JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Zhenzhan Xu,Xiaolin Ma,Fengting He,Mingjie Lu,Jinqiang Zhang,Shuaijun Wang,Pei Dong,Chaocheng Zhao
Electro-Fenton (EF) is considered to be an effective technology for the purification of organic wastewater containing antibiotics, but the construction of accessible and efficient heterogeneous EF catalytic materials still faces challenges. In this study, an iron foam-derived electrode (FeO x /if-400) was prepared by a simple method (chemical oxidation combined heat treatment). The fabricated electrode presented great EF degradation efficiency under wide pH range (almost completely removing 50 mg L −1 TNZ within 60 min) and maintained great stability after consecutive operation (>95% removal after six cycles). Also, the FeO x /if-400 electrode showed good purification ability for pharmaceutical wastewater as evaluated by the quadrupole time-of-flight mass spectrometry and the three-dimensional excitation-emission matrix fluorescence spectroscopy . Based on experimental results, characterization analysis, and density functional theory (DFT) calculations, the EF reaction mechanism of FeOx/if-400 electrode and the organics degradation pathways in simulated and real matrices were proposed. Significantly, the biotoxicity assessment of the degradation intermediate products was revealed by ECOSAR software and relative inhibition of E. coli , which fully proved the environmental friendliness of the EF process by the FeO x /if-400 cathode. This work provides a green and effective EF system, showing a promising application potential in the field of organic wastewater treatment containing antibiotic contaminants.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Huanxin Zhao,Yuqi Liu,Dan Wu,Huixin Yu,Xuejun Zhang,He Wang,Xiaoyuan Shang,Mingyi Lv
The development of single atom catalysts (SACs) with superior catalytic performance is a long-term goal for peroxymonosulfate (PMS) activation in advanced oxidation processes (AOPs). A novel SACs that single Co atoms anchored on CuO with enriched oxygen vacancies (O v ) is synthesized successfully by choosing a metal oxide as the carrier creatively. 100% of tetracycline (TC) can be removed by Co–CuO (O v )/PMS system within 3 min. The corresponding reaction rate constant is 3.1068 min −1 , which is much higher than that of CuO (O v ), ZIF-CoN 4 -C, Co–CuO (without O v ) and Co NP –CuO (O v ), respectively. Co(II) is the primary source of radical pathway (·OH and SO 4 · - ), and its regeneration is promoted by Cu(Ⅰ). The enriched O v is the major contribution to the nonradical pathway, which promotes the singlet oxygen ( 1 O 2 ) generation together with accelerates the electron transfer from TC to catalyst-PMS*. Besides, the Co–CuO (O v ) exhibits an excellent stability and anti-interference capability. This study highlights a novel strategy to promote PMS activation by incorporating the single metal atoms on a metal oxide carrier with defects to accelerate the redox of dominate metal and stabilize the metal atoms simultaneously, which may inform the design for the next generation of SACs in AOPs.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Xiupeng Yue,Yaping Zhang,Yongping Shan,Kai Shen,Wentao Jiao
Electrokinetic transport followed by electrical resistance heating activation of peroxydisulfate is a novel in situ soil remediation method. However, the strategy of electrokinetic transport coupled with electrical resistance heating and the comprehensive evaluation of restored soil need to be further explored. In this study, a lab-scale simulation device for in situ electrokinetic transport coupled with electrical resistance heating activation of peroxydisulfate was constructed to monitor the transport and transfer of peroxydisulfate, target pollutants, and process parameters, and the physicochemical properties and bacterial community of treated soil were evaluated. The results showed that adding 10 wt% peroxydisulfate to both the anode and cathode resulted in the optimized transfer rate and cumulative concentration of peroxydisulfate under electrokinetics. After 8 h, the cumulative concentration of peroxydisulfate reached 66.15– 166.29 mmol L −1 , which was attributed to the migration of a large amount of S 2 O 8 2− from the cathode to the soil under electromigration . Additionally, the anodic interfacial electric potential was improved, which was more conducive to electroosmotic transport of peroxydisulfate from the anode chamber. By alternating electrokinetic transport and electrical resistance heating activation of peroxydisulfate for two cycles, the phenanthrene degradation efficiency in four evenly distributed wells between electrodes reached 75.4 %, 87.6 %, 92.3 %, and 94.4 %. With slight variations in soil morphology and structure, the electrokinetic transport coupled with electrical resistance heating activation of peroxydisulfate elevated the soil fertility index. The abundance and diversity of bacterial communities in treated soil recovered to above the original soil level after 15 days. Our findings may support the application of electrokinetic transport coupled with electrical resistance heating activation of peroxydisulfate as a promising green ecological technology for the in situ remediation of organic-contaminated soil.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Mudassir Habib,Meesam Ali,Tehreem Ayaz,Ali Shan,Guilu Zeng,Zhengyuan Zhou,Shuguang Lyu
Rapid growth and industrialization have become a major threat to water contamination with carcinogenic chlorinated hydrocarbons such as trichloroethylene (TCE). Therefore, this study aims to assess the TCE degradation performance through advanced oxidation process (AOP) using catalyst FeS 2 in combination with oxidants persulfate (PS), peroxymonosulfate (PMS), and hydrogen peroxide (H 2 O 2 ) in PS/FeS 2 , PMS/FeS 2 , and H 2 O 2 /FeS 2 systems, respectively. TCE concentration was analyzed using gas chromatography (GC). The results found the trend for TCE degradation by the systems was PMS/FeS 2 >PS/FeS 2 >H 2 O 2 /FeS 2 (99.84, 99.63, and 98.47%, respectively). Degradation of TCE was analyzed at different pH ranges (3–11) and maximum degradation at a wide pH range was observed for PMS/FeS 2 . The analysis using electron paramagnetic resonance (EPR) and scavenging tests explored responsible reactive oxygen species (ROS) for TCE degradation and found that HO• and SO 4 − • played the most effective role. The results of catalyst stability showed PMS/FeS 2 system the most promising with the stability of 99, 96 and 50% for the first, second and third runs, respectively. The system was also found efficient in the presence of surfactants (TW-80, TX-100, and Brij-35) in ultra-pure water (89.41, 34.11, 96.61%, respectively), and actual groundwater (94.37, 33.72, and 73.48%, respectively), but at higher reagents dosages (5X for ultra-pure water and 10X actual ground water). Furthermore, it is demonstrated that the oxic systems have degradation capability for other TCE-like pollutants. In conclusion, due to its high stability, reactivity, and cost-effectiveness, PMS/FeS 2 system could be a better choice for the treatment of TCE contaminated water and can be beneficial for field application.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Surfaces and Interfaces
·
2023
·
IF 6.2
Yanxi Chen,Jieqiong Kang,Zhenjie Li,Mingshan Zhu,Renli Yin
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) have raised wide attention due to the efficient degradation of pollutants. However, the low efficiency in PMS activation is still a challenge for practical application. Herein, an economic Co 2 P catalyst with surface-active center was constructed for PMS activation to induce fast degradation of carbamazepine (CBZ). Particularly, the removal ratio of CBZ in the Co 2 P/PMS system could achieve at 98% in 10 min, accompanied with the removal ratio of total organic carbon (TOC) reached 60% in 60 min. Characterizations indicated that interfacial transformation of Co δ+ to Co 2+ promoted electron-rich Co center formation, which supplied electrons for PMS to produce SO 4 • – and •OH that were responsible for the efficient degradation of CBZ. Furthermore, potential interferences from the real water matrix, dosage of the catalyst and PMS, and variation of initial pH were carefully studied for practical applications. Besides, three possible degradation pathways of CBZ were proposed and the toxicity of the products was predicted. However, the generation of more toxic intermediates was found in the system for the radical (SO 4 • – and •OH) oxidation is a non-selective oxidation process. Particularly, we expect that this work can provide new insights into the regulation of reaction mechanisms, degradation routes and safe transformation in PMS-AOPs for wastewater treatment .
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xinxin Li,Linchuan Cong,Yupeng Wu,Nan Lin,Fangbing Liu,Deyuan Xin,Fuyu Han,Jin Yang,Weitong Chen,Haibo Lin
Electrochemical methods for catalytic furfural conversion have drawn significant interest in both academic and industrial research communities. Paired electrocatalytic conversion has been identified as a promising strategy for reducing energy consumption and promoting carbon neutrality. To optimize product distribution and conversion efficiency, we have developed a divergent paired electrochemical upgrading approach for furfural in acidic environments, with a focus on prioritizing strong gas evolution reactions and product transformations. The high electrocatalytic activity of CuSn/CuF@Cu prepared by electrodeposition can effectively inhibit the hydrogen evolution. The performance of the electrocatalysts and the pathways of electrocatalytic hydrogenation (ECH) of furfural to 2-methylfuran (MF) were investigated by combination of experiments and the density functional theory (DFT) calculations. A stable Ti/PbO 2 electrode with high oxygen evolution overpotential was prepared for anodic electrocatalytic oxidation (ECO) and the product transformation route was described. The conversion of furfural to maleic acid (MA) and MF in acidic environment was successfully achieved. In the paired electrosynthesis system, the electrons generated from anodic ECO of furfural are utilized in valuable and controllable cathodic ECH. It significantly and continuously reduces the power cost associated with renewable energy sources and further promotes the development of biomass electrochemical conversion.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Qingqing Li,Zhujuan Ren,Yutong Liu,Chibin Zhang,Jiadi Liu,Rong Zhou,Yuanqing Bu,Feifei Mao,Hua Wu
Developing hierarchical and efficient catalysts with multiple active sites to activate peroxymonosulfate (PMS) for the degradation of persistent organic contaminants is crucial, whereas it's still a challenge. Herein, a novel petal-like N -doped porous carbon embedded with ultrafine cobalt oxide nanoparticles (NPs) (named as Co 3 O 4 /NC) was unprecedentedly fabricated via the pyrolysis of N -enriched Co-MOF (named as Co-TA), where the unique hierarchical structure, rich active sites and large specific area were contributed to improve the excellent catalytic activity toward tetracycline hydrochloride (TCH). As expected, the removal efficiency of TCH in Co 3 O 4 /NC/peroxymonosulfate system was 96.4 % within 30 min, extraordinary superior to direct air-calcining nano-Co 3 O 4 , commercial Co 3 O 4 and Co-TA, in which the kinetic constant was 10.4 times higher than pure Co-TA. Besides, above 97 % removal efficiency of TCH was maintained over a wide pH range of 5–9, and 71 % of total organic carbon (TOC) could be eliminated. The TCH degradation was mainly characterized by the coexistence of multiple active substances using EPR analysis, where SO 4 · − and 1 O 2 were the dominant contributors. The degradation pathways of TCH were also clarified based on theoretical calculation and HPLC-TOF-MS 2 data. This work can extend the application of metal–organic frameworks (MOFs)-derived nanocatalysts in the environment field, and may offer a promising metal oxide heterogeneous catalyst for the rapid elimination of persistent organic pollutants by sulfate radical-based advanced oxidation processes (SR-AOPs).
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2022
·
IF 8.634
Jun Zhang,Chengyu Li,Sheng Hu,Jing Gu,Haoran Yuan,Yong Chen
In the present study, CuO and Cu 2 O were employed in H-transfer transformation of bio-based furfural (FFR) using methanol as both the solvent and an in-situ hydrogen source , to clearly elucidate the catalytic mechanism of copper oxides (CuO x , x = 0.5, 1) during the reaction. A number of characterization techniques including XPS , H 2 -TPD, in-situ FTIR, etc., were undertaken to track the state of copper species. Owing to the synergistic effect of in-situ generated H 2 , Cu 0 species and CuO x derived Brønsted/Lewis acid sites, FFR could be efficiently hydrogenated into FA and subsequently deoxygenated into MF in methanol. The combined results from in-situ characterizations and experiments show that the FFR-to-FA (FA, furfuryl alcohol) and FFR-to-MF (MF, 2-methylfuran) conversions largely depended on the hydrogen production capability from methanol reforming and FFR adsorption strength over CuO x . Density functional theory (DFT) calculations demonstrated that the CuO(200) surface revealed lower free energy and energy barriers for methanol reforming and FFR transfer hydrogenation. This study provides a promising guidance for reasonably designing copper-based materials in the hydro-upgrading of bio-based unsaturated molecules into value-added chemicals in methanol without external H 2 supply.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POLYMERS AND THE ENVIRONMENT
·
2022
·Vol. 30
·期 12
·5252-5262
·
IF 4.705
Cheng Bing-Xu,Lu Chen-Chen,Li Qing,Zhao Si-Qi,Bi Chang-Shun,Wu Wei,Huang Chong-Xing,Zhao Hui
A type of waterborne polyurethane (WPU) with excellent self-healing and recyclable properties was successfully prepared by introducing Diels–Alder (DA) reaction groups into it. FT-IR was used to verify the successful synthesis of samples and the retro-DA reaction in the WPU-DA films. It was found that the self-healing efficiency of the WPU-DA-4/4 films was 72.8%. After four cycle times, the self-healing efficiency could still achieve 49.7%. Moreover, the WPU-DA film could be applied as the positive friction layer to prepare a triboelectric nanogenerator (TENG). Working in contact-separation mode, the electrical outputs with 2 × 2 cm 2 area can reach 58 V, 3.2 µA, 17.6 nC, respectively. It is also interesting to find that the electrical output properties of the TENG after damage-healed can be restored to more than 90% of the original one. The cross-linked WPU had good reprocessability and had great potential application prospects in intelligent materials.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yulong Yuan,Minghua Nie,Caixia Yan,Leliang Wu,Wenbo Dong,Mingjun Ding,Peng Wang
This study investigated for the first time the potential of the novel combination of peroxymonosulfate (PMS) and carbonate (CO 3 2− ) toward bisphenol S (BPS) under solar light irradiation. Compared with the Na 2 CO 3 /PMS and solar/PMS system, the solar/Na 2 CO 3 /PMS system significantly reduces the time required for the degradation of BPS. The excellent removal performance is possible due to the synergistic effect between enhanced light absorption and PMS activation, which accelerated the decomposition of PMS to generate more reactive oxygen species. Scavenging tests and electron paramagnetic resonance analysis revealed that the singlet oxygen ( 1 O 2 ) was the dominant oxidant formed and contributed to BPS elimination with a small proportion of superoxide anion radical (O 2 •– ), rather than sulfate radical (SO 4 •− ) and hydroxyl radical (HO•). The addition of Cl − could promote the degradation of BPS, but the addition of HA and a higher HCO 3 − concentration inhibited this process. The presence of SO 4 2− and NO 3 − slightly promote the degradation of BPS. Besides, the solar/Na 2 CO 3 /PMS system represented significant degradation efficiency in a wide initial pH range (5.02–10.96). Such a system is favorable for the application in actual water matrices such as domestic wastewater, river water, lake water, and tap water. Meanwhile, based on the intermediates identified, the possible degradation pathways of BPS were proposed. In addition, most of the degradation intermediates of BPS were less toxic to different organisms than the parent compound. Moreover, the highly efficient degradation of several typical organic contaminants was also achieved using the solar/Na 2 CO 3 /PMS system under simulated and natural solar light irradiation. This study provides a novel idea and demonstrates the great potential for the elimination of organic pollutants in water.
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Yangke Long,Shixin Huang,Jianlin Sun,Dan Peng,Zuotai Zhang
Highly dispersed iron nanoclusters on carbon (FeNC@C) hold great promise for wastewater purification in Fenton-like reactions. The microenvironment engineering of central Fe atom is promising to boost the activation capacity of FeNC@C, which is however remains a challenge. This study developed a self-sacrificed templating strategy to S, N-codoped carbon supported Fe nanoclusters (FeNC@SNC) activator and find the key role of sulfur heteroatoms in regulating the electron structure of Fe sites and final activation property. Investigations revealed that the FeNC@SNC composite exhibited unusual bifunctional activity in both peroxymonosulfate (PMS)- and periodate (PI)-based Fenton-like reactions. We also offered insights into the differences between the degradation of organics by the FeNC@SNC/PMS and FeNC@SNC/PI systems. Specifically, under identical conditions, the FeNC@SNC/PMS system delivered a higher oxidation capability and stronger resistance to nontarget matrix constituents, but showed more severe Fe leaching than the FeNC@SNC/PI system. Furthermore, while mediated electron-transfer process was identified as the major route for pollutant decomposition in both systems, the high-valent Fe-oxo species [Fe (IV)] was the auxiliary reactive species found only in the FeNC@SNC/PMS system. Based on these findings, our results provide profound insights into the design of active and durable Fe-based activators toward highly efficient Fenton-like reactions.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ATMOSPHERIC ENVIRONMENT
·
2022
·
IF 5.755
Jinwen Li,Qingcai Chen,Dongjie Guan
Atmospheric aerosols contain organic compounds that can form triplet organics ( 3 C*) excited by sunlight, which plays a significant role in the aging process of aerosols. The formation characteristics of 3 C* of aerosol components with different polarities were investigated, including highly polar water-soluble matter (HP-WSM), humic-like substances (HULIS), and methanol-soluble matter (MSM). Carbon analysis, probe method and electron paramagnetic resonance were used to investigate the photochemical properties of ambient samples. The coupling effect of generation of 3 C* and reactive oxygen species (ROS) between different aerosol components was also examined. The results showed that the 3 C* generation characteristics are strongly dependent on the polarity of these components. HULIS has the strongest generation ability of 3 C*, and the MSM contributes the most to the total generation of 3 C*. It was found that the high-energy triplet states ( E T ≥ 250 kJ mol −1 ) of HULIS and HP-WSM components account for up to 80% of the water soluble components. These 3 C* have an important contribution to the photochemically generation of ROS, and the generated ROS of different components are also different, which is determined by the chromophore composition of complex organic compounds. A tyrosine-like chromophore is the main substance leading to the formation of water-soluble 3 C*, while the highly oxidized HULIS chromophore plays a leading role in the water-insoluble component. This study also found that there is a coupling effect between HP-WSM and HULIS on 3 C* and ROS generation. The generation rate of 3 C* increases by about 40% after mixing, but the generation of 1 O 2 is severely reduced. In general, this study provided deep insights into the generation characteristics and aging impact of the triplet state on atmospheric aerosols.
✓ 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）