CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Yaling Wang,Maolin Wang,Qing Xie,Xiyun Cai
We report new activated persulfate systems with cyclodextrin (CD)-coated Fe 3 O 4 @Fe 0 nanoparticles (Fe 3 O 4 @Fe 0 -CD) that are characterized by both highly activating persulfates and rapidly accessing hydrophobic PAHs. Fe 3 O 4 @Fe 0 -β-CD displays chain-like structure of core–shell Fe 3 O 4 @Fe 0 nanoparticles coated with a CD layer (about 5.9 nm). CD coating stabilizes the polycrystalline structure of Fe 3 O 4 @Fe 0 nanoparticles and accelerates mass transfer of PAHs in water, thereby making Fe 3 O 4 @Fe 0 -β-CD intrinsically stable and reactive. Fe 3 O 4 @Fe 0 -β-CD/PS, featured by high yields of highly reactive Fe(IV), had about 30-fold rate constants of naphthalene (Nap) in water as much as Fe 3 O 4 @Fe 0 /PS. Fe 3 O 4 @Fe 0 -β-CD/PS completely removed Nap in water during 13 of total 18 supplementations of Nap and/or PS, whereas Fe 3 O 4 @Fe 0 /PS completely removed Nap only at the first supplementation of Nap. Likewise, Fe 3 O 4 @Fe 0 -β-CD/PS completely removed Nap in simulated groundwater, and degraded four PAHs in soils by >63%. This study may provide a technical basis for the developments of new PS activators to remove recalcitrant hydrophobic contaminants in water and soils.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Tao Chen,Fangpei Ma,Zhe Chen,Menglin Xie,Ting Li,Yu Zhou,Jun Wang
Solar-driven benzene oxidation with dioxygen (O 2 ) provides a green and sustainable alternative for phenol production, but the construction of heterogeneous photocatalysts remains a huge challenge for efficient conversion under visible light irradiation and ambient conditions. Herein, we reported a facile microwave assisted strategy for the defect engineering of two-dimensional (2D) tungsten oxide while well maintaining the original crystalline architecture. Abundant oxygen vacancies were constructed on the 2D tungsten oxide, which remarkably promoted photochemical (light harvesting, charge separation and transfer) and O 2 activation behaviors, this promotion effect was further strengthened by the hybridization with Pt species with the formation of Schottky junction. The champion catalyst enabled a high phenol yield of 11.3% with a selectivity of 91% in the visible-light-driven benzene hydroxylation with atmospheric O 2 at room temperature. The catalyst can be facilely recovered and reused with stable activity. The oxygen vacancies and Pt co-catalyst were demonstrated to play vital roles in the photocatalytic formation of the reactive oxygen species (hydroxyl radials, ·OH) for effective oxidation.
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CHEMOSPHERE
·
2023
·
IF 8.8
Yaxiong Zeng,Qizheng Zhuo,Liyan Dai,Baohong Guan
The molecular nest structured catalysts have demonstrated better performance than the traditional supported catalysts. However, they have not been tried in antibiotics or other organic pollutants removal from water by advanced oxidation processes (AOPs). Here we synthesized Mn anchored zeolite molecular nest (Mn@ZN) for the catalytic ozonation of cephalexin (CLX), which is the widely used antibiotic and also a refractory pollutant in water. The ozonation catalyzed by Mn@ZN achieves 97% of CLX degradation in only 2 min and a reaction rate constant of 0.2454 L·mg −1 ·s −1 , which is 79.2 times higher than that of the non-catalytic ozonation. Even after ten cycles, the 0.46Mn@ZN/O 3 still achieves a CLX degradation efficiency higher than 88% in 2 min, presenting an excellent stability. Mn ions stabilized by the molecular nests facilitate Lewis acid sites and oxygen vacancies, providing active sites for O 3 sorption and decomposition into ·O 2− and 1 O 2 through electrons transfer for the radical reaction with CLX. DFT calculation indicates that both the oxygen vacancy formation energy and the O 3 adsorption energy of Mn@ZN are reduced by the Mn species introduction. This study finds a fascinating catalyst of Mn@ZN for the catalytic ozonation of antibiotics, and also a smart design strategy for zeolite confined metals catalysts for water treatment .
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Wood Material Science & Engineering
·
2023
·
IF 2.2
Zhiping Wang,Anmin Huang,Shifeng Zhang,Yingying Su,Yuejin Fu
Wood emits volatile organic compounds (VOCs) that can affect people’s health and air quality. Based on advanced oxidation processes (AOPs), sulfate radicals produced via thermally-activated persulfate (Na2S2O8, KHSO5) can minimize VOCs. This research aims to apply this technique to minimize the VOC content in Pinus radiata. The results showed that terpenes and alcohols were the main VOCs emitted from Pinus radiata, which were greatly minimized using four treatments; however, acetic acid and 3-furaldehyde emissions increased. Furthermore, the temperature and oxidizing agent contributed to VOC degradation. Characterization results, including FTIR, XRD, color tests, and compressive strength indicated that the AOP treatment caused only a slight decline in the wood properties, while effectively reducing VOC emissions by as much as 32.75–61.05%.
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ANALYTICA CHIMICA ACTA
·
2023
·
IF 6.2
Yue Tang,Xiangqiang Zhan,Jia Zheng,Zhengmin Xie,Shuangju Zhu,Yuangen Wu
The long-term and excessive use of organophosphorus pesticides (OPs) leads to hazardous residues in the environment, which threatens human health to a considerable extent. Colorimetric methods can quickly and readily identify pesticide residue , but they still have various challenges in accuracy and stability. Herein, a smartphone-assisted and non-enzymatic colorimetric biosensor was constructed for rapid monitoring of multiple OPs based on the enhanced effect of aptamer on the catalytic ability of octahedral Ag 2 O. It was demonstrated that the aptamer sequence could enhance the affinity of colloidal Ag 2 O to chromogenic substrates, and accelerate the generation of oxygen radicals such as superoxide radical (·O 2 − ) and singlet oxygen ( 1 O 2 ) from dissolved oxygen, thereby significantly increasing the oxidase activity of octahedral Ag 2 O. The color change of the solution can be easily converted to the corresponding RGB values by a smartphone for quantitative and rapid detection of multiple OPs. Hence, the smartphone-based and visual biosensor of multiple OPs was acquired with limit of detection of 10 μg L −1 , 28 μg L −1 and 40 μg L −1 for isocarbophos , profenofos and omethoate , respectively. The colorimetric biosensor also exhibited good recoveries in several environmental and biological samples, showing that it may have broad application prospects for detecting OPs residues.
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Reaction Chemistry & Engineering
·
2023
·Vol. 8
·期 8
·1981-1992
·
IF 3.9
Li Sun,Mengying Sun,Yuan Zhi,Hua Zhang,Yuejin Shan,Binlin Dou,Jian Chen,Lixin Zhang
The continuous-flow (C-F) reduction process has been limitedly applied in the treatment of dyeing wastewater owing to the weak catalytic performance of the reactors employed. In this work, a small tubular packed reactor and its module are designed, fabricated and used for the C-F reduction of nitro and azo compounds in dyeing wastewater. Here, Au–Co–CoOx-coated glass beads with superior catalytic activity are chosen as packing materials, prepared without any toxic chemical agents. By means of the reactor, 4-nitrophenol (4-NP) can be completely removed and its removal rate is determined to be 100 μmol h−1. After that, a novel strategy for the tandem module is proposed to further enhance the removal rate of 4-NP. Based on the tandem module, the removal rate of 4-NP can be dramatically boosted to 1900 μmol h−1. Meanwhile, the rate constant for the C-F reduction of 4-NP can reach up to 0.44 s−1. Furthermore, the tandem module displays satisfactory operating stability, reusability and reliability in real water samples. In addition, the tandem module first achieves the C-F reduction of 2-nitrophenol, 3-nitrophenol, methyl red and methyl orange. Clearly, the reactor and its module can effectively extend the application of the C-F reduction process in dyeing wastewater treatment.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2023
·
IF 3.9
Hongyu Liu,Xin Wen,Jun Zhang,Huan Zhang,Junfu Wei
Catalytic oxidation of contaminants by peroxomonosulfate (PMS) was coupled with membrane filtration to realize high-performance removal of dyes. CoFe 2 O 4 (CFO) was enwrapped and cross linked in calcium alginate (CaAlg) to form CFO−CaAlg composite membrane. The introduction of CFO could not only activate PMS, but also enhanced the stability, hydrophilic property and crosslinking degree of the composite membrane. The final removal rate was enhanced greatly benefiting from the synergistic effect of filtration and catalytic degradation. The removal rate increased from 75% (filtration) to 98% by coupling with catalytic degradation. More importantly, purified water could be obtained immediately instead of waiting for purifying the whole feed solution due to the superiority of cross flow filtration . Radicals quenching and electron spin resonance (ESR) analysis experiment confirm that SO 4 · − contributed 25% and 1 O 2 contributed 75% in catalytic degradation. The composite membrane was effective for different type of dyes and could be reused only being backwashed by purified water because the catalyst CoFe 2 O 4 could recover from Co 3+ to Co 2+ by itself during the process. This study opens a new path of rapid water purification and immediate drinking water supply.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Zixin Zhang,Guohe Huang,Yongping Li,Xiujuan Chen,Yao Yao,Peng Zhang,Shaojie Ren,Mengna Li,Yifei Luo,Ning Chen,Renfei Feng
Homogeneous electro-Fenton (EF) technique is effective to mitigate membrane fouling through oxidizing organic foulants by hydroxyl radicals (HO·), but suffers from acid pH working environment (2.5 ∼ 3.5), low iron recyclability, and iron sludge accumulation. Herein, we developed a heterogeneous EF catalytic membrane to overcome these problems. A FeOCl@NCNT-functionalized ceramic membrane (FeOCl@NCNT/CM) was prepared to control the membrane fouling caused by humic acid (HA). At near neutral pH (∼ 6.0), the membrane enabled the in-situ generation of HO·. It also imparted an effective regeneration of Fe(II) through cathodic reduction and the electron transfer to Fe(III) from pyrrolic-N. The continuously generated HO· could oxidize the HA on/in the membrane, thus effectively mitigating membrane fouling. Electrostatic repulsion also contributed to fouling control by reducing the adhesion of negatively charged HA on the membrane. In continuous electrification mode, the FeOCl@NCNT/CM showed a superior antifouling ability. The water flux of the membrane at an applied voltage of −2.2 V was 1.79 times as high as that without voltage. Both reversible and irreversible membrane fouling were greatly reduced, and the transition of membrane fouling mechanism from pore blockage to cake filtration was significantly delayed. In intermittent electrification mode, the membrane exhibited an excellent self-cleaning performance. The fouled membrane showed considerable water flux recovery ratios (> 95%) after the EF cleaning at −2.2 V. The excellent antifouling and self-cleaning properties, low energy consumption, good stability and reusability of the FeOCl@NCNT/CM make it promising for the in-situ control of membrane fouling in water treatment.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Can Feng,Heng Zhang,Yi Ren,Mengfan Luo,Siying Yu,Zhaokun Xiong,Yang Liu,Peng Zhou,Bo Lai
Zerovalent iron (ZVI)-based Fenton-like processes have been widely applied in degrading organic contaminants . However, the surface oxyhydroxide passivation layer produced during the preparation and oxidation of ZVI hinders its dissolution and Fe(III)/Fe(II) cycling, and restricts the generation of reactive oxygen species (ROS). In this study, copper sulfide (CuS) was found to effectively enhance the degradation of diverse organic pollutants in the ZVI/H 2 O 2 system. Moreover, the degradation performance for the actual industrial wastewater (i.e., dinitrodiazophenol wastewater) in the ZVI/H 2 O 2 system was impressively improved by 41% with CuS addition, and the COD removal efficiency could reach 97% after 2 h of treatment. Mechanism investigation revealed that the introduction of CuS accelerated the sustainable supply of Fe(II) in the ZVI/H 2 O 2 system. Specifically, Cu(I) and reductive sulfur species (i.e., S 2– , S 2 2– , S n 2– and H 2 S (aq)) from CuS directly induced efficient Fe(III)/Fe(II) cycling. The iron-copper synergistic effect between Cu(II) from CuS and ZVI expedited Fe(II) generation from ZVI dissolution and Fe(III) reduction by formed Cu(I). This study not only elucidates the promotion effects of CuS on ZVI dissolution and Fe(III)/Fe(II) cycling in ZVI-based Fenton-like processes, but also provides a sustainable and high-efficiency iron-based oxidation system for removal of organic contaminants.
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Environmental Progress & Sustainable Energy
·
2023
·Vol. 42
·期 5
·e14140
·
IF 2.8
Li Hua,Taozhi Cheng,Ting Wei
Advanced oxidation based on persulfate applied for the removal of organic pollutants has received widespread attention. Here, combining hydrothermal synthesis and a high-temperature calcination approach, we constructed an effective copper oxide-modified biochar from wood waste ( Ginkgo biloba rods) for the removal of bisphenol A (BPA) from contaminated waterways. The modified biochar with copper oxide in its structure (CuO/BC) exhibited a densely arranged needle-shaped structure different from pristine timber waste biochar (BC). CuO/BC can activate persulfate efficiently, and the removal rate of BPA could reach 100% within 20–30 min, approximately three times higher than that of BC. Moreover, CuO/BC was more suitable for treating BPA wastewater under alkaline conditions. The stability of CuO/BC, reaction intermediates, and possible degradation pathway were investigated. These results demonstrate the potential of the application of CuO/BC for organic wastewater treatment and shed light on a new approach to develop wastewater treatment materials that are carbon-based and cost-effective.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Qiwen Pan,Fei Lin,Ruiqi Liu,Yilin Li,Xinyue Zhang,Rui Luo,Lingling Cai,Yang Liu,Wuguo Deng,Liru He
Nanocatalysts provide a platform for developing anti-tumor strategies by activating intratumoral chemical catalysis to produce highly toxic reactive oxygen species (ROS). However, the biological effect of nanocatalysts on tumor cells, which is pivotal for effective nanotherapy treatment, remains poorly understood. Herein, we present a general and facile method of synthesizing Fe/Ni-layered double hydroxides (LDHs) for enhanced apoptosis- and ferroptosis-induced cancer nano-therapy, as well as a potential mechanism underlying the anti-tumor effect based on transcriptome sequencing. An analysis of the chemical structure suggests that the Fe atoms interact strongly with the Ni atoms in Fe/Ni-LDH. Compared with Fe-OH and Ni-OH, Fe/Ni-LDH exhibited significantly better ROS-catalytic activity, with a V max of 5.015 × 10 −2 μM·s −1 , and generated massive amounts of •OH and O 2 •− radicals, enabling outstanding chemo-dynamic therapy. Both in vitro and in vivo experiments indicated a robust apoptosis-induced cell death pathway, increased intracellular oxidative stress, and accumulation of lipid peroxide (LPO), promoting ferroptosis-involved cancer-cell death, which was further confirmed by transcriptome sequencing. The Fe/Ni-LDH biocatalyst not only provides a robust nanoplatform for tumor suppression but also encourages further exploration and applications of nanobiocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Junjing Li,Yu Wang,Bin Zhao,Jing Ding,Jun Zhang,Menghua Yin,Zhaohui Zhang,Shumin Ma,Yaqian Liu,Zilin Tan,Hongwei Zhang,Liang Wang,Dionysios D. Dionysiou
In this work, a nickel-cobalt bimetallic organic framework (NiCo-MOF) was introduced as an intermediate layer to synthesize a Pd/NiCo-MOF/Nickel foam composite electrode, which was applied for electrocatalytic hydrodechlorination (ECH) of chlorinated pharmaceuticals and personal care products (PPCPs). The introduction of the NiCo-MOF structure dramatically improved the catalytic activity compared with the common Pd/Nickel foam electrode. Combined with transmission electron microscope and X-ray absorption fine structure analysis, catalyst on Pd/NiCo-MOF/Nickel foam surface had smaller particle size. The removal of the Pd/NiCo-MOF/Nickel foam electrode for chloramphenicol (CAP) reached more than 95 % at 40 min, while the removal of the Pd/Nickel foam electrode was only approximately 55 %. In this study, the active atomic hydrogen (H*) adsorbed on the Pd and NiCo-MOF structures is the critical active species to remove chlorinated PPCPs by Pd/NiCo-MOF/Nickel foam electrode. Density functional theory (DFT) was used to calculate and investigate the adsorption strength of the composite electrode structure for CAP, the product and H*. This work provided a new method to achieve higher catalytic performance and reactivity operability and longevity of catalytic materials through the synergism of a NiCo-MOF interlayer with Pd particles.
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