SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Da Ouyang,Yun Chen,Ruihuan Chen,Wenying Zhang,Jingchun Yan,Mingyue Gu,Jing Li,Haibo Zhang,Mengfang Chen
1,4-Dioxane degradation under both batch-scale and column experiments has been investigated within the biochar activated peroxymonosulfate (PMS) system for in-situ remediation of 1,4-dioxane contaminated groundwater. In case of the batch experiments, the 1,4-dioxane degradation efficiencies were significantly increased with the increased biochar pyrolysis temperatures. The optimized 1,4-dioxane degradation efficiency at 89.2% was achieved with 1.0 g L −1 of biochar (E800) and 8.0 mM PMS. In the absence of PMS, the breakthrough rates of 1,4-dioxane in biochar packed column experiments under the dynamic flow conditions were relatively slow compared with those in sand packed columns. Simultaneously, based on the integrated areas (IA) from the 1,4-dioxane breakthrough curves , the degradation efficiency at 70.2% was estimated in biochar packed column (W E800 :W Sand = 1:9) under continuous injections of 16.0 mM PMS. Electron paramagnetic resonance (EPR) indicated that hydroxyl, sulfate and superoxide radicals were generated within the biochar/PMS systems and alcohol quenching experiments suggested that the dominated hydroxyl and sulfate radicals were responsible for 1,4-dioxane degradation. The findings of this study suggested that the biochar activated PMS system is a promising and cost-effective strategy for the remediation of 1,4-dioxane contaminated groundwater.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Yunjin Yao,Xiaoyan Liu,Huanhuan Hu,Yinghao Tang,Hongwei Hu,Zhenshan Ma,Shaobin Wang
Fe, N atoms deposited on porous biochar (Fe-N@BC) composites were synthesized and employed as an efficient catalyst for organic pollutant removal and Cr VI reduction. Naturally abundant, renewable and N -rich pomelo peel as a carbon and nitrogen source and unsubstituted phthalocyanine/iron phthalocyanine complexes as a Fe and nitrogen resource were used to develop the Fe-N@BC via a carbonization process. It is found that Fe-N@BC hybrids have homogeneous dispersion of Fe and N atoms on 3D hierarchically porous biochar, which significantly improves the performance toward the detoxification of organic pollutants using peroxymonosulfate as an oxidant, as well as the reduction of hexavalent chromium by formic acid as a reductant. Furthermore, the effects of Fe loading and pyrolytic temperature on catalysis were comprehensively analyzed and optimized. The excellent activity of Fe-N@BC in acid media can be attributed to the high dispersion of Fe species, high content of doped nitrogen as well as hierarchical micro-mesopores, which induce to expose more active sites for catalysis. Owing to the structure-enabled acidic stability, Fe-N@BC efficiently retains its activity as well as its structural stability after several cycles of reactions. This work provides a new approach to construct Fe, N -doped biochar as an effective catalyst for the detoxification of organic and inorganic pollutants.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Vietnam Journal of Chemistry
·
2021
·Vol. 59
·期 6
·813-822
·
IF 0
Nguyen Trung Dung,Vu Dinh Thao,Nguyen Nhat Huy
In this study, the CuCoFe-layered double hydroxide was employed for the degradation of glyphosate in water via peroxymonosulfate (PMS) activation. Scanning electron microscopy, X-ray powder diffraction, energy-dispersive X-ray spectroscopy, Fourier-transform infrared spectroscopy, and Brunauer-Emmett-Teller analyses were used to characterize the material. The effects of the catalytic system, initial solution pH, and catalyst and PMS dose on the degradation efficiency of glyphosate were investigated. The results indicated that after 6 min the CuCoFe-LDH/PMS system can degrade 99.54 % of glyphosate (100 mg/L) using 100 mg/L of CuCoFe-LDH, 200 mg/L of PMS, and pH 11. In addition, radical quenching experiments prove that the reactive oxygen species (e.g., SO 4 ●- , HO ● , O 2 ●– , and 1 O 2 ) are formed and SO 4 ●- plays a decisive role in glyphosate degradation. Moreover, the CuCoFe-LDH catalyst is reusable and stable with a glyphosate removal efficiency of 90.34 % after five continuous degradation cycles.
✓ 已验证
产品关联
DOI
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Peizhen Yang,Songrong Li,Liang Xiaofu,An Xiaojing,Dongfang Liu,Wenli Huang
The degradation of organic contaminants via traditional radical-dominated advanced oxidation processes (AOPs) under high salinity conditions was limited due to side reactions between coexisting inorganic anions and radicals. Herein, a nonradical oxidation process via peroxymonosulfate (PMS) activation by CuO/MXene for treating high-salinity organic wastewater was developed. Rapid removal efficiency of target pollutant carbamazepine (CBZ) was significantly enhanced to 95.88% within 20 min by CuO/MXene under high salinity conditions (NaCl, 200 mM), compared to the efficiency of 4.30% exhibited by PMS alone. Besides, CBZ maintained a higher removal efficiency of > 81.04% in complex highly saline wastewater composed of eight common inorganic anions. Radical quenching experiments and electron paramagnetic resonance (EPR) analysis confirmed that radical and nonradical oxidation processes were involved in the catalytic process. However, singlet oxygen ( 1 O 2 ) was identified as the primary reactive species, and its contribution rate to CBZ degradation was > 73.58% in a wide pH range (3.0-9.0). The oxygenated functional groups and the interaction between CuO/MXene and PMS facilitated the production of 1 O 2 . The degradation pathway was proposed based on the detection of intermediates. This work provided a new inspiration for the decontamination of organic contaminants under high salinity conditions via a nonradical oxidation process.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Chengcheng Xu,Jing Deng,Shijun Zhu,Xiao Ling,Songtu Shen,Hongguang Guo,Qiongfang Wang,Xueyan Li
The introduction of ascorbic acid (AA) into Fe(III)/PS system exhibited extremely high activity on the removal of N,N-diethyl- meta -toluamide (DEET) and other pollutants. The removal efficiency of DEET within 30 min reached 90.13%, its dynamic curve obeyed second-order kinetic model and the k obs was calculated to be 0.150 L·mg −1 ·min −1 . Compared with other reducing agents, AA was tested to be the most suitable. The optimal dosages of Fe(III), PS and AA were tested to be 0.1, 1.0 and 0.5 mM, respectively. Furthermore, the introduction of AA extended the working pH to 2.5–9.3. Common anions posed different degrees of inhibition on DEET degradation at relatively high concentration, while a small dosage of HCO 3 − (<1 mM) abnormally exerted a positive role. In terms of reaction mechanism, scavenger experiment and EPR observation illustrated that ·OH and ·SO 4 − dominated DEET degradation, yet slight Fe(Ⅳ) was also found during the reaction, which indicated that Fe(Ⅳ) may also contribute to DEET removal. Different from the rapid consumption of Fe(II) in Fe(II)/PS system, Fe(II) in Fe(III)/PS/AA system entered a dynamic equilibrium state in the later stage of the reaction, which can decompose PS to form ·SO 4 − continuously. Furthermore, the reduction and chelation ability of AA both functioned a key role. According to the degradation intermediates identified by LC-MS analysis, the degradation pathways of DEET could be divided into two directions, which covered opening benzene ring and removing side chain.
✓ 已验证
产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2021
·
IF 0
Shenyu Lan,Chuan Yu,Enya Wu,Mingshan Zhu,Dionysios D. Dionysiou
Ambient water motions presented in urban drainage systems is a rich source of renewable mechanical energy. Harvesting this energy to trigger the generation of reactive oxygen species (ROS) for water purification is a desirable yet underexplored solution. Herein, the water flow from a spiral reactor to simulate pipeline drainage was utilized to provide mechanical energy to power itself to initiate the piezo-response of molybdenum disulfide (MoS2) that was added into water flowing in the reactor. The piezocatalytic degradation efficiency of benzothiazole by MoS2 reached 94.8% after 24 cycles (ca. 144 s), which was 8.8 and 4.9 times higher than that of quiescent solution of MoS2 and non-piezoelectric commercial MoS2, respectively. Furthermore, the water flow-driven system can be extended to degrade different kinds of organic contaminants, including benzotriazole and various antibiotics (enrofloxacin, ciprofloxacin, metronidazole, etc.). All target pollutants were degraded with electric energy per order EEO in the range of 0.0161 to 0.0616 kW h/m3. In this process, the running water from the spiral reactor drove MoS2 to generate piezoelectric charges, which in turn reacted with dissolved oxygen and water to generate ROS including the hydroxyl radical, superoxide anion, and singlet oxygen to decompose the target pollutants. The system retained piezo-degradation efficiencies (>80%) in different aqueous matrices including rainwater, saline water, and pharmaceutical sewage and could be reused four times maintaining a good performance (>90%). This investigation provides a facile self-powered piezocatalytic process by harnessing ambient energy from the water flow of simulated water drainage to purify wastewater.
✓ 已验证
产品关联
DOI
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Wenjie Wu,Liang Bai,Yenan Song,Yuanting Su,Kai Jiang,Haitao Sun,Guangyin Zhen,Yan Shen,Qinghong Yuan,Zhuo Sun
Graphene-based catalysts have been widely applied for catalytic ozonation. However, as it is difficult to obtain graphene with high structural precision, it is currently unfeasible to comprehend the relationships between the intrinsic structure of the layered carbon catalysts with its catalytic activities. Here, an advanced plasma-assisted etch strategy was used to fine tune the ozonation activity of monolayered graphene films by tailoring the defect types. Raman mapping indicated that the defects of the as-prepared monolayered graphene films were predominantly sp3, vacancy, and boundary-type defects, respectively. The roles and contributions of these active defects in manipulating the oxidative potential of monolayered graphene films were revealed by quenching experiments, electron paramagnetic resonance results, and density functional theory calculations. The catalytic results showed that the monolayered graphene films with boundary-like defects exhibited the best catalytic performance toward the degradation of sulfamethoxazole. This work contributes new insights into the design of high-efficiency carbonaceous catalysts by structuring additional defective sites.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
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.
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
·
2023
·
IF 12.8
Yun-Jie Wang,Chen-Xuan Li,Yan Meng,Zhi-Yan Guo,Shuo Cui,Xian-Zhong Fu,Hou-Qi Liu,Wen-Qi Xia,Wen-Wei Li
Low-pressure catalytic membranes allow efficient rejection of particulates and simultaneously removing organics pollutant in water, but the accumulation of dissolved organic matters (DOM) on membrane surface, which cover the catalytic sites and cause membrane fouling, challenges their stable operation in practical wastewater treatment. Here we propose a ferric salt-based coagulation/co-catalytic membrane integrated system that can effectively mitigate the detrimental effects of DOM. Ferric salt (Fe 3+ ) was in the wastewater, serving both as DOM coagulant to lower the membrane fouling and as a co-catalyst with the membrane-embedded MoS 2 nanosheets for perxymonosulfate (PMS) activation and pollutant degradation. The membrane functionalized with 2H-phased MoS 2 nanosheets showed improved hydrophilicity and fouling resistance relative to the blank polysulfone membrane. Attributed to the DOM coagulation and co-catalytic generation of surface-bound radicals for decontamination at membrane surface, the catalytic membrane/PMS/ Fe 3+ system showed much less membrane fouling and 2.6 times higher pollutant degradation rate in wastewater treatment than the catalytic membrane alone. Our work imply a great potential of coagulation/co-catalytic membrane integrated system for water purification application.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Longjie Liu,Zeyang Lu,Wanling Cai,Gary Owens,Zuliang Chen
Reduced graphene oxide/iron nanoparticles (rGO/FeNPs) synthesized by the chemical method have been used in Fenton oxidation of organic contaminants , yet little is known about biosynthesized rGO/FeNPs using green tea extract (GT) as how to activate persulfate in sulfate radical-based advanced oxidation processes . In this study, rGO/FeNPs were used to activate peroxydisulfate (PDS) for 17β-estradiol (βE 2 ) and estriol (E 3 ) removal. The rGO/FeNPs-PDS system removed 83.6% of βE 2 and 62.5% of E 3 within 240 min, which was confirmed by a combination of adsorption and degradation via both radical and non-radical pathways. Four main reactive species in βE 2 and E 3 degradation were observed, i.e., hydroxyl radical (·OH), sulfate radical (SO 4 ·− ), singlet oxygen ( 1 O 2 ) and electron transfer , with the respective contributions of ·OH (32.9 and 34.7%), SO 4 ·− (16.1 and 19.7%), 1 O 2 (12.2 and 14.1%) and electron transfer (8.0 and 7.2%). Analysis of X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FTIR), Electron Paramagnetic Resonance (EPR) and electrochemical measurements all indicated that beside the well-known role of Fe, C O from rGO through the generation of ·OH, SO 4 ·− , 1 O 2 and electron transfer, as well as GT through electron transfer also participated in the activation of PDS. Finally, the degradation pathways of βE 2 /E 3 were proposed. Overall, this study provides a new insight into the biosynthesis of rGO/FeNPs to activate PDS for the oxidation of mixed emerging contaminants .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2023
·
IF 7.4
Yanqing Shi,Cai Guo,Huajing Zhou,Liang He,Shaoyun Shan,Tianding Hu
Rational modulation of the local electron density of Cu active site is the key to improve the efficient transfer hydrogenation (CTH) of furfural (FF) on the surface of catalysts with low Cu-loadings. In this paper, a CuMgAl/LSC catalyst with lower Cu content (<3.5 % wt ) was prepared by using porous biochar as a carrier and exploiting the local dispersion and electron-modulation effects of structural elements of hydrotalcite laminates. CTH experiments showed that the conversion of FF and the selectivity of FA could reach more than 99.0 % in isopropanol solution at 170 °C and within 1 h. Catalyst characterization and density functional theory (DFT) calculations demonstrated that the Cu(I) species was the main active site during the CTH process of FF. Doping laminate metals (i.e., Mg, Al) can not only form electron-rich centers by local electron modulation of the active site through the coordination structure of Cu-O-M, lowering its D-band center and achieving higher catalytic activity; Due to the Jahn-Teller effect, the local spatial misalignment of Cu sites formed, which can reduce the risk of over-hydrogenation and improve the FA selectivity. In addition, it can be also found that the Coulomb tractive force of reactive intermediates can lead to the crystal surface reconstruction and structure deterioration of Cu species. The new discovery of the deactivation mechanism can provide a reference for the future design of copper-based catalysts in CTH process of FF.
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 48
·期 4
·1757-1770
·
IF 3.3
Ling Tao,Jiepu Zhang,Fangke Yu
In this study, in order to achieve efficient activation of persulfate, we added MoS2 as a co-catalyst to the iron, cobalt and nitrogen modified biochar (Fe–Co–N–BC) catalytic system. Analytical methods such as scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) demonstrated that the MoS2/Co–Fe–N–BC catalytic materials were successfully prepared. In the MoS2/Fe–Co–N–BC/PMS system, 97.5% of PFOA was removed within 180 min with Kobs of 0.074 min−1. Composites with different mass ratios of MoS2 and Co–Fe–N–BC/PMS in the non-homogeneous PMS system both exhibit excellent catalytic efficiency for TOC removal. In particular, MoS2/Fe–Co–N–BC obtained extraordinary catalytic efficiency through synergistic radical (SO4˙−, ˙OH) and non-radical (1O2, FeIV and FeV) processes, which was proved by the quenching experiments and the EPR testing. The analysis of the activation mechanism reveals that the three redox ion pairs Fe2+/Fe3+, Co2+/Co3+ and Mo4+/Mo6+ simultaneously participated in the activation of PMS, realizing multi-path electron transfer. And MoS2 played an excellent co-catalysis role in promoting the cycling of the valence states of the ions. Compared to Fe3+ and Co3+, the low valence states of Fe2+ and Co2+ can activate PMS more rapidly and produce more ˙OH and SO4˙−. However, the recycling efficiency of Fe2+ and Co3+ in the Fe–Co–N–BC system is low, and the presence of MoS2 improves the efficiency of Fe3+ and Co3+ reduction to Fe2+ and Co2+, respectively. The possible degradation pathways of PFOA were proposed. This study provides some references for the design of polymetallic-doped catalysts to degrade difficult-to-degrade organic pollutants.
✓ 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）