SCIENCE OF THE TOTAL ENVIRONMENT
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2018
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IF 4.61
Shizong Wang,Jianlong Wang
Carbamazepine is one of pharmaceutical and personal care products (PPCPs) and has been widely used to treat depression and seizures, and it cannot be effectively removed during the conventional wastewater treatment processes . In this study, three processes were used for the carbamazepine degradation, including single radiation, radiation in the presence of peroxymonosulfate (PMS) and radiation followed by PMS oxidation. The results show that radiation in the presence of PMS could enhance the degradation and mineralization of carbamazepine, decreasing the absorbed dose required for completely degrading carbamazepine from 800 Gy to 300 Gy, no matter what the molar ratio of PMS to carbamazepine was. The radiation followed by PMS oxidation significantly increased the mineralization, and the maximum mineralization achieved 46.5% at the dose of 600 Gy. Eight intermediates were tentatively identified. Compared to single radiation process, the radiation in the presence of PMS enhanced the transformation of intermediates and the release of ammonium ion. In real wastewater , the radiation in the presence of PMS could effectively remove carbamazepine and considerably decreased the biological toxicity of the wastewater containing carbamazepine.
研究领域:
环境科学
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水处理工程
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毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Junmei Luo,Shufeng Bo,Yanan Qin,Qingda An,Zuoyi Xiao,Shangru Zhai
The excessive discharge of goat manure has placed a serious burden on the environment and accordingly how to transform this type of waste into functional materials is of practical significance yet remains challenging. Herein, surface-loaded cobalt/biochar (Co-GMC-900) was successfully prepared for the first time by carbonizing Co-impregnated goat manure waste. The Co-GMC-900 exhibited excellent performance in activating peroxymonosulfate (PMS) to degrade ciprofloxacin (CIP), which could remove 96.5% of CIP within 30 min. Additionally, in the cycle experiments, the Co-GMC-900 presented robust stability due to the synergy of excellent magnetism, inherent ellipsoid of goat manure and strengthened interactions between cobalt nanoparticles and graphitized biochar network. In the light of a series of characterization analyses, carbonization temperature played a crucial role in tailoring the physicochemical properties (crystal structure, graphitized degree, the ratio of C=O groups and specific surface area) of composites. Based on detected active species, radical process (SO 4 •− , • OH and O 2 •− ) in conjunction with the non-radical process ( 1 O 2 and charge transfer) resulted in the CIP degradation, in which the radical process mainly contributed to the degradation process, and Co 0 played a leading role in the radical process. Favorably, this work might provide great promise for utilizing goat manure waste in a valuable manner and simultaneously achieving environmental remediation.
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Chen Ling,Chaolin Li,Aiping Liang,Wenhui Wang
Microplastics (MPs) pose a severe threat to the environment and human health, and effective treatment techniques are urgently desired to prevent the global spread of MPs pollution. However, efficient degradation of MPs remains difficult. Herein, vacuum ultraviolet (VUV) activated peroxymonosulfate (PMS) was firstly proposed as a promising technique for the degradation of polyethylene MPs. The weight loss of MPs reaches as high as 51.5% under mild conditions ([PMS] = 32 mmol/L, initial pH = 7, [MPs] = 1 g/L, [Time] = 48 h), which is the record performance achieved at room temperature and ambient pressure for MPs degradation. The excellent degradation performance is uncovered to originate from the synergistic effect of VUV and activated PMS. Direct photolysis of VUV can rapidly oxidize the surface of MPs to reduce its hydrophobicity and thus enhance the adsorption of reactive oxidation species (i.e., SO 4 ⋅− and HO ⋅ ) rooted from the VUV activated PMS, which was further confirmed by DFT calculations. The degradation of MPs repeatedly undergoes the process of VUV photolysis oxidation of the surface, degradation via VUV/UV/PMS-derived reactive oxidation species, shedding, and re-exposure of the new surface via VUV photolysis oxidation. This study highlights the unique role of the VUV photolysis in MPs degradation, paving a new route for designing practical MPs pollution remediation techniques.
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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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Baokang Xu,Xiao Zhang,Yue Zhang,Shiwen Wang,Peng Yu,Yongjun Sun,Xi Li,Yanhua Xu
The nonradical pathway selectively oxidizes pollutants with less interference from environmental factors, which can effectively improve the environmental suitability of peroxymonosulfate (PMS) activation. Herein, a Co-doped nanotubular carbon nitride catalyst (Co-CNNT) based on CoN x sites was constructed for stable and efficient PMS activation with a better specific surface area, number of CoN x sites, and electron transfer capability than Co-doped lamellar carbon nitride catalyst (Co-CN). Co-CNNT improved PMS utilization efficiency (∼50%) and enhanced the contribution of the electron transfer pathway to tetracycline (TET) degradation. The enhanced ability of Co-CNNT to adsorb PMS leads to Co-CNNT–PMS* generated by PMS at the CoN x site, which raises the Co-CNNT surface potential and allows PMS to be activated in a manner that captured electrons. Thus, the Co-CNNT/PMS system could effectively destroy electron-rich or low-potential pollutants within 24 min. The stronger environmental adaptability allows it to maintain catalytic activity in complex aqueous matrices, achieving effective oxidation of diluted tetracycline-based pharmaceutical wastewater. This paper reveals the effects of carbon nitride morphology control strategies on the properties of CoN x active sites and PMS activation mechanisms, providing new insights into the induction of nonradical PMS activation pathways.
研究领域:
环境科学
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催化
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水处理
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ronghao Wu,Xin Hu,Yihui Li,Yongfu Li,Yanjiang Cai,Peikun Jiang,Bing Yu
Constructing bimetallic nanostructures with specific crystalline phases provides an attractive strategy to develop highly efficient catalysts and explore structure-dependent catalytic properties. Herein, a new iron-based bimetallic catalyst consisting of amorphous MnO 2 and crystalline α-Fe 2 O 3 was synthesized for peroxymonosulfate (PMS) activation, named as a-MnO 2 /α-Fe 2 O 3 . The results show that the removal efficiency of sulfamethoxazole is over 90% within 120 min by the a-MnO 2 /α-Fe 2 O 3 in the presence of PMS at broad pH conditions ranging from 3 to 9. Furthermore, a complete degradation of bisphenol A (BPA) is achieved within 2 min in the a-MnO 2 /α-Fe 2 O 3 /PMS system under optimum conditions, and the BPA degradation rate constant of 1.67 min −1 outperforms most reported Fe- and Mn- based catalysts. The results of electron paramagnetic resonance analysis, quenching tests and Raman spectroscopy analysis show that the mechanism for the a-MnO 2 /α-Fe 2 O 3 -based PMS activation is dominated by the formation of activated surface-PMS complexes. ≡Mn(Ⅳ)–OH and ≡Fe(III)–OH of a-MnO 2 /α-Fe 2 O 3 are active sites for PMS adsorption to form inner-sphere complexes (≡Mn(Ⅳ)-OOSO 3 - ) through the replacement of surface hydroxyl groups. Finally, the a-MnO 2 /α-Fe 2 O 3 exhibits a remarkable removal efficiency of over 99% for BPA in column-bed tests conducted over 600 cycles, demonstrating its immense potential for practical applications.
研究领域:
环境科学
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催化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jinming Feng,Jincheng Mu,Qiong Peng,Yang Xiao,Baojun Liu
Cobalt-based oxides have attracted extensive attention in heterogeneous catalytic peroxymonosulfate (PMS) activation towards emerging pollutants degradation, while the improvement of their catalytic performance is still a severe challenge. Herein, a CoO x ultrathin nanosheet composed of in situ interfacial Co 3 O 4 and CoO (CoO x -Ar-350) was synthesized and employed in PMS activation for micro-contaminates removal. The catalyst shows 100 % bisphenol A (BPA) conversion within 2 min ([BPA] = 20 mg/L, [Catalyst] = 20 mg/L, [PMS] = 200 mg/L) with a remarkable reaction rate of 2.69 min −1 , which is 3.84 and 2.66 times of pure Co 3 O 4 and CoO, respectively. Characterization and theoretical calculation results indicates that the interfacial synergy between Co 3 O 4 and CoO could modulate the adsorption behavior and enhance the electron acceptance of PMS, which boosts the breaking of O-O bonds and the generation of reactive oxygen species (ROS) and thereby the pollutant removal efficiency. The ROS quenching and capture experiments demonstrate that the enhanced OH and 1 O 2 play significant contribution during the degradation process. This work provides a novel in situ interfacial engineering for the development of highly efficient catalyst and reveals the activity enhancement mechanism for PMS activation.
研究领域:
环境科学
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催化
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水处理
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Shishun Wang,Shuang Gai,Kui Cheng,Zhuqing Liu,Markus Antonietti,Fan Yang
The degradation efficiency of organic contaminants using Fenton-like system based on Fe(II) and peroxymonosulfate (PMS) has been hindered by the rapid transformation from Fe(II) to Fe(III) and the slow regeneration of Fe(II). To address this challenge, artificial humic acid (AHA) derived from biomass was incorporated into Fe(III)/PMS system to build AHA/Fe(III)/PMS system. The results demonstrated that the degradation rate of atrazine (ATZ) in AHA/Fe(III)/PMS system (98.83%) is significantly superior to those in Fe(III)/PMS (16.51%) and AHA/PMS system (41.76%) within 90 min. Furthermore, Fe(II) measurement experiments revealed that AHA exhibited more significant iron-reducing potential. The analysis of FTIR, 3D-EEM, and liquid NMR indicated that AHA possessed more structures with reductive potential in comparison to commercial humic acid (CHA) and humic acid extracted from lignite (LHA). The results of persistent free radicals indicated that CHA possessed oxidative potential, which also accounted for the lowest Fe(II) concentration in those system containing CHA. Furthermore, quenching experiments, EPR analysis, and PMSO probe analysis have indicated the presence of reactive species such as •OH, SO 4 •- , and Fe(IV) within AHA/Fe(III)/PMS system. The degradation products from ATZ were identified and determined to exhibit reduced toxicity relative to parent compound. Collectively, these findings presented an in-depth understanding to reactivate Fe(III)/PMS system, offering a promising alternative strategy for efficient degradation of organic pollutants in water treatment processes.
研究领域:
环境科学
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水处理技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2024
·
IF 5.5
Shengrong Liu,Boyang Wang,Yimeng Huang,Xing Xu,Yujiao Kan,Yanan Shang
Background Advanced oxidation processes (AOPs) based on sulfate radicals (SO 4 •– ) have proven to be highly effective in degrading organics in wastewater. Carbon-based materials have emerged as promising catalysts for activating persulfate, which generates environmentally friendly sulfate radicals (SO 4 •– ), for remediation purposes. The nitrogen doping technique is an effective method for site-specific regulation and can significantly enhance the performance of carbon-based catalysts, which could promote the application of carbon-based catalysts in the future. Endogenous and exogenous nitrogen sources can provide nitrogen sources for N doping. However, there are few reports on the comparison of the structure and catalytic mechanism of these two types of N-doped biochar. It is also of great significance to reveal the mechanisms of constructing catalytic sites using endogenous and exogenous nitrogen. Methods Herein, the preparation of endogenous nitrogen-doped biochar (BC) was achieved by using soybean as the precursor material, which is rich in natural nitrogen-containing components of proteins. Subsequently, the BC was doped by mixing it with urea and pyrolysis, resulting in the preparation of exogenous nitrogen-doped biochar (NBC). Significant findings The characterization of XRD and HRTEM showed that g-C 3 N 4 formed in NBC. The results of catalytic degradation and quenching experiments demonstrate that the exogenous nitrogen-doped catalysts have a better performance than endogenous nitrogen-doped catalysts. The OFL removal rate in BC/PMS was higher than that in the BC/PMS system (71.68% vs. 61.83 %). The k obs in NBC/PMS are also higher than that in BC/PMS (0.00943 min −1 vs. 0.01369 min −1 ). The NBC could be a promising catalyst for PMS activation in practical application. DFT results showed that the g-C 3 N 4 generated from exogenous nitrogen can improve PMS activation performance in the g-C 3 N 4 /graphene bilayer structure. The influence on the charge distribution of surrounding carbon materials makes endogenous nitrogen doping a good choice for optimizing the local performance of the material in the absence of natural nitrogen components.
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
Small
·
2024
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IF 13
Yi Shen,Yongliang Pan,Chao Zhu,Haizhong Zhang,Jun Wang,Renlan Liu,Qile Fang,Shuang Song,Baoliang Chen
In the domain of heterogeneous catalytic activation of peroxymonosulfate (PMS), high-valent metal-oxo (HVMO) species are widely recognized as potent oxidants for the abatement of organic pollutants. However, the generation selectivity and efficiency of HVMO are often constrained by stringent requirements for catalyst adsorption sites and electron transfer efficiency. In this study, a single-atom catalyst, Cu SA /CN P&S, is synthesized featuring multiple types (planar/axial) of heteroatom coordination via an H-bond-assisted self-assembly strategy. It is confirmed that CuN 3 active centers with axial S coordination are uniformly distributed in a carbon matrix modified by planar P atoms. Cu SA /CN P&S activated PMS to selectively generate Cu (III) ═OH species as the primary reactive oxygen species (ROS). The pseudo-first-order kinetic rate for bisphenol A degradation reached 1.51 min −1 , a 17.57-fold increase compared to the unmodified Cu SA /CN catalyst. Additionally, the Cu SA /CN P&S catalyst demonstrates high efficiency and durability in removing contaminants from various aqueous matrices. Theoretical calculations and experimental results indicate that the intrinsic electric field generated by distal planar P atoms enhances electron transfer efficiency within the carbon matrix. Meanwhile, axial S coordination elevates the d-band center and tunes the e g * band broadening of Cu, thereby enhancing the adsorption selectivity for the terminal oxygen of PMS. This multitype coordination synergistically mitigates the issues of low selectivity and yield of HVMO species.
研究领域:
环境科学
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催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Environmental Science-Water Research & Technology
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2024
·
IF 3.5
Haoxiang Yan,Jianzheng Zhen,Yuyuan Yao
Developing a facile preparation method to construct separable and recyclable Fenton-like catalysts holds great significance in the field of environmental remediation. Herein, a rapid dopamine (DA) polymerization strategy to modify melamine foam (MF) was proposed for the construction of bulk foam catalytic materials, which was further utilized for peroxymonosulfate (PMS) activation to degrade organic pollutants. Taking advantage of the chelation between dopamine's catechol group and Fe3+, as well as the oxidative environment provided by H2O2, DA could encapsulate and polymerize on the surface of MF within 2 h to obtain the MF@Fe@PDA catalyst. Detailed experimental results demonstrated that MF@Fe@PDA could efficiently activate PMS to achieve almost 100% removal of bisphenol A (BPA) in 20 min, and the corresponding turnover frequency (TOF) value was one order of magnitude higher than that of the homogeneous (Fe2+, Fe3+) and nanoparticle (Fe0) catalysts. The high activity of the MF@Fe@PDA/PMS system stemmed from the Fe sites and carbonyl group (CO), which could induce the activation of PMS for the rapid generation of singlet oxygen (1O2), sulfate radical (SO4˙−) and hydroxyl radicals (˙OH). Meanwhile, the coexisting bicarbonate ions (HCO3−) in the MF@Fe@PDA/PMS system could enhance the generation of 1O2, thereby accelerating the degradation of BPA. Moreover, a flow-through system assisted by the bulk MF@Fe@PDA catalyst was constructed for organic pollutant degradation. Overall, these findings may open up new possibilities for developing highly efficient catalysts for wastewater remediation.
研究领域:
环境科学
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
Water
·
2024
·Vol. 16
·期 20
·2997
·
IF 3
Qin Liu,Huali Zhang,Kanghui Zhang,Jinxiu Li,Jiaheng Cui,Tongshan Shi
Organic pollutants entering water bodies lead to severe water pollution, posing a threat to human health. The activation of persulfate advanced oxidation processes using carbon materials derived from MOFs as substrates can efficiently treat wastewater contaminated with organic pollutants. This research uses NH2-MIL-101(Fe) as a substrate, doped with Fe2+and Co2+, to prepare Fe/Co-CNs through a one-step carbonization method. The surface morphology, pore structure, and chemical composition of Fe/Co-CNs were investigated using characterization techniques such as XRD, SEM, TEM, XPS, FT-IR, BET, and Raman. A comparative study was conducted on the performance of catalysts with different Fe/Co ratios in activating PMS for the degradation of organic pollutants, as well as the effects of various influencing factors (the dosage of Fe/Co-CNs, the amount of peroxymonosulfate (PMS), the initial pH of the solution, the TC concentration, and inorganic anions) on the catalyst’s activation of persulfate for TC degradation. Through radical quenching experiments and post-degradation XPS analysis, the active radicals in the FeCo-CNs/PMS system were investigated to explain the possible mechanism of TC degradation in the Fe/Co-CNs/PMS system. The results indicate that Fe/Co-CNs-2 (with a Co2+doping amount of 20%) achieves a degradation rate of 93.34% for TC (tetracycline hydrochloride) within 30 min when activating PMS, outperforming other Co2+doping amounts. In addition, singlet oxygen (1O2) is the main reactive species in the reaction system.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Xiaofei Ren,Yubo Wang,Guicong Hu,Qingbin Guo,Dengzheng Gao,Peng Huang,Wenbing Zhang,Li Wang,Xiaolong Hu
In this study, Fe 3 O 4 /sepiolite composites as peroxymonosulfate (PMS) catalysts were successfully synthesized via a simple water bath method for tetracycline (TC) degradation. The results indicated that the composite with 70% Fe 3 O 4 loading amount exhibited the highest TC degradation efficiency (90.12%), and its reaction rate constant (0.02193 min −1 ) was around 2.07 times higher than that of pure Fe 3 O 4 . The enhanced catalytic activity was mainly attributed to the uniform deposition of Fe 3 O 4 nanoparticles with smaller grain size (17.24 nm) on sepiolite , leading to the larger specific surface area (120.61 m 2 /g) and more exposed reaction active sites. The electron paramagnetic resonance (EPR) and quenching experiments displayed that 1 O 2 species played the predominant roles in TC degradation process. Besides, potential catalytic mechanisms and degradation pathways of TC were proposed. The toxicity of TC was reduced during the degradation process. Overall, this work can provide a new strategy for the rational design of promising mineral-based PMS catalyst for the wastewater treatment .
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）