COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Xiangyu Peng,Jiayi Tian,Shuai Zhang,Wei Xiao,Xiaozhen Tian,Yubin Wang,Juanqin Xue,Dashi Lei
Rational design of photoelectrode with high visible light utilization rate and separation efficiency of electron-hole pairs is the key step in photoelectrocatalytic technology. In this work, Z-Scheme photoelectrocatalyst (ZTO/rGO/Ag/AgBr) was synthesized by hydrothermal and photo-reduction process. Comparing with pure Zn 2 SnO 4 (ZTO), adding reduced graphene oxide (rGO) effectively improved electrons transfer efficiency. Notably, the addition of Ag/AgBr not only broaden the visible light response range of ZTO, but also accelerated the separation of photo-generated electron-hole pairs, and constructed all-solid-state Z-Scheme heterojunction . Meanwhile, DFT calculation showed that Ag metal on rGO surface could act as active site for organic dyes degradation . Moreover, the addition of extra bias potential during photoelectrochemical process not only accelerate the migration of carriers, but also inhibit the recombination of photo-generated electron-hole pairs. Methylene blue (MB) could be effectively removed during photoelectrochemical reaction process, which was attributed to hydroxyl radical (•OH) and superoxide radical (•O 2 - ). In this work, Z-Scheme transfer pathway, assisted photoelectrocatalytic technology, is a feasible strategy for improving catalytic performance.
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Catalysts
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2022
·Vol. 12
·期 10
·1207
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IF 4.501
Chenliu Tang,Zhicheng Long,Yidan Wang,Dongze Ma,Xiaobiao Zhu
This study investigated the inhibition effects of sulfate on ferrous ion-activated persulfate oxidation of azo dye reactive brilliant red X-3B. The experimental results showed that the degradation efficiency of reactive brilliant red X-3B decreased from 100% to 63% in 60 min when the initial concentration of sulfate increased from 0 to 3 g/L. The ferrous/persulfate molar ratio had remarkable influence on persulfate oxidation capability in presence of sulfate. SO42−could coordinate with Fe2+and Fe3+in generating FeSO4ion pairs as well as FeSO4+or Fe(SO4)2−complexes, which were difficult to activate persulfate and reduced the regeneration of Fe2+. Radicals quenching and electron paramagnetic resonance experiments showed that ·OH and SO4·−were responsible for the oxidation of reactive brilliant red X-3B; however, the addition of sulfate significantly inhibited the generation of SO4·−, and then the generation of ·OH. Moreover, the corresponding Nernst equation indicated that high concentration of sulfate reduced the oxidation potential of SO4·−/SO42−. Experimental results proved that the adverse effects of sulfate on the persulfate oxidation could be counteracted either by batch addition of ferrous or by adding Ba2+to remove SO42−in the system.Keywords:persulfate;sulfate;sulfate radicals;reactive brilliant red X-3B
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Shizong Wang,Jianlong Wang
This study prepared the carbon-supported cobalt catalyst (Co-C-X) for activating peroxymonosulfate (PMS), and investigated the effect of co-pyrolysis temperature of graphitic carbon nitride (g-C 3 N 4 ) and vitamin B 12 on the catalytic activity. It was found that with the increase of co-pyrolysis temperature, the catalytic activity of Co-C-X increased, due to the different coordination structures of cobalt. At 500 °C (Co-C-500), cobalt existed as CoO; while it was single atom Co at 600 °C (Co-C-600); and small size CoO at 700 °C (Co-C-700). Co-C-X could activate PMS to produce hydroxyl radicals, sulfate radicals, high-valent cobalt-oxo and singlet oxygen, which depended on the pyrolysis temperature. Although Co-C-700 had the highest catalytic activity, the leaching cobalt was also highest (3.23 mg/L), compared with that of Co-C-500 (0.27 mg/L) and Co-C-600 (0.14 mg/L). Co-C-600 had fast degradation for atrazine, nitrobenzene , bisphenol A, phenol and 4-chlorophenol, which also had wide pH range and high tolerance to inorganic ions.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Jie Tian,Junyan Wei,Yeping Liang,Ruixue Guo,Beibei Li,Ruijuan Qu,Dongmei Zhou,Zunyao Wang,Ping Sun
This study aimed to investigate the catalytic performance of Fe 3 O 4 /ZnO in the ozonation of 1-hexyl-3-methyl imidazolium bromide ([HMIM]Br). The Fe 3 O 4 /ZnO composite was prepared by a quick and convenient two-step coprecipitation method, and the optimum mass ratio of Fe 3 O 4 :ZnO was determined as 1:8. The structure, surface morphology, and chemical composition of the Fe 3 O 4 /ZnO composites were studied by characterization methods. The degradation efficiency of [HMIM]Br reached 96% in 5 min in catalytic ozonation with the Fe 3 O 4 /ZnO composite, an increase of 20% compared with ozonation alone. Moreover, the pseudo-first-order rate constant was 1.5 times higher than ozonation alone. With the increase in the catalyst dosage, the degradation efficiency of [HMIM]Br first improved and then decreased, and the optimum dosage was 0.25 g/L. The increase in pH value and the introduction of Cu 2+ effectively promoted the catalytic ozonation of [HMIM]Br with Fe 3 O 4 /ZnO, while the reducing inorganic ions inhibited the ozonation reaction. Different water matrices had little influence on the catalytic performance of Fe 3 O 4 /ZnO. Radical scavenging and EPR experiments showed that hydroxyl radicals (•OH), superoxide radicals (O 2 •- ) and singlet oxygen ( 1 O 2 ) were the main active species in this system. Meanwhile, product identification showed that the degradation of [HMIM]Br mainly included hydroxylation, imidazole ring cleavage and bond cleavage. Toxicity prediction illustrated that the catalytic ozonation of [HMIM]Br could effectively reduce its toxicity. The efficiency, toxicity, reusability, and stability experiments suggested that the developed catalyst, Fe 3 O 4 /ZnO composite, had promising prospects in catalytic ozonation.
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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Guangli He,Yunhe Lai,Yanzhen Guo,Hang Yin,Binbin Chang,Man Liu,Shouren Zhang,Baocheng Yang,Jianfang Wang
Designing plasmonic photocatalysts with spatially controlled catalytic sites is an effective strategy to boost the sunlight-driven chemical transformation efficiency through plasmonic enhancement. Herein, we describe a facile method for the synthesis of TiO2-tipped Au nanobipyramids (NBPs) to give (Au NBP)/t-TiO2 nanodumbbells. The surfactant cetyltrimethylammonium bromide concentration is the key factor in the construction of this type of unique nanostructure. The photocatalytic aerobic oxidative coupling of amines using the plasmonic photocatalysts with the dumbbell-like and core@shell structures indicates that the TiO2-tipped ends for the photo-reduction and the exposed adjacent Au surface for the photo-oxidation on (Au NBP)/t-TiO2 can significantly improve the photocatalytic activity. The underlying mechanism of the photocatalytic oxidative coupling of benzylamine over (Au NBP)/t-TiO2 has been thoroughly investigated. Both experimental and simulation results for (Au NBP)/t-TiO2 and (Au nanorod)/t-TiO2 confirm the important effect of the plasmonic hotspots on the enhancement of the photocatalytic activity.
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PubMed
高影响因子
Catalysts
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2022
·Vol. 12
·期 11
·1455
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IF 4.501
Ting Gao,Ke Zhang,Qiuhui Zhu,Qingyun Tian,Hui Wang,Wei Zhang,Jiangyushan Liang,Jingqi Lin,Ahmed A. Allam,Jamaan S. Ajarem,Peter K. J. Robertson,Chuanyi Wang
Photocatalysis is an effective technology for NO removal even at low concentrations in the ambient atmosphere. However, the low efficiency of this advanced process and the tendency of producing toxic byproducts hinder the practical application of photocatalysis. To overcome these problems, the Bi@Ba2TiO4/BaBi4Ti4O15photocatalytic composites were successfully prepared by a one-step hydrothermal method. The as-synthesized photocatalysts exhibited an efficient photocatalytic performance and generated low amounts of toxic byproducts. X-ray diffraction studies show that Bi3+is successfully reduced on the surface of Ba2TiO4/BaBi4Ti4O15(BT/BBT). After L-Ascorbic acid (AA) modification, the photocatalytic NO removal efficiency of Bi@Ba2TiO4/BaBi4Ti4O15is increased from 25.55% to 67.88%, while the production of the toxic byproductNO2is reduced by 92.02%, where the initial concentration of NO is diluted to ca. 800 ppb by the gas stream and the flow rate is controlled at 301.98 mL·min−1in a 150 mL cylindrical reactor. Furthermore, ambient humidity has little effect on the photocatalytic performance of theBi@Ba2TiO4/BaBi4Ti4O15, and the photocatalyst exhibits excellent reusability after repeated cleaning with deionized water. The improved photocatalytic effect is attributed to the addition of AA in BT/BBT being able to reduce Bi3+ions to form Bi nanoparticles giving surface plasmon effect (SPR) and generate oxygen vacancies (OVs) at the same time, thereby improving the separation efficiency of photogenerated carriers, enhancing the light absorption, and increasing the specific surface areas. The present work could provide new insights into the design of high-performance photocatalysts and their potential applications in air purification, especially for NO removal.Keywords:photocatalysis;BaBi4Ti4O15;surface plasmon effect;NO removal
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APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Qi Zhao,Ye Yuan,Luyan Zhang,Liang Qiao,Cheng Ding,Kangshun Wang,Hongpeng Li,Jun Ma,Panpan Wang,Tianming Chen,Feihong Wang
Nonmetal doping is widely used in the modification of titanium dioxides (TiO 2 ) for photocatalytic applications. As a typical two-dimensional layered nanomaterial, the excellent physical and chemical properties of MXene materials have been the focus of current research. In this study, carbon and fluorine co-doped MXene derived TiO 2 nanosheets (labelled as C-F-TiO 2 ) were successfully synthesized and used as catalysts for degrading 2,4,6-trichlorophenol (2,4,6-TCP) under UV light irradiation. The C-F-TiO 2 with ultrathin nanosheet structure enhanced light absorption range and decreased the bandgaps. The degradation efficiency of 2,4,6-TCP by C-F-TiO 2 was over 99 % in 90 min, and the degradation rate was more than twice that of commercial TiO 2 . The degradation rate still remained about 90 % in 90 min after five cycles. The results of quenching experiments and electron spin resonance (ESR) illustrated that more reactive oxygen species (ROS) were generated in the C-F-TiO 2 /UV system, which was 1.5 times that of commercial pure TiO 2 , and • O 2 – was the dominant ROS for 2,4,6-TCP degradation. This study provided insight to utilize physicochemical characteristics of MXene to synthesize non-metal co-doped TiO 2 nanosheet as a catalyst, exhibiting excellent reactivity in the potential application for organic pollutant degradation.
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ENVIRONMENTAL TECHNOLOGY
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2022
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IF 3.475
Sheng Sheng,Jingjing Fu,Siyuan Song,Yuxuan He,Jin Qian,Ziyang Yi
The increasing use of fluoroquinolone antibiotics, which are found in various environmental media, is a constant threat to ecological safety and human health. In this paper, SrFeO3@MoS2 heterogeneous catalyst was prepared to activate peroxymonosulfate (PMS) for the degradation of levofloxacin (LVO). The characteristics of SrFeO3@MoS2 samples were studied and the optimum conditions for the removal of LVO by SrFeO3@MoS2/PMS system were investigated. The removal of LVO by the SrFeO3@MoS2-0.3/PMS system could reach 96.06% within 20 min of reaction. The effect of inorganic anions (SO42−, Cl−, NO3− and H2PO4−) commonly found in actual water bodies on catalytic reaction was explored. The reusability investigation revealed that the catalyst could still remove 88.06% of LVO within 20 min after four cycles. Moreover, SO4•−, •OH and 1O2 were identified by Electron Paramagnetic Resonance (EPR) tests and scavenger experiments, where the SO4•− and •OH were dominant reactive species. Combining with the XPS characterisation, the activation mechanism of SrFeO3@MoS2-0.3/PMS was proposed, and the oxygen vacancies and transition metals on the sample surface were active sites of PMS activation. Furthermore, the possible degradation pathways of LVO were well-established based on the detected intermediates.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2022
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IF 7.926
Hussein Abdelraouf,Jing Ding,Jiayi Ren,Guanshu Zhao,Fanyang Zhou,Shuyan Guan,Xuedong Zhai,Qingliang Zhao
A novel and short-term preparation method was conducted to fabricate pristine BiVO 4, and Gadolinium (Gd) doped BiVO 4 photocatalysts at sub-100 °C. The optical, structural, morphology, microstructure, and compositional characteristics of the fabricated photocatalysts were examined, which illustrated that the doping of Gd stabilized the existence of the tetragonal phase structure and enlarged the specific surface area of the pristine BiVO 4 . The comparison of the photocatalytic performance, preparation power consumption , and preparation cost showed the superiority of Gd doped BiVO 4 photocatalyst fabricated by the Short-Term Synthesis Method at sub-100 °C. The ofloxacin (OFL) removal rate with 5%, 7%, and 10% Gd-BiVO 4 photocatalysts was 1.53, 1.61, and 1.83 times that with pristine BiVO 4 under sunlight, respectively. The degradation performance of target contaminants, including diclofenac, tetracycline HCl , ofloxacin, rhodamine B, and sulfadiazine, was demonstrated after one hour of sunlight irradiation with 5% Gd-BiVO 4 , achieving the removal efficiencies of 98.63%, 98.07%, 97.98%, 92.09%, and 78.56%, respectively. The effect of various factors on the removal performance was revealed, indicating that SO 4 2− and H 2 PO 4 − had a remarkable inhibitory effect on the degradation. The 5% Gd-BiVO 4 also showed excellent reusability and stability after five-cycle runs. The photogenerated holes (h + ) and the superoxide radicals ( • O 2 − ) were the predominant generated active species , and the possible photocatalytic mechanism for the degradation of organic contaminants was proposed. Simple prepared Gd-BiVO 4 photocatalysts were revealed to be a practical and potential choice for efficiently degrading contaminants with sunlight as green energy.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Wenjie Kuang,Zhang Yan,Jinxiu Chen,Xiaotang Ling,Wenxiao Zheng,Weijun Huang,Chunhua Feng
Electrochemical oxidation has been demonstrated to be a useful method for removing biorefractory organic pollutants in mature landfill leachate but suffers from low efficiency in eliminating ammonium because of its resistance to being oxidized by HO• or free chlorine (FC) at decreased pH. Here, we propose a new bipolar membrane-electrochlorination (BPM-EC) process to address this issue. We found that the BPM-EC system was significantly superior to both the undivided and divided reactors with monopolar membranes in terms of elevated rate of ammonium removal, attenuated generation of byproducts (e.g., nitrate and chloramines), increased Faradaic efficiency, and decreased energy consumption. Mechanistic studies revealed that the integration of BPM was helpful in creating alkaline environments in the vicinity of the anode, which facilitated production of surface-bound HO• and FC and eventually promoted in situ generation of ClO•, a crucial reactive species mainly responsible for accelerating ammonium oxidation and selective transformation to nitrogen. The efficacy of BPM-EC in treating landfill leachates with different ammonium concentrations was verified under batch and continuous-flow conditions. A kinetic model that incorporates the key parameters was developed, which can successfully predict the optimal number of BPM-EC reactors (e.g., 2 and 5 for leachates containing 589.4 ± 5.5 and 1258.1 ± 9.6 mg L–1 NH4+-N, respectively) necessary for complete removal of ammonium. These findings reveal that the BPM-EC process shows promise in treating ammonium-containing wastewater, with advantages that include effectiveness, adaptability, and flexibility.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Xiaoqing Meng,Hua Li,Su Yan,Zengping Ning,Quan Yuan,Chengshuai Liu,Lixiang Zhou,Guanyu Zheng
Zero-valent iron (ZVI) activated Fenton-like processes have been proposed to inactivate ARB that carry diverse antibiotic resistance genes (ARGs) in wastewater, whereas they exhibit very low capacity of degrading ARB-carrying ARGs. Our previous study has revealed that pre-acidification can make cell inactivation and lysis. Thus, the present study investigated the effect of pre-acidification on the inactivation of a multi-drug resistant bacterium Pseudomonas putida MX-2 and the simultaneous degradation of carried seven ARGs by ZVI/H 2 O 2 and ZVI/PDS processes. Results showed that the pre-acidification of bacterial solution to acidic pH greatly promoted the degradation of carried ARGs from 0.14 to 0.17 logs to 2.48–2.97 logs at the meanwhile of almost completely inactivating P. putida MX-2 in both ZVI/H 2 O 2 and ZVI/peroxydisulfate (PDS) processes. Moreover, the pre-acidification seriously lysed the bacterial cells, released the carried ARGs into the extracellular environment, and facilitated the degradation of extracellular ARGs (e-ARGs) by the generated radicals. During the degradation of the resultant e-ARGs, they were fragmented to short fragments by ZVI/H 2 O 2 and ZVI/PDS processes. The treatment of real wastewater containing P. putida MX-2 further validated the promoting effect of pre-acidification on the degradation of carried ARGs. Therefore, it is extremely crucial to lyse the cells of ARB efficiently via acidification or other methods to promote the degradation of carried ARGs greatly, which may also be applicable for other advanced oxidation processes to reduce antibiotic resistance in wastewater effectively.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Zhe Zhao,Wuming Xie,Zijun Huang,Haiming Cai,Yuemeng Ji,Baocong Zhao
The antibiotic florfenicol (FF) discharged into the aquatic environment may cause serious water pollution. Therefore, an effective way to eliminate FF antibiotics from the water bodies should be proposed. Herein, MIL-53(Al)-supported nano zero-valent iron (NZVI@MIL-53(Al)) was synthesized and applied to activate hydrogen peroxide (H 2 O 2 ) to spark the Fenton reaction for FF antibiotics removal. The characterization results demonstrated the successful loading and good dispersion of NZVI onto MIL-53(Al). 100 % FF antibiotics degradation could be achieved under the optimal reaction conditions, including an initial FF antibiotics concentration of 20 mg L −1 , initial solution pH of 3.0, NZVI@MIL-53(Al) dose of 25 mg L −1 , and H 2 O 2 concentration of 0.2 mM. And after four cycles, the FF antibiotic degradation efficiency was still 81.18 %. The lowest tolerance for HCO 3 − was observed while the degradation activity was maintained at the presence of Cl − and HA. EPR measurement and free radical quenching experiment showed that ·OH was the main reactive specie in the NZVI@MIL-53(Al)/H 2 O 2 system. FF antibiotics degradation involved hydroxylation reactions (electrophilic substitution), dehalogenation, hydrolysis, and cleavage based on the UPLC-MS/MS analysis and DFT calculation. Noteworthy, 0.247 mg L −1 of F − and 1.2 mg L −1 of Cl − were detected in the solution after the reaction due to the breakage of the stable C–Cl bond and C–F bond. Finally, this work revealed that the NZVI@MIL-53(Al), with high stability and recyclability, could be a potential heterogeneous catalyst for treating antibiotic wastewater.
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