SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Jiayu Feng,Fei Wang,Chi Wang,Kai Li,Ping Ning,Xin Sun,Lijuan Jia
A series Ce m Cu n O x /HZSM-5 sorbents were introduced to remove PH 3 in low-temperature and low-oxygen environments. The effects of copper loading and cerium doping on the adsorption–oxidation performance of the sorbents were investigated. Experimental results showed that doping with 1 wt% of cerium (Ce 1 Cu 30 O X /HZSM-5) could significantly improve the performance of the sorbent. The PH 3 breakthrough capacity was identified as 114.36 mg(PH 3 )•g sorbent -1 . In addition, after three thermal regeneration cycles, the sorbent still has ideal performance. X-ray diffractometer (XRD) and X-ray photoelectron spectroscopy (XPS) analyses exhibited that CuO was the main active species, and Ce-doping can increase the chemisorption oxygen on the surface of the sorbent. BET results demonstrated that the introduction of cerium could improve the specific surface area and pore volume of sorbent. Hydrogen temperature-programmed reduction (H 2 -TPR) and scanning electron microscope (SEM-EDS) indicated that cerium species played an important role in uniformly dispersing copper species on the HZSM-5 surface and improving the oxidation performance of sorbent. Moreover, the reaction products and mechanisms were also investigated by XRD, XPS, and in-situ FTIR spectra. The results indicated that the consumption of CuO and the accumulation of phosphorus species (e.g., P, P 2 O 5 , and Cu 3 P) on the surface and inner pores of the sorbent were the primary reasons for the deactivation of the sorbent.
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
·
2024
·
IF 8.1
Yeshuang Wang,Mingxian Duan,Zhelin Su,Chao Yang,Yuxiao Wang,Tian Kou,Jiawei Kou,Huiling Fan
Cu–1,3,5-benzenetricarboxylate (Cu–BTC) exhibited potential for hydrogen sulfide (H 2 S) removal, however, its sulfur capacity is limited due to it relies only on the adsorption reaction path. Herein, a series of Fe-doped Cu–BTC materials (denoted as x Fe–Cu–BTC) were synthesized to enhance H 2 S removal capacity via a adsorption–oxidation bifunctional synergism mechanism. The prepared materials were characterized using various techniques, and their H 2 S removal performance was measured under dry and ambient conditions. The experimental results demonstrated that the 18%Fe–Cu–BTC shown the optimal breakthrough sulfur capacity of 122.8 mg S/g, marking a 2.1-fold and 10.3-fold improvement over pure Cu–BTC and Fe–BTC, respectively. The characterization analyses revealed that the Cu 2+ active sites initially react with H 2 S to form CuS, while the incorporated Fe 3+ sites trigger the oxidation of CuS, yielding elemental sulfur, Cu 2+ and Fe 2+ . The resultant Cu 2+ and Fe 2+ further engage in reactions with H 2 S to form CuS and FeS, thereby enhancing the H 2 S removal capacity via dual reaction pathways of adsorption and oxidation. Additionally, appropriate Fe doping increased the specific surface area and pore volume of Cu–BTC, which exposed more active sites and improved molecular diffusion. Based on the obtained findings, a plausible desulfurization mechanism involving adsorption and oxidation synergism for remove H 2 S was proposed.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Huimin Hu,Qiwu Zhang,Chao Wang,Min Chen,Qian Wang
Soluble Fe(IV) has been proposed as primary reactive species in advanced oxidation technology, however, Fe(IV) in solid-state oxidant is rarely reported. This study reports a facile synthesis of CaMn 1-x Fe x O 3 (0.1 ≤ x ≤ 0.7) containing high ratio of Fe(IV) by low-temperature calcination of the ball milling precursor and evaluates its adsorption-oxidation performances of As(III). Although Fe(IV) and Mn(IV) inside CaMn 1-x Fe x O 3 both act as electron acceptor species, with × for Fe ratio increased, charge transport capability and oxidation performance of As(III) to As(V) of the CaMn 1-x Fe x O 3 materials can be raised dramatically with more iron incorporated. With sample CaMn 0.3 Fe 0.7 O 3 , the maximal adsorption capacity for As(III) reaches 120.78 mg/g with the ratio of oxidized As(V) as high as 86.4% in a wide pH range of 2 ∼ 10. More importantly, excellent cyclability and stability are observed and 83% of the initial adsorption-oxidation capacity still retains even after 5 cycles, and leaching concentrations of the metal ions (Fe/Mn) are far below the emission standard (0.5 mg/L). With an aid of environment-friendly ball milling process, the idea to obtain high valent Fe by a simple incorporation into a specific crystalline structure of perovskite offers a new approach for synthesizing active oxidizing species of Fe(IV). Further, the synthesis of solid oxidants would transform the redox reactions from a liquid phase reaction process to a solid–liquid reaction process, which could be conducive to the occurrence of in-situ oxidation and fixation of pollutants to reduce their mobility, and much contribution is expected to the development of advanced oxidization process in wastewater treatment using the easy handling solid-state oxidants.
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
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Jiayu Feng,Fei Wang,Chi Wang,Kai Li,Xin Sun,Ping Ning
In this study, an NH3 plasma-treated Cu/HZSM-5 sorbent was introduced to simultaneously remove H2S and PH3 in low-temperature and low-oxygen environments. The effects of the Cu loading amounts, modification methods, and plasma-treatment conditions on the adsorption–oxidation performance of the sorbents were investigated. From the performance test results, the sorbent treated by NH3 plasma with the specific energy input (SEI, electrical input energy to the unit volume of gas) value of 1 J·mL–1 (Cu/HZSM-5-[S1]) was identified as having the highest breakthrough capacities of 108.9 mg S·g–1 and 150.9 mg P·g–1 among all of the materials tested. After three times of regeneration, the sorbent can still maintain the ideal performance. The results of Fourier transform infrared (FT-IR) spectroscopy and CO2 temperature-programmed desorption (CO2-TPD) indicated that the NH3 plasma treatment can introduce amino groups (functional groups) onto the sorbent surface, which greatly increases the number and strength of the basic sites on the sorbent surface. Results of N2 adsorption/desorption isotherms and scanning electron microscopy–energy dispersive spectroscopy (SEM–EDS) showed that the morphology of the sorbent changed after the plasma treatment, which exposed more active sites (copper species). In situ IR spectra showed that the amino groups are continuously consumed during the reaction process, indicating that these amino groups can help sorbents to capture gas molecules. Moreover, X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses indicated that CuO is the main active species and the consumption of CuO and accumulation of the reaction products on the surface and inner pores of the sorbent are the primary reasons for the deactivation of the sorbent.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Junzhuo Cai,Shuhong Liu,Yu Bon Man,Xiaoxun Xu,Zhanbiao Yang,Changlian Xu,Guiyin Wang,Chengyi Huang,Gang Yang,Guochun Lv,Xin Qi,Ming Hung Wong,Zhang Cheng
The pretreatment of tetracycline production wastewater (TPW) is of great environmental significance in improving its biodegradability and reducing the risk of resistance genes. A novel sequential adsorption-oxidation pulses (SAOP) electrochemical method was proposed, and 95.6 % of tetracycline hydrochloride (TCH) was removed in 60 min with the enhancement of BOD 5 /COD Cr from 0.18 to 0.44. The results of in-situ electrochemical electron magnetic resonance and electro-adsorption experiments indicate that the mild negative pulse makes the targeting TCH electromigration and adsorb on an electrode surface, and then the positive pulse forces TCH to be oxidized. Presumable mechanisms for enhancing TCH removal was proposed as (1) ameliorative mass transfer, (2) the pre-adsorbed TCH modifies the electrode surface to facilitate subsequent oxidation or ROS generation. The pretreatment of SAOP reduces the toxicity of TPW on activated sludge and decreases its inhibition of cell activity. Finally, considering the intended use, the performance of SAOP was validated in actual TPW. The pretreatment results are achieved in terms of removal and biodegradability, as well as reduction of resistance genes’ accumulation in the biochemical unit. This research provides a novel method for solving the contradiction between mass and charge transfer in the electrochemical oxidation of positively charged pollutants and a reproducible readily method for the electrochemical pretreatment of recalcitrant antibiotic production wastewater.
研究领域:
环境科学
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废水处理
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抗生素污染控制
✓ 已验证
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 91
·88897-88903
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IF 3.289
Na Wang,Xiaofeng Li,Jing Yang,Yuxia Shen,Jin Qu,Song Hong,Zhong-Zhen Yu
To enhance the recyclability while maintaining the high efficiency for the removal of organic dyes, monolithic polyurethane@reduced graphene oxide@manganese dioxide (PU@RGO@MnO2) hybrid sponge with a hierarchical structure and satisfactory flexibility is fabricated by self-assembly of RGO on a PU sponge followed by uniform coating of MnO2 nanoparticles onto RGO by means of an in situ redox reaction between RGO and KMnO4. RGO acts as an ideal substrate to accommodate MnO2 nanoparticles and prevents their aggregation, whereas the numerous hydrophilic MnO2 nanoparticles play dual roles of adsorption and catalytic degradation of methylene blue (MB) dye. The resultant hybrid sponge shows a hierarchical porous structure that provides fast transport channels and abundant active sites, benefiting the diffusion and removal of MB. By enhancing the mass transfer with the help of a micro-pump, the monolithic hybrid sponge acts as a filter for dye removal. Under the dynamic mode, the adsorption efficiency of the PU@RGO@MnO2 hybrid sponge for MB (50 ppm, 30 mL) reaches 94% after 20 min, whereas it is as low as 5% under the static mode. With the assistance of H2O2, the removal efficiency of the hybrid sponge is 96% at first time under the dynamic mode, whereas it is only 14% in the static mode. The monolithic hybrid sponge is highly efficient in adsorption and catalytic degradation of MB based on an adsorption–oxidation–desorption process. Even after being used 4 times, it still maintains excellent removal efficiency and recyclability.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2022
·Vol. 39
·期 1
·96-108
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IF 3.146
Zeng Xingye,Adesina Adeyemo,Li Ping,Wang Hanlu,Zhou Rujin
Ti-containing Mobil composition of matter-twenty-two (Ti-MWW) zeolite was prepared via a two-step post-synthesis process and then characterized by X-ray fluorescence, nitrogen adsorption-desorption isotherms, Fourier transform infrared absorption spectra, X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectra. These results indicate that the textural properties of MWW were well preserved after acid treatment and incorporation of titanium. An adsorptive-oxidative desulfurization (AODS) system was successfully developed on the basis of a model oil containing dibenzothiophene (DBT) with the as-prepared Ti-MWW being the catalyst and adsorbent and cumene hydroperoxide (CHP) being the oxidant. The parameters influencing the desulfurization performance were systematically investigated. These parameters include the Ti-MWW dosage, the reaction temperature, the stirring speed, the molar ratio of CHP to DBT and the additions of olefins and aromatics to the system. The conversion rate of DBT reached 99.6% via the catalytic oxidation process and the turnover frequency was 40.1 h −1 . Meanwhile, the oxidation products of DBT were removed by Ti-MWW adsorption. The recycling and regeneration performance of Ti-MWW were also investigated, and the DBT conversion reached 99.5% using the regenerated Ti-MWW. This work provides useful information for the construction of solvent-free oxidative desulfurization systems using a zeolite.
研究领域:
化学工程
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环境科学
·
催化材料
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 46
·22143-22150
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IF 3.925
Yanwen Guo,Xingjian Liu,Bing Hu
A novel supported deep eutectic solvent (DES) TBAB/PEG-200 was prepared by loading DES TBAB/PEG-200 onto mesoporous silica by the sol–gel method. The properties of the supported deep eutectic solvent TBAB/PEG-200 were characterized by FT-IR, XRD, SEM, BET analysis, and TG. The adsorption oxidation desulfurization system was studied using environmentally friendly H2O2 as an oxidant and typical heterocyclic sulfide dibenzothiophene (DBT) was dissolved in n-octane as a simulated oil. After the optimization of preset experimental parameters, the DBT content in the simulated oil could be removed deeply and effectively under the optimal reaction conditions m(25%-DES/SiO2) = 0.20 g, T = 60 °C, O/S = 14, t = 60 min. The catalyst was reused more than 9 times with no significant decrease in the desulfurization rate. Finally, the possible adsorption oxidative desulfurization mechanism was proposed.
研究领域:
材料科学
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环境工程
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2022
·Vol. 48
·期 11
·4517-4536
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IF 3.134
Yang Zizhen,Wang Siya,Chen Ou,Wang Zhengwei,Xu Jundong,Zheng Shuqin
In this paper, FeMn-ZSM-5/MOR(FeMn-Z/M) catalyst was synthesized through in-situ crystallization and wet impregnation method and used as heterogeneous Fenton-like catalyst for degradation of indigo carmine (IC) in aqueous solution. The catalysts were characterized using XRD, BET, SEM, EDS, FT-IR and XPS techniques. The experimental results showed that Fe and Mn were successfully doped onto the ZSM-5/MOR(Z/M) surface. The combination of ZSM-5 and mordenite (MOR) not only enhanced the adsorption capacity of contaminant, but also had more active sites. Degradation experiments and the valence variations indicated that Fe and Mn had a significant synergistic effect. The results of IC degradation experiments under different conditions showed that the optimum conditions (FeMn mass ratio = 1:2, FeMn-Z/M = 25 mg, H 2 O 2 = 0.5 ml, pH = 3), the degradation rate of IC reaches 99% in 20 min. Reaction analyses showed that catalyst follow a first-order reaction kinetic. The degradation of IC could be divided into two stages: adsorption/oxidation (After adsorption, oxidative degradation begins) and Fenton-like reaction. Free radicals quenching studies analyzed verified that the dominant free radicals within FeMn-Z/M Fenton-like system were hydroxyl radical (·HO) and hydro-peroxy radical (·HO 2 ), ·HO 2 was the main free radical in the adsorption/oxidation stage. The possible catalytic mechanism was proposed. Finally, the synthesized FeMn-Z/M catalyst had better performance than other IC removal methods, and had good degradation efficiency and high reusability after multiple runs.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Sciences
·
2023
·
IF 6.9
Yongqi Yan,Xinyu Yang,Ping Ning,Chi Wang,Xin Sun,Fei Wang,Peng Gao,Kai Li
In this study, non-thermal plasma (NTP) was employed to modify the Cu/TiO 2 adsorbent to efficiently purify H 2 S in low-temperature and micro-oxygen environments. The effects of Cu loading amounts and atmospheres of NTP treatment on the adsorption-oxidation performance of the adsorbents were investigated. The NTP modification successfully boosted the H 2 S removal capacity to varying degrees, and the optimized adsorbent treated by air plasma (Cu/TiO 2 -Air) attained the best H 2 S breakthrough capacity of 113.29 mg H 2 S/g adsorbent , which was almost 5 times higher than that of the adsorbent without NTP modification. Further studies demonstrated that the superior performance of Cu/TiO 2 -Air was attributed to increased mesoporous volume, more exposure of active sites (CuO) and functional groups (amino groups and hydroxyl groups), enhanced Ti-O-Cu interaction, and the favorable ratio of active oxygen species. Additionally, the X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) results indicated the main reason for the deactivation was the consumption of the active components (CuO) and the agglomeration of reaction products (CuS and SO 4 2− ) occupying the active sites on the surface and the inner pores of the adsorbents.
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
·
2020
·
IF 4.3
Qiyuan Chen,Lifen Liu
Emissions of volatile organic compounds (VOCs) air pollutants adversely affected human health and air quality. A novel reactor is designed by a bio-anode chamber with a PVDF/CFC diffusion membrane module and a catalytic air cathode chamber with persulfate and activated carbon fiber (ACF) based photocathode . Peroxysulfate is activated to generate oxidizing species that promote toluene removal and oxidation together with UV photolysis and photo-electrochemical catalysis. This new reactor as air pollution control technique is able to continuously remove toluene gas from an air stream that sequentially flows through firstly the cathode chamber where UV photolysis, photo-electrochemical (PEC) oxidation are integrated with activation of peroxymonosulfate (PMS), then flows through the bio-anode chamber where adsorption/diffusion and biodegradation take place in microbial fuel cell (MFC). This integrated system exhibits high efficiency in toluene removal (∼95 %, ∼100 ppm toluene) with stable power output (cell voltage: 0.40 V) under UV light illumination. In addition, the existence of reactive species such as OH, O 2 − and SO 4 - radicals are confirmed by EPR tests. The results show that both ·OH and SO 4 - are involved in the toluene oxidative degradation with the addition of PMS, where SO 4 - plays a predominant role, indicating that combination of photolysis, cathodic adsorption/oxidation with anodic adsorption/diffusion and biodegradation provides a promising way for VOCs removal and simultaneous electricity generation at room temperature.
研究领域:
环境科学
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化学工程
·
生物技术
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Umar Abdulbaki Danhassan,Xin Zhang,Riying Qi,Mahmoud M. Ali,Kuichuan Sheng,Hongjian Lin
Pristine biochar (PBC) is flourishing in adsorptive oxidation for pollutants remediation as an alternative to carbon adsorbents derived from coal/petroleum carbon sources, multistep, and hash synthesis. However, it is widely overlooked for aqueous S 2- remediation because the rational design of biochar with proper conductive and porous structure is challenging. Cobalt or iron ion was impregnated in biomass to produce biochar with different porous and conductive structures and explore S 2- adsorptive oxidation mechanism. Finding suggests cobalt and iron ions facilitate biomass decomposition to remove volatile matter, which transforms them into elemental cobalt (Co 0 ) or magnetite (Fe 3 O 4 ) on biochars (BC-Co) or (BC-Fe) and improves the porous structure. BC-Co benefitted from superior mesopores to adsorb S 2- 2.4 and 35 times faster than PBC and BC-Fe, achieving 811 ± 146 mg-S 2- /g maximum capacity. BC-Fe removed S 2- far less than PBC because Fe 3 O 4 on its surface blocked S 2- diffusion channel to the active site. It is postulated that S 2- was removed from water via external and internal diffusion and adsorption and oxidation at active sites. S 2- diffuses from bulk liquid to film near the biochar pore and into the pores via pore and surface diffusion to the active site, where it is adsorbed and oxidized to elemental sulfur or sulfate by quinone , semiquinone, or hydroxyl radicals at the wall of biochars. This study has documented fundamental information for developing mesoporous electroactive biochar for contaminant removal.
研究领域:
环境科学
·
化学工程
·
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）