CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Tian-Yu Liu,Cong Wang,Yong-Zhe Han,Chang Bai,Hai-Tao Ren,Yong Liu,Xu Han
Bi 2+x WO 6 are a group of reactive photocatalysts in the photooxidation of various contaminants. However, their catalytic reactivity in the persulfate (PS)-based oxidation processes in the absence of light is still unknown. In this study, Bi 2.15 WO 6 shows a high reactivity in the catalytic oxidation of bisphenol A (BPA) by PS in the absence of light under alkaline conditions, and 20 mg L -1 BPA can be rapidly removed within 30 min at pH 10.0 with the low stoichiometry ratio of 1.79 between consumed PS and removed BPA. Characterizations of the oxidation products indicate that 98.4% of soluble BPA has been oxidatively polymerized to BPA polymers, instead of being oxidized to CO 2 and H 2 O. FTIR, Raman, XPS and electrochemical analyses confirm that surface Bi(III) is the reactive site for the adsorption of BPA and PS, which then initiates reactions between BPA and PS. DFT calculations reveal that the O-O bond in PS is moderately activated via the nonradical pathway after adsorbing on Bi(III), instead of being decomposed to SO 4 •− , followed by H-abstraction from BPA by the activated PS with the formation of phenoxyl radicals and the subsequent polymerization to BPA polymers. The apparently lower energy barrier from adsorbed BPA (Δ G = 0.056 eV) than that from dissolved BPA (Δ G = 0.263 eV) further reveals that H-abstraction from adsorbed BPA to the activated PS on the surface of Bi 2.15 WO 6 is more favorable than that from dissolved BPA. This study gives new insight on the efficient removal of recalcitrant contaminants via the H-abstraction pathway.
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
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2022
·Vol. 101
·期 1
·354-367
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IF 2.5
Yun Liu,Xiaopan Jiao,Fuli Zhang,Daojian Cheng,Wensheng Qin
Supported non-noble metal catalysts for the selective oxidation of furfural into high-value chemicals have attracted considerable attention. Herein, an atom-level-isolated, cobalt-catalyst-supported N-doped carbon (Co SAs-N@C) was synthesized through a metal cobalt–tannic acid coordination assembly strategy. The obtained Co SAs-N@C with 7.68 wt% of Co content was qualitatively and quantitatively characterized by X-ray diffraction, X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy, high-angle annular dark-field scanning transmission electron microscopy, inductively coupled plasma optical emission spectrometer, and X-ray absorption fine structure techniques. From the structural properties, potassium thiocyanate poisoning, and acid leaching, it was found that the atomic-dispersed CoNx species of the catalyst acts as the active site and plays a vital role in its highly effective oxidative esterification activity. The catalytic mechanism of this reaction is involved in radical oxidation, as confirmed by electron paramagnetic resonance spectra. The density functional theory calculations revealed that the reaction pathway proceeds as a hemiacetal pathway. Interestingly, the Co SAs-N@C catalyst also showed satisfactory catalytic activity for the aerobic oxidation of furfural. Unexpectedly, the Co SAs-N@C catalyst still possessed excellent stability and recyclability without loss of activity after five reuses.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Jun Li,Ge Gou,Hailing Zhao,Chao Liu,Naiwen Li,Longguo Li,Bo Tan,Bo Lai
CoFe 2 O 4 -CeO 2 composites with different CoFe 2 O 4 content were synthesized and used as catalysts for peroxymonosulfate (PMS) activation in water purification. Under the conditions of 200 mg/L 15%CoFe 2 O 4 -CeO 2 and 0.15 mM PMS, complete atrazine degradation was achieved in the 15%CoFe 2 O 4 -CeO 2 /PMS system. The pseudo-first-order rate constant ( k obs ) in 15%CoFe 2 O 4 -CeO 2 /PMS system (0.224 min −1 ) was 2.4 and 4.8 times of that in CoFe 2 O 4 /PMS system (0.092 min −1 ) and (CoFe 2 O 4 + CeO 2 )/PMS system (0.047 min −1 ). The main reactive species were verified through various quenching experiments and electron paramagnetic resonance tests, and the concentration of two main radicals was calculated. In addition, the interaction between CoFe 2 O 4 and CeO 2 involving Co(III)/Co(II), Fe(III)/Fe(II), and Ce(IV)/Ce(III) redox recycle for accelerating the degradation of organic compounds was explored. In addition, different from Cl − , HCO 3 − and NO 3 − , H 2 PO 4 − could promote atrazine degradation in 15%CoFe 2 O 4 -CeO 2 /PMS system by improving sulfate radical concentration in the reaction system. The main degradation intermediates of atrazine in the 15%CoFe 2 O 4 -CeO 2 /PMS and CoFe 2 O 4 /PMS systems were compared, as well as the degradation pathways. The toxicity analysis based on luminescent bacteria Vibrio fischeri indicated the superiority of 15%CoFe 2 O 4 -CeO 2 /PMS than CoFe 2 O 4 /PMS systems for ATZ degradation.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Guirong Ye,Jinghong Zhou,Renting Huang,Yingjun Ke,Yecan Peng,Yongxin Zhou,Yu Weng,Chutong Ling,Weixi Pan
Fenton sludge was converted into magnetic sludge-based biochar (SMBC) using a one-step pyrolysis process and employed as a novel heterogeneous catalyst to activate hydrogen peroxide (H 2 O 2 ) for the oxidative removal of methylene blue (MB). The crystal structure and catalytic activity of SMBC are strongly affected by the pyrolysis temperature. X-ray powder diffraction, Mössbauer, and scanning electron microscope-energy dispersive spectrometer analyses were conducted to determine the crystal phase transfer of iron (Fe) oxides at different pyrolytic temperatures and retention times. The results revealed that the catalytic efficiency of SMBC was strongly related to the crystal phase of Fe oxides. The catalyst obtained at 800 °C for 1 h exhibited superior catalytic properties and degraded 98.56% of the MB (100 mg·L −1 ) in 3 min via the synergistic effect of Fe 3 O 4 , Fe 0 , and biochar. Free radical quenching experiments and electron paramagnetic resonance studies demonstrated that ·OH, O 2 · − and 1 O 2 participated in the H 2 O 2 system, and·OH radicals were promptly generated owing to the catalysis of the SMBC. Aging tests were repeated for four cycles in three conditions to examine the stability of the material. The results showed that SMBC was relatively stable in non-aerated and aqueous conditions, but its activation performance was severely inhibited in an oxygen environment. Furthermore, the catalytic ability of SMBC was maintained at 88.13% after the 4th run. This study presents a cost-effective method of converting ferric sludge to an environmentally friendly catalyst that enables H 2 O 2 activation for degrading refractory organic contaminants .
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Jun Wang,Ying Zhao,Chunting Li,Zijun Yu,Yang Zhang,Yuan Li,Xiaoyao Tan,Shaomin Liu,Shaobin Wang,Xiaoguang Duan
Hierarchically porous iron/nitrogen-doped carbons (Fe-N-PC) were developed for the oxidation of ibuprofen (IBP) with peroxymonosulfate (PMS). The incorporation of trace-level iron and nitrogen dopants promoted the catalytic performance remarkably, leading to 4.8, 16.4 and 22.9-fold enhancement over N-doped carbon (N-PC), porous carbon (PC), and Fe-doped carbon (Fe-PC), respectively. Fe(III) was anchored in nitrogen-coordinated pots (Fe-N x ) in the sp 2 -hybridized carbon network, and graphitic-N could synergistically boost the catalysis. Notably, methyl phenyl sulfoxide (PMSO) transformation, quenching tests, in situ electrochemical analysis and Raman spectroscopy verified high-valent iron-oxo species and direct electron transfer pathway accounted for pollutant oxidation. The relationship between the kinetic constants (ln k obs ) and the oxidation peak potential ( E op ) of pollutants was established with good correlation, manifesting particular selectivity toward oxidizing electron-rich pollutants and great immunity to background inorganic ions and natural organic matters (NOMs) for real wastewater treatment . The deactivation mechanisms of Fe-N-PC were revealed via surface oxidation and dopant refabrication. This work delicates to deepen the understanding of the nonradical mechanisms and structure-oriented PMS activation by engineered carbonaceous materials .
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PubMed
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WATER RESEARCH
·
2022
·
IF 13.4
Haolin Xu,Rundong Chen,Sheng Liang,Zhenchao Lei,Wenxiao Zheng,Zhang Yan,Jianxin Cao,Chaohai Wei,Chunhua Feng
The formation of chlorinated byproducts represents a significant threat to the quality of the effluent treated using electrochemical advanced oxidation processes (EAOPs), thus spurring investigation into alleviating their production. This study presents a new strategy to minimize the release of chlorinated intermediates during the electrochemical oxidation of Ni-EDTA by establishing a dual mixed metal oxide (MMO)/Fe anode system. The results indicate that the dual-anode system achieved a substantially higher rate (0.141 min − 1 ) of Ni-EDTA destruction and accordingly allowed a more pronounced removal of aqueous Ni (from 39.85 to 0.63 mg L − 1 ) after alkaline precipitation, compared with its single MMO anode (0.017 min − 1 of Ni-EDTA removal, with 14.38 mg L − 1 Ni remaining) and single Fe anode (insignificant Ni-EDTA removal, with 38.37 mg L − 1 Ni remaining) counterparts. Compared to reactive chlorine species (RCS) produced from the single MMO anode system, Fe(IV) was in situ generated from the dual-anode system and was predominantly responsible for the attenuation of chlorinated byproducts and thus the decrease in the acute toxicity of the treated solution (evaluated using luminescent bacteria). The Fe(IV)-dominated dual-anode system also exhibited superior performance in removing multiple pollutants (including organic ligands, Ni, and phosphite) in the real electroless plating effluent. The findings suggest that the strategy for Fe(II) transition to Fe(IV) by active chlorine paves a new avenue for yielding less chlorinated products with lower toxicity when EAOPs are used to treat chloride-containing organic wastewater.
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LANGMUIR
·
2022
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IF 4.331
Jinling Li,Hui-Ling Peng,Changchun Wen,Peijing Xu,Xing-Can Shen,Cunji Gao
The therapeutic effect of photothermal therapy (PTT) and photodynamic therapy (PDT) is severely limited because of the shallow tissue penetration depth of the first near-infrared (NIR-I) light. Multifunctional nanotheranostics irradiated by the second near-infrared (NIR-II) light have received wide interest with respect to deeper tissue penetration, and sonodynamic therapy (SDT) synergistic phototherapy can achieve the complete elimination of tumors. Herein, we successfully constructed a single NIR-II light-induced nanotheranostic using cerium oxide (CeO2–x) with abundant oxygen vacancies for photoacoustic imaging-guided SDT-enhanced phototherapy for the first time. CeO2–x with surface crystalline disorder showed extensive NIR-II region absorption and an outstanding photothermal conversion ability. In addition, the CeO2–x layer with numerous oxygen defects can promote the separation of holes and electrons by ultrasound irradiation, which can remarkably enhance the efficacy of phototherapy to achieve high-efficiency tumor ablation. CeO2–x was surface modified with hyaluronic acid (HA) to prepare CeO2–x@HA to allow active tumor targeting efficiency. Both cell and animal experiments confirmed that all-in-one CeO2–x@HA exhibited a high therapeutic efficacy of SDT-enhanced PDT/PTT under 1064 nm laser irradiation, which achieved complete tumor eradication without systemic toxicity. This study significantly broadened the application of NIR-II-responsive CeO2–x for photoacoustic imaging-mediated SDT-enhanced phototherapy to the highly efficient and precise elimination of tumors.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Xi Li,Wenwen Zhang,Zhenxue Liu,Shiwen Wang,Xiao Zhang,Baokang Xu,Peng Yu,Yanhua Xu,Yongjun Sun
Co-based heterogeneous catalysts exhibit relatively high performance on peroxymonosulfate (PMS) activation for antibiotic pollution control in water. But the aggregation and loss of active components limit their expanded application. In this study, a 3D rose-like MoS 2 was designed and synthesized to anchor Co in its special lamellar structure and achieve its high dispersion. 98.9% of tetracycline (TC) was removed within 60 min with a mineralization rate of 50.5% under neutral condition. The accelerated valence cycle between Co 2+ and Co 3+ was the key to PMS activation and TC degradation. And the lamellar structure of MoS 2 endowed the catalyst with better stability and inhibited Co leaching. The influences of common anions (Cl − , HCO 3 − , H 2 PO 4 − , and SO 4 2− ) and humic acid in aqueous solution on TC degradation were systematically investigated. The catalytic mechanism of PMS activation and the generation of reactive oxygen species (ROS) over Co@MoS 2 were deeply investigated. The reduced biotoxicity of the intermediates indicated the potential of Co@MoS 2 /PMS system for the control of environmental risks caused by TC. This work provided a new insight for the design of metal-doped heterogeneous catalyst with high stability and a new direction for the remediation of antibiotic contamination in water.
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ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Tianyao Shen,Xiaojing Wang,Peng Xu,Chunyan Yang,Jiaqin Li,Peng Wang,Guangshan Zhang
Dielectric barrier discharge plasma (DBDP) is an emerging and promising advanced oxidation process (AOP) for wastewater treatment . After investigating the effect of input voltage, O 3 (generated by dielectric barrier discharge), and peroxydisulfate (PDS) dosage, the DBDP O3 /PDS system was established. With the assistance of PDS, the atrazine (ATZ) removal efficiency increased from 69.67% to 82.46% within 25 min. Synergistic effect calculation suggests that there were markedly synergies between DBDP, O 3 , and PDS. Under the effect of SO 4 −• , the total organic carbon (TOC) removal and dechlorination efficiency were significantly improved. In addition, the DBDP O3 /PDS system maintained the ATZ removal efficiency at a high level over a wide range of initial pH values. According to quenching experiments and electron paramagnetic resonance (EPR) detection, the dominant radical for ATZ degradation in the DBDP O3 /PDS system was HO • . A possible degradation pathway of ATZ was proposed based on density functional theory (DFT) analysis, quadrupole-time of flight-liquid chromatography/mass spectrometry (Q-TOF-LC/MS) results, and related literature. The acute toxicity to aquatic minnows and the developmental toxicity of intermediate products prediction confirmed that the DBDP O3 /PDS system could effectively reduce ATZ toxicity. The electrical energy per order ( E EO ) was 7.10 kWh m −3 order −1 illustrating that the DBDP O3 /PDS was a more energy-economic system than other energy-intensive processing technologies .
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Peng Xu,Peng Wang,Xiang Li,Rui Wei,Xiaojing Wang,Chunyan Yang,Tianyao Shen,Tong Zheng,Guangshan Zhang
CuO-Fe 2 O 3 /MXene was fabricated using a rapid microwave hydrothermal method and used for the enhanced peroxymonosulfate (PMS) activation and atrazine (ATZ) degradation. The ATZ degradation rate could reach up to nearly 100% within 60 min at pH = 6.4, with low dosage for CuO-Fe 2 O 3 /5% MXene (0.1 g‧L -1 ) and PMS (0.37 mM). Experimental results and DFT calculations showed that coexisting matter had little influence on ATZ degradation at low concentrations, indicating the excellent anti-interference capability of the system. Circulation and interaction of ≡Fe(III)/≡Fe(II) and ≡Cu(II)/≡Cu(I) produced SO 4 •- and •OH, O* and SO 5 •- could participate in the formation of 1 O 2 . Then, ATZ degradation pathways, including dealkylation, dichlorination-hydroxylation, alkyl hydroxylation, alkyl oxidation, olefination, and deamination-hydroxylation processes, were proposed based on DFT calculations and ESI-QTOF-MS/MS data. QSAR analysis illustrated that most intermediates were more environmentally friendly than ATZ. This study developed novel materials with superior catalytic performance for elimination of refractory organic pollutants in wastewater.
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LANGMUIR
·
2022
·
IF 4.331
Qiangtao Zhu,Dongyu Pan,Yangyi Sun,Dongming Qi
Hollow structures in TiO2 materials can enhance the photocatalytic properties by reducing the diffusion length and improving the accessibility of active sites for the reactants. However, existing approaches for preparing hollow TiO2 materials have two drawbacks that restrict their engineering applicability: first, a heavy reliance on templates to form a hollow structure, which makes the preparation laborious, complicated, and costly; second, difficult-to-achieve high crystallization while maintaining the small grain size in calcinated TiO2, which is crucial for enhancing photocatalytic activity. Herein, a simple, effective method is proposed that not only enables the preparation of hybrid TiO2–SiO2 hollow spheres without the template fabrication and removal process via microemulsion technology but also achieves both high crystallization and a small grain size in calcinated TiO2 at once through the calcination of amorphous TiO2 with organosilane at a high temperature of 850 °C. The prepared TiO2–SiO2 hollow spheres with tunable sizes demonstrate high photocatalytic activity with a maximum k value of 133.74 × 10–3 min–1, which is superior to commercial photocatalyst P25 (k = 114.97 × 10–3 min–1). In addition, Au can be doped in the hybrid TiO2–SiO2 shell to gain Au-doped hollow spheres that show a high k value of up to 694.14 × 10–3 min–1, which is 6 times larger than that of P25 and much better than that reported in the literature. This study not only provides an effective approach to stabilize and tune the grain growth of the TiO2 photocatalyst during calcination but also enables the simple preparation of hollow TiO2-based materials with controllable hollow nanostructures.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Li Chen,Tahir Maqbool,Ghazanfar Nazir,Congyu Hou,Yulong Yang,Jianning Guo,Xihui Zhang
Endocrine disrupting compounds (EDCs) in the aquatic systems are of growing concerns that could undermine drinking water safety. In this study, manganese (III) oxide (Mn 2 O 3 ) based catalytic ceramic membrane (CCM) was developed for the activation of peroxymonosulfate (PMS), and its applicability has been tested in degrading the ten different EDCs (including bisphenol analogs (BPs)) in drinking water. The CCMs were synthesized at different calcination temperatures i.e., 850, 950, and 1150 °C. Optimal performance of CCMs/PMS was achieved at a higher degree of calcination. The CCMs/PMS has shown a potential to effectively degrade the EDCs at higher concentrations (mg/L) to trace levels (ng/L). The CCMs/PMS system adopted a non-radical pathway of degrading the EDCs through the extensive generation of singlet oxygen ( 1 O 2 ), as confirmed using quenching experiments and electron paramagnetic resonance (EPR) spectroscopy. 1 O 2 -based oxidation process showed special selectivity for the decontamination of phenols and bisphenols. The long-term performance of CCMs/PMS showed good stability in degradation of the EDCs in drinking water, also with efficient mineralization (TOC removal >55%) and negligible release of Mn (0.004 wt%Mn/min). CCMs/PMS system also showed high potential in improving water quality by reducing the disinfection byproducts (DBPs) formation potential, highest recorded for bromodichloromethane (CHCl 2 Br, 100%) and lowest for dichloroacetic acids (TCAA, ∼50%). The study provided a highly efficient catalytic ceramic membrane based advanced oxidation process (AOPs) for effective degradation multiple of EDCs in drinking water, and the findings of this work can be a baseline for full-scale water treatment applications.
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