CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Maolin Wang,Yaling Wang,Xudong Jing,Jiahui Xu,Min Li,Qing Xie,Xiyun Cai
Iron-activated persulfate (PS) systems commonly suffer from the poor Fe(III)/Fe(II) redox cycle in groundwater and soils, due to the rapid oxidation of Fe(II) by both PS-related and naturally occurring oxidative substances. Maintaining the Fe(III)/Fe(II) redox cycle is necessary to achieve the high efficiency and stability of iron-activated persulfate systems toward aromatic contaminants (e.g., PAHs) in groundwater and soils. Herein, we discover the mixtures of dithionite (DTN) and zerovalent iron (ZVI) to synergistically activate PS, and develop highly efficient, stable DTN-ZVI/PS systems for PAHs removal in groundwater and soils. DTN and intermediates sulfite/thiosulfate initiated reduction of ZVI-derived Fe(III) species in DTN-ZVI/PS systems. This reaction accelerated the Fe(III)/Fe(II) redox cycle and coated ZVI with FeS x , both favoring the generation of HO and SO 4 − . DTN-ZVI/PS exhibited Nap removal of >90% in water during 11 of 15 supplementations of Nap and/or PS, 1.4–2.4 times ZVI/PS. Similarly, 0.47–4.3 fold increments of Nap removal k obs were obtained in five chemical types of groundwater, and 1.3–2.4 fold increments of PAHs removal in soils. This study may provide a technical basis to develop new Fe-activated oxidation systems for groundwater and soil remediation .
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Changhui Zhou,Jinhua Li,Yan Zhang,Jing Bai,Pengbo Wang,Bo Zhang,Lina Zha,Mingce Long,Baoxue Zhou
Sulfurous and nitrogenous oxides, including NO x and SO 2 , and the generated substances NO x - and SO 3 2- widely exist in air and water as pollutants and thus are difficult to control in the environment. In this study, we designed a novel photoelectrocatalytic (PEC) system for the efficient conversion of SO 2 and NO x in mixed gases and NO x - and SO 3 2- in wastewater to N 2 and SO 4 2- , respectively, by activating SO 3 2- to form SO 3 • - . The key ideas include the conversion of SO 3 2- from SO 2 and efficient activation of SO 3 2- into SO 3 • - and further conversion into SO 4 • - by the MoS 2 /Fe 2 O 3 photoanode. Simultaneously, NO 3 - /NO 2 - originating from NO x was rapidly reduced to NH 4 + on the CuNW@CF cathode. Ultimately, the generated NH 4 + was selectively oxidized to N 2 by SO 4 • - and SO 4 • - was reduced to SO 4 2- . The results indicated that 99.9 % of TN was removed and 100 % of SO 3 2- was converted to harmless SO 4 2- . This study provides new insights into the treatment of sulfurous and nitrogenous oxides in air and water.
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Nanoscale
·
2023
·Vol. 15
·期 20
·9214-9228
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IF 6.7
Wenting Li,Shikai Liu,Yangyang Zhang,Jialing Zhou,Rumin Li,Shili Gai,Lei Zhong,Piaoping Yang
Numerous research studies have proved that lactate is pivotal in tumor proliferation, metastasis, and recurrence, so disrupting the lactate metabolism in the tumor microenvironment (TME) has become one of the effective methods of tumor treatment. Herein, we have developed a versatile nanoparticle (HCLP NP) based on hollow Prussian blue (HPB) as the functional carrier for loading α-cyano-4-hydroxycinnamate (CHC), and lactate oxidase (LOD), followed by coating with polyethylene glycol to enhance chemodynamic therapy (CDT) and the antimetastatic effect of cancer. The obtained HCLP NPs would be degraded under endogenous mild acidity within the TME to simultaneously release CHC and LOD. CHC inhibits the expression of monocarboxylate transporter 1 in tumors, thereby interrupting the uptake of lactate from the outside and alleviating tumor hypoxia by reducing lactate aerobic respiration. Meanwhile, the released LOD can catalyze the decomposition of lactate into hydrogen peroxide, further enhancing the efficacy of CDT by generating plenty of toxic reactive oxygen species through the Fenton reaction. The strong absorbance at about 800 nm endows HCLP NPs with excellent photoacoustic imaging properties. Both in vitro and in vivo studies have demonstrated that HCLP NPs can inhibit tumor growth and metastasis, providing a new possibility for tumor therapy.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Hexiang Wang,Chenliu Tang,Luwei Wang,Zhirong Sun,Xiang Hu
A MOF-derived carbon material containing CoFe alloy (Co/Fe@NPC-500) by calcining N-doped Co/Fe bimetallic MOF at a lower temperature was successfully synthesized as a cathode in electro-Fenton process for ceftazidime (CAZ) degradation. The presence of Co could accelerate the transfer of electrons from C atoms of carbon material to Fe, thus increasing the content of low-valent metals in the material, which had been demonstrated by characterizations and density functional theory (DFT) calculations. Thanks to the integrity of the MOF structure, the synergistic effect between Fe and Co, Co/Fe@NPC-500 cathode showed efficient removal efficiency for CAZ completely removed within 60 min and obtained a total organic carbon (TOC) removal rate of 52.1% at 90 min. Besides, based on the results of HPLC-MS and DFT calculations, the degradation pathway of CAZ was proposed. This study provides some useful information for the preparation of MOF-derived carbon materials containing low-valent metals for electro-Fenton process.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Yue Gao,Yanan Xue,Kai Zhen,Jiacheng Guo,Xuejiao Tang,Peng Zhang,Cuiping Wang,Hongwen Sun,Jizhou Wu
The remediation of soil contaminated with hydrophobic organic pollutants has attracted great public concern. In the present study, a novel catalyst using biochar supported ferro ferric oxide modified by carboxymethyl cellulose (CMC-Fe 3 O 4 /BC) was developed to activate the Fenton reaction for hazardous hydrophobic organic pollutants , and the degradation mechanisms were analyzed in terms of free radicals , electron transfer pathways and degradation intermediates. The results showed that the CMC-Fe 3 O 4 /BC-activated H 2 O 2 system degraded nearly 100% of pyrene in the aqueous system after a 1440-min reaction. The catalyst was also applied to remediate industrial field soil contaminated with PAHs and γ-HCH. The removal rate of the total pollutants reached 61.1% after a 10-day reaction, which was higher than that of Fe 3 O 4 /BC without modification. CMC enabled the Fe 3 O 4 particles to more equably distribute on the BC surface, further effectively activating H 2 O 2 to generate more ⋅OH and forming different degradation products compared to the Fe 3 O 4 /BC. Additionally, the CMC-Fe 3 O 4 /BC-activated H 2 O 2 system obviously enhanced electron transfer on the BC surface. Thus, the PAHs and γ-HCH could be degraded via electron transfer pathways.
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Reaction Chemistry & Engineering
·
2023
·Vol. 8
·期 8
·1981-1992
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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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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Xindan Fan,Qintie Lin,Kehuan Xu,Junli Zheng,Jian Sun,Hengyi Fu,Yuxin Liu,Yongjie Ma,Jin He
Considering that high concentrations of ciprofloxacin (CIP) are generally ecotoxic and persistent in water bodies, the refractory degradability has not been addressed in depth. In this study, an N-doped modified graphitized iron-based carbon nanomaterial (0.8 N@FeCS) was prepared by hydrothermal synthesis for the rapid degradation of ciprofloxacin by activated peroxydisulfate. More importantly, the N-doped nitrogen configuration in the iron-based carbon material is pyridine nitrogen, pyrrole nitrogen and graphite nitrogen. The nitrogen modification imparts a new twist to the CIP degradation system: a shift from a common free radical reaction to a nonradical process ( 1 O 2 and electron transfer pathways). The degradation intermediates were identified by LC-MS analysis and density functional theory (DFT), it is suggested that the possible CIP degradation pathway. In conclusion, the process of catalytic activation results in removal of CIP, and this study provides a new perspective for the removal of antibiotics from aqueous solutions.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
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2023
·
IF 3.9
Huiqi Zheng,Xiaorong Meng,Yingzi Yang,Jin Chen,Shanshan Huo
The influence of surface charge density of nanofiltration (NF) membranes could due to enhanced electrostatic interaction through electrically assisted. In this study, the hydroxylated BaTiO 3 /Ti 3 C 2 T x (HBT)@polyvinyl alcohol (PVA) (HBTA) composite NF membranes were prepared by crosslinking HBT on the surfaces of NF membranes. The optimized HBTA-0.06 sample exhibited a water contact angle of 43.7°, zeta potential of −13.73 mV (pH = 6.5), average effective pore size of 0.319 nm, and pure water permeance of 55.1 L·m –2 ·h –1 . At an applied electric field of 3 V, the rejection rates of LiCl, NaCl, KCl, RbCl, and MgCl 2 determined for HBTA-0.06 reached 73.3%, 60.1%, 53.6%, 49.4%, and 59.8%, respectively. HBTA-0.06 has good stabilization properties that are especially advantageous for water purification , indicating good long-term filtration stability within 168 h. Furthermore, HBT doping significantly increased the charge density of the HBTA membranes and the rejection efficiency of chloride salts, both chlorine radicals (·Cl) and hydroxyl radicals (·OH) generation pathways were proposed under electrochemical assistance. Hence, electrical assistance represents a novel and effective technique for enhancing the salt rejection properties of multifunctional composite NF membranes.
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ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Huan He,Fan Li,Kunqian Liu,Juhong Zhan,Xiaoxia Wang,Chaochao Lai,Xiaoxia Yang,Bin Huang,Xuejun Pan
Disinfection treatment is an indispensable water purification process, but it can leave trace concentrations of disinfectant in the purified water. Disinfectants oxidation can age plastic pipes and release hazardous microplastics and chemicals into drinking water . Lengths of commercially-available unplasticized polyvinyl chloride and polypropylene random copolymer water pipe were ground into particles and exposed to micro-molar concentrations of ClO 2 , NaClO, trichloroisocyanuric acid, or O 3 for up to 75 days. The disinfectants aged the plastic and changed its surface morphology and functional groups. Meanwhile, disinfectants could significantly promote the release of organic matter from plastic pipes into the water. ClO 2 generated the highest concentrations of organic matter in the leachates from both plastics. Plasticizers , antioxidants and low molecular weight organic matter were detected in all of the leachates. Leachate samples inhibited the proliferation of CT26 mouse colon cancer and induced oxidative stress in the cells. Even trace concentrations of residual disinfectant can constitute a drinking water risk.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
·
IF 13.6
Chen Wang,Huanran Liu,Peng Sun,Jingjing Cai,Mingxing Sun,Haijiao Xie,Guoqing Shen
Single-atom dispersed catalysts (SACs) have gained considerable attention in organic contaminants remediation due to their superior reactivity and stability. However, the complex and costly synthesis processes limit their practical applications in environmental protection. Herein, a facile and cost-effective single-atom iron catalyst (Fe-SA/NC) anchored on nitrogen-doped porous carbon was first fabricated by using waste biomass as a carbon source. The Fe-SA/NC catalyst exhibited outstanding performance with a high turnover frequency of 1.72 min −1 toward antibiotics degradation via peroxymonosulfate activation . ECOSAR program and algae growth experiments demonstrated that the byproducts produced during the sulfamethoxazole degradation process were not detrimental to the aquatic environment. Radical quenching and electron paramagnetic resonance experiments revealed that Fe-SA/NC remarkably promoted 1 O 2 production in PMS-assisted reaction, and thus 1 O 2 contributed as much as 78.77% to sulfamethoxazole degradation. As indicated by experiment and density functional theory (DFT) calculations, FeN 2 O 2 configuration serves as the active site. DFT calculations further presented the most rational generation route of 1 O 2 as PMS→OH* →O* → 1 O 2 . We also designed Fe-SA/NC embedded spherical pellets for contaminants elimination at the device level. This study offers new insights into the synthesis of SACs from waste biomass and their practical application in environmental remediation.
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JOURNAL OF CONTROLLED RELEASE
·
2023
·
IF 10.8
Chuang Yang,Zheng Chen,Min Wei,Shen Hu,Mengyuan Cai,Nan Wang,Yunan Guan,Fangyuan Li,Qiang Ding,Daishun Ling
Ferroptosis has recently become an attractive strategy to combat the chemoresistance of cancer cells, but the intracellular ferroptosis defense system greatly challenges the efficient ferroptosis induction. Herein, we report a ferrous metal-organic framework-based nanoagent (FMN) that inhibits the intracellular upstream glutathione synthesis and induces self-amplified ferroptosis of cancer cells, for reversing chemoresistance and boosting chemotherapy. The FMN is loaded with SLC7A11 siRNA (siSLC7A11) and chemotherapeutic doxorubicin (DOX), which shows enhanced tumor cell uptake and retention, thus ensuring the effective DOX delivery and tumor intracellular iron accumulation. Importantly, the FMN simultaneously catalyzes the iron-dependent Fenton reaction and triggers the siSLC7A11-mediated suppression of upstream glutathione synthesis for intracellularly self-amplified ferroptosis, which further inhibits P-glycoprotein activity for DOX retention, and regulates the expression of Bcl-2/Bax to reverse the apoptotic resistance state of tumor cells. The FMN-mediated ferroptosis is also demonstrated in ex vivo patient-derived tumor fragment platform. Consequently, FMN successfully reverses cancer chemoresistance and achieves a highly efficient in vivo therapeutic efficacy in MCF7/ADR tumor-bearing mice. Our study provides a self-amplified ferroptosis strategy via inhibiting intracellular upstream glutathione synthesis, which is effective to reverse cancer chemoresistance.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 19
·13716-13727
·
IF 3.3
Caihong Wang,Yong Liu,Fengshen Han,Yongzhe Han,Tianyu Liu,Haitao Ren,Xu Han
Using metal-free catalysts is widely recognized as a promising approach toward wastewater remediation because of the absence of metal leaching. However, the oxidation products involved in the oxidation process and the corresponding mechanisms are still not clear. In this work, N-doped carbocatalysts (CN) were fabricated using as-prepared g-C3N4 and glucose solution, and the reactivity of the as-prepared catalysts was optimized by controlling calcination temperature. Correspondingly, increasing the calcination temperature promotes the catalytic oxidation of BPA. The positive correlations between the contents of pyridinic-N and graphitic-N and the kobs values of BPA oxidation, as well as XPS analysis indicate the important roles of pyridinic-N and graphitic-N in BPA oxidation. According to the series of characterizations of the oxidation products and Raman analysis of the reaction process, the moderately activated persulfate (PS) on the CN catalyst is the predominant species in BPA oxidation and BPA can be oxidized to BPA polymers with high selectivity by H-abstraction under alkaline conditions. This work highlights the important role of the moderate activation of PS in the polymerization of phenolic contaminants under alkaline conditions, which enriches our understanding of the oxidation of aromatic contaminants by PS under alkaline conditions.
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