CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Lu-Lu Zhou,Peng-Xi Liu,Ying Ding,Jia-Rui Xi,Li-Juan Liu,Wei-Kang Wang,Juan Xu
Heterogeneous catalysts with hierarchically porous structure are highly efficient to catalyze chemical reactions. In this work, two-dimensional (2D) nano-flakes assembled flower-like NiO is fabricated and utilized for activating peroxydisulfate (PDS) to degrade organic pollutants bisphenol A (BPA). The results demonstrate that the prepared catalyst exhibits well organized flower structure composed of uniform 2D nano-flakes. PDS combines with the catalyst to form surface-activated NiO-PDS complex, subsequently depriving electrons from BPA. For the optimized NiO-12 catalyst, large specific surface area and hierarchically porous structure benefit to exposes abundant active sites while low resistance promotes electrons transfer, bringing the high BPA degradation rate constant of 0.28 min −1 under the condition of 20 mg/L initial concentration. NiO-12 exerts a capability of catalyzing PDS to mineralize 34% of practical packaging wastewater. This study provides a new strategy to fabricate hierarchical 2D porous catalysts for persulfate activation, with application potential in practical wastewater treatment.
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DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 48
·17911-17919
·
IF 4.39
Can Wang,Ruikang Zhang,Yucong Miao,Qihui Xue,Borong Yu,Yuanzhe Gao,Zhangang Han,Mingfei Shao
TiO2-based nanosheet materials with a core–shell structure are expected to be one of the promising photocatalysts for the degradation of organic pollution. It is a challenge to synthesize TiO2 by the desired nucleation and growth process, so most reported TiO2 core–shell photocatalysts are prepared using TiO2 as a core material. Layered double hydroxides (LDHs) are considered ideal platforms to grow TiO2in situ and further serve as additional components to improve the separation of photogenerated charge carriers. In this work, we report the design and fabrication of anatase TiO2-coated ZnAl-layered double oxide (LDO@TiO2) nanosheets, which involve the in situ growth of TiO2 on ZnAl-LDH followed by subsequent calcination treatment. The resulting LDO@TiO2 photocatalyst yields typical core–shell nanosheet morphology with a mesoporous structure, exhibiting excellent photodegradation and mineralization efficiency for organic pollution.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Yuexiang Wang,Hui Zhou,Jing Kong,Ming Shen
A broad-spectrum responsive organic-inorganic heterojunction was synthesized by in-situ self-assembled perylene diimide (PDIsm) through π-π stacking onto the surface of flower-like BiOCOOH. The PDIsm/BiOCOOH with different compositions exhibited enhanced photocatalytic degradation of levofloxacin under visible light irradiation. Among them, 10% PDIsm/BiOCOOH had the best photocatalytic activity, which was 4.6 and 14.1 times higher than pure PDIsm and BiOCOOH, respectively. The enhancement of photocatalytic activity was mainly attributed to the introduction of PDIsm which significantly improved the light absorption in almost the whole visible light range. Besides, the formed heterojunctions facilitate the separation and transfer of photogenerated charge carriers. In addition, after five cycles of degradation, the degradation rate of the PDIsm/BiOCOOH composite for levofloxacin hydrochloride remained above 75%, indicating its good photocatalytic activity and stability. Furthermore, free radical capture experiments and electron spin resonance experiments verify that •O 2 ‾ and h + were the active species generated in the photocatalytic process. Combining the experimental results of high-performance liquid chromatography-mass spectrometry, a possible photocatalytic reaction mechanism was proposed. This work provides a way to prepare an efficient organic-inorganic photocatalyst , which can potentially be utilized in environmental remediation under visible light.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Xu Chen,Linfeng Su,Shaojie Zhang,Li Yi,Hao Yang,Yingjie Wen,Jie Sun,Zhiyi Lu
The aluminosilicate-based heterogeneous catalysts hold great promise for industrial catalytic ozonation ; however, the lack of exploration into novel active sites and mechanism studies has impeded their development. In this work, we demonstrate that labile oxygen (O lab ) can be generated in mullite (mullite-O lab ) by the introduction of extra Al-O 4 tetrahedral units. In our experiments, mullite-O lab exhibits excellent performance in terms of catalytic ozone activation, with a degradation rate of 87.4 % within 15 min for nonbiodegradable atrazine, corresponding to a high quasi-first-order rate constant ( k , 0.112 min −1 ), while the degradation constant is close to 0 for mullite without O lab . Operando Raman and density functional theory (DFT) simulations further reveal that O lab activates ozone via a novel surface peroxide pathway to generate surface O lab -O* species with a high oxidizing ability. The mullite-O lab is stable with an average Al 3+ leaching of 0.339 ppm during cycling, meeting the effluent discharge standard of the total Al. Moreover, we achieve the kilogram synthesis of mullite-O lab , which shows promising activity in the catalytic ozonation of acrylic fiber wastewater, with the chemical oxygen demand (COD) and total organic carbon (TOC) removal rates of 46.0 %±4.8 % and 24.9 %±2.8 % for 5 cycles. This work is the first to demonstrate the role of O lab in ozone activation and provides an advanced mullite-O lab catalyst for future nonbiodegradable wastewater treatment .
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CATALYSIS LETTERS
·
2023
·
IF 2.8
Su Zheng,Sun Yu,Zhang Qi,Wang Jia,Zhou Wenqi,Zhou Suyin,Zhang Jinlong,Liu Yongdi,Zhou Liang,Lei Juying
Photocatalytic cofactor regeneration often encounters the problem of insufficient stability of reduced nicotinamide adenine dinucleotide hydrogen (NADH) regeneration due to the influence of reactive oxygen species. Here, we obtained Pt-loaded CdS nanorods (CdS NRs) with a one-dimensional (1D) rod-like structure by simple hydrothermal and photo-deposition methods. The yield of NADH improved by 52.54% within 40 min. Superoxide radical (·O 2 − ) had been proven to be the main reactive species that leaded to unwanted oxidation after NADH regeneration. After loading Pt, the formation of Schottky junctions between Pt and CdS NRs promoted the separation and migration of photogenerated carriers, resulting in a tendency of ·O 2 − to shift toward hydroxyl radical (·OH). ·OH produces additional intermediates in the oxidation of NADH compared to ·O 2 − , which inhibits the unwanted oxidation of NADH. Meanwhile, the conduction band position of Pt/CdS shifted positively and the ability to reduce O 2 was weakened, thus the ·O 2 − in the system was reduced, which weakened the oxidation of NADH and significantly improved the stability of NADH regeneration. These studies provide a new reference for applying loaded metal catalysts to the stable regeneration of NADH. Graphical Abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Jiayu Du,Decai Liu,Zhiyong Zhang,Huiying Ai,Ming-Lai Fu,Wenjie Sun,Baoling Yuan
The widespread use of chlorine during disinfection has led to the problems of disinfection by-products (DBPs). Recently, the combination of ultraviolet (UV, 254 nm) and vacuum ultraviolet (VUV, 185 nm) with chlorine has been considered a promising strategy to mitigate the formation of DBPs. This study systematically evaluated the efficacy of six different disinfection methods in abating humic acid (HA), a common precursor of DBPs (UV-Chlorine, VUV/UV-Chlorine, Chlorine-UV, Chlorine-VUV/UV, UV/Chlorine, and VUV/UV/Chlorine). Under 40 mJ/cm 2 UV fluence and 3 mg/L chlorine dose, the synergistic processes yielded DBP levels below 20 μg/L, whereas sequential disinfection resulted in DBP levels exceeding 100 μg/L. Additionally, there was no significant difference in the formation of DBPs between the two methods of chlorination followed by irradiation. However, for irradiation followed by chlorination, the addition of VUV led to an increase of 50 μg/L in trihalomethanes (THMs). As the irradiation time increased, the inclusion of VUV demonstrated enhanced control of DBP levels in the sequential disinfection process. Moreover, compared to UV/Chlorine, at 13 mg/L chlorine dose in VUV/UV/Chlorine process, the inclusion of VUV expedited the appearance of peak DBPs by two minutes and reduced the peak value by 25.6 %, but the DBP yield was 12.9 times higher than that at a chlorine dose of 3 mg/L. This study, comparing six combination disinfection methods, will provide deeper insights into precursor abatement and DBP control during drinking water disinfection.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Longjie Liu,Zeyang Lu,Wanling Cai,Gary Owens,Zuliang Chen
Reduced graphene oxide/iron nanoparticles (rGO/FeNPs) synthesized by the chemical method have been used in Fenton oxidation of organic contaminants , yet little is known about biosynthesized rGO/FeNPs using green tea extract (GT) as how to activate persulfate in sulfate radical-based advanced oxidation processes . In this study, rGO/FeNPs were used to activate peroxydisulfate (PDS) for 17β-estradiol (βE 2 ) and estriol (E 3 ) removal. The rGO/FeNPs-PDS system removed 83.6% of βE 2 and 62.5% of E 3 within 240 min, which was confirmed by a combination of adsorption and degradation via both radical and non-radical pathways. Four main reactive species in βE 2 and E 3 degradation were observed, i.e., hydroxyl radical (·OH), sulfate radical (SO 4 ·− ), singlet oxygen ( 1 O 2 ) and electron transfer , with the respective contributions of ·OH (32.9 and 34.7%), SO 4 ·− (16.1 and 19.7%), 1 O 2 (12.2 and 14.1%) and electron transfer (8.0 and 7.2%). Analysis of X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FTIR), Electron Paramagnetic Resonance (EPR) and electrochemical measurements all indicated that beside the well-known role of Fe, C O from rGO through the generation of ·OH, SO 4 ·− , 1 O 2 and electron transfer, as well as GT through electron transfer also participated in the activation of PDS. Finally, the degradation pathways of βE 2 /E 3 were proposed. Overall, this study provides a new insight into the biosynthesis of rGO/FeNPs to activate PDS for the oxidation of mixed emerging contaminants .
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Hui Wang,Yuhan Xiong,Yi He,Lingru Kong,Lan Ding,Rui Wu,Xin-Lei Gao,Jie Ding,Nanqi Ren
Covalent organic frameworks (COFs) have attracted great attention in photocatalysis, but the high recombination rate of photo-induced electron − hole pairs limits their photocatalytic performance. We report a synergy strategy based on the donor − acceptor (D-A) effect and Au clusters to enable the effective transfer and separation of photogenerated electrons to rationally fabricate visible light driven photocatalyst (MT-COF-Au) for the degradation of benzotriazole (BTA). MT-COF-Au displayed superior photocatalytic activity. The degradation efficiency of BTA was 93 % within 110 min, which was significantly improved 6.7 times than COF. For BTA degradation, O 2 − played a prominent role based on reactive species trapping experiments. The products of the last stage of the reaction were ketone, imidazole, acetamide, and nitrogen, which were formed via ring opening and isomerization reactions. MT-COF-Au could be reused for at least 5 cycles without significantly deteriorating its catalytic activity. Experiments and theory calculations confirmed the electron transfer mode and photocatalytic mechanism. This work provides new prospects for the design and synthesis of high-efficiency photocatalyst photocatalysts.
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MICROCHIMICA ACTA
·
2023
·Vol. 191
·期 1
·1-11
·
IF 5.7
Guo Zhanghong,Zhou Lin,Chen Xuan,Song Qijun
Carbon-coated copper nanocrystals (CuNCs) with peroxidase-like activity were hydrothermally prepared by using copper acetate, citric acid (CA) and histidine (His) as the precursors. Various shaped CuNCs, including urchin-like, slab-like and spherical appearance were facilely prepared by addition of different amount of NaNO 2 in the precursor solutions. When 3,3′,5,5′-tetramethylbenzidine (TMB) was used as the substrate, the CuNCs with urchin-like appearance have greatest peroxidase-like activity and their Michaelis–Menten constant ( K m ) and the maximum rate constant (ν max ) are respectively 8.8 and 1.2 times higher than that obtained from horseradish peroxidase (HRP). The production of reactive oxygen species (ROS) was confirmed by radical quenching and electron spin resonance (ESR) tests. Subsequent studies have found that the CuNCs catalyzed color reaction of TMB can be selectively quenched by the environmental pollutant 2,4-dinitrophenylhydrazine (2,4-DNPH). Thus a new colorimetric method for the determination of 2,4-DNPH with a linear range of 0.60–20 µM was developed and a limit of detection (LOD) as low as 0.166 µM was achieved. The results obtained not only reveal the tunability of the peroxidase-like activity of Cu-based nanomaterials, but also provide a new method for the sensitive determination of environmental contaminate. Graphical abstract
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 48
·期 4
·1757-1770
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IF 3.3
Ling Tao,Jiepu Zhang,Fangke Yu
In this study, in order to achieve efficient activation of persulfate, we added MoS2 as a co-catalyst to the iron, cobalt and nitrogen modified biochar (Fe–Co–N–BC) catalytic system. Analytical methods such as scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) demonstrated that the MoS2/Co–Fe–N–BC catalytic materials were successfully prepared. In the MoS2/Fe–Co–N–BC/PMS system, 97.5% of PFOA was removed within 180 min with Kobs of 0.074 min−1. Composites with different mass ratios of MoS2 and Co–Fe–N–BC/PMS in the non-homogeneous PMS system both exhibit excellent catalytic efficiency for TOC removal. In particular, MoS2/Fe–Co–N–BC obtained extraordinary catalytic efficiency through synergistic radical (SO4˙−, ˙OH) and non-radical (1O2, FeIV and FeV) processes, which was proved by the quenching experiments and the EPR testing. The analysis of the activation mechanism reveals that the three redox ion pairs Fe2+/Fe3+, Co2+/Co3+ and Mo4+/Mo6+ simultaneously participated in the activation of PMS, realizing multi-path electron transfer. And MoS2 played an excellent co-catalysis role in promoting the cycling of the valence states of the ions. Compared to Fe3+ and Co3+, the low valence states of Fe2+ and Co2+ can activate PMS more rapidly and produce more ˙OH and SO4˙−. However, the recycling efficiency of Fe2+ and Co3+ in the Fe–Co–N–BC system is low, and the presence of MoS2 improves the efficiency of Fe3+ and Co3+ reduction to Fe2+ and Co2+, respectively. The possible degradation pathways of PFOA were proposed. This study provides some references for the design of polymetallic-doped catalysts to degrade difficult-to-degrade organic pollutants.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Jiayu Zhang,Shan Qiu,Fengxia Deng
The electro-Fenton (EF) process generates H 2 O 2 through the 2e- oxygen reduction reaction (ORR), which is subsequently activated to •OH by iron-based catalysts. To alleviate the potential risk of external Fe-based catalysts, along with metal dissolution in acidic or neutral environments, in this study we employed oxygen-doped carbon nanotubes (OCNT) as a bifunctional, metal-free cathode to establish a metal-free EF process for organic pollutant degradation. The results demonstrate that the metal-free electrode has excellent H 2 O 2 accumulation (12 mg L −1 cm −1 ) and degrades sulfathiazole (STZ) with 97.05 % efficiency in 180 min with an explanation kinetic of 0.0189 min −1 . For the first time, this enhancement came from the dual active site centers in OCNT: Ⅰ) -COOH and defects active sites were responsible for H 2 O 2 production, Ⅱ) then -C O triggered H 2 O 2 into •OH, avoiding the introduction of metal-based catalysts. These findings suggest that the EF system with in situ oxygen-doped cathodes have great potential for treating antibiotic wastewater.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Binbin Tan,Jing Wang,Yao Deng,Huidi Zhang,Jiang Wang,Zhihao Zhang,Wenlei Wang
The key to enhancing the activation efficiency of peroxydisulfate (PDS) lies in facilitating the adsorption of PDS and accelerating the rate of electron transfer at the interface. In this work, the oxygen vacancy (Ovs) concentration of ultrathin Bi 4 Ti 3 O 12 (BTO) was controlled in situ by high-energy electron beam bombardment. BTO V -300 exhibited a significant activation effect on PDS. The degradation rate constant ( k obs ) for the removal of ciprofloxacin (CIP) was measured to be 0.2080 min −1 under visible light irradiation, which was 3.71 times greater than that of the original BTO. Density functional theory calculations uncovered the principal role of oxygen vacancies as active sites for PDS activation. Introducing OVs significantly boosted the adsorption energy of PDS on BTO and lengthened the O O bond of PDS. This study represents the potential mechanism behind the activation of PDS by BTO V and provides valuable insights for enhancing the photoactivation efficiency of PDS.
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