Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Rumeng Wang,Hongyan Zhai,Wenjing Luo,Wen Liu,Zhengkai Zhuang,Min Ji
Carbonaceous catalysts are highly efficient in activation of persulfate thus attracting much attention in pollutant control. A reduced graphene oxide (rGO 600 ) was carefully prepared via thermal annealing graphene oxide to activate peroxydisulfate (PDS) for generating nonradical and radical degradation pathways of diclofenac (DCF) in this study. The rGO 600 had multifunctional groups, high defective degree (vacancies, C O and C−O−C; abundant reactive sites to activate PDS) and specific surface area. In the rGO 600 /PDS/DCF system, DCF was fast adsorbed on the surface and degraded via 1 O 2 , electron transfer complex and O 2 •− . The rGO 600 /PDS/DCF system was resistant to the presence of Cl − and NO 3 − . Reductive NO 2 − and humic acid significantly retarded the absorption and activation of PDS by rGO 600 . Ten intermediate products from DCF were tentatively identified and proposed by using high-resolution mass spectrometry . The major adsorption sites for DCF and major catalytic sites for PDS were not exactly the same sites. The coexist of abundant reactive oxygen species (ROS)-generation sites and adsorbed DCF on the adsorption sites should favor the quick utilization of the generated ROS. The multifunctional sites on rGO 600 improved the activation of PDS with pseudo first-order kinetics and the degradation of DCF.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Meiqi Li,Na Chen,Huan Shang,Cancan Ling,Kai Wei,Shengxi Zhao,Biao Zhou,Falong Jia,Zhihui Ai,Lizhi Zhang
Heavy metals chelated with coexisting organic ligands in wastewater impose severe risks to public health and the ambient ecosystem but are also valuable metal resources. For sustainable development goals, the treatment of heavy metal complexes wastewater requires simultaneous metal–organic bond destruction and metal resource recovery. In this study, we demonstrated that a neutral pH electro-Fenton (EF) system, which was composed of an iron anode, carbon cloth cathode, and sodium tetrapolyphosphate electrolyte (Na6TPP), could induce a successive single-electron activation pathway of molecular oxygen due to the formation of Fe(II)-TPP complexes. The boosted •OH generation in the Na6TPP-EF process could decomplex 99.9% of copper ethylene diamine tetraacetate within 8 h; meanwhile, the released Cu ions were in situ deposited on the carbon cloth cathode in the form of Cu nanoparticles with a high energy efficiency of 2.45 g kWh–1. Impressively, the recovered Cu nanoparticles were of purity over 95.0%. More importantly, this neutral EF strategy could realize the simultaneous removal of Cu, Ni, and Cr complexes from real electroplating effluents. This study provides a promising neutral EF system for simultaneous heavy metal complexes wastewater treatment and resource recovery and sheds light on the importance of molecular oxygen activation in the field of pollutant control.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Xianhu Long,Zhaokun Xiong,Rongfu Huang,Yahan Yu,Peng Zhou,Heng Zhang,Gang Yao,Bo Lai
Herein, an electrochemical (EC) system was applied as “co-catalyst” to enhance the activation of peroxymonosulfate (EC/Fe(III)/PMS) for efficient Sulfamethoxazole (SMX) degradation. The cathodic reduction reaction can facilitate electron transfer to Fe(III) and trigger the sustainable Fe(III)/Fe(II) redox cycle. Unexpectedly, in addition to hydroxyl radical ( OH) and sulfate radical (SO 4 •− ), non-radicals mechanism including singlet oxygen ( 1 O 2 ) and Fe(IV) were also found involved in EC/Fe(III)/PMS system. The degradation of SMX in EC/Fe(III)/PMS system was accomplished by the collaboration of radicals and non-radicals oxidation . The generation routes and mechanisms of involved reactive oxygen species (ROS) were explored. The relative contributions of OH, SO 4 •− , and nonradical species for the degradation of SMX were calculated to 4.75 %, 25.31 %, and 69.94 %, respectively. Besides, multiple degradation pathways of SMX were proposed by identifying the formed byproducts. The EC/Fe(III)/PMS process could efficiently degrade SMX under the influence of co-existing ions and inactivate pathogens in the wastewater.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Zhenchao Lei,Ziyuan Huang,Yimin Lin,Yuwei Liu,Zhang Yan,Wenxiao Zheng,Huanxin Ma,Zhi Dang,Chunhua Feng
The corrosion of Fe(0) in the presence of O 2 in nature can lead to the oxidation of organic compounds, but the efficiency is very limited. Herein, attempts were made to establish a galvanic system that separates the anodic Fe(0) oxidation reaction and the cathodic O 2 reduction reaction using an air-breathing cathode. Compared with the chemical Fe(0)/O 2 system, it exhibited a substantially higher capability of destroying a variety of pollutants, such as organic dyes (12 types), phenol , nitrobenzene , acetaminophen, phenol, and ethylenediaminetetraacetic acid. The degradation rate constant of a model dye (i.e., Rhodamine B) increased from 0.047 min − 1 (chemical) to 1.412 min −1 (galvanic) under the passive air-breathing condition. The electric circuit design promoted Fe(0) dissolution to Fe(II) and triggered electron transfer that drives O 2 reduction to H 2 O 2 , two important species responsible for the generation of HO • at high abundance. In addition, the galvanic Fe(0)/O 2 system produces electricity while destroying pollutants. Tests with real Ni plating wastewater further demonstrated the capability of the system to oxidize complexed organics and phosphite. This study provides a new strategy for boosting the oxidative capacity of the Fe(0)/O 2 system, which shows promise for acid wastewater treatment .
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CHEMOSPHERE
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2022
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IF 8.943
Qiang Wang,Haibo Liu,Peixun Zhai,Fuwei Sun,Tianhu Chen,Ziyang Chu,Dong Chen,Xuehua Zou
In this study, a new low-cost carbon-based material was prepared via the carbonization of methylene blue adsorbed halloysite (CMH) at different temperatures in a nitrogen atmosphere, which was named CMH-T (T-Temperature). The performance of CMH-T was explored and the effects of initial pH values, catalyst dosage, phenol (PE) concentrations, peroxymonosulfate (PMS) concentrations, and water background compounds on PE degradation were investigated systematically. The results indicated that CMH800 exhibited the best performance to activate PMS for degrading PE. Specifically, 92% PE was degraded within 30 min with a constant rate ( k obs ) of 0.1186 min −1 in the CMH800/PMS system. Furthermore, CMH800 was efficient over a wide pH range (pH 3–9) and showed a slight inhibition to inorganic anions. Quenching experiments, electron spin resonance (ESR) analysis, and electrochemical analysis confirmed that PE was degraded through non-radical pathways dominated by single oxygen ( 1 O 2 ) and mediated electron transfer processes in the CMH800/PMS system. In addition, the predicted toxicity of intermediates through ECOSAR software based on QSAR (Quantitative Structure - Activity Relationship) model indicated that most of the intermediates had a low risk to water environment. Therefore, the CMH800 has a good potential for wastewater treatment applications.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Huizhong Chi,Wenbiao Jin,Jianqiao Zhang,Yibin Xiu,Tao Xu
In recent years, there has been growing interest in the mechanism (radical or nonradical) of persulfate activation processes. In this study, the enhancement of naproxen (NPX) degradation in a Cu 0 /peroxymonosulfate (PMS) system by complexing reagents was investigated. Surprisingly, neocuproine (NCP) alters the nature of reactive species in the Cu 0 /PMS system. A high-valent copper species, Cu(III)-NCP, was found to dominate NPX degradation rather than radicals under acid conditions for the first time. Moreover, systematically designed experiments revealed that the Cu(III)-NCP complex was a strong selective oxidant that reacted with organics through a single electron transfer pathway. Meanwhile, the degradation efficiency of NPX was highly dependent on the solution pH and dosage of Cu 0 and NCP, but was irrelevant to the concentration of NPX. Additionally, the enhancement of NCP on other copper based PMS activation systems (i.e., Cu 2+ /HA/PMS and Cu 0 /HA/PMS systems) was investigated. Considering that the released copper can be removed by a simple precipitation method to meet the effluent standards, the new complex-enhanced Cu 0 /PMS system provided a new method to enhance the degradation efficiencies of pollutants by a copper-catalyzed Fenton-like system.
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Acta Biomaterialia
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2022
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IF 10.633
Kai Sun,Jiaying Yu,Jinzhong Hu,Jian Chen,Jia Song,Zhixin Chen,Zhuoer Cai,Zhuoxuan Lu,Liming Zhang,Zhifei Wang
The delivery of salicylic acid or its derivatives to tumor tissue in the form of nanomedicine is critical for the studies on their potential synergistic mechanism in tumor therapy and chemoprevention considering the dangerous bleeding in the high-dose oral administration. To deepen the understanding of their role in adjusting immunosuppressive tumor microenvironment (ITM), herein, we firstly developed a hypoxia-sensitive Fe-5,5′-azosalicylic acid nanoscale coordination polymer nanomedicines (FeNCPs) via a “old drugs new tricks” strategy for synergistic chemodynamic therapy (CDT) and remodulation of ITM to elevate antitumor immunotherapy effect. PEGylated FeNCPs could be reductively cleaved to release 5-aminosalicylic acid (5-ASA) and ferric ions by azo-reductase under hypoxic conditions, which could induce tumor cell death by Fenton reaction-catalysis enhanced CDT and 5-ASA-converted carboxylquinone to promote the production of •OH. Meanwhile, cyclooxygenase-2 (COX-2) and its enzymatic product prostaglandin E 2 (PGE 2 ), as immune negative regulatory molecules, can promote tumor progression and immune tolerance . The released 5-ASA as a COX inhibitor could suppress the expression of PGE 2 , and Fe 3+ was employed to reeducate M2-like tumor-associated macrophages (TAMs) to M1-like phenotype, which could initiate antitumor immune response to reach better antitumor immunotherapy. This work broadens the application of salicylic acid derivatives in antitumor immunotherapy, and provides a new strategy for their “old drugs new tricks”. Statement of Significance Cyclooxygenase-2 (COX-2) and its enzymatic product prostaglandin E2 (PGE 2 ), as immune negative regulatory molecules, facilitate the differentiation of immune cells into immunosuppressive cells to build the immunosuppressive tumor microenvironment, which can promote tumor progression and immune tolerance. Thus, down-regulation of COX-2/PGE 2 expression may be a key approach to tumor treatments. Meanwhile, as a class of inhibitors of COX-2/PGE 2 , the potential mechanism of aspirin or 5-aminosalicylic acid has been a mystery in tumor therapy and chemoprevention. To expand the application of aspirin family nanomedicine in biomedicine , herein, we firstly developed a hypoxia-sensitive Fe-5,5′-azosalicylic acid nanoscale coordination polymer nanomedicines via a “old drugs new tricks” strategy for synergistic chemodynamic therapy and remodulation of immunosuppressive tumor microenvironment to elevate antitumor immunotherapy effect.
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ANALYTICAL CHEMISTRY
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2022
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IF 8.008
Jing Lei,Wei Liu,Yan Jin,Baoxin Li
Defect engineering is an effective strategy to improve the catalytic activity of metal oxides, and quantitative characterization of surface defects is thus vital to the understanding and application of metal oxide catalysts. Herein, we found that ZnO nanoparticles with oxygen vacancy could trigger the luminol–H2O2 system to emit a strong chemiluminescence (CL), and the CL intensity was strongly dependent on the oxygen vacancy of the ZnO nanoparticles. The mechanism of this CL reaction was discussed by means of the electron-spin resonance spectrum, X-ray photoelectron spectrum (XPS), and CL spectrum. The oxygen vacancy-dependent CL was attributed to the ability of the oxygen vacancy to readily adsorb and further dissociate H2O2 into active •OH radicals. Taking advantage of this oxygen vacancy-dependent CL, we presented one method for quantifying the oxygen defects in ZnO. Compared with the current evaluation techniques (XPS and Raman spectroscopy), this CL method is rapid, low-cost, and easy to operate. This work introduces the CL technique into the field of material structure–property evaluation, and provides a new approach for exploring the defect function in ZnO defect engineering.
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APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Shiwei Gao,Zheng Wang,Haoran Wang,Yannan Jia,Nannan Xu,Xue Wang,Jiahao Wang,Chenyue Zhang,Tian Tian,Wei Shen
In the present study, B-doped biochar (BBC) materials with different B contents were prepared and used for the adsorption/degradation of oxytetracycline (OTC) through the activation of peroxydisulfate (PDS). The catalytic activity of BBC was improved to different degrees compared with that of pristine BC owing to enhanced OTC adsorption and PDS activation. Furthermore, the best adsorption and degradation achieved in this study was when the ratio of boric acid to biochar was 2:1, and we defined it as BBC 2 . The degradation rate of OTC (20 mg/L) after 120 min was increased to 94% by adding BBC 2 and PDS. Furthermore, B-doping increased the BC pore size and introduced Lewis-acidic sites to its surface for PDS activation. The effects of PDS concentration, initial pH, and catalyst dosage on the removal of OTC were also evaluated. Using free-radical-quenching experiments, two main pathways for OTC degradation were identified, i.e., that via radicals on the BBC surface and that via non-radicals ( 1 O 2 ) in solution. B atom doping positively charged the adjacent C atoms, thus allowing direct electron transfer with S 2 O 8 2− and facilitating the generation of 1 O 2 . Furthermore, the C O groups generated upon BBC activation also generate 1 O 2 in a similar manner. Finally, nine OTC degradation products were identified and two possible degradation pathways were proposed.
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Journal of Cleaner Production
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2022
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IF 11.072
Jinxin Li,Wencheng Ma,Dan Zhong,Kefei Li,Jun Ma,Shaobo Zhang,Xuan Du
Oxygen vacancies (V O ) constructing in metallic compounds have been verified to enhance hydrogen peroxide (H 2 O 2 ) activation for pollutants treatment. However, the interactions between surface V O concentration and H 2 O 2 were still ambiguous. In this study, perovskites with different surface V O concentration were successfully prepared by a simple sol-gel process. Experimental results showed that A-site cation deficient was capable of distorting FeO 6 octahedra in Ca 1−x FeO 3-δ (x = 0, 0.1, 0.2) orthorhombic perovskites for the regulation of surface V O concentration. Afterwards, Ca 0.9 FeO 3-δ exhibited excellent catalytic activity and stability for tetracycline (TC) degradation, which was 4 times higher of catalytic enhancement than that of the raw Ca 1.0 FeO 3-δ . Moreover, up to 9, 17 and 27 times of catalytic enhancement as compared with commercial Fe 3 O 4 , ɑ-FeOOH and Fe 2 O 3 towards TC degradation. Based on electron spin resonance and free radical quenching experiments, the hydroxyl radical (∙OH) was the main active species for the catalytic degradation of TC. Meanwhile, higher or lower surface V O concentration was harmful to the production of ∙OH. Additionally, the toxicity of TC degradation by-products exhibited a decreasing trend according to the results of toxicological simulation. This work provides a new strategy for designing an efficient and promising heterogeneous Fenton-likes catalyst for environmental remediation.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
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IF 6.76
Chaochao Jiang,Caihong Qin,Mengke Guo,Jiayu Huang,Dongjie Yan,Xiaoqing Dang
A non-thermal plasma with a wet scrubber (NTP + WS) was used to degrade gaseous toluene. Compared with the NTP + WS/H 2 O system, the toluene and by-product ozone removal efficiencies were increased by 10% and 85% in the NTP + WS/Fe 2+ system, respectively. For 60 ppm toluene degradation, the maximum mineralization rate (MR) of toluene (61%) was obtained, at the optimum Fe 2+ concentration of 50 mg/L. During catalytic oxidation, the removal efficiency of toluene was limited by its solubility in WS systems. In addition, decreased Fe 2+ concentration and accumulation of organics led to the system deactivation. The EPR and quenching experiments verified the presence and contribution of hydroxyl radicals (4.6%) and superoxide radicals (3.8%) to the removal efficiency of toluene. Based on the radicals and intermediates detected in the gas and liquid phases, a degradation mechanism for toluene in the NTP + WS/Fe 2+ system was proposed.
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ACS Nano
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2022
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IF 18.027
Shikai Liu,Wenting Li,Hengxing Chen,Jialing Zhou,Shuming Dong,Pengyu Zang,Boshi Tian,He Ding,Shili Gai,Piaoping Yang,Yanli Zhao
Nanosystem-mediated tumor radiosensitization strategy combining the features of X-ray with infinite penetration depth and high atomic number elements shows considerable application potential in clinical cancer therapy. However, it is difficult to achieve satisfactory anticancer efficacy using clinical radiotherapy for the majority of solid tumors due to the restrictions brought about by the tumor hypoxia, insufficient DNA damage, and rapid DNA repair during and after treatment. Inspired by the complementary advantages of nitric oxide (NO) and X-ray-induced photodynamic therapy, we herein report a two-dimensional nanoplatform by the integration of the NO donor-modified LiYF4:Ce scintillator and graphitic carbon nitride nanosheets for on-demand generation of highly cytotoxic peroxynitrite (ONOO–). By simply adjusting the Ce3+ doping content, the obtained nanoscintillator can realize high radioluminescence, activating photosensitive materials to simultaneously generate NO and superoxide radical for the formation of ONOO– in the tumor. Obtained ONOO– effectively amplifies therapeutic efficacy of radiotherapy by directly inducing mitochondrial and DNA damage, overcoming hypoxia-associated radiation resistance. The level of glutamine synthetase (GS) is downregulated by ONOO–, and the inhibition of GS delays DNA damage repair, further enhancing radiosensitivity. This work establishes a combinatorial strategy of ONOO– to overcome the major limitations of radiotherapy and provides insightful guidance to clinical radiotherapy.
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