APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Shihu Cao,Shugang Zheng,Tianci Liu,Jinhao Liu,Yaqi Yin,Dan Feng,Yunqing Liu,Dayi Qian,Jiangwei Shang,Xiuwen Cheng
Herein, we identified interfacial oxygen vacancy-metal (O V -Ni) dual-sites within a NiFe 2 O 4 /Ni@NC composite as the definitive structural origin for dictating the selective evolution of singlet oxygen ( 1 O 2 ) from peroxymonosulfate (PMS) activation. The catalyst was fabricated via in-situ pyrolysis of a Ni-MOF on NiFe 2 O 4 nanoparticles, and its mechanism was elucidated through a combination of in-situ spectroscopy, kinetic analysis, and density functional theory (DFT) calculations. This 1 O 2 -driven catalysis achieved an 11-fold enhancement in the levofloxacin degradation rate, with the interfacial synergy lowering the non-radical pathway’s energy barrier by 0.037 eV. We conclude that these engineered dual-sites deterministically control reaction selectivity, as proven by the first experimental trapping of a surface-bound 1 O 2 precursor. This work establishes a design blueprint for advanced non-radical catalysts by transforming the approach from serendipitous discovery to predictable, interface-driven design.
研究领域:
环境催化
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材料化学
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物理化学
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纳米催化
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水处理技术
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Huan Chen,Yan Zhao,Zhe Zhang,Bo Niu,Yayun Zhang,Donghui Long
In this work, a cobalt phthalocyanine catalyst with axial pyridine coordination anchored on carbon nanotubes (CoPc-Py-CNT) was developed for enhanced peroxymonosulfate (PMS) activation toward singlet oxygen ( 1 O 2 ) evolution. Axial pyridine coordination induces Co 3 d -N 2 p rehybridization, elevating the Co d z 2 orbital energy level to strengthens d-p orbital hybridization with the oxygen atom in PMS, thereby lowering the activation energy barrier for O-O bond cleavage. The CoPc-Py-CNT/PMS system exhibits an 8.3-fold increase in ciprofloxacin degradation rate and nearly quantitative selectivity in aromatic alcohol oxidation to corresponding aldehydes compared to axially unmodified CoPc-CNT. CoPc-Py-CNT maintains excellent performance in both continuous-flow and 50 L pilot-scale water treatment systems, with minimal cobalt leaching (<20 μg L −1 ) and negligible ecotoxicity. This work proposes a tailored symmetry-breaking strategy via axial coordination to modulate the electronic structure of SACs, offering a robust platform for 1 O 2 -mediated water remediation and selective oxidation reactions in green chemistry applications.
研究领域:
环境化学
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催化
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材料科学
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水处理
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绿色化学
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配位化学
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DOI
高影响因子
DYES AND PIGMENTS
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2019
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IF 4.018
Jinjin Guo,Xiaoyu Wang,Shuxian Zhu,Lu Liu,Xiaofeng Jiang,Dongdong Ban,Lidong Li
We combined the unique natural oxygen transporting function of red blood cells (RBCs) with photosensitive nanocomposites to create biomaterials with strong singlet oxygen ( 1 O 2 ) generation. During cold storage for a long time, structural changes to RBCs may occur, which reduce their oxygen carrying capacity. The nanocomposite developed herein featured dual emission characteristic, which enabled evaluation of the status of the RBCs. On the basis of energy transfer from the conjugated polymer to iridium(III) complexes, the formed nanocomposites show intense, long-lived and oxygen-sensitive emission. When modified with 1,2-distearoyl- sn -glycero-3-phosphoethanolamine- N -[methoxy(polyethyleneglycol)-2000], the nanocomposites non-invasively entered RBCs through hydrophobic interactions . We measured the quenching effect of oxygen on the emission of the iridium(III) complexes. The differential fluorescent signals and fluorescence lifetime images indicated the storage history of the RBCs. RBCs in good condition stored oxygen. When engineered with nanocomposites, RBCs generated large amounts of cytotoxic 1 O 2 upon irradiation. These decorated RBCs might serve as a new kind of photosensitive biomaterial.
研究领域:
生物材料学
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医学工程
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光动力治疗
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DOI
高影响因子
BIOCONJUGATE CHEMISTRY
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2018
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IF 4.485
Zheng Ruan,Wei Miao,Pan Yuan,Liu Le,Lijuan Jiao,Erhong Hao,Lifeng Yan
NIR photosensitizer is attractive for photodynamic therapy (PDT). Low-power light irradiation and imaging-guided PDT makes it possible to increase tissue penetration depth. The pyrrole-substituted iodinated BODIPY (BDPI) molecule was designed and synthesized, and it possesses an intense NIR absorption and emission band, and exhibits a high singlet oxygen quantum yield (ΦΔ = 0.80) which leads remarkable cytotoxicity upon low power illumination (IC50 = 0.60 μg/mL, 6.1 mW/cm2). After being encapsulated with biocompatibility polypeptide PEG–PLys, polymeric micelles nanoparticles (PBDPI NPs) was obtained that are water-dispersed and passively tumor-targetable. Such enhanced accumulation in tumor area makes it easily traced in vivo due to its NIR fluorescence. In addition, such nanoparticles offer an unprecedented photodynamic therapeutic effect by using a low-power irradiation light, which makes it possible to kill cancer cells in deep tissue efficiently.
研究领域:
生物医学工程
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肿瘤学
·
材料科学
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DOI
高影响因子
MOLECULES
·
2026
·Vol. 31
·期 17
·2946
·
IF 5.1
Jie Teng,Yuzhen Zhang,Xiangbo Ma,Wencheng Zhu,Pu Li,Mingguo Peng
17β-Estradiol (E2), a highly bioactive steroid estrogen, poses potential ecological risks even at trace concentrations in aquatic environments. In this study, a nanoconfined Co-based catalyst (Co@Cin) was employed to activate peracetic acid (PAA) for efficient E2 degradation. Microscopic and spectroscopic characterizations indicated that Co-containing species were highly dispersed within the CNT-based architecture, while the graphitic tubular framework was largely preserved. Compared with PAA alone, CNTs, Co@Cinalone, and the externally loaded Co@Cout/PAA system, Co@Cin/PAA exhibited substantially faster E2 degradation. Pseudo-first-order kinetic analysis further demonstrated the enhanced degradation kinetics of the internally confined system. Importantly, ICP analysis showed comparable Co loadings for Co@Cinand Co@Cout, while Co@Cinretained a markedly higher Co-normalized apparent kinetic activity, indicating that its enhanced performance cannot be explained simply by differences in total Co loading. Moreover, Co@Cinexhibited substantially lower Co leaching than Co@Coutand maintained considerable catalytic activity over five consecutive cycles, demonstrating improved stability of the confined Co species. The degradation performance was influenced by initial E2 concentration, catalyst dosage, PAA concentration, and pH, while Cl−and NO3−showed negligible effects and humic acid and CO32−caused only moderate inhibition. Scavenging experiments and controlled TEMP-EPR measurements with appropriate blank and control systems supported a dominant contribution of singlet oxygen (1O2), with radical pathways playing only minor roles. The enhanced performance is therefore associated with the nanoconfined reaction environment, which promotes efficient PAA activation while stabilizing the Co species. This work extends nanoconfinement-regulated PAA oxidation to the treatment of the highly bioactive steroid estrogen E2 and provides a quantitative assessment of the activity–stability advantages of internally confined Co species.
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PubMed
高影响因子
Fundamental Research
·
2022
·
IF 0
Qianqian Yang,Zhiyuan Feng,Yanbo Zhou,Hongying Zhao,Guohua Zhao
High concentrations of inorganic ions in saline wastewater pose adverse effects on hydroxyl radical (HO • )-dominated technologies. Here, we report a unique strategy for boosting singlet oxygen ( 1 O 2 ) generation via coactivation of oxygen and peroxymonosulfate (PMS) by regulating the electron transfer regime in the photoelectrochemical process. The Fe-N bridge in atomic Fe-modified graphitic carbon nitride (denoted SA-FeCN) favors the construction of electron-defective Fe and electron-rich N vacancies (Nvs) to accelerate directional electron transfer. The produced intermediate (HSO 4 O···Fe−Nvs···O O) as a chemical channel accelerates the directional electron transfer from PMS to further reduce O 2 to form activated products (SO 5 •− , O 2 •− ), thereby transforming O 2 into 1 O 2 . An optimized 1 O 2 generation rate of 39.4 μmol L − 1 s − 1 is obtained, which is 15.7–945.0 times higher than that in traditional advanced oxidation processes. Fast kinetics are achieved for removing various phenolic pollutants in a nonradical oxidation pathway, which is less susceptible to the coexistence of natural organic matter and inorganic ions. The COD removal for coal wastewater and complex industrial wastewater in real scenarios is found to reach a value of 90%-96% in 3 h. This work provides a new direction for boosting the 1 O 2 generation rate, especially for the selective degradation of target electron-rich contaminants in saline wastewater.
研究领域:
环境科学
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化学工程
·
材料科学
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ENVIRONMENTAL RESEARCH
·
2020
·
IF 5.715
Li Liu,Yunong Li,Wei Li,Ruixue Zhong,Yeqing Lan,Jing Guo
Co 3 O 4 –SnO 2 /rice straw biochar (RSBC) was prepared for the first time via calcining oxalate precipitation precursor dispersed on the surface of RSBC and used as a catalyst for activating PMS to degrade sulfisoxazole (SIZ). The results demonstrated that Co 3 O 4 –SnO 2 /RSBC possessed much better catalytic performance than Co 3 O 4 , Co 3 O 4 –SnO 2 , Co 3 O 4 /RSBC, and SnO 2 /RSBC, which is ascribed to the synergy of Co 3 O 4 , SnO 2 and RSBC. Approximately 98% of SIZ (50 mg/L) was decomposed by PMS (1 mmol/L) activated with Co 3 O 4 –SnO 2 /RSBC (0.1 g/L) within 5 min. The optimal degradation efficiency of SIZ was realized at the initial pH 9. Co 3 O 4 –SnO 2 /RSBC also displayed remarkable stability and reusability, and the degradation rate of SIZ maintained over 90% even after the fifth recycle run. The electron paramagnetic resonance (EPR) technique and quenching experiments proved singlet oxygen ( 1 O 2 ) to be the main reactive oxygen species (ROS) responsible for the SIZ decomposition in the Co 3 O 4 –SnO 2 /RSBC/PMS system. On the basis of the characterization analysis, the identification of the ROS and the SIZ degradation products , the possible mechanism and pathways of the SIZ degradation by a combination of PMS and Co 3 O 4 –SnO 2 /RSBC were further proposed. This study provides not only a new insight into non-radical mechanism for the heterogeneous activating PMS over Co 3 O 4 –SnO 2 /RSBC to degrade organic pollutants but also an eco-friendly synthetic route for exploring novel and efficient catalysts.
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高影响因子
Redox Biology
·
2020
·
IF 9.986
Lei Zeng,Meng-Di Wang,Sheng-Li Ming,Guo-Li Li,Peng-Wei Yu,Yan-Li Qi,Da-Wei Jiang,Guo-Yu Yang,Jiang Wang,Bei-Bei Chu
Emerging viral pathogens cause substantial morbidity and pose a severe threat to health worldwide. However, a universal antiviral strategy for producing safe and immunogenic inactivated vaccines is lacking. Here, we report an antiviral strategy using the novel singlet oxygen ( 1 O 2 )-generating agent LJ002 to inactivate enveloped viruses and provide effective protection against viral infection. Our results demonstrated that LJ002 efficiently generated 1 O 2 in solution and living cells. Nevertheless, LJ002 exhibited no signs of acute toxicity in vitro or in vivo . The 1 O 2 produced by LJ002 oxidized lipids in the viral envelope and consequently destroyed the viral membrane structure, thus inhibiting the viral and cell membrane fusion necessary for infection. Moreover, the 1 O 2 -based inactivated pseudorabies virus (PRV) vaccine had no effect on the content of the viral surface proteins. Immunization of mice with LJ002-inactiviated PRV vaccine harboring comparable antigen induced more neutralizing antibody responses and efficient protection against PRV infection than conventional formalin-inactivated vaccine. Additionally, LJ002 inactivated a broad spectrum of enveloped viruses. Together, our results may provide a new paradigm of using broad-spectrum, highly effective inactivants functioning through 1 O 2 -mediated lipid oxidation for developing antivirals that target the viral membrane fusion process.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Bao-Cheng Huang,Gui-Xiang Huang,Jun Jiang,Wu-Jun Liu,Han-Qing Yu
Carbon-based materials are recognized as promising candidates for pollutant degradation because of their environmental benignity. Massive and cost-effective production and efficient recovery of carbon-based catalysts are crucial to apply this technology. However, various nanostructured carbons with different dimensions are usually utilized as precursors while not considering their complex preparation procedures and the high costs of ingredients. Moreover, catalyst separation and recovery are not given sufficient attention. In this work, a calcium salt-assisted pyrolysis strategy is proposed to tune the catalytic site formation of carbon-based catalysts. Results show that blending equal amounts of Ca2+ (calcium chloride) and organic precursors could greatly improve the catalytic activity of the carbonated product to activate peroxymonosulfate for pollutant degradation. In addition, the proposed synthetic strategy is universal to most of the readily accessed and cost-effective organic precursors. Singlet oxygen is identified as the main reactive oxidant for pollutant removal in the catalytic reaction. By cross-linking calcium ions and alginate as a hydrogel to immobilize the catalyst, the carbon material could be readily recovered. Furthermore, a long-term continuous-flow reactor test is conducted to validate the effectiveness of applying the immobilized catalyst to treat a synthetic wastewater with 0.5 mM bisphenol A. As a result, a green synthesis and immobilization strategy for persulfate catalysts is successfully established, and the prepared catalyst might be applied for wastewater treatment through using calcium salt in two purposes.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Qihui Zhang,Dan He,Xinran Li,Wei Feng,Cong Lyu,Yifeng Zhang
Peroxymonosulfate (PMS) has gained attention as oxidant for SR-AOPs. It is essential to develop a stable heterogeneous catalyst with strong hydrophilicity and high electron transfer capability for PMS activating. In this study, cobalt oxyhydroxide (CoOOH) was synthesized and activated PMS for degradation of 2,4-dichlorophenol (2,4-DCP) aiming to assess the feasibility of CoOOH/PMS system. 50 mg/L of 2,4-DCP could be 100% degraded within 120 min with 0.20 g/L CoOOH and 6 mM PMS. CoOOH/PMS system possessed a high degradation efficiency (0.0462 min −1 ), which was about 10 and 4 times higher than Co 3 O 4 /PMS and CoFe 2 O 4 /PMS system, respectively. Furthermore, it was found that CoOOH/PMS system displayed effective catalytic performance over broad pH range (e.g. 3–9). Importantly, the quenching tests revealed that 1 O 2 was identified as dominant reactive oxygen species (ROS). Co (Ⅲ) was rapidly reduced to Co (Ⅱ) owing to the efficient electron transfer rate performance of CoOOH in the catalytic reaction. Then, the regeneration of Co (Ⅱ) facilitated CoOH + owing to the surface of CoOOH with sufficient hydroxyl group, which is crucial for PMS activation and reactive oxygen species-ROS generation. This study proposed an alternative technology based on peroxymonosulfate catalyzed by cobalt-based hydroxide for waste water treatment.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Shanshan Yang,Pingxiao Wu,Junqin Liu,Meiqing Chen,Zubair Ahmed,Nengwu Zhu
For eliminating organic pollutants from wastewater, Fe 0 or Fe 0 -composites as catalyst for peroxymonosulfate (PMS) activation have attracted increasing attention in advanced oxidation processes. In this work, a novel Fe 0 -montmorillonite composites (Fe-Mt-C-H 2 ) have been prepared by thermal reduction and used as an activator for PMS to remove bisphenol A (BPA). The removal efficiency of BPA (25 mg·L −1 ) and total organic carbon (TOC) were 99.3% and 70.6%, respectively, in the presence of Fe-Mt-C-H 2 (0.4 g·L −1 ) and PMS (1 mM) at pH of 3. Electron paramagnetic resonance (EPR) spectroscopy and radical scavenger studies demonstrated that superoxide radical (O 2 − ) and singlet oxygen ( 1 O 2 ) were the crucial reactive oxygen species (ROS) in the Fe-Mt-C-H 2 /PMS system rather than sulfate (SO 4 − ) and hydroxyl radical (·OH). Besides, it was found that pH had a great influence on the catalytic oxidation rate of BPA and the Fe-Mt-C-H 2 exhibited best catalytic performance and reusability at initial pH of 3. Furthermore, the constituents of the iron surface oxidation layer at different initial pH were investigated with X-ray photoelectron spectroscopy studies, which indicated that the major constituents were Fe 3 O 4 in acidic solution and contained α-Fe 2 O 3 , FeO and FeSO 4 (s) in alkaline or neutral solution. The findings of this study provide new insights into the activation mechanism of PMS by Fe 0 -composites and exhibit a promising application of Fe-Mt-C-H 2 in wastewater treatment.
研究领域:
环境科学
·
化学工程
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Luwei Zhai,Fengchun Li,Yuhai He,Xia Chen,Xuan Zhang,Yawei Gu,Chongqing Xu,Guihuan Yan,Xiaojing Feng,Wenqiang Jiang
The present investigation involved the synthesis of sulfur-doped CoFe 2 O 4 (S-CoFe 2 O 4 ) catalysts by a straightforward co-precipitation and calcination technique. These catalysts were subsequently employed for the degradation of norfloxacin (NOR) utilizing activated perodisulfate (PDS). At the optimal level of sulfur doping, the efficiency of NOR removal in the S-CoFe 2 O 4 -3/PDS system can achieve a high percentage of 98.2%. Furthermore, the study also examined the impact of starting pH, catalyst dosage, PDS dose, several common inorganic anions, and humic acid on the breakdown of NOR. The study of free radicals and singlet oxygen activation mechanisms in the S-CoFe 2 O 4 /PDS system is facilitated through the implementation of free radical quenching experiments and electron paramagnetic resonance (EPR) techniques. The suggested breakdown mechanism of NOR in the S-CoFe 2 O 4 /PDS system was determined through the analysis of degradation products using high-performance liquid chromatography-mass spectrometry (HPLC-MS). The Biotoxicity Analysis Software (TEST) was employed to assess the toxicity of NOR and its breakdown products.
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