JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Sainan Sun,Guanghua Huang,Jiawei Tang,Fazhi Xie,Xiao Wang,Qiang Guo,Hongshuai Kan,Meng Qiao,Yanpeng Liu,Yi Liu,Zixiao Zhu,Xu Zhao,Ran Mao,Bo Yang
Considering the potential eutrophication risk of phosphonate and scarcity of phosphorus resources, the oxidation of organically-bound phosphorus to orthophosphate (ortho-P) is an important prerequisite for high-value phosphorus recovery. This study investigated efficiency and mechanism of different categories of phosphonates oxidation to ortho-P by classical Fenton and practical electrochlorination Fenton-like processes. The target phosphonates included two categories: nitrogen-free phosphonates (NF-PPs), i.e. 2-phosphonobutane-1,2,4-tricarboxylic acid (PBTC) and 1-Hydroxyethane-1,1-diphosphonic acid (HEDP), and aminophosphonates (A-PPs), i.e. Nitrilotris(methylene phosphonic acid) (NTMP) and diethylenetriamine penta(methylene phosphonic acid) (DTPMP). The results showed that ortho-P conversion for both NF-PPs and A-PPs by classical Fenton process were below 35 %, even though the content of Fe(II) and H 2 O 2 were high enough to neglect the influence of phosphonate-Fe(II) complexation on Fenton reaction initiation. While electrochlorination Fenton-like process greatly enhanced ortho-P conversion of HEDP, NTMP and DTPMP. Potent oxidation relied on generation of HClO, Fe IV O 2+ , and 1 O 2 rather than HO•. In particular, PBTC failed to decompose effectively by electrochlorination Fenton-like process possibly due to chlorine resistance. The non-N-element group was inferred to serve as a decisive role in phosphonates decomposition. This study provided the first systematic description of oxidation rules and mechanism characteristics of diverse phosphonates under classical Fenton and electrochlorination Fenton-like treatment.
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CHEMICAL ENGINEERING JOURNAL
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2012
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IF 3.461
Weizhao Yin,Jinhua Wu,Ping Li,Xiangde Wang,Nengwu Zhu,Pingxiao Wu,Bo Yang
Nitrobenzene (NB) in groundwater has posed significant health risks because of its persistence and high toxicity. In this study, batch experiments were performed to evaluate the effects of initial pH, iron dosage, oxygen and common dissolved anions including Cl − , SO 4 2− , NO 3 − , HCO 3 − , PO 4 3− and humic acid on the NB reduction by zero-valent iron (ZVI). The NB removal increased with the decrease of initial solution pH and a removal efficiency of 88.7% was obtained at an initial pH value of 7.0. The reduction process followed the pseudo-zero-order kinetic model when the iron dosage was 0.5 g L −1 and the corresponding rate constant k 0 was 1.76 mg L −1 h −1 . But it showed a better fit with the pseudo first order kinetics when iron dosage ranged from 1.0 g L −1 to 5.0 g L −1 with the corresponding rate constant k 1 between 0.16 h −1 and 0.76 h −1 . Oxygen inhibited NB reduction due to its competing for electrons from ZVI and the generation of iron oxides. In comparison to the anaerobic system, a 17.1% decrease of NB removal was observed in the air-water system. Improvement of NB removal was observed in the present of Cl − , SO 4 2− and NO 3 − , while bicarbonate would be an inhibitor if its concentration exceeds 50 mg L −1 . The NB reduction was significantly inhibited by PO 4 3− and humic acid since they could form inner-sphere complexes on iron surface. The reaction even ceased as their concentrations reached 8 and 18 mg L −1 , respectively.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Qingshan Zhao,Dejian Xu,Libo Wang,Shihao Cui,Qinlian Liu,Xuan Han,Zhiyuan Wang,Hui Ning,Mingbo Wu
Heteroatom doping provides an effective approach to regulating the catalytic properties of single-atom catalysts for chemical reactions. However, the economical and controllable production of efficient single-atom catalysts with tailored coordination structures presents a formidable challenge. In this study, we demonstrate a novel core-shell confinement strategy to fabricate a single-atom iron catalyst on carbon nanoshells (Fe-N/S-C) for the bifunctional selective reduction of nitroarenes and epoxidation of olefins. Through the encapsulation of polydopamine-coated nano-Fe 2 O 3 within sulfur-rich petroleum asphalt, atomically dispersed Fe-N 3 S 1 with asymmetric coordination were meticulously engineered through one-step thermal treatment, obviating the need for additional sources of iron, nitrogen, or sulfur. Under mild reaction conditions, the Fe-N/S-C catalyst achieved a complete conversion of p-nitrophenol with over 99 % selectivity and a high overall turnover frequency (TOF) of 116.9 h −1 . Meanwhile, the Fe-N/S-C catalyst could also accomplish an 80.2 % conversion in the epoxidation of styrene with a high selectivity of 93.6 %. The remarkable catalytic activities, as well as exceptional stability, notably surpass those of reported single-atom Fe-N-C and noble metal catalysts. Experimental results and theoretical calculations indicate that the negative charge induced by sulfur doping efficiently modulates the electron distribution of the active center and enhances the adsorption/desorption and activation of the reaction substrates, thereby accelerating the catalytic processes involved in selective reduction and oxidation. This work offers a promising approach to the development of cost-effective and potent catalysts for chemical transformations.
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WATER RESEARCH
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2025
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IF 12.4
Han Li,Jinrui Shi,Tao Fu,Jinwei Liu,Xiangtian Peng,Liangjie Wang,Huifang Sun,Yi Xu,Huazhang Zhao
High-temperature wastewaters can themselves activate peroxydisulfate (PDS) to remove aromatic contaminants via polymerization. This, however, may result in an insufficient carbon source for denitrification during biochemical treatment, and the formed polymers, without a proper reuse method, will be costly to handle as hazardous waste. This study demonstrates that the addition of NaOH can suppress the polymerization of aromatic contaminants, which is observed not only in simulated wastewater but also in actual coking wastewater (ACW). Taking phenol as an example, the formation of phenoxy radical (PhO•) through the reaction between SO 4 •- and phenol is the crucial step for phenol polymerization. The addition of NaOH can convert sulfate radicals (SO 4 •– ) to hydroxyl radicals (HO•), and simultaneously, HO• can quickly consume PhO•. Both processes contribute to the inhibition of phenol polymerization. After treatment with heat/NaOH/PDS, the biodegradability of ACW is significantly enhanced with a relatively low carbon source loss (around 16%). Moreover, Fourier transform-ion cyclotron resonance mass spectrometry analysis indicates that the transformation of polyphenols to highly unsaturated and phenolic compounds is beneficial for the biodegradability improvement of ACW. Therefore, the NaOH/PDS system is an effective way to utilize waste heat and enhance the biodegradability of wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Wei Song,Zhaosheng Lei,Hongze Fang,Caixia Fu,Yan Cang,Yuning Fang,Ruigang Wang,Bin Li,Xing Du,Zhihong Wang,Zhiwei Zhao
Sulfate radicals-based advanced oxidation process (SO 4 − -AOPs) exhibits remarkable efficacy for emerging contaminants (ECs) eradication. In this work, we utilized natural Fe II -siderite as a catalyst with dithionite (DTN) and peroxymonosulfate (PMS) precursors to engineer the Fe II -siderite&DTN/PMS system. Carbamazepine (CBZ) elimination efficiency exceeded 90% in 10 min with reactive species of SO 4 − and OH, even in the anaerobic condition due to the sufficient oxidation species source from broken peroxy bond. The system generated various radicals (e.g., SO 4 − , SO 3 − , OH, and SO 5 − ) through redox cycles involving Fe II -siderite, DTN, and PMS, with Fe II /Fe III interconversion driven by PMS oxidation and DTN reduction. Enhanced electron shuttling and Fe II /Fe III interconversion at the phase interface, the rate-limiting step in iron-based AOPs, facilitated PMS activation. CBZ degradation followed four pathways including deacylation, ring-opening oxidation, hydroxylation, decarboxylation, and deketonization, with reactive sites at CBZ-7C and CBZ-8C identified by LC-MS/MS and density functional theory (DFT). Oxygen consumption rate (OCR) toxicity assessments revealed persistent toxicity of intermediates, yet the Fe II -siderite&DTN/PMS system detoxified them effectively based on T.E.S.T. evaluation. And the system demonstrates potential for ECs remediation, particularly in high salinity waters, due to the significant enhancement of higher Cl − concentrations.
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ACS Nano
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2025
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IF 16
Xiao Ge,Xinya Liu,Jinze Xu,Xiyang Zheng,Li-jiao Tian,Xiaozhi Wang
Rational regulation of the coordination environment of single-atom catalysts (SACs) is a promising yet challenging strategy to enhance their activity. Here, we introduce an O atom into the second coordination shell of Co–N4 sites via a simple thermal treatment, forming a Co–N4–ON matrix to boost photosynthetic hydrogen peroxide (H2O2) production. This modification significantly alters the electronic structure of the Co site, bringing the d-band center closer to the Fermi energy and elevating the conduction band of Co–N4–CN to enhance its reducing capacity. Density functional theory (DFT) calculations reveal intensified charge redistribution and a reduced work function in Co–N4–ON, facilitating O2 adsorption. Notably, Co–N4–ON exhibits the lowest O2 adsorption energy, indicating a stronger interaction between Co–N4–O and O2, which is further strengthened by orbital hybridization and charge transfer at their interface, leading to enhanced O2 activation. The optimized Co–N4–ON catalyst demonstrates superior O2 reduction capabilities with the lowest energy barrier during H2O2 desorption. Consequently, it achieves a H2O2 production rate of 3098.18 μmol g–1 h–1 under neutral conditions, which is 2.6 times higher than that of Co–N4–CN. Moreover, it maintains a production rate of 1967.79 μmol g–1 h–1 over 10 h in a continuous flow reactor under natural sunlight and ambient air, highlighting its durability and practicality. This study underscores the crucial role of the second coordination shell in SACs and offers valuable insights into their atomic-level structure–activity relationships, thus contributing to advancements in catalyst design for efficient photosynthetic H2O2 production.
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Journal of Water Process Engineering
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2025
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IF 6.7
Chen-Yan Hu,Li-Li Hu,Tian-Yang Zhang,Xin-Yu Yang,Hao Liu,Jia-Nan Chen,Ling-Mei Gao,Zheng-Yu Dong
Emerging contaminants (ECs) have received widespread attention. In this study, the Far-UVC (222 nm) combined with chlorine (UV 222 /chlorine) system is used to remove ECs from water. The results reveal that carbamazepine (CBZ) was effectively degraded by the UV 222 /chlorine system, with a degradation efficiency of 92.5 % within 45 min at a UV fluence of 666 mJ cm −2 and a chlorine concentration of 200 μM. Quenching experiments indicate that HO• and Cl• play a major role in the UV 222 /chlorine system. The steady-state concentrations of HO• (3.85 × 10 −14 M), Cl• (8.55 × 10 −14 M), and ClO• (9.13 × 10 −12 M) in the UV 222 /chlorine system is determined by using probe method. The degradation of CBZ by UV 222 /chlorine system (92.5 %) is significantly better than that of UV 222 alone (32.3 %) and the UV 254 /chlorine system (78.3 %) at the same UV dose. In addition, the UV 222 /chlorine system exhibits excellent EE/O performance of 0.53 KWh/L, effectively reducing resource consumption. Compared with the UV 222 /peracetic acid (PAA) system, the UV 222 /chlorine system shows higher degradation efficiency for CBZ in a wide pH range of 4 to 9. In addition, the presence of Cl − and HCO 3 − shows no significant impact on both the UV 222 /chlorine and UV 222 /PAA systems. The UV 222 /chlorine system is expected to become a promising alternative to traditional UV and chlorine disinfection techniques in water treatment . This study provides technical support for promoting the practical application of the UV 222 /chlorine system.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2025
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IF 4.6
Xiulian Yin,Yingjin Li,Mingjie Wei,Yanni Ji,Qinghua Cao,Xiangfen Xue
Spectral retrieval method plays a crucial role in spectral analysis technology. Nevertheless, research in this area has not received the requisite advancement for fluorescence excitation-emission matrix (EEM) spectroscopy, which has been widely used in environmental monitoring and other fields. In this work, we developed a spectral retrieval method, the contour line-based image pattern recognition (CLIPR) technique, to interpret the EEM spectrum. A three-level retrieval mechanism, including the primary feature Lib1, qualitation Lib2 and quantitation Lib3 has been set up. Optimization efforts have been conducted on the accuracy and efficiency of noise removing, feature extraction and image retrieval methods. To demonstrate the technique, four model pollutants with very similar chemical structures and a metal-organic framework (MOF), MOF-74 (Zn), as a fluorescence probe providing more dimensional information were used. A total of 28 × 4 EEM map images were modeled and validated using the leave-one-out cross-validation method. Two batches with 5 × 4 samples each as unknown samples were selected to evaluate the performance of the CLIPR method. When taking the weight value set with 0.8, 0.1 and 0.1, for the validation sets with the concentration greater than 50 μM, the intra class similarity is above 79.61 % and the accuracy reached 98.81 % (83/84). The best quantitative result is PhNH 2 -S1, with the RMSE/True value 3.09 % and R 2 0.99. For the unknown sets, when Batch 1 greater than 35 μM and Batch 2 greater than 50 μM, the recognition accuracy reaches 100 %. The research results indicate that the model has a certain degree of stability and generalization and it is feasible to apply spectral retrieval method to interpret EEM information. We have taken a step forward in laying the foundation for large-scale reference data preparation in this field.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Hao Du,Bo Shen,Rubin Huo,Yuxin Hui,Chao Chen,Aoxiang Liu,Zhe Zhang,Chunjuan Li,Bingjie Ni,Derek Hao,Qi Wang
In this work, we synthesized perylene-3,4,9,10-tetracarboximide/WO 3 (PDINH/WO 3 ) with strong hetero-interfacial interactions (SHIs) to enhance the three-electron oxygen reduction reaction (3e - ORR) for hydroxyl radicals (•OH) generation toward micropollutants degradation and antibacterial applications. Experimental and density functional theory (DFT) computational results revealed that WO 3 facilitates the 2e - oxygen reduction pathway for H 2 O 2 production, while the organic PDINH component strengthens the adsorption of *H 2 O 2 intermediates, promoting their subsequent 1e - reduction to •OH. The optimized system enabled exceptional •OH production, with excellent tetracycline degradation and robust antibacterial activity, alongside 120 h stability with < 5 % activity loss in continuous-flow wastewater treatment, even under high-salinity, extreme pH, and natural organic matter interference. This work establishes SHIs as a universal design principle for steering 3e - ORR pathways. The findings offer transformative opportunities for energy-efficient environmental remediation, demonstrating exceptional resilience in complex real-world wastewater systems.
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Cell Reports Physical Science
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2025
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IF 7.3
Jingyi Xiong,Jiawei Zhang,Xufan Zheng,Tianyu Hu,Huimin Xiang,Yuda Li,Biao Xiao,Xunchang Wang,Renqiang Yang
Summary Fluorescence sensing technology has been extensively used in the field of explosives monitoring for highly sensitive trace detection and early warning systems. However, these advancements have been hindered by a significant reliance on professional technicians and a low degree of automation. Here, we present a cloud-based website that encapsulates a deep-learning-assisted technique based on the PaddlePaddle You Only Look Once (PPYOLO) model and integrates a highly sensitive external fluorescence sensor. This approach, combined with a deep learning model, streamlines the detection of nitro explosives, enhancing automation levels and efficiency. The cloud-based interface and self-developed portable sampling software offer a user-friendly, interactive, and portable system. Moreover, the model boasts a target recognition accuracy (bounding box mean average precision [bbox_map]) of up to 99%, making it capable of automatically extracting six independent color signals from images and providing detection results. These results suggest that the proposed method could provide promising perspectives for the future development of efficient and portable explosives detection systems.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Ting Zhou,Wenyi Dong,Xuechuan Li,Weigang Liu,Mengke Qiang,Hongjie Wang
High-valent ferric oxide species (HV-Fe(IV)) has been increasingly explored to selectively and efficiently remove pollutants from wastewater owing to its high reduction potential, long lifetime, and valuable resistance to anions. However, the directional production of HV-Fe(IV) and its mechanism remain challenging. Herein, a biochar-based catalyst with monoatomic Fe-trans-N 2 O 2 configuration and rich COOH group (SAFe-NKBC) was rationally constructed via KOH and supramolecular organic framework co-pyrolysis. As a result, the SAFe-NKBC/PMS system exhibited exceptional catalytic performance, achieving rapid sulfamethoxazole degradation (97.4% within 10 min) and TOC removal (73.1%). Mechanistic investigations revealed the cooperative catalytic role of single-atom Fe-trans-N 2 O 2 and COOH in biochar support via surface-confinement effect in boosting peroxymonosulfate activation and directional HV-Fe(IV) generation, mediating spatially coupled electron transfer and promoting selective oxidation pathways. Furthermore, a structure–activity relationship for various para-substituted anilines was systematically established via quantitative structure–activity relationship modeling based on different adsorption and oxidation descriptors. The valid descriptors were confirmed to predict reactivity, offering a molecular-level framework for water purification. Meanwhile, the catalyst demonstrated excellent resistance to matrix interference, long-term stability in flow-through systems, and significantly reduced toxicity of degradation byproducts, underscoring its potential in sustainable and precision-oriented water remediation. This work offered new insights into rational SAC design and reactivity prediction for sustainable water remediation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Shizong Wang,Jianlong Wang,Bo Lai
This study investigated the role of support-driven coordination environments in regulating peroxymonosulfate (PMS) activation by single-atom cobalt catalysts. Atomically dispersed cobalt was anchored on graphene oxide (Co/GO) and silica (Co/SiO 2 ) to compare their catalytic pathways and stability. Both catalysts enabled efficient degradation of sulfamethoxazole (SMX), achieving mineralization efficiencies of 36.4 % for Co/GO and 42.7 % for Co/SiO 2 after 60 min. Co/SiO 2 also showed superior structural stability and reduced cobalt leaching during reaction. Mechanistic studies revealed that Co/GO favored the direct formation of Co(IV)=O species, whereas Co/SiO 2 promoted surface-bound radicals, which is attributed to its higher cobalt coordination number and stronger metal-support interactions. Furthermore, both catalysts were incorporated into polyvinylidene fluoride membranes, which maintained high SMX removal efficiency during 7 days of continuous operation with real municipal wastewater. These findings underscore the crucial role of support effects in tailoring PMS activation and offer insights for designing stable single-atom catalysts for water treatment.
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