ACS Applied Materials & Interfaces
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2021
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IF 9.229
Xiaosheng Du,Linzhao Jin,Sha Deng,Mi Zhou,Zongliang Du,Xu Cheng,Haibo Wang
Conventional polymeric phase change materials (PCMs) exhibit good shape stability, large energy storage density, and satisfactory chemical stability, but they cannot be recycled and self-healed due to their permanent cross-linking structure. Additionally, the high flammability of organic PCMs seriously restricts their applications for thermal energy storage (TES). Therefore, it is urgently required to explore PCM composites exhibiting superior recyclability, good self-healing capability, and excellent flame retardancy simultaneously. Herein, tri-maleimide end-capped cyclotriphosphazene flame retardant (TMCTP) was synthesized via the nucleophilic substitution between 1,3,5,2,4,6-triazatriphosphorine-2,2,4,4,6,6-hexachloride and N-(2-hydroxyethyl)maleimide. Then, novel dynamically cross-linked PCM composites (FPCMs) with superior recyclability, good self-healing capability, and excellent flame retardancy were fabricated by bonding PEG and TMCTP to polymeric skeleton via reversible furan/maleimide Diels–Alder (DA) reaction. TMCTP, which covalently and dynamically binding in the polymeric FPCMs, acted not only as an efficient flame retardant for reducing the flammability of PCM composites but also as dynamic cross-linking skeletons for thermally induced self-healing and recycling. Differential scanning calorimetry (DSC) analysis confirmed the reversible energy storage and release ability of FPCMs. Due to its reversible DA covalent bonds, the introduction of TMCTP endowed the FPCMs with considerably increased self-healing efficiency (up to 93.1%) and recyclability efficiency (94.6%). Moreover, with the introduction of TMCTP into FPCMs, the heat release rate (HRR) and total heat release (THR) significantly decreased, while the char residue and limiting oxygen index (LOI) value increased, confirming that the flame retardancy of FPCMs greatly improved. Hence, the synthesized FPCMs show enormous potential in TES applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Xin Chen,Ming Zhang,Haowei Qin,Jiancheng Zhou,Quanhao Shen,Ke Wang,Wenshuai Chen,Maochang Liu,Naixu Li
The perovskite-type LaFeO 3 serves as a promising photo-Fenton-like catalyst, but its low adsorption ability and catalytic activity inhibit the effective removal of ofloxacin. Herein, the LaFeO 3 and lignin-biochar composites were fabricated by a facile sol–gel pyrolysis route. As compared with LaFeO 3 nanoparticles, the LaFeO 3 /lignin-biochar composites showed better adsorption and degradation ability due to the synergistic effect between LaFeO 3 nanoparticles and lignin-biochar. Compared with LaFeO 3 , the adsorption capacity of LaFeO 3 /lignin-biochar for ofloxacin increased from 0.72 to 30.4 mg·g −1 . Importantly, this catalyst exhibited the improved degradation efficiency of ofloxacin during 75 min (95.6 % for LaFeO 3 /lignin-biochar Vs 53.4 % for LaFeO 3 ) as the adsorption process was combined with the photo-Fenton-like process. Notably, the lignin-biochar in the LaFeO 3 /lignin-biochar composites decreased the bandgap of LaFeO 3 nanoparticles from 2.10 eV to 1.79 eV due to the interface interaction between LaFeO 3 and lignin-biochar, facilitating the enhanced photo-Fenton-like activity. The hydroxyl radicals that were generated in the photo-Fenton-like process effectively induced the oxidative degradation of ofloxacin, which was confirmed by free radical capture experiments and ESR characterization. Moreover, the photo-Fenton-like degradation pathway of ofloxacin was proposed according to LC-MS analyses, and the toxicity analysis of degradation intermediates was further carried out. Hence, the LaFeO 3 /lignin-biochar composite was a promising photo-Fenton-like catalyst to eliminate ofloxacin via coupling of adsorption and photo-Fenton-like processes.
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Vietnam Journal of Chemistry
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2021
·Vol. 59
·期 6
·813-822
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IF 0
Nguyen Trung Dung,Vu Dinh Thao,Nguyen Nhat Huy
In this study, the CuCoFe-layered double hydroxide was employed for the degradation of glyphosate in water via peroxymonosulfate (PMS) activation. Scanning electron microscopy, X-ray powder diffraction, energy-dispersive X-ray spectroscopy, Fourier-transform infrared spectroscopy, and Brunauer-Emmett-Teller analyses were used to characterize the material. The effects of the catalytic system, initial solution pH, and catalyst and PMS dose on the degradation efficiency of glyphosate were investigated. The results indicated that after 6 min the CuCoFe-LDH/PMS system can degrade 99.54 % of glyphosate (100 mg/L) using 100 mg/L of CuCoFe-LDH, 200 mg/L of PMS, and pH 11. In addition, radical quenching experiments prove that the reactive oxygen species (e.g., SO 4 ●- , HO ● , O 2 ●– , and 1 O 2 ) are formed and SO 4 ●- plays a decisive role in glyphosate degradation. Moreover, the CuCoFe-LDH catalyst is reusable and stable with a glyphosate removal efficiency of 90.34 % after five continuous degradation cycles.
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Journal of Cleaner Production
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2021
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IF 9.297
Banghao Du,Gongduan Fan,Shangwu Yang,Zhuoyi Chen,Jing Luo,Weiwei Yu,Junyi Yu,Qi Wei,Yushan Lu
Reactive oxygen species (ROS) play a considerable role in the catalytic reaction for removing organic pollutants, however, the generation and transformation mechanism by catalyst with light and ultrasonic irradiation still requires intensive investigation. In this study, a novel Er 3+ -CdS/MoS 2 (ECMS) composite was synthesized, and the synergetic degradation effects for 17β-estradiol (17β-E2) during the sonophotocatalytic (SPC) process were investigated. The contribution of ROSs for eliminating 17β-E2 during the SPC process through quenching experiments was generally ranked in the following order: superoxide radical (•O 2 − ) ≈ hole (h + ) > hydroxyl radical (•OH) > H 2 O 2 > singlet oxygen ( 1 O 2 ). •OH plays a crucial role in 17β-E2 removal by ECMS under sonocatalysis and photocatalysis conditions. The transformation process among ROSs was further analyzed and elucidated in the light of the probe measurement results with positive or negative correlation among ROSs. Besides, we observed a phenomenon that the generated concentration of •O 2 − rises first and then falls during the SPC process, which might be attributed to the formation of 1 O 2 via the oxidation of h + or recombination with •OH. This work clarifies the underlying mechanisms of sonophotocatalytic generation and transformation of ROSs in depth.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
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IF 9.028
Shuhui Sun,Chao Shan,Zhichao Yang,Shu Wang,Bingcai Pan
Phosphonate is an important category of highly soluble organophosphorus in contaminated waters, and its oxidative transformation into phosphate is usually a prerequisite step to achieve the in-depth removal of the total phosphorus. Currently, selective oxidation of phosphonate into phosphate is urgently desired as conventional advanced oxidation processes suffer from severe matrix interferences. Herein, we employed 1-hydroxyethylidene-1,1-diphosphonic acid (HEDP) as a model phosphonate and demonstrated its efficient and selective oxidation by the Cu(II)/H2O2 process at alkaline pH. In the presence of trace Cu(II) (0.020 mM), 90.8% of HEDP (0.10 mM) was converted to phosphate by H2O2 in 30 min at pH 9.5, whereas negligible conversion was observed by UV/H2O2 or a Fenton reaction (pH = 3.0). The oxidation of HEDP by Cu(II)/H2O2 was insignificantly affected by natural organic matters (10.0 mg TOC/L) and various anions including chloride, sulfate, and nitrate (10.0 mM). The complexation of Cu(II) with HEDP coupling Cu(III) produced in situ enabled an intramolecular electron transfer process, which features high selective oxidation. Selective degradation of HEDP was further validated by adding stoichiometric H2O2 into an industrial effluent, where the existing Cu(II) could serve as the catalyst. This study also provides a successful case to trigger selective oxidation of trace pollutants of concern upon synergizing with the nature of the contaminated water.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Tao Zhou,Yi Han,Wei Xiang,Chen Wang,Xiaohui Wu,Juan Mao,Mingjie Huang
Heterogeneous catalytic activation mechanisms of peroxydisulfate (PDS) by transition metal oxides are generally attributed to the interactions between catalysts and PDS, however, the role of the co-existed organic substrate was largely overlooked in the past studies. In this work, phenol was selected as the target organic pollutant in a CuO/PDS system to evaluate its deep-seated role in participating in the effective activation of PDS. First, optimized reaction conditions as pH of 6.0, CuO of 5.96 g·L −1 and PDS of 2.5 mM were obtained by the response surface methodology (RSM) with a phenol degradation efficiency of 84.0%. It was further found that pre-adsorption of phenol or PDS led to obviously different performances in the phenol degradation with/without the radical scavengers. Two different activation pathways of PDS, i.e., the non-radical pathway mediated by surface deprotonated phenol to generate 1 O 2 and the radical pathway mediated by structural Cu(I)/Cu(II) to produce SO 4 − , were therefore proposed, and the former was predominant in the CuO/PDS/phenol system. In addition, HCO 3 − and HPO 4 2− could strongly inhibit the phenol degradation while Cl − and NO 3 − only performed negligible effects. NaOH washing could regenerate the surface hydroxyl groups and recover the catalytic ability of CuO. The result of this study integrated the interactions among the catalyst, oxidant and substrate, providing new insights into environmental-friendly PDS activation processes.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Xin Liu,Peng Xu,Qi Fu,Runhan Li,Chenxi He,Wenxuan Yao,Lei Wang,Shiqi Xie,Zhiyi Xie,Jingwei Ma,Qiulai He,John C. Crittenden
Zero-valent copper activated peroxymonosulfate (ZVC/PMS) system was widely used to degrade refractory contaminants due to being highly effective. However, the low reactivity and easy dismutation of cuprous species (Cu(I)) in acid condition limited its efficiency. In our study, ZVC coupled with ferrous ion (Fe(II)) promoted PMS to degrade orange II. Multiple oxidants including Cu(III), OH and SO 4 − made main contribution on orange II degradation in the Fe(II)/ZVC/PMS system. In the Fe(II)/ZVC/PMS system, ZVC generated Cu(I) by H + corrosion and PMS oxidation, and Cu(I) reacted with oxygen producing hydrogen peroxide. Then, Fe(II) and Cu(I) catalyzed hydrogen peroxide and PMS to generate Cu(III), OH and SO 4 − , and thereinto Fe(III) was reduced to Fe(II) by ZVC and Cu(I). In the Fe(II)/ZVC/PMS system, water matrix including humic acid, sulfate and nitrate had no significant impact on orange II degradation, while chloride restrained the degradation of orange II. The Fe(II)/ZVC/PMS system exhibited great degradation for orange II in tap water, lake water and well water. Additionally, the Fe(II)/ZVC/PMS system degraded more than 90% of methyl orange, rhodamine B, acetaminophen, ibuprofen, propranolol and diclofenac. Through adjusting the final reaction solution to pH 8.5 and subsiding, the discharge of total copper met the II-level environmental quality standards for surface water in China (1 mg/L). Hence, the study provided a promising method to induce PMS for enhanced degradation of contaminants.
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Chemistry-An Asian Journal
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2021
·Vol. 16
·期 20
·3194-3201
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IF 4.568
Jun Wu,Xinyue Yan,Wenrui Wang,Ming Jin,Yuhang Xie,Chengbing Wang
Graphical Efficient, stable, and low-cost N-doped graphitic carbon embedded CoNi bimetallic alloy nanocatalysts were developed for the catalytic transfer hydrogenation of biomass-derived furfural to value-added furfuryl alcohol with isopropanol as hydrogen donor. The synergy enabled by bimetallic alloys and abundant N-based Lewis-base sites and surface Co−N active species were responsible for the excellent catalytic performance. The development of efficient, stable, and cost-effective heterogeneous catalysts for catalytic transfer hydrogenation (CTH) of biomass-derived furfural (FAL) is highly desired. Herein, series of N-doped graphitic carbon embedded CoNi bimetallic alloy nanoparticles were fabricated and used for the CTH of FAL to value-added furfuryl alcohol (FOL) with renewable isopropanol as hydrogen donor. Intrinsic catalytic activity examination indicated the catalytic performance of Ni x Co y @NGC (x:y=1 : 3, 1 : 1, 3 : 1) nanocatalysts were sensitive to their chemical compositions. The optimal Ni 1 Co 1 @NGC nanocatalyst with Ni/Co mole ratio of 1 : 1 afforded a largest FOL yield of 89.3% with nearly full conversion of FAL. The synergistic effect enabled by bimetallic alloys and the abundant N-based Lewis base sites and surface Co−N active species were revealed based on systematic structural characterization, responsible for the excellent catalytic efficiency of bimetallic Ni 1 Co 1 @NGC nanocatalyst for CTH of FAL.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Ge Song,Xuedong Du,Yang Zheng,Pei Su,Yunping Tang,Minghua Zhou
To promote the reduction of Fe 3+ and improve the mineralization of organic pollutants , a novel electro-Fenton coupled with sulfite (Fe 3+ -EF/sulfite) process was constructed, which was superior to Fe 3+ -EF process in terms of carbamazepine (CBZ) degradation and mineralization with 5.99 times enhancement in degradation rate constant and 15.7 times enhancement on TOC removal. The complexation of Fe 3+ and sulfite prevented the precipitation of Fe 3+ , reduced Fe 3+ to Fe 2+ , and accelerated the iron cycle, so that H 2 O 2 utilization efficiency (0.051 mg TOC mg H2O2 −1 ) was greatly improved and electric energy consumption was greatly reduced (0.081 kWh g −1 TOC). The quenching experiments and EPR test confirmed that the reactive species, such as SO 3 •- , SO 4 •- , • OH, O 2 •- and 1 O 2 were responsible for the degradation of CBZ. This process also expanded the pH application range from 3 to 9 with satisfactory CBZ removal efficiency. This work verified the suitability of the Fe 3+ -EF/sulfite process for different sulfites (sulfite and bisulfite), typical pollutants (atrazine, sulfamethazine, rhodamine B) and real wastewater with 2.1–18.7 folds enhancement in degradation rate. The Fe 3+ -EF/sulfite process can achieve deep mineralization with low cost and simple operation, which has a broad and cost-effective application prospect in removal of refractory organic pollutants.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-12
·
IF 14.919
Xie Chao,Lin Longfei,Huang Liang,Wang Zixin,Jiang Zhiwei,Zhang Zehui,Han Buxing
Selective cleavage of C-C bonds is very important in organic chemistry, but remains challenging because of their inert chemical nature. Herein, we report that Zn/NC-X catalysts, in which Zn 2+ coordinate with N species on microporous N-doped carbon (NC) and X denotes the pyrolysis temperature, can effectively catalyze aerobic oxidative cleavage of C(CO)-C bonds and quantitatively convert acetophenone to methyl benzoate with a yield of 99% at 100 °C. The Zn/NC-950 can be applied for a wide scope of acetophenone derivatives as well as more challenging alkyl ketones. Detail mechanistic investigations reveal that the catalytic performance of Zn/NC-950 can be attributed to the coordination between Zn 2+ and N species to change the electronic state of the metal, synergetic effect of the Zn single sites with their surrounding N atoms, as well as the microporous structure with the high surface area and structural defects of the NC.
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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
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2021
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IF 7.664
Yuan Cao,Min Zhi Rong,Ming Qiu Zhang
To tackle the challenge of manufacturing highly filled composite materials via melt compounding and injection molding , the authors proposed a novel approach based on Diels-Alder (DA) chemistry. Polycaprolactone oligomers (PCL olig , M w = 2000 g/mol) were firstly crosslinked by DA bonds, and then the resultant network PCL olig -DA was also connected to maleimide functionalized Al 2 O 3 particles (Al 2 O 3 -M) via DA bonds. Upon being heated to the retro-DA reaction temperature, the covalent adaptable composite network exhibited low viscosity due to de-crosslinking, enabling melt processing and well dispersion of high-concentration fillers. During the subsequent cooling, the composite network was regained because of DA reaction, benefiting increase of the composite’s strength . Consequently, the contradictory requirements for molecular weight of matrix polymer under the circumstances, which had better to be as low as possible during the manufacturing but as high as possible in the ultimate composites, were skillfully satisfied.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Jie Tan,Zhifeng Li,Jie Li,Yuan Meng,Xiaolong Yao,Yuhui Wang,Yong Lu,Tingting Zhang
Bifunctional oxygen-doped graphitic carbon nitride (OCN) was fabricated to activate peroxymonosulfate (PMS) for degrading imidacloprid (IMD). The modulated electronic structure of OCN promoted the adsorption, electron transfer , and formation of the redox site of PMS. The light absorption capacity, and the separation and migration speed of photogenerated carriers of OCN were increased. Consequently, 94.5% of IMD (3.0 mg/L) was removed by OCN-10/PMS process in 2.0 h. Compared with g-C 3 N 4 /PMS (0.048 h −1 ), the IMD degradation rate constant of OCN-10/Vis/PMS system (1.501 h −1 ) was increased by 30.3 times. The PMS oxidation on electron-deficient C atoms and holes, the PMS reduction around electron-rich O atoms and photogenerated electrons, and the multiple reactions of superoxide radical were the sources of the main active species singlet oxygen. Moreover, even under different pH conditions, coexisting anions, humic acid , and other neonicotinoid pesticides , the OCN-10/Vis/PMS system still showed acceptable applicability. Finally, mass spectrometry identified that hydroxylation and N-dealkylation of amines were the primary degradation pathways of IMD. This paper demonstrates an environmental-friendly combined activation strategy of PMS that can be operated day and night with low energy consumption, aiming to pave the way for developing metal-free photocatalysts for high-efficient environmental purification based on advanced oxidation coupling technology .
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