater with the effect of bromide.

研究领域: 环境科学 · 分析化学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Application of CaO2-enhanced peroxone process to adjust waste activated sludge characteristics for dewaterability amelioration: Molecular transformation of dissolved organic matters and realized mechanism of deep-dewatering

Dongdong Ge,Weixiang Wu,Guangming Li,Yuhui Wang,Guobiao Li,Yanting Dong,Haiping Yuan,Nanwen Zhu

Sludge dewaterability is commonly poor due to the hydrophilic biopolymeric substances. The highly efficient oxidation process is of great significance for extracellular biopolymers disintegration and bound water discharge. This work investigated the novel CaO 2 -enhanced peroxone (CaO 2 /O 3 ) process to adjust sludge characteristics for dewaterability enhancement and focused on the molecular composition and transformation of dissolved organic matters (DOM). CaO 2 /O 3 (60/40 mg/gTS (total solid)) treatment showed more powerful sludge solubilization of 57.8% and cell death proportion of 46.1% over single CaO 2 or O 3 treatment. Hydrophilic extracellular polymeric substances, especially protein-like substances, were substantially degraded, and their conformation turned to be more hydrophobic, and carbohydrate-like, aminosugars-like, and lignins-like substances increased in CaO 2 /O 3 process. Meanwhile, CaO 2 /O 3 handling resulted in more decomposition of CHO-containing compounds than N-containing or S-containing compounds. Subsequently, 60 mg/gTS PFS (polyferric sulfate) reflocculation exerted a strengthened role in eliminating proteins & lipids-like, lignins-like, and unsaturated hydrocarbons-like substances, and especially S-containing compounds, which compensated for the unsatisfactory removal effects of these substances in the CaO 2 /O 3 oxidation process. Therefore, the CaO 2 /O 3 -PFS treated sludge with less hydrated DOM easily harvested deep-dewatering in pressure filtration. Furthermore, it was noteworthy that the presence of CaO 2 created an alkaline environment and served as the source of sustained-release H 2 O 2 , which accelerated O 3 decomposition and greatly improved • OH generation. These findings provided molecular insight into a novel sludge conditioning approach for ideal dewaterability based on the CaO 2 -enhanced peroxone process in sludge treatment.

研究领域: 环境工程 · 污水处理 · 化学工程
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Journal of Water Process Engineering · 2025 · IF 6.7

Transformation of dissolved organic matter at molecular level during UV222/chlorine process

Chen-Yan Hu,Jia-Nan Chen,Ling-Mei Gao,Xiao-Cong Ma,Ming Zheng,Xi-Wei Yang,Jia-Qi Yang,Tian-Hong Qiu,Hai-Qing Ding,Zheng-Yu Dong

The krypton chloride (KrCl*) excimer lamp (222 nm) has become a novel light source used in UV-based advanced oxidation processes (UV-AOPs). Recently, a large number of studies have explored the application of UV 222 /chlorine process in water treatment. However, the transformation patterns of widely present dissolved organic matter (DOM) in water in this process is still unknown, especially at the molecular level. This study investigated the removal, component changes, and potential mechanisms of DOM during UV 222 /chlorine process, with humic acid as a typical DOM. The results showed that the removal efficiency of DOC and UV 254 by UV 222 /chlorine process can reach up to 56.0 % and 69.8 %, significantly higher than that of UV 222 alone and chlorine alone. Electron paramagnetic resonance (EPR) experiments have confirmed that HO•, Cl• and 1 O 2 are the main active species in the reaction. The formation of disinfection by-products (DBPs) was detected. Compared to the UV 254 /chlorine process, the UV 222 /chlorine process can significantly reduce the formation of DBPs, mainly due to the higher removal rate of DBPs precursors. The molecular changes of DOM were analyzed using FT-ICR MS method. The active species generated in the system can cause multi-pathway transformation of phenolic compounds, while the conversion of aliphatic substances can undergo dealkylation reactions. This study provides valuable insights into the molecular transformation of DOM in the Far-UVC/chlorine process, which will help promote the application of Far-UV technology in water treatment.

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WATER RESEARCH · 2025 · IF 12.4

Far-UVC photolysis of chlorine to mitigate ultrafiltration membrane fouling: Unraveling the molecular transformation mechanism of natural organic matter

Xiaoxiang Cheng,Yaoyao Feng,Peijie Li,Kunyu Chen,Tao Yang,Yan Jin,Xinsheng Luo,Daoji Wu

Fouling of ultrafiltration (UF) membranes by natural organic matter (NOM) remains a persistent challenge. Herein, far-ultraviolet (Far-UVC) photolysis of chlorine was developed as a pretreatment to solve the membrane fouling problem arising from NOM. The findings demonstrated that Far-UVC/NaClO pretreatment efficiently increased membrane flux while reducing reversible and irreversible fouling resistance by 80.0 % and 47.1 %, individually. Specifically, Cl • , ClO • and HO • were identified by quenching and probing experiments to play key roles in NOM degradation. Interfacial free energy analysis revealed that Far-UVC/NaClO pretreatment markedly enhanced the repulsive force between contaminant and membrane, thus reducing the tendency of membrane pore clogging. Through molecular-level reaction analysis, unsaturated and aromatic compound macromolecules were decomposed into small molecules, thus reducing membrane pore clogging. Mass difference analysis further revealed the degradation pathways of NOM, which mainly included decarboxylation, dealkylation, and oxygen addition reactions. Moreover, chlorine disinfection by-products (Cl-DBPs) such as trichloroacetic acid, dichloroacetic acid, chloral hydrate and trichloromethane were detected following post-chlorination. Subsequent UF process effectively reduced the formation of DBPs by 19.3–34.3 %. This study demonstrates the application potential of Far-UVC-based oxidation technology to mitigate membrane fouling resulting from NOM.

研究领域: 环境工程 · 水处理技术 · 膜分离科学 · 氧化过程 · 天然有机物化学 · 自由基反应机理 · 消毒副产物控制
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Journal of Environmental Sciences · 2024 · IF 5.9

Coupled transformations of manganese and dissolved organic matter molecules during iron (oxyhydr)oxide-catalyzed oxidation of Mn(II)

Xixian Huang,Bing Yang,Ye Dou,Yang Ding

The abiotic oxidation of divalent manganese (Mn(II)) and the formation of Mn oxides are important geochemical processes, which control the mobility and availability of Mn as well as element cycling and pollutant behavior in soils. It was found that iron (oxyhydr)oxides can catalyze Mn(II) oxidation , but the effects of the coexisting dissolved organic matter (DOM) molecules on the catalysis of different iron (oxyhydr)oxides for Mn(II) oxidation are poorly understood. Herein, we investigated Mn(II) oxidation under the impacts of the interactions between iron (oxyhydr)oxides (i.e., ferrihydrite, goethite and hematite) and DOM molecules. Simultaneously, we elucidated the variations of DOM composition and properties. Our results indicated that the catalysis of iron (oxyhydr)oxides for Mn(II) oxidation was significantly inhibited by DOM. Moreover, DOM had less inhibiting effect on the catalysis of ferrihydrite for Mn(II) oxidation and the formation of Mn oxides (e.g., hausmannite and buserite) relative to goethite and hematite, which was partially because of the higher electron transfer capacities of ferrihydrite. Meanwhile, DOM molecules with high nominal oxidation state of carbon (NOSC), molecular weight, unsaturation and aromaticity were selectively adsorbed and oxidized by Mn oxides , including the oxygenated phenols and polyphenols. The newly formed molecules mainly belonged to phenols depleted of oxygen and aliphatics. Furthermore, NOSC was a key molecular characteristic for controlling DOM composition during DOM adsorption and oxidation by Mn oxides when iron minerals were present. Overall, our research contributes to understanding Mn(II) oxidation mechanisms under heterogeneous systems and behaviors of DOM molecules in the environment.

研究领域: 环境地球化学 · 土壤化学 · 水文地球化学 · 有机-矿物相互作用 · 元素生物地球化学循环
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ACS Applied Nano Materials · 2023 · IF 5.9

Ultrasmall Zeolite Subcrystal Catalyst Devoid of Intracrystalline Diffusion Limitation for Bulk Molecule Conversion

Ke Du,Zhizheng Sheng,He Li,Lou Gao,Tianlan Yan,Jiayu Yu,Di Pan,Zhichao Tan,Songhai Xie,Jing Ju,Yahong Zhang,Yi Tang

Constructing zeolite catalysts with excellent mass transfer and active site accessibility is the key to improving their catalytic efficiencies. Herein, a zeolite subcrystal catalyst with high short-range ordering but X-ray amorphism is prepared to minimize the existing molecular mass-transfer barrier of conventional zeolite catalysts. Various characterizations confirm its size of smaller than 10 nm, definite MFI framework, complete opened micropore channel, and abundant accessible acid sites. Moreover, physical and chemisorption results reveal that the high short-range ordering MFI zeolite subcrystal possesses negligible intracrystalline diffuse limitation and utmost accessibility for the active site. As anticipated, the zeolite subcrystal catalyst not only demonstrates high cracking efficiency in polyolefin cracking reactions but also exhibits outstanding catalytic activity and resistance to carbon deposition in macromolecular furfuryl alcohol etherification reaction. The controlled MFI zeolite subcrystal catalyst synthesis strategy is expected to extend to a variety of microporous materials.

研究领域: 化学工程 · 催化 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Unravelling molecular transformation of dissolved organic matter in UV/Dichloroisocyanurate, UV/Chlorine, and UV/Chloramine processes using high Resolution mass spectrometry

Quanfa Zhong,Wangbao Gong,Guangjun Wang,Jun Xie,Jianshu Zhao,Qinghai Jin,Xiaoming Ma,Zhangxin Wang,Di He

This study utilized Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) to investigate the molecular-level transformation of dissolved organic matter (DOM) during treatment with the novel UV/dichloroisocyanurate (NaDCC) process. Comparisons were made with conventional UV/hypochlorite (NaClO) and UV/monochloramine (NH 2 Cl) processes to assess the feasibility and environmental risks of UV/NaDCC. Results showed that UV/NaDCC and UV/NaClO had comparable and stronger DOM mineralization effects than UV/NH 2 Cl. Notably, UV/NaDCC treatment more effectively reduced DOM aromaticity, fluorescence, and apparent molecular weight, producing more oxidized and saturated molecules. Kendrick mass defect (KMD) analysis indicated that demethylation and carboxylation reactions played key roles in UV/NaDCC treatment, supported by a greater number of precursor-product pairs. The UV/NaDCC system produced substantial chlorinated and N-containing byproducts (Cl-BPs and N-BPs). Among the Cl-BPs, species formed via + 2Cl reaction ( e. g. , +H 2 Cl 2 O 2 , +Cl 2 O) were dominant, similar to the UV/NaClO system. The N-BPs with higher nitrogen content ( e. g. , N3 and N4) were more abundant than in UV/NH 2 Cl. The UV/NaDCC system produced the highest concentrations of TCM and DCAN, whereas the UV/NaClO system yielded the highest concentration of DCAA. Toxicity tests revealed that UV/NaDCC effluent displayed the highest toxicity. To the best of our knowledge, this study provides the first molecular-level insight into DOM transformation in UV/NaDCC treatment, offering theoretical and practical guidance for its application.

研究领域: 环境化学 · 水处理技术 · 质谱分析 · 有机物分析 · 副产物生成 · 毒理学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Unveiling molecular transformations and mechanisms of soil organic matter during thermal remediation across temperatures

Han Gao,Shang Gao,Lei Wang,Zhen Song,Xiaolei Qu,Minli Wang,Tao Long,Jinzhong Wan

Thermal treatment is a commonly applied soil remediation technique that can also change the properties of soil. However, few studies looked into the transformation and mechanism of soil organic matter (SOM) at the molecular level when contaminated soil undergoes thermal remediation. Herein, FT-ICR MS, pyrolysis gas chromatography mass spectrometry (Py-GC–MS), and size exclusion chromatography-diode array detector-fluorescence detector-organic carbon detector (SEC-DAD-FLD-OCD) were used to unveil the molecular transformation mechanism of SOM under 100 °C and 400 °C treatments. The macromolecules transformed to humic and fulvic components after 400 °C treatment, while few transformations occurred after 100 °C treatment. The molecules decreased with the increase in temperature. After 400 °C treatment, over 99 % of the molecules were newly produced, which were mainly aromatic (66 %) and lignin-like (19 %) components. After 100 °C treatment, most of the molecules (73.6 %) were reserved. The unsaturation and aromatic structures of SOM increased significantly after the 400 °C treatment, while the changes were relatively minor after the 100 °C treatment. The fracture of the carbon skeleton, cyclization, and H abstraction reactions were the main mechanisms for the molecular transformation of SOM during 400 °C treatment, while volatilization was the main transformation scheme during 100 °C. Statistical results of pyrolysates show the increase of aromatic components, and the molecular markers reflected the increase of condensed organic carbon and the decrease of phenols, alkene components during 400 °C treatment. The sorption of PAHs for soil decreased after treatment, owing to the loss and transformation of SOM. This study advances the mechanistic understanding of transformation in SOM molecular signatures during thermal treatment.

CAS / MDL: 129-00-0 91-20-3 85-01-8
研究领域: 环境科学 · 土壤化学 · 分析化学 · 有机地球化学
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