CHINESE CHEMICAL LETTERS
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2023
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IF 9.1
Han-Qing Zhao,Peili Lu,Fei Chen,Chen-Xuan Li,Rui Yan,Yang Mu
Sulfide oxidation under aerobic conditions can produce active oxygen for the transformation of organic pollutants in aquatic environments. However, the catalytic performance of transition metal-supported carbon material on this process is poor understood. This study found that Co-loaded carbon nanotubes (CNTs) was able to realize the efficient aerobic transformation of antibiotic ciprofloxacin (CIP) by sulfide, with the pseudo -first order reaction rate constant improved from 0.013 h −1 without catalyst to 0.44–0.71 h −1 with 100 mg/L Co-loaded CNTs. Singlet oxygen ( 1 O 2 ) was the main active specie playing key roles in the process of CIP aerobic transformation with presence of Co-loaded CNTs. Mechanism studies indicated that the excellent electron transfer ability of Co-loaded CNTs might play an important role to promote the electron transfer and facilitate the formation of intermediate H 2 O 2 and 1 O 2 . Additionally, the Co-loaded CNTs/sulfide system effectively reduced the acute toxicity of organic pollutant, and Co-loaded CNTs showed remarkable cycling stability and negligible leaching. This study gives a better understanding for the Co-loaded CNTs mediated aerobic antibiotics transformation by sulfide, and provide a reference for the application of Co-loaded carbon materials on organics aerobic transformation by sulfide.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2023
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IF 5.2
Xuyang Zou,Jiangzhang Wang,Guojun Lv,Tao Wang,Chaoyi Zhou,Yan Chen,Jialing Shen,Shihao Su,Zhongmin Liu
Impregnation handlement can load highly dispersed CuO nanoparticles on the Fe-MFI zeolite and effectively enhances its catalytic activity in the tetracycline degradation reactions, but encounters serious re-usability problems. In this work, Fe-MFI zeolite-encapsulated copper oxide CuO@Fe-MFI was prepared via one-step hydrothermal synthesis and utilized as heterogeneous catalyst for the removal of tetracycline. The obtained 2CuO@1Fe-MFI zeolite presented a external surface area of 270 m 2 /g, which was almost 5.5 folds of 2CuO/1Fe-MFI zeolite obtained by impregnation handlement. In addition, there may be a near-neighbor effect between encapsulated CuO and framework iron evidenced by the shifts of UV–Vis absorption bands as well as binding energies for Fe 2p and Cu 2p. At pH = 7.0, 2CuO@1Fe-MFI zeolite attained the largest tetracycline removal rate of 99.6% within 20 min at experimental conditions: [TCE] = 50 mg/L, [Catalyst] = 0.5 g/L, [PMS] = 1.0 g/L, 323 K, and the biggest degradation rate constant of 2.42 min −1 , which was almost 11.1 folds of that for 2CuO/1Fe-MFI zeolite. The large external surface area and near-neighbor effect together gave rise to the excellent tetracycline degradation performance for 2CuO@1Fe-MFI zeolite. On the same time, the obtained 2CuO@1Fe-MFI zeolite can be reused for more than five times. Quenching experiments and EPR characterizations demonstrated the reactive species for tetracycline removal over 2CuO@1Fe-MFI zeolite were •OH, SO 4 • − , •O 2 − and 1 O 2 species, and moreover 1 O 2 served as the major active species. Furthermore, possible tetracycline degradation pathways over 2CuO@1Fe-MFI zeolite were proposed.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Zilong Zhao,Yatao Ren,Shuyu Qi,Zigong Ning,Xing Wang,Wenyi Dong,Hongjie Wang
Heavy metal complexes pose a challenge in terms of their resistance to removal due to their stable and intricate structure. In this study, we explored the utilization of Fe and N co-doped biochar derived from rice husk (Fe-N-RHBC) as catalytic particle electrodes in a three-dimensional electro-Fenton (3D-EF) system for the decomplexation and removal of a model pollutant, Ni-EDTA. The characterization analysis and comparison of catalytic activities confirmed the beneficial effects of Fe and N co-doping on various aspects, such as the types of active sites, interfacial electron transfer properties, and H 2 O 2 decomposition capacity. Compared to other investigated oxidation systems, the 3D-EF process demonstrated rapid removal of Ni-EDTA within the initial minute, with a maximum H 2 O 2 utilization of 99.1% after 30 min. The prepared catalytic particle electrodes exhibited high stability and catalytic capacity even after three consecutive cycles. Throughout the reaction, several processes, including anode oxidation, particle electrode polarization, catalysis, and adsorption of Fe-N-RHBC, as well as cathodic electro-deposition, synergistically contributed to the treatment of Ni-EDTA. The surface-bound O 2 − radicals and 1 O 2 generated by the Fe-N-RHBC catalytic particle electrode played a crucial role in the decomplexation and removal of Ni-EDTA. Building upon these findings, we further proposed potential mechanisms for the removal of Ni-EDTA in the 3D-EF system using the Fe-N-RHBC catalytic particle electrode.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jun Hu,Wenji Cai,Shangkun Li,Jun Wu,Zhimin Qiang
Cupric and cuprous oxides (CuO and Cu 2 O) are the main corrosion products of copper pipes; peroxymonosulfate (PMS) is a good drinking water disinfectant; micropollutants are ubiquitous in the factory waters. Corrosion products influence the micropollutant transformation under the action of disinfectants. This study compared the conversion of diatrizoate (DTZ) with PMS as a disinfectant under the catalysis of CuO (Cu(II)PS) and Cu 2 O (Cu(I)PS). The pseudo-first-order constant ( k obs ) for the DTZ degradation in the Cu(II)PS was 11.8 times that in the Cu(I)PS, with values of 0.092 and 0.0078 min −1 , respectively. SO 4 − and HO played dominant roles in the Cu(II)PS, while O 2 − and 1 O 2 were the primary contributors in the Cu(I)PS. The yield ratio of reactive species were 92.8% and 69.6% in the Cu(II)PS and Cu(I)PS, respectively. The DTZ degradation was promoted by the increase of CuO dose, while inhibited by the increase of Cu 2 O dose (0.1–1.0 g L −1 ). In both Cu(II)PS and Cu(I)PS, the DTZ degradation was enhanced by the increasing PMS dose (10–100 mg L −1 ) and neutral pH (7.0), whereas weakened by water matrix (NOM, HCO 3 − and Cl − ). The total organic iodine was mainly converted to IO 3 − with a ratio of 45.3 and 7.4% in the Cu(II)PS and Cu(I)PS, respectively. In the Cu(II)PS, the DTZ transformation was mainly through the amide hydrolysis followed by amino oxidation and stepwise deiodination followed by hydroxyl addition. However, hydroxyl addition is not thought to occur in the Cu(I)PS since the related intermediates have not been identified. The study helps to comprehensively understand the conversion of iodine-containing micropollutants in copper pipes when PMS is a disinfectant.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Heng Li,Xiaoying Jin,Qin Li,Zuliang Chen
Slow electron migration in iron sulfide nanoparticles (C-FeS NPs) synthesized by co-precipitation severely limits the activation performance of hydrogen peroxide (H 2 O 2 ). Herein, a biofunctional FeS NPs (P-FeS NPs) derived from Pinus massoniana Lamb biomass, with interface coupling effect, was used for enhanced H 2 O 2 activation and norfloxacin (NOR) degradation. It was discovered that P-FeS NPs exhibited superior catalytic activity (100%) compared to C-FeS NPs (53.1%). Fe atoms of FeS NPs and hydroxyl groups (–OH) of Pinus massoniana Lamb biomass were mutually coupled to produce Fe-OH interfacial sites, which significantly increased the generation of multi-reactive species by accelerating the transfer of electrons across interfaces. Additionally, radical quenching tests elucidated that singlet oxygen ( 1 O 2 ) (66.6%) played a leading role, while hydroxyl radicals (•OH) (14.5%) and superoxide radicals (•O 2 – ) (18.9%) were secondary oxidants. Finally, P-FeS NPs showed a high tolerance to a wide range of pH conditions and could remove 96.4% NOR from wastewater. Overall, this work generates important insights into understanding how green sustainable interfacial catalysts can accelerate catalytic activity.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Jun Chen,Shangqing Xia,Xiaohong Yang,Xue Li,Zhaoming Chen,Zihui Song,Yutong Wang,Zongsheng Zhan,Jie Jin,Dongliang Shao
New technology is required for the effective disinfection of pathogenic bacteria in water. A novel type of activator material (Fe-Mg-Mt-SS) was prepared using bimetallic iron-magnesium (Fe-Mg), montmorillonite (Mt), and sewage sludge carbon (SS) and applied it for disinfection. The specific surface area of Fe-Mg-Mt-SS was 115.72 m 2 /g, and the spatial structure of Fe-Mg-Mt-SS was orderly and layered. Mt played a role in frame support, and Fe-Mg was integrated into the structure in an orderly manner. Fe-Mg-Mt-SS effectively activated persulfate (PS) to disinfect Escherichia coli ( E. coli ) in water, with a disinfection rate of 7.00 lg of E. coli within 80 min in the PS/Fe-Mg-Mt-SS system, and the high disinfection rate was stable under different pH and elevated temperatures. Fe-Mg-Mt-SS showed broad spectrum disinfectant efficiency against other bacteria ( Staphylococcus aureus, Pseudomonas aeruginosa, and Bacillus subtilis ). Fe-Mg-Mt-SS activated PS killed E. coli mainly by producing hydroxyl and oxygen radicals, which damaged the E. coli cell membrane. Bimetallic activation with Fe and Mg synergistically activated PS, graphitised SS had more orderly spatial and laminar structures, and Mt improved the thermal stability and layer spacing of Fe-Mg-Mt-SS, which facilitated better metal insertion and improved its activation properties. The preparation of Fe-Mg-Mt-SS and activation of PS provide a new technology for the disinfection of pathogenic bacteria in water.
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BIORESOURCE TECHNOLOGY
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2023
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IF 11.4
Shuo Li,Yingnan Liu,Heshan Zheng,Junfeng Niu,Yoong Kit Leong,Duu-Jong Lee,Jo-Shu Chang
Corn straw and sludge-derived biochar composite (BC) loaded with CoFe 2 O 4 was successfully prepared to activate peracetic acid (PAA) for efficient degradation of tetracycline hydrochloride (TCH). Within 60 s, 96 % TCH removal efficiency was achieved through a non-free radical degradation pathway, primarily driven by singlet oxygen ( 1 O 2 ). The mechanism involves the electron-rich groups on the biochar surface, which facilitate the cleavage of the PAA O O bond to generate •O 2 − / 1 O 2 and provide electrons to induce the formation of high-valent Fe(IV) and Co(IV). The oxygen vacancies on the surface of the CoFe 2 O 4 -loaded biochar composite (CFB-2) contribute partially to 1 O 2 production through their transformation into a metastable intermediate with dissolved oxygen. Moreover, elevated temperatures further enhance PAA activation by CFB-2, leading to increased reactive oxygen species (ROS) production through PAA decomposition, thereby promoting TCH removal. This study offers new insights into the catalysis of metal-loaded biochar for efficient TCH degradation via non-free radical generation.
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ACS Catalysis
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2023
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IF 12.9
Wei Lin,Yi Chen,Yuexing Zhang,Yongsheng Zhang,Jianshe Wang,Liucheng Wang,Chunbao Charles Xu,Renfeng Nie
Ni–ReOx bimetallic catalysts (Ni–ReOx/TiO2) were prepared through a successive impregnation method, which is extremely active in furfural (FAL) hydrogenation to tetrahydrofurfuryl alcohol (THFOL) under mild reaction conditions. For instance, high FAL initial reaction rate (439.4 mmol/g-Ni/h) and THFOL formation rate (80.4 mmol/g-Ni/h) were achieved over Ni–5ReOx/TiO2, which are 13.2 and 6.6 times higher than those of Ni/TiO2, respectively. The unique catalyst reactivity derives from rich Lewis acidic ReOx and intimate electron interaction of ReOx with Ni NPs. Kinetic studies reveal that ReOx decoration decreases the activation barrier of −C═O hydrogenation other than the furan ring. Mechanism studies show that ReOx has a good affinity for C═O and H2 and favors hydrogen spillover and C═O bond activation on Ni, thus reinforcing the synergistic effect of Ni and ReOx. This catalyst is versatile for various furan aldehydes and is relatively stable for 5 times recycling, showing relative potential for industrial application.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Guosheng Zhang,Huiwen Ding,Jianqiao Wang,Pengfei Xiao
This study reports the preparation of an affordable Ni-doped CoMoO 4 catalyst (Ni X Co 1−X MoO 4 (X = 0–1)) via a hydrothermal method by substituting Co with Ni and investigated the performance and mechanism of Ni X Co 1−X MoO 4 catalyzing peroxymonosulfate (PMS) to degrade organic pollutants for the first time. Based on characterization, it can be observed that the synthesized Ni 0.5 Co 0.5 MoO 4 catalyst exhibited excellent surface properties and structural stability. Under optimal conditions, Ni 0.5 Co 0.5 MoO 4 and PMS synergistically achieved over 95% degradation of chloroquine phosphate (CQP) within 20 min, demonstrating superior performance. The degradation system maintained high efficiency under interference different interfering substances in aqueous media, exhibiting excellent tolerance and practicality. Elemental analysis and mechanistic studies of the catalyst showed that Ni doping promoted the reduction between Co 2+ /Co 3+ and Mo 4+ /Mo 6+ , which is critical for catalyst durability and reusability. The quenching experiment and electron paramagnetic resonance (EPR) show that the 1 O 2 generated through non-free radical pathways represented the predominant reactive species. A total of 19 intermediates were detected by LC-MS during degradation and possible pathways for CQP degradation were proposed and toxicity evaluation. After 5 cycles, the catalyst still showed good stability. Ni 0.5 Co 0.5 MoO 4 challenges including poor activation, metal ion leaching and low recovery of transition metal catalysts were addressed. This work offers new insights for the design of atom-doped spinel catalysts for catalytic oxidation and mechanism research. The Ni 0.5 Co 0.5 MoO 4 /PMS catalytic system can be extended to the treatment of other organic pollutants and even applied in the processing of high-concentration organic wastewater that requires rapid treatment, offering broader prospects for practical applications.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2023
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IF 5.8
Zhong Dengjie,Liu Peng,Liu Yi,Xu Yunlan
The Zn/Fe@N-doped porous graphitic carbon catalyst (Zn/Fe@PCN) was successfully produced through one-step pyrolysis of g-C 3 N 4 and Zn/Fe-MOF and was used for the activation of persulfate (PS) for the degradation of RhB. The Zn/Fe@PCN/PS system was able to degrade 95.92% of RhB in 30 min at a rate of 0.6453 min −1 when RhB was concentrated at 50 mg L −1 . The efficient degradation of RhB is primarily realized through the synergistic activation of PS by Zn, Fe, and N to produce reactive oxygen species 1 O 2 , \(\cdot{\mathrm{O}}_2^-\) , \(\cdot \mathrm{SO}_4^-\) , and ·OH. Zn 0 /Fe 0 in Zn/Fe@PCN forms a galvanic cell with carbon to release electrons to join in the activation of PS. The doping of Zn not only provides sufficient electrons for the activation of PS but also promotes the effective reduction of Fe 2+ and thus the Fe 2+ /Fe 3+ cycle. The N doping accelerates the electron transfer during the reaction progress.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Wei Lin,Yuexing Zhang,Zixu Ma,Zhiwei Sun,Xiaolong Liu,Chunbao Charles Xu,Renfeng Nie
Selectivity controlling is a crucial and challenging issue for the hydrogenation of furfural (FAL) to cyclopentanone (CPO). Herein, Ni 3 Sn 2 -ReO x /TiO 2 is synthesized via successive impregnation and exhibits full conversion and 92.5 % CPO selectivity under 3.0 MPa H 2 at 140 °C, which are much higher than those of Ni/TiO 2 and Ni 3 Sn 2 /TiO 2 . Characterizations show that Ni 3 Sn 2 is the main active phase that remarkably restrains the over-hydrogenation of the furan ring, while ReO x plays an electrophile or Lewis acid site to activate C-OH of furfuryl alcohol and induces its rearrangement. DFT calculations verify that Sn doping weakens the furan ring adsorption on Ni 3 Sn 2 and shifts its adsorption configuration, which consequently inhibits side reactions and favors the metal-acid (Ni 3 Sn 2 -ReO x ) synergy. The catalyst is stable, recyclable and also active at even 0.5 MPa H 2 and 80 °C. This study provides an advanced strategy for the rational design of superior catalysts for tuning product selectivity, with practical potential for upgrading biomass-derived platform molecules.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Xiaoyue Zhou,Yunying Liu,Yingqi Miao,Wenwen He,Yanan Pan,Adela Jing Li,Junhao Qin,Huashou Li,Renli Yin,Rongliang Qiu
Piezo-photocatalytic processes based on heterogeneous catalysts, by establishing electronic fast track to realize electronic storage and conversion, are proved to be effective ways to improve the efficiency of PMS activation. Herein, α-SnWO 4 /ZnO catalyst with p-n heterojunction was constructed to testify the piezo-photocatalytic effect on peroxymonosulfate (PMS) activation for pollution control. The decomposition rate of carbamazepine (CBZ) in the piezo-photocatalytic PMS activation process by α-SnWO 4 /ZnO heterojunction was 12.6 and 5.2 times to that by ZnO and α-SnWO 4 processes, respectively. In addition, the total organic carbon (TOC) removal rate of CBZ reached 89%, and TOC in the actual water body was also effectively removed. Free radical quenching and detection experiments showed that nonradicals ( 1 O 2 ) and free radicals (O 2 − , OH) were the mainly active species of the process, by which the toxicity of the intermediates of CBZ was significantly reduced by the combination of the radical and nonradical pathways through hydroxylation and singlet oxygen oxidation . Furthermore, the influences of the experimental factors, including the initial pH, PMS concentration, temperature and reuse of catalysts on CBZ degradation were evaluated. Notably, the activation energy (Ea) in this work was calculated as 34.2 kJ mol −1 , which was lower than that of other reported systems. Overall, this work can scientifically guide the design of high-performance piezo-photocatalysts to use common metals for efficient activation of PMS as economical alternatives over expensive rare metal catalysts for water purification.
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