ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2018
·
IF 6.653
Yuan Chen,Xu Zhang,Shixiang Feng
Contributions of excited triplet state of humic acid (3HA*) and superoxide radical anion (O2•–), which is mainly generated via the reaction of O2 with HA-derived reducing intermediates (HA•–), to phenol transformation were revealed using acetaminophen, 2,4,6-trimethylphenol and tyrosine as probe molecules. Phenol transformation was initiated by 3HA*, leading to the formation of the phenoxyl radical (PhO•), but the distribution of transformation intermediates was codetermined by 3HA* and HA•–. The influence of HA•– essentially resulted from the production of O2•–, which affected the fate of PhO•. PhO• could undergo dimerization, or react with O2•–, leading to either phenol peroxide formation (radical addition) or phenol regeneration (electron transfer). In addition, PhO• could bind to HA or react with HA radicals, particularly in the absence of O2 and O2•–. These PhO• reactions were dependent on the reduction potential and structure of PhO•. This study also proved that the reaction of phenol with 1O2 and the reaction of PhO• with O2•– lead to the same oxidation product. The contributions of 3HA* and its generated 1O2, HA•– and its generated O2•– to phenol transformation were pH-dependent.
研究领域:
环境化学
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物理化学
·
分析化学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yuhang Zhang,Jin Qian,Peifang Wang,Yuxuan He,Bianhe Lu,Sijing Tang,Kailin Xu
In this study, ternary magnetic nanocomposites (SrTiO 3 /CoFe 2 O 4 /rGO, SCG) doped with cobalt ferrite and loaded with rGO were successfully synthesized, and utilized to rapidly activate PMS to degrade LVF. After evaluating the efficacy of samples with different loading loads, SCG-1 (1 % wt rGO loading) was selected for further testing due to its optimal catalytic activity (degradation efficiency reached 87.4 % in 5 min). Quench experiments and electron paramagnetic resonance (EPR) analysis showed that SO 4 − , 1 O 2 , OH were the main active substance involved in LVF degradation. Based on the redox cycle of Co and Fe ions and the platform provided by perovskite and rGO, the reaction can be carried out quickly. The vulnerable sites and possible degradation pathways of LVF were further analyzed by density functional theory (DFT) calculation and LC-MS/MS analysis, and the developmental toxicity and ecological risk of intermediate products were determined based on toxicity assessment software (T.E.S.T). This study provided a new vision for realizing rapid antibiotic degradation in water environments and provided theoretical support for the subsequent research on novel nanomaterials.
研究领域:
环境科学
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纳米技术
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水处理
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材料科学
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产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Geng Li,Zhuoyu Cai,Kun Su,Yuxin Zhao,Ying Zhu,Jiangang Han,Yuwei Pan,Weinan Xing,Guangyu Wu
In recent years, advanced oxidation technologies employ peroxynitrite activation have exhibited exceptional effectiveness in eliminating various emerging contaminants. In this study, different calcination temperatures were used to derive Co 3 O 4 nanospheres with varying surface morphologies . This method effectively addresses the issue of high cost associated with high-performance catalyst synthesis or poor catalytic performance of low-cost catalysts. The active species like O 2 •− , •OH, SO 4 •− , 1 O 2 played significant role in TC degradation and 1 O 2 was the dominant reactive oxygen species (ROS). The study also proposed possible degradation pathways based on the 15 intermediates identified through HPLC-MS. Furthermore, the developmental toxicity of the identified intermediates was evaluated using a quantitative conformational relationship prediction method. This paper delves into the reaction mechanism of Co 3 O 4 nanospheres in the activation of PMS and examines the impact of surface morphology on their catalytic performance, providing a new approach to developing a persulfate catalyst that is cost-effective and has high catalytic performance, with a simple synthesis step.
研究领域:
环境科学
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化学工程
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材料科学
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高级氧化技术
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催化
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Qi Zhang,Wei Li,Siyuan Cao,Xu Yin,Hongwei Zhu,Liankai Gu,Haoming Chen,Xiaoyuan Zhang,Weiqing Han,Kajia Wei
Precisely controlling atomic occupancy in edge-sharing sites remains challenging and limits the application of spinel oxides in advanced oxidation processes (AOPs). Herein, a series of inverse spinel oxides featuring edge-sharing Co Oh -O-Mn Oh (Oh means octahedral) configurations were designed to leverage inter-octahedral electronic redistribution and spin-state modulation, thereby enhancing catalytic performance for peroxymonosulfate (PMS) activation and pollutant degradation. The energy redistribution induced by this structure enhances the O-p/Mn-d orbital hybridization, accelerates the electron transfer kinetics between Co and Mn, and promotes the generation of high-valent cobalt-oxo (Co IV =O) species and singlet oxygen ( 1 O 2 ), thereby increasing the degradation efficiency of organic pollutants. The optimized Co-Mn inverse spinel achieved complete BPA removal within 15 min, exhibiting 11.4-fold enhancement in PMS activation efficiency than unmodified cobalt oxide, and with < 6.5 % average efficiency deviation at 100 mM ionic concentration. This study offers a strategy for the precise design of edge-sharing reactive sites in inverse spinel oxides and their application in AOPs.
研究领域:
环境催化
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高级氧化技术
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材料化学
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无机化学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Shengnan Huang,Fan Tian,Jiawei Dai,Xuesong Tian,Guangfang Li,Yunling Liu,Zhiquan Chen,Rong Chen
Chlorophenols (CPs) treatment in water is a huge challenge due to its native robustness and harmful chlorinated by-products in degradation. In this work, we developed a specific BiO 2-x with high density Bi-O-Bi-O vacancy via a facile hydrothermal process. Extraordinary CPs removal ability under near infrared (NIR, >700 nm) is achieved over the as-prepared product. The presence of vacancies not only induced strong interactions between CPs and photocatalyst, but also promoted singlet oxygen ( 1 O 2 ) and photogenerated holes (h + ) generation. Furthermore, the generated 1 O 2 is found mainly originating from lattice oxygen release and the superoxide radicals ( O 2 − ) oxidation from BiO 2-x . Such performance could be well-maintained under wide pH range as well as in the presence of different constitutes in water matrix. This work unravels a unique function of BiO 2-x photocatalyst for CPs decomposition and provide a rational design of highly efficient photocatalysts toward optimization of pollutants degradations.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 26
·5255-5263
·
IF 6.331
Jiansheng Liu,Xueqin Qing,Qin Zhang,Ningyue Yu,Mengbin Ding,Zhaohui Li,Zhen Zhao,Zhiling Zhou,Jingchao Li
Photodynamic therapy (PDT) has provided a promising approach for the treatment of solid tumors, while the therapeutic efficacy is often limited due to the hypoxic tumor microenvironment, resulting in tumor metastasis. Herein, we report an oxygen-producing proenzyme hydrogel (OPeH) with photoactivatable enzymatic activity for PDT enabled metastasis-inhibiting combinational therapy of breast cancer. This OPeH based on alginate is composed of protoporphyrin IX (PpIX) conjugated manganese oxide (MnO2) nanoparticles, which act as both the photosensitizer and oxygen-producing agent, and singlet oxygen (1O2)-responsive proenzyme nanoparticles. In the hypoxic and acidic tumor microenvironment, MnO2 can generate 1O2 to promote PpIX-mediated PDT with an amplified 1O2 generation efficiency, which also triggers the cleavage of 1O2-responsive linkers and cascade activation of proenzymes for cancer cell death. This combinational therapy upon photoactivation not only greatly inhibited the tumor growth, but also suppressed lung metastasis in a mouse xenograft breast tumor model, which is impossible in the case of PDT alone. This study thus provides a proenzyme hydrogel platform with photoactivatable activity for metastasis-inhibiting cancer therapy with high efficacy and safety.
研究领域:
癌症治疗
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纳米医学
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生物医学工程
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肿瘤微环境研究
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产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2026
·
IF 12.8
Lumeng Jia,Wenchao Yu,Xiangting Hou,Mengxue Li,Qi Shi,Zhaoyong Bian,Hui Wang
Photoelectrocatalytic (PEC) in situ hydrogen peroxide (H 2 O 2 ) production offers a green strategy for activating singlet oxygen ( 1 O 2 ) and degrading refractory organic pollutants. However, it suffers from low cathode yield, sluggish anode kinetics, mass-transfer losses, and low selectivity for 1 O 2 . This study ingeniously designed an S-O double vacancy β-In 2 S 3 -Er/Yb@WO 3 -Ov S-type heterojunction full-spectrum photoanode, offered new perspectives on in situ oxygen reduction at the photoanode for H 2 O 2 generation, and presented a dual-electrode cooperative PEC system. In the experiment, double vacancies at the photoanode acted as electron traps, accumulating electrons. Meanwhile, an applied bias voltage, more electrons on the surface, and weakly acidic and oxygen-permeable conditions the electrons trapped by vacancies, together with conduction band electrons, were conducive to driving the in-situ two-electron oxygen reduction reaction to H 2 O 2 formation at the photoanode. O vacancies dominated interfacial adsorption and catalysis, while S vacancies served as electron traps for charge separation, forming a complementary synergy. Coupled with charge modulation at the S-scheme heterojunction interface, accelerating photogenerated carrier separation and preserved highly reactive holes, providing key conditions for 1 O 2 generation. β-In 2 S 3 -Er/Yb@WO 3 -Ov photoanode realized in-situ oxygen reduction reaction-induced H 2 O 2 production and cathodic H 2 O 2 activation simultaneously. Both routes yield ·OOH/·O 2 - intermediates, which were oxidized by holes to form 1 O 2 , thereby enabling efficient carbamazepine removal (98.4%, k app = 0.093 min -1 ), efficient 1 O 2 production (53.13 μmol L -1 min -1 ), and low energy consumption (0.155 kWh m -3 -log). This work presents an advanced PEC strategy for the synergistic synthesis of H 2 O 2 and 1 O 2 , offering a promising approach for high-efficiency environmental remediation.
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jingwei Yan,Lin Gong,Senyou Chai,Cong Guo,Wei Zhang,Hongyou Wan
The dual effect of chloride anions (Cl − ) on sulfate radical-advanced oxidation process (SR-AOP) systems has recently garnered increasing attention, particularly the inhibitory effects of Cl − on the degradation of organic pollutants. However, few studies have characterized the promoting effect of Cl − on SR-AOPs. Our study investigated the effect of Cl − on the degradation of levofloxacin (LVF) in peroxymonosulfate (PMS) with ZIF-67/VTM (Z-VTM) as an activator. With the addition of Cl − , singlet oxygen ( 1 O 2 ) was the dominant driver of LVF degradation in the Cl − /Z-VTM/PMS system, which differed from the dominant role of HOCl (generated from Cl − ) in the degradation of organic pollutants in previous studies. To the best of our knowledge, our study is the first to describe the conversion of HOCl to 1 O 2 in a Cl − /Z-VTM/PMS system. 1 O 2 was effectively generated in Cl − containing water at a 3.0–9.0 pH range. This work provides novel insights into the formation of ROS from HOCl during the degradation of organic pollutants in SR-AOPs, which is of great significance for the removal of organic pollutants in wastewater with high salt concentrations.
研究领域:
环境科学
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水处理
·
化学工程
·
污染物降解
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Shihua Zhang,Shuang Dai,Qiao Huang,Jincan Huang,Shengqiang Hei,Peng Wang,Biming Liu
The confinement effect triggered by nano-confinement systems in the advanced oxidation processes has received extensive attention. In this study, the strategy of constructing stable confined Co 3 O 4 @SiO 2 materials and activating peroxymonosulfate (PMS) was adopted to successfully achieve the efficient removal of enrofloxacin (EON). The removal efficiency of EON by Co 3 O 4 @SiO 2 (0.08 g/L) could reach 99 % at pH 0 of 7 and PMS of 0.2 g/L, and the optimal degradation rate could reach 0.147 min −1 , which was 9.6 times higher than that of the unconfined system. The reaction process was mainly driven by the synergistic interaction between the non-radical 1 O 2 and the interfacial electron transfer network, and the formation of oxygen vacancies within the reaction system accelerated the degradation process. Density functional theory calculations further showed that the confinement effect of SiO 2 aerogel stabilized the Co 3 O 4 nanoparticles, the charge transfer efficiency between Co 3 O 4 @SiO 2 and PMS was optimized, and at the same time, Co 3 O 4 was the key active site for EON degradation. This research can provide an effective strategy for the activation of PMS by SiO 2 aerogel confined structure to remove antibiotic pollutants.
研究领域:
环境科学
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材料化学
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高级氧化过程
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纳米材料
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污染物降解
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Chenguang Li,Yanlei Zhang,Shiqi Yin,Qin Wang,Yuanyuan Li,Qiang Liu,Liuqingqing Liu,Xianxiang Luo,Lingyun Chen,Hao Zheng,Fengmin Li
p -Phenylenediamines (PPDs), an important type of rubber antioxidants, have received little study on their environmental fate , particularly for their vital photodegradation process in water environment. Accordingly, N -(1,3-dimethylbutyl)- N′ -phenyl-1,4-phenylenediamine (6PPD), as a representative of PPDs, was investigated experimentally and theoretically for its photodegradation in water. Rapid photodegradation occurred when 6PPD was exposed to illumination especially UV region irradiation. Under acidic conditions, the photodegradation of 6PPD accelerated mainly due to the increased absorption of long wavelength irradiation by ionized 6PPD. Nine photodegradation products (e.g., 6PPD - quinone (6PPDQ)) of 6PPD were identified by an ultra-performance liquid chromatography QTOF mass spectrometry . Molar yields of photoproducts such as 6PPDQ, aniline, 4-aminodiphenylamine, and 4-hydroxydiphenylamine were 0.03 ± 0.00, 0.10 ± 0.01, 0.03 ± 0.02, and 0.08 ± 0.01, respectively. Mechanisms involved in 6PPD photodegradation include photoexcitation , direct photolysis, self-sensitized photodegradation, and 1 O 2 oxidation , as demonstrated by electron paramagnetic resonance (EPR) analysis, scavenging experiments, and the time-dependent density functional theory (TD-DFT). Notably, the toxicity of the reaction solution formed during the photodegradation of 6PPD was increased by the formation of highly toxic products (e.g., 6PPDQ). This study provides the first explanation for photodegradation mechanisms of 6PPD and confirms the pathway of 6PPDQ produced by the photoreaction in water environment.
研究领域:
环境科学
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化学
·
毒理学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Teng Huang,Fan Tian,Zhipan Wen,Guangfang Li,Ying Liang,Rong Chen
Bi/Bi 2 WO 6-x heterostructures has been successfully prepared by a facile one-step hydrothermal method. By maneuvering reaction time and Bi/W molar ratio of the precursors, we have been able to selectively introduce oxygen vacancy and metallic Bi into Bi 2 WO 6 nanostructures. The obtained Bi/Bi 2 WO 6-x heterostructures with more oxygen vacancy and moderate metallic Bi exhibit significantly improved photocatalytic activity for the photodegradation of bisphenol A (BPA) and its analogues due to its great ability for the generation of singlet oxygen ( 1 O 2 ), which has proven to work as the main reactive oxygen species during photocatalysis. It is also found the 1 O 2 concentration is highly depended on and modulated by the content of oxygen vacancy and metallic bismuth. Besides, we also demonstrate that the obtained Bi/Bi 2 WO 6-x products display efficient photocatalytic performance toward BPA derivatives degradation and enhanced stability to resist the interferences in the water matrix.
研究领域:
环境科学
·
材料科学
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DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 9
·1-16
·
IF 2.4
Hu Rui,Wang Haiyin,Luo Jiahui,Song Jianjun,Jia Haiyuan
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) have been proven to be an effective method for the removal of tetracycline in water. In this study, the Co 3 O 4 /molecular sieve catalyst synthesized by the incipient wetness impregnation method was used for PMS activation. The effect of specific surface area on the catalytic performance of Co 3 O 4 /molecular sieve catalyst was investigated and analyzed in detail by characterization techniques. In the Tetracycline hydrochloride (TCH) degradation experiment, the Co 3 O 4 /13X catalyst exhibited the highest specific surface area (490.584 m 2 /g) and provide abundant active sites, enabling 98.0% TCH degradation within 30 min under optimal conditions (1.5 g catalyst, 0.3 mM PMS, pH 8.0, 25℃), with a reaction rate constant (k obs ) of 0.0977 min -1 . In addition, the degradation mechanism of TCH was explored using electron paramagnetic resonance (EPR) spectroscopy and quenching experiments. It was confirmed that free radicals (SO 4 •− , •OH, O 2 •− ) and non-free radical species ( 1 O 2 ) generated during the reaction play a crucial role in the degradation process of TCH. In summary, the Co 3 O 4 /13X catalyst, when activating PMS, exhibits a remarkable synergistic effect on the degradation of TCH, and shows good repeatability and environmental adaptability. This study provides valuable insights into the design and optimization of catalysts for degrading antibiotic pollutants in water treatment processes. Graphical
研究领域:
环境科学
·
催化
·
水处理
·
化学工程
·
污染物降解
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）