Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Hui Li,Siyang Li,Lide Jin,Zhen Lu,Minghui Xiang,Chen Wang,Wenbing Wang,Jin Zhang,Chunyang Li,Haijiao Xie
The synergistic catalytic degradation of metal carbon-based composites is a feasible strategy to improve the efficiency of advanced oxidation processes (AOPs) by means of green chemistry. In this work, Fe 3 S 4 nanoparticles were anchored on the surface of peanut shell biochar to prepare magnetic Fe 3 S 4 /biochar (Fe 3 S 4 /BC) composites, which were applied to activate peroxymonosulfate (PMS) to degrade 2,4,6-trichlorophenol (2,4,6-TCP). The addition of biochar not only reduced the aggregation of Fe 3 S 4 nanoparticles, but also accelerated the electron transfer rate, and the constructed C-O-Fe bridges accelerated the regeneration of Fe(Ⅱ), which made Fe 3 S 4 /BC have better catalytic performance than pure Fe 3 S 4 even though the use of metal sulfides was reduced. Fe on the surface of Fe 3 S 4 /BC was the catalytic reaction center. The dominant role of sulfate radical (SO 4 ·- ) and hydroxyl radical (HO·) on the degradation of 2,4,6-TCP was verified by electron paramagnetic resonance (EPR) and free radical quenching experiments. The mechanism of C-O-Fe bridges was verified by density functional theory (DFT) calculation. The mechanism of PMS activation by Fe 3 S 4 /BC was elucidated by electrochemical impedance spectroscopy (EIS) and X-ray photoelectron spectroscopy (XPS). Based on the detection results of intermediate products, the possible degradation pathways to 2,4,6-TCP were proposed. This work provides new insights into the synergistic catalytic mechanism of metal carbon-based sulfides and promotes the development of environmentally friendly and efficient metal carbon-based catalysts.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Mengmeng Dou,Jin Wang,Zhaokun Ma,Boru Gao,Xue Huang
In the study, an efficient ‘1 + 1 > 2′ synergistic coupling system driven by visible light consisting of mesoporous g-C 3 N 4 (MCN) and persulfate (PS)was constructed. The free radical transformation, electron transfer and non-covalent interaction between the MCN layer and PS in the system were explored via experiments and DFT calculations. The similarity for the fate of the seven β-lactam antibiotics with typical structures in the oxidation system was studied systematically in depth. First, the consistencies and differences of the seven antibiotics were summarized from three aspects: three-dimensional structures, electron cloud distributions, and the vulnerable sites. Notably, the selective differential degradation of β-lactam antibiotics in the MCN/PS system was speculated to be related with the molecular ionization potential (MIP), as a key index to describe the difficulty of oxidation. The distribution relationship between MIP and the oxidation kinetic constant ( K ) was explored and showed the following trend: a higher MIP indicates a weaker ability to provide electrons, and this leads to a greater resistance to oxidative degradation. In total, four main oxidation pathways of β-lactam antibiotics were systematically summarized combining HPLC-QTOF-MS and the simplified Fukui function calculation. The toxicity assessment of intermediate products provided by the T.E.S.T software of USEPA also shows a decreasing trend in the oxidation process. In the end, the superior practicability and stability of the MCN/PS system was verified by complex environment simulation and cyclic test. This research clarified the selective differential degradation mechanism of β-lactam antibiotics and provided a possible idea for the effective removal of refractory organic pollutants in water.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Ningning Dong,Lifa Ge,Pei Chen,Wei Wang,Fatang Tan,Xinyun Wang,Xueliang Qiao,Po Keung Wong
Stable, cheap and environmentally friendly CaO 2 was widely used to remediate environmental pollution, especially in advanced oxidation process (AOP) systems. However, its non-radical activation was still a huge challenge. In this study, the non-radical activation of CaO 2 nanoparticles was realized by MgNCN/MgO composites for efficient remediation of organic and heavy metal-contaminated wastewater. The presented CaO 2 -based AOP system exhibited excellent degradation performance towards tetracycline (TC) and methylene blue (MB) over a broad pH range, accompanied with the weak influences of common coexisting anions and natural water sources. Singlet oxygen ( 1 O 2 ) was verified as the dominant active species for organics degradation, and the coordination between MgNCN and MgO in MgNCN/MgO composites played a crucial role in the non-radical activation of CaO 2 nanoparticles. More importantly, the AOP system could not only degraded effectively organic pollutants, but also remove simultaneously heavy metal ions in wastewater. 100 mg/L CaO 2 and MgNCN/MgO could successfully remediate the complex pollution consisting of 10 mg/L MB and 100 mg/L Cd 2+ . Furthermore, the degradation intermediates of MB and the solid residues after treating pollutants were analyzed in detail to reveal the degradation process and conversion products.
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Journal of Materials Chemistry A
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2021
·Vol. 10
·期 6
·3146-3158
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IF 12.732
Xingkui Guo,Fan Yang,Xiaolu Sun,Chuang Han,Yujiao Bai,Guanjun Liu,Wenbo Liu,Rongguo Wang
A novel separation-free poly(N,N′-dimethylacrylamide)–titanium dioxide/copper sulfide (PDMAA–TiO2/CuS) hydrogel photocatalyst with the synergistic effect of adsorption and photocatalysis has been successfully developed by a facile two-step method involving a homogeneous polymerization process and a chemical precipitation approach. The catalyst not only shows strong capability to adsorb organic pollutants, but also provides multidimensional quality and electron transfer channels owing to the formation of a heterojunction between TiO2 and CuS nanoparticles as confirmed by TEM and PL spectra. Furthermore, the effects and mechanisms of adsorption and photodegradation of sulfaclozine as the target contaminant are investigated. The adsorption process of sulfaclozine on the composite hydrogel followed a pseudo-second-order rate equation and fitted in Langmuir monolayer adsorption. The photodegradation and mineralization of sulfaclozine reached 97.86% and 67.53%, respectively, when sulfaclozine degradation by the PDMAA–TiO2/CuS hydrogel achieved balance within 22 h. The intermediates of sulfaclozine degradation are identified through HPLC-MS, and the sulfaclozine degradation pathway is proposed. Therefore, this work might provide new insights to develop environmentally friendly separation-free high efficiency catalysts for the degradation of organic contaminants.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Jiabin Chen,Jie Xu,Tongcai Liu,Qi Wang,Nan Li,Yalei Zhang,Libin Yang,Xuefei Zhou
Peracetic acid (PAA) is an emerging oxidant and disinfectant increasingly used in wastewater treatment. Tetracyclines (TCs) are extensively consumed antibiotics, and frequently detected in the wastewater and surface water. Herein, PAA was found to show high reactivity towards TCs for the first time. This reaction follows the second-order kinetics with the rate constant ( k 2,app ) rapidly raised from pH 5 to 7, and then slightly increased to pH 9. Degradation of TCs by PAA was slightly influenced by water components, thus maintaining high efficiency in the real waters. Theoretical calculations revealed the electrons mainly concentrated on the B-ring of TCs, implying the B-ring as the reactive moieties for PAA oxidation. Transformation product analysis confirmed that oxidation of TCs by PAA mainly proceeded via hydroxylation and N-demethylation. Finally, PAA-promoted oxidation could remarkably reduce the antibacterial activity of TCs.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Xiaowen Liu,Yuanyuan Liu,Xin Zhang,Xiaodan Miao
In recent years, the development of low-cost and reusable green catalysts to reduce the organic pollutant of 4-nitrophenol (4-NP) into the utilizable intermediate of 4-aminophenol (4-AP) had attracted more and more attention. Herein, we reported a facile strategy to synthesize 3D N-doped graphene/bismuth (NGR/Bi) composites with efficient catalytic properties for 4-NP reduction. TGA exhibited NGR/8Bi catalyst came close to reach the maximum load of Bi (weight ratio 67%). NGR/8Bi catalyst had an apparent rate constant of 0.595 min −1 . After 8 min of catalytic reaction , the conversion of 4-NP reached 99.15%. Doped N facilitated the uniform distribution of Bi on graphene and improved the specific surface area and porosity of the catalyst, all of which contributed to the improvement of catalytic performance. The good reusability was attributed to that the microstructure of catalyst had not been changed significantly after used. The 3D network similar to aerogel made NGR/8Bi very easy to recycle and reuse. EPR spectra showed that H* active free radical was responsible for the conversion of 4-NP. This work revealed that the total surface area of metal particles in metal catalyst composites could affect catalytic performance essentially due to the surface plasma resonance effect.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Gen Wang,Lei Ge,Zhuoyue Liu,Xiurong Zhu,Shengjiong Yang,Kun Wu,Pengkang Jin,Xiangkang Zeng,Xiwang Zhang
Heterogeneous activation of peroxydisulfate (PDS) by transition metal oxides offers a promising strategy for organic pollutants removal but suffers from low electron transfer efficiency. Herein, layered MgO supported CuO nanoparticles was prepared by thermal conversion of metal-phenolic networks of Cu 2+ /Mg 2+ and tannic acid. CuO nanoparticles (∼2 nm) were spatial monodispersed on layered MgO, inducing the formation of electron deficient Cu 3+ and surface oxygen vacancies and thus facilitated adsorption and activation of PDS. The electron-rich CuO/MgO hybrid catalysts manifested good catalytic performance of PDS activation for organic pollutants removal. At 0.18 g/L of CuO/MgO hybrid catalyst and 0.2 mM of PDS, complete removal of bisphenol A (BPA) was achieved with a high kinetic constant (0.1 min −1 , 50 min). Quenching experiments, electron paramagnetic resonance tests, PDS decomposition behaviors, electrochemical analysis and in situ ATR-FTIR and Raman spectroscopy revealed a nonradical pathway of electron transfer for PDS activation. The CuO/MgO hybrid catalysts exhibited wide working pH range from 3 to 11, selective oxidation capability, good resistance to halide ion and high utilization efficiency of PDS, and thus would be a promising candidate for wastewater remediation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Zhendong Yu,Jiachen Ma,Xiaoyi Huang,Yuancai Lv,Yifan Liu,Chunxiang Lin,Rongni Dou,Xiaoxia Ye,Yongqian Shi,Minghua Liu
In this study, the S modified iron-based catalyst (S-Fe@C) for activating peroxydisulfate (PDS) was fabricated by heating the S-MIL-101 (Fe) precursor at 800 °C. The resulted S-Fe@C composite mainly consisted of carbon, Fe 0 , FeS, FeS 2 , and Fe 3 O 4 , and showed strong magnetism. Compared with Fe@C obtained from MIL-101 (Fe), the S-Fe@C exhibited much higher performance (1.5 times larger) on PDS activation and the S-Fe@C/PDS could rapidly degrade various organic pollutants in 5 min under the attack of the species of SO 4 - · , 1 O 2 , electro-transfer and Fe(IV). The S element in enhancing the PDS activation mainly involved two mechanisms. Firstly, the doped S could speed up the electron transfer efficiency, resulting in a promotion on PDS decomposition; secondly, the S 2- S 2 2- or S 0 could achieve the circulation of Fe 2+ and Fe 3+ , leading to the formation of non-radicals Fe(IV) and 1 O 2 .
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高影响因子
ACS Applied Polymer Materials
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2021
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IF 4.089
Wenzhuo Zhu,Shuai Zhou,Jian Wang,Wen Sun,Jinxing Chen,Ming He
Natural soft materials can generate a reversible transition between soft and tough states triggered by environmental stimuli. Inspired by this, various synthetic hydrogels with dynamic reversible crosslinks are developed. In this study, a weak coordination-induced dynamic crosslinked hydrogel is successfully synthesized. High concentrations of Ca2+ ions are coordinated with acrylamide, which then catalyze ammonium persulfate decomposition for rapid polymerization to a polyacrylamide (PAAm)/Ca hydrogel at room temperature. The preassembled coordination provides sufficient crosslinks, accompanied by enhanced hydrogen bonding during dehydration, which together endows the gel with high mechanical properties. This weak coordinated crosslinked structure is affected by humidity, leading to a wide range of mechanical properties of the gel, with the tensile strength ranging from 44.2 kPa to 5.6 MPa, elastic modulus from 17.3 kPa to 2.2 MPa, and toughness from 312.3 kJ/m3 to 7.8 MJ/m3. Additionally, Ca2+ ions preferentially coordinate with amides in the hydration process, and the gel exhibits an abnormal hydration phenomenon under low humidity. The gel with high polymer content has a higher water loss ratio and volume shrinkage. On this basis, we design an asymmetric bilayer structure gel and realize the curling and stretching of leaves and petals. Interestingly, the bilayer gel exhibits reversible adhesion properties and the tearing energy is up to 3985.9 J/m2 under low humidity. This principle may provide ideas and inspiration for producing hydrogels with adjustable mechanical strength and develop a route to construct versatile stimulus-responsive materials.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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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.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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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.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Libin Fu,Fenna Lide,Yaobin Ding,Chengjun Wang,Jizhou Jiang,Jia Huang
Photolysis of bromophenols and nitrogen cycle are two common processes in the natural water bodies. In the study, effect of hydroxylamine (HA), an intermediate of nitrogen cycle, on UV photolysis of bromophenols in the aqueous solution was investigated under different conditions. It was found that HA presence not only changed formation of reactive species, also varied degradation pathways of 2,4,6-tribromophenol (TBP). During photolysis of TBP, carbon-centered radicals (C ), H and e aq − were produced, while new radicals of OH, NO 2 and NH 2 were produced after addition of HA. Moreover, the added HA greatly inhibited hydrolysis of C via the reaction between them, thereby depressing formation of hydroxylated intermediates (e.g., monohydroxylated 2,6-dibromophenol), and improving debromination of TBP in UV/HA/TBP system. It is worth noting that two new nitro/amino byproducts of concern were detected in UV/HA/TBP system. They are proposed to be generated from the combination of C with NO 2 and NH 2 . Furthermore, nitro/amino byproducts were one of the major sink pathways of HA in UV/HA/TBP system. This is the first article to demonstrate the formation of nitro/amino byproducts form photodegradation of phenolic compounds in the presence of HA, and to clarify reaction mechanism for generation of OH, NO 2 and NH 2 from HA activation during photolysis of bromophenols in the aqueous solution.
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