Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Xiao Zhou,Yabo Wang,Xuqian Wang,Yongkui Zhang
Peroxymonosulfate (PMS) activation technology represents an efficient approach to generate reactive oxygen species for treating pharmaceutical pollutants, and the fabrication of effective catalysts is of great significance for PMS activation technology. In this study, iron-manganese (Fe-Mn) layered double oxides (LDO) with flaky structure formed by metal oxide nanoparticles were synthesized by coprecipitation-calcination method and used to activate oxidant PMS to generate reactive oxygen species so as to realize the degradation of sulfathiazole (STZ). Benefiting from the well-dispersed structure and synergistic effect between bimetallic oxides, about 90% of STZ (20 mg L −1 ) could be removed with the dosage of catalyst (LDO-400, 0.4 g L −1 ) and PMS (0.4 g L −1 ) in 40 min catalysis process. Quenching experiments and in-situ electron paramagnetic resonance (EPR) analysis revealed that radical pathways dominated by surface-bound SO 4 − • and •OH were involved in the removal of STZ in LDO-400/PMS system. Besides, EPR and linear sweep voltammetry (LSV) analysis indicated the non-radical pathways containing 1 O 2 and electron transfer also contributed to STZ degradation. Five consecutive cycles were conducted to prove the stability and reusability of LDO-400. The intermediates in the STZ degradation process were identified to propose the STZ degradation pathways. Particularly, ecological structure-activity relationship (ECOSAR) predicted the relatively low ecological risk of LDO-400/PMS system for STZ degradation. This study not only proves the advantages of synergistic effect between bimetallic oxides, but also enriches the design strategy of environmental remediation.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Kexin Yin,Yanan Shang,Dongdong Chen,Baoyu Gao,Qinyan Yue,Xing Xu
Versatile persulfate-based catalytic mechanisms induced by highly-effective single atom catalysts (SACs) have been intensively reported, which was mainly ascribed to the versatile coordinated-structures of SACs. However, the origin of these different mechanisms from the specific properties of pollutants has been ignored. In this work, eight kinds of pollutants were selected and the half-wave potential (φ 1/2 ) values representing their redox potentials were determined. A good correlation between the redox potential characteristics of pollutants and their oxidation performances/pathways in manganese single-atom catalyst (Mn-SAC)/PMS system can be confirmed. The φ 1/2 values of different pollutants showed a good correlation with the energy gaps between the pollutants and Mn-SAC/PMS complexes as well as their electrophilicity indexes, which confirmed the redox potential of pollutants was essential to the electron-transfer oxidation in Mn-SAC/PMS system. Based on the new insights in this work, we will be able to unveil the sources of Fenton-like systems with tunable oxidation processes.
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Catalysis Science & Technology
·
2018
·Vol. 8
·期 23
·6241-6251
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IF 5.365
Zhuang Guo,Linbi Zhou,Hongbin Cao,Yongbing Xie,Jiadong Xiao,Jin Yang,Yi Zhang
The electro-peroxone (E-P) process normally exhibits low efficiency in organic degradation in acid solution due to the limited rate constant of the reaction between O3 and H2O2 (peroxone reaction). In this paper, a C3N4–Mn/CNT composite material was synthetized and characterized with XRD, FTIR, SEM and XPS. With the function of the C3N4–Mn/CNT catalyst, the substrate oxalic acid (OA) was completely degraded in the E-P process within 30 min at pH 3, while only 15% degradation could be achieved after 60 min without the catalyst. The comparison of different reaction systems using the C3N4–Mn/CNT catalyst confirmed that the catalyst promoted the peroxone reaction, rather than the catalytic ozonation or electro-Fenton like reaction. Correlating the XRD and XPS analysis with the degradation data using the C3N4–Mn/CNT catalyst, we deduced that Mn coordinated with nitrogen was the active site for the peroxone reaction. Furthermore, the catalyst showed good chemical and catalytic stability in five cycles of the E-P process for OA degradation.
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CHEMICAL ENGINEERING JOURNAL
·
2018
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IF 6.735
Kunlun Yang,Jiasheng Zhou,Zimo Lou,Xurui Zhou,Yuanli Liu,Yizhou Li,Shams Ali Baig,Xinhua Xu
Fe-Mn binary oxides (FMBO) with different Fe/Mn molar ratios were synthesized to investigate the influence of the changed iron oxides forms and the manganese oxide on the removal efficacy of Sb(V) from water under neutral pH. The characterization tests by electron microscopy and X-ray diffraction spectroscopy showed that FMBO gradually changed from granular to aciculiform or fibrous structure and their crystalline degree increased with the decreasing Mn content. The ferric oxides in FMBO transformed from 2-L ferrihydrite-like substance with amorphous state to goethite or lepidocrocite with high crystalline as the amount of added Mn reduced during the preparation. The Sb(V) adsorption rates and capacities of FMBO both decreased and the influence of pH on the Sb(V) removal became greater with the decreasing Mn oxide content. All the results indicated that the addition of Mn could greatly improve the Sb(V) removal performance of FMBO through promoting the formation and preventing the transformation of amorphous ferric oxide in FMBO during the preparation, whose Sb(V) adsorption ability was confirmed to be stronger than that of goethite or lepidocrocite. Further exploration indicated the complexation reaction between Sb(V) and amorphous ferric oxide played a key role in Sb(V) adsorption by FMBO. Meanwhile, FMBO with a Fe/Mn molar ratio of 3:1 (FMBO 3 ) exhibited excellent regeneration performance and the amorphous iron oxide in FMBO 3 gradually transformed into crystalline iron oxide during the consecutive recycling.
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Journal of Materials Chemistry A
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2017
·Vol. 5
·期 45
·23641-23650
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IF 8.867
Zhong-Jie Jiang,Si Cheng,Haibo Rong,Zhongqing Jiang,Jianlin Huang
A general method has been developed for the synthesis of the spindle-like MFe2O4/C (M = Zn, Co, Ni, Mn). The synthetic procedure involves the preparation of mixed metal organic frameworks (i.e. Fe2M-MOFs) and their subsequent calcination. The obtained MFe2O4/C spindles show an intriguing structure, which consists of carbon coated secondary MFe2O4 nanoparticles with an interconnected carbon network. This makes them highly promising as the active materials for various applications with enhanced performance. For example, when used as the anode for lithium ion batteries (LIBs), the MFe2O4/C spindles exhibit higher reversible capacities and higher cycling stability in comparison to the MFe2O4 materials reported previously. Most interestingly, these MFe2O4/C spindles exhibit good morphology preservation during cycling. This shows that the volumetric expansion of MFe2O4 upon lithiation leads to the leaching of some active materials to the surface of the MFe2O4/C spindles along the percolation channels. This alleviates the volumetric expansion energy and prevents the structural destruction of MFe2O4/C spindles. The leached active materials do not detach from the MFe2O4/C spindles and participate in the lithiation/delithiation reactions throughout the whole cycling process, giving the MFe2O4/C spindles with high specific capacity and good durability. The approach reported here is highly versatile and might be applicable to the synthesis of other MFe2O4/C spindles for various applications.
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Analytical Methods
·
2017
·Vol. 9
·期 31
·4609-4615
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IF 1.9
Xuelian Wu,Xiaodong Lv,Jixiang Wang,Lin Sun,Yongsheng Yan
Based on the room-temperature phosphorescence (RTP) peculiarity of Mn-doped ZnS quantum dots (QDs), a bifenthrin sensor was fabricated by coupling molecular imprinted polymers (MIPs) on the surface of silane modified QDs via atom transfer radical polymerization (ATRP). The stepwise synthesis was realized with ZnS QDs-NH2-Br as the initiator, methacrylic acid (MAA) as the functional monomer, divinylbenzene (DVB) as the cross-linker, CuBr as the catalyst and 2,2′-bipyridine as the complexant. The smart RTP probe for bifenthrin was gained by surface molecular imprinting technology (SMIT) that can not only produce the stable RTP intensity of Mn-doped ZnS QDs, but can also enable more efficient recognition of the target molecule. The results presented show that the detection limit of the probe was 16.7 μg L−1. The RTP stability, selectivity and sensitivity of the bifenthrin sensor were evaluated by using a spectrophotometer. The high sensitivity was due to an electron-transfer mechanism between the target and the QDs, and the particular selectivity was due to SMIT. Therefore, this novel strategy combines RTP of Mn-doped ZnS QDs with ATRP to use the best aspects of both. It offers the advantages of straightforward preparation and processing, fast response, low toxicity and optical stability, so it is very promising for the detection of bifenthrin.
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LANGMUIR
·
2025
·
IF 3.9
Hua Zhong,Qin Qin,Zhuozhuo Wang,Hua Zhang,Yanling Qiu,Daqiang Yin,Xiaochang Liu,Zhiliang Zhu
Water pollution caused by emerging contaminants poses significant environmental and health risks, while the management of invasive algal biomass remains an underutilized resource. This study presents a novel Fe/Mn-modified in situ N-doped Enteromorpha prolifera-derived biochar catalyst (Fe/Mn/EP), addressing the dual challenges of efficient peroxymonosulfate (PMS) activation and utilization of invasive algal biomass. Through a straightforward one-step pyrolysis approach, the obtained catalyst integrated nitrogen functionalities and bimetallic active sites, enabling it to achieve an outstanding catalytic performance. It completely degraded carbamazepine (CBZ) in water samples within 30 min. The degradation process relied on the synergy between radical and nonradical pathways, primarily dominated by singlet oxygen (1O2) and superoxide radicals (·O2–). Specifically, in situ nitrogen doping, particularly involving pyrrole and graphite nitrogen, enhanced PMS activation by regulating the electronic properties and increasing the density of active sites. The degradation of CBZ significantly reduces the toxicity of the system by analysis prediction based on quantitative structure–activity relationship. The Fe/Mn/EP catalyst demonstrated broad adaptability across various emerging pollutants and real water matrices. This work highlights a sustainable strategy to transform problematic algae into high-performance biochar-based catalysts, offering a scalable solution for water pollution remediation.
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PubMed
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Xuan Chang,Tingting Duan,Jiashen Feng,Ying-Xia Li
The common use of peroxides in the remediation of malodorous black water may lead to the activation of heavy metals in sediment when eliminating black and odorous substances. The mechanisms of heavy metal interactions with dissolved organic matter (DOM) in response to in situ capping have not been elucidated, but this information could guide the optimization of capping materials. We developed a capping material consisting of hydrothermally carbonized sediment (HCS), hydrated magnesium carbonate (HMC) and sodium percarbonate (SPC) and used microcosm experiments to investigate the dynamics of Mn and Cu at the sediment–water interface in malodorous black water. The results showed that HCS, HMC and SPC contributed multiple functions of mechanical protection, chemical isolation and oxygen provision to the new caps. HMC promoted the conversion of Mn/Cu into carbonate minerals. The optimal mass proportions were 25 % HCS, 60 % HMC and 15 % SPC based on the mixture design. In situ capping altered the fate and transformation of metals in the sediment-overlying water profile in the short term through Mn immobilization and Cu activation. The complexation of Cu(II) ions was significantly stronger than that of Mn(II) ions. In situ capping had a significant effect on the order of complexation of different fluorescent DOM molecules with Mn(II)/Cu(II) ions: microbial byproducts and fulvic acid-like components were preferentially complexed with Cu(II) ions after capping, while phenolic and humic acid-like components preferentially interacted with Mn(II) ions. Humic-like components bound to Cu were affected the most by capping treatment, whereas protein-like components were relatively weakly affected. Our study provides valuable knowledge on the impact of in situ capping on DOM–metal complexes.
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PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yipeng Wang,Kun Wang,Xuchan Wang,Qingliang Zhao,Junqiu Jiang,Ruiyuan Xue,Luzi Yuan
Heavy metals (HMs) in wastewater, including Cd, Pb and Ni, were toxic and needed urgent treatment. Using biochar as an adsorbent to purify HM-containing wastewater is effective. However, there are few studies on screening of high-efficiency modifier and comparing their adsorption capacity. Herein, three different modification methods, including heteroatomic doping (urea), alkali hydroxide (NaOH) and chemical oxidation (KMnO 4 ), were used to improve removal ability of HMs by biochar. The difference in impregnation solution resulted in completely differences in microscopic morphology, physicochemical properties and adsorption efficiency of modified biochar. Biochar modified by KMnO 4 (Mn-BC) had significantly better adsorption capacity for Cd, Pb and Ni, reaching 46.40 mg/g, 80.20 mg/g and 18.65 mg/g, respectively, compared with raw biochar and other modification biochar, which might be due to the highest surface area and pore volume, lower zeta potential and loaded MnO x onto Mn-BC surface. Chemical and monolayer adsorption was dominant during adsorption of HMs. After adsorption, HMs were detected on the Mn-BC surface in the form of carbonate, hydroxide or oxide. Mineral precipitation and cation exchange were the dominant mechanisms during adsorption, accounting for 17.4%-41.8% and 43.0%-77.2%, respectively. Moreover, according to the correlation analysis, the increase in biochar pH, pore volume and degrees of carbonization were beneficial for HM adsorption. Mn-BC could adapt to a wider pH range (pH=4–6), and its adsorption capacity would not be interfered by coexisting ions (50 mg/L). This research proved advantages of biochar with KMnO 4 modification and highlighted its application in treatment of wastewater contaminated with multiple HMs.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Ruifeng Zhang,Jingjing Tang,Jing Yang,Chuanyun Yang,Qiuyan Niu,Gang Wen
Tetracycline (TC) is a widely used antibiotic, which poses a significant threat to aquatic environments. In this study, the backwashing sludge with different Fe/Mn mass ratio was obtained by adjusting the concentration of Fe 2 + and Mn 2+ in the influent water of filters. After dehydrating, drying and thermal treatment, the sludge was prepared as Fe-Mn binary catalysts to activate peroxymonosulfate (PMS) for removing TC from water. The removal performance, influence factors, and the degradation mechanism were investigated. The results indicated the prepared Fe-Mn sludge catalysts could effectively activate PMS to degrade TC and the activity was significantly influenced by the Fe/Mn ratio in the influent water. With Fe/Mn of 1:1 and 6:1, the sludge could be directly used as high activity catalysts; with Fe/Mn of 3:1, thermal treatment at 400 °C was required to enhance the activity. The fluidized-bed experiments showed that the Fe-Mn sludge catalysts had excellent activity stability and the ion leaching experiment indicated that the safe operational pH for the sludge catalysts should be above 5. The identification and quantification of reactive oxygen species proved that Mn was more beneficial to the generation of 1 O 2 , while Fe was more beneficial to the generation of SO 4 •─ and •OH, and TC was primarily degraded by 1 O 2 . Finally, based on the results of LC-MS characterization, the degradation pathway of TC was proposed, and the toxicity of the intermediates was assessed. The results provide new insights into the utilization of the Fe-Mn waste sludge as PMS catalysts for antibiotic removal.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Wei Wang,Ruibo Wei,Qinghan Zhu,Ziming Fu,Ruixia Zhong,Haiwang Wang,Jian Qi
The greenhouse effect caused by direct emissions of lean methane from coal mining is 25 times greater than that of CO 2 . To reduce the methane content in the atmosphere, it is imperative to develop high-activity, stable, and low cost methane-catalyzed combustion catalysts. In this work, a series of Mn-doped Co 3 O 4 hollow nanocages with dodecahedral shape were prepared using the metal-organic framework (MOF) material ZIF-67 as a template, combined with an in-situ growth method and a high-temperature calcination process. The optimized hollow structure Mn 0.6 /Co 3 O 4 -H (T 90 = 302 °C) exhibited higher catalytic activity than the solid structure Mn 0.6 /Co 3 O 4 -S (T 90 = 387 °C). On the one hand, Mn 0.6 /Co 3 O 4 -H has abundant O ads /O latt (0.61) and high Co 3+ /Co 2+ (1.11) content, which increases the adsorption of reactive molecules. In addition, the adsorption of methane by the Mn 0.6 /Co 3 O 4 -H catalyst reached 0.77 cm 3 /g at 273 K, increasing the methane concentration inside the catalyst. Concurrently, the hollow structure also establishes fast mass and heat transfer channels, leading to a significant improvement in the catalytic performance. The new catalyst developed in this study provides a new perspective and insight for reducing methane emissions during coal mining and reducing its negative impact on the environment.
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ACS Applied Energy Materials
·
2025
·
IF 5.5
Hongjie Chen,Yixuan Su,Yucong Chen,Minghan Bao,Mingjun Wu,Junyang Chen,Weitao Chen,Qiang Ru
The inherent low electronic conductivity of NASICON-type Na4MnV(PO4)3 (NMVP) impedes its use in advanced energy storage. Herein, we address this challenge by introducing a citric acid-derived carbon coating to elevate the material’s conductivity and electrochemical performance. By precisely tailoring the configuration of the carbon layer, we fabricated Na4MnV(PO4)3 encapsulated by a carbon coating (NMVP@C) and constructed a 3D hierarchical architecture with incorporated V(III) and Mn(II) states, which prompts the reversible redox reaction, augments Na+ storage capability, and mitigates volume expansion during cycling. The optimal cathode manifests superior rate capability and a long life span with 107.5 mA h g–1 at 1 C and 82.5% capacity retention over 5000 cycles at 20 C. The hard carbon//NMVP@C full cell confirms practical applicability with good electrochemical performance. This work underscores the pivotal interplay among the carbon layer, Na+ mobility, and structural integrity in NASICON cathodes, offering a pathway to develop high-performance and cost-effective cathode materials for sodium-ion batteries.
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