CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Sitao Wang,Zhijie Liu,Bolun Pang,Yuting Gao,Santu Luo,Qiaosong Li,Hailan Chen,Michael G Kong
Antibiotics are widely used to treat or prevent infectious diseases in human and veterinary medicine. Excessive residues in the aquatic environment lead to increasingly prominent antibiotic pollution; therefore, it is urgent to develop sustainable strategies for rapidly degrading antibiotics. In this study, a highly synergetic effect for norfloxacin (NOR) remediation is achieved by coupling underwater bubble plasma formation with a Fe (III)–S (IV) system due to the efficient utilization of reactive species in chain reactions. The degradation rate using synergetic approach can reach 76.4% within 50 min discharge, and further increases significantly to 94.4% after 5 h post-discharge. The effects of pulsed peak voltage and Fe (III)/S (IV) dosage on NOR removal are characterized. The existence of hydroxyl radicals ( • OH) and sulfate radicals (SO 4 •− ) are proved by electron spin resonance spectrometer (ESR) during degradation. Furthermore, radical scavenger experiments demonstrate that • OH and SO 4 •− play a crucial role in degradation. Underwater bubble plasma provides the oxic and acidic liquid environment for the Fe (III)–S (IV) system to accelerate the self-perpetuating chain reactions. These reactions not only introduce SO 4 •− and generate more • OH during plasma-on, but also induce their regeneration and further prolong the degradation process during plasma-off through plasma-generated effects. Finally, the degradation intermediates of NOR are identified, and a possible degradation pathway is proposed. The possible contribution weight of each approach on the degradation rate is speculated. These new findings offer promising applications for developing a technology with real potential for the treatment of organic compounds in industrial wastewater treatment.
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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Shasha Wei,Li Liu,Xuan Huang,Yichuan Zhang,Fusheng Liu,Liang Deng,Emiliano Bilotti,Guangming Chen
Organic thermoelectric (TE) composites and flexible devices have gained a rapid development in recent decade. Herein, a flexible and foldable film of poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)/single-walled carbon nanotube (PEDOT:PSS/SWCNT) composite is fabricated by post-treatment with an ionic liquid (IL), and an S-shape TE generator (TEG) is designed to harvest heat from human body via a vertical temperature gradient. After being post-treated with IL of bis(trifluoromethane)sulfonimide lithium salt (LiTFSI), the PEDOT:PSS/SWNCT composite displays an improved electrical conductivity from 1063 ± 80 to 1562 ± 170 S cm–1, with an almost constant Seebeck coefficient of ∼21.9 μV K–1 with a 30 wt % content of SWCNT. The TE properties exhibit excellent stability against repeated bending or folding cycles. Furthermore, an S-shape architecture is designed for TEG assembling, which enables effective utilization of a vertical temperature gradient between the human body and surroundings. The present study proposes a universal strategy for harvesting heat using a wearable TEG via a vertical temperature gradient, which represents great prospects for application in self-powered wearable electronics.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Rongsheng Ning,Heliang Pang,Zhongsen Yan,Zhenyu Lu,Qiankun Wang,Zengling Wu,Wenxin Dai,Lingshan Liu,Zhongsheng Li,Gongduan Fan,Xianzhi Fu
The development of high efficient photocatalysts for antibiotics contamination in water remains a severe challenge. In this study, a novel step-scheme (S-scheme) photocatalytic heterojunction nanocomposites were fabricated from integrating AgCl nanoparticles on the MIL-100(Fe) octahedron surface through facile multi-stage stirring strategy. The S-scheme heterojunction structure in AgCl/MIL-100(Fe) (AM) nanocomposite provided a more rational utilization of electrons (e - ) and holes (h + ), accelerated the carrier transport at the junction interface, and enhanced the overall photocatalytic performance of nanomaterials . The visible-light-driven photocatalysts were used to degrade sulfamethazine (SMZ) which attained a high removal efficiency (99.9%). The reaction mechanisms of SMZ degradation in the AM photocatalytic system were explored by electron spin resonance (ESR) and active species capture experiments, which superoxide radical (•O 2 - ), hydroxyl radical (•OH), and h + performed as major roles. More importantly, the SMZ degradation pathway and toxicity assessment were proposed. There were four main pathways of SMZ degradation, including the processes of oxidation , hydroxylation, denitrification, and desulfonation. The toxicity of the final products in each pathway was lower than that of the parent according to the toxicity evaluation results. Therefore, this work might provide new insights into the environmentally-friendly photocatalytic processes of S-scheme AM nanocomposites for the efficient degradation of antibiotics pollutants.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Jinhang Yang,Jiangli Sun,Shuo Chen,Danquan Lan,Zhihong Li,Zuji Li,Jingwen Wei,Zebin Yu,Hongxiang Zhu,Shuangfei Wang,Yanping Hou
Development of efficient and stable photocatalysts is of essential for photocatalytic degradation of refractory organics in wastewaters. Herein, the novel S-scheme MoSe 2 /AgBr (MS/AB) heterojunctions were synthesized for antibiotics degradation. Various characterization results showed that the S-scheme MS/AB photocatalysts exhibited efficient carriers’ separation and strong redox potential. Tetracycline (TC) (20 mg/L) degradation efficiency of 81.4% was achieved using the 5MS/AB within 90 min at pH of 9, superior to those of the counterparts. Photogenerated carriers' transfer and photocatalytic reaction mechanism of the S-scheme MoSe 2 /AgBr heterojunction were deduced by DFT calculation, in-situ XPS and work function calculation. Moreover, possible degradation pathways of TC were proposed based on identified intermediates, and most of the intermediates showed lower toxicity than that of TC. The 5MS/AB photocatalyst also showed great stability and excellent antibacterial effect. This study advances the design of efficient photocatalysts and enriches related mechanisms.
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ORGANIC PROCESS RESEARCH & DEVELOPMENT
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2022
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IF 3.858
Jianjiong Li,Shanshan Yu,Yingang Wang,Peiyuan Yao,Qiaqing Wu,Dunming Zhu
(S)-2-Aminobutane, d-alanine, and d-homoalanine are important intermediates for the production of various active pharmaceutical ingredients and food additives. The preparation of these small chiral amine or amino acids with high water solubility still demands searching for efficient methods. In this work, we identified an ω-transaminase (ω-TA) from Sinirhodobacter hungdaonensis (ShdTA) that catalyzed the kinetic resolution of racemic 2-aminobutane at a concentration of 800 mM using pyruvate as the amino acceptor, leading to the simultaneous isolation of enantiopure (S)-2-aminobutane and d-alanine in 46% and 90% yield, respectively. In addition, (S)-2-aminobutane (98% ee) and d-homoalanine (99% ee) were isolated in 45% and 93% yield, respectively, in the kinetic resolution of racemic 2-aminobutane at a concentration of 400 mM coupled with deamination of l-threonine by threonine deaminase. We thus developed a biocatalytic process for the practical synthesis of these valuable small chiral amine and d-amino acids.
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Polymers
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2022
·Vol. 14
·期 4
·699
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IF 4.967
Linlin Wang,Jie Zhou,Lei Li,Shengyu Feng
Supramolecular elastomers integrated with high mechanical toughness and excellent self-healing ability offer attractive applications in various fields such as biomedical materials and wearable electronics. However, the multistep preparation process for creating functional polymer precursors and the expensive stock materials required are two factors that limit the widespread use of supramolecular elastomers. Herein, for the first time, poly(β-hydroxyl amine)s generated by amine-epoxy polymerization were used in the development of supramolecular polymer materials. Based on the novel silicon-containing poly(β-hydroxyl amine)s synthesized by the polymerization between 1,3-bis(3-glycidyloxypropyl)tetramethyldisiloxane and 3-amino-1,2-propanediol, dually cross-linked supramolecular elastomers with both hydrogen bonding and metal coordination were achieved, displaying adjustable mechanical properties with the tensile strength varying from 0.70 MPa to 2.52 MPa, respectively. Thanks to the dynamic nature of the supramolecular interactions, these elastomers exhibited favorable hot-pressing reprocessability and excellent self-healing performance, with the healing efficiency reaching up to 98% at 60 °C for 48 h. Potential applications for photoluminescent materials and flexible electronic devices were demonstrated. We believe that its simplicity of synthesis, adjustable mechanical properties, and robust self-healing capacities bode well for future applications of this new supramolecular elastomer.Keywords:dual-cross-linked elastomer;supramolecular elastomer;poly(β-hydroxyl amine);self-healing
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Ya Xiong,Teng Liu,Xinyu Wang,Wendi Liu,Yanjun Xue,Xiaoli Zhang,Can Xiong,Jian Tian
Ultrathin CdS nanosheets (NSs) are intriguing in photocatalytic hydrogen evolution . Severe photo-corrosion and rapid recombination of electrons and holes, however, impair their applications. To solve this problem, a novel step-scheme (S-scheme) 2D CdS/W 18 O 49 heterostructure with strong interfacial interactions and large contact interface has been successfully designed. Due to the ultrathin structure of CdS, defect-rich W 18 O 49 NSs-assembled network, unique 2D heterostructure and state-of-the-art S-scheme mode, 40 wt% CdS/W 18 O 49 (CW40) shows a prominent photocatalytic H 2 production rate of 15.4 mmol g −1 h −1 . Besides, the apparent quantum efficiency of CW40 is up to 15.4 % under light at λ = 370 nm. Besides, the as-prepared CW40 can protect CdS from photo-corrosion, exhibiting outstanding stability over 24 h circular reaction. Our work provides an out-of-box solution to broaden the application potential of certain catalysts with inherent drawbacks and offers fresh insight into the design and preparation of highly-efficient 2D heterostructures for versatile applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yuanchao Pei,Yaxin Zhang,Jie Ma,Yang Zhao,Zhiyong Li,Huiyong Wang,Jianji Wang,Ran Du
Development of porous adsorption materials tethered with functional groups was favorable to establish a more efficient, stable and broad-spectrum metal ions removal strategy from water. In this work, carboxyl functional poly(ionic liquid)s@MOF composites were prepared through in situ polymerization of ILs monomers inside MOF pores. Their thermophysical property, structure and morphology were characterized by different techniques. These PILs@MOF composites were proposed as universal and efficient adsorbents to remove selected rare earth metal ions (La 3+ , Sm 3+ , Nd 3+ ) and heavy metal ions (Pb 2+ , Cd 2+ ) from water medium. Effect of pH value and composite dosage on the adsorption efficiency were studied in detail. The optimized adsorption efficiency as high as 99.8 % could be found for the selected metal ions by PIL@MIL-101. In addition, the isotherms, kinetics and thermodynamic parameters of the adsorption process were also determined, and these results imply that the Langmuir model and pseudo-second-order model fitted well with the experimental data. Thermodynamic parameters revealed spontaneous and exothermic nature of the adsorption process. A plausible mechanism for the adsorption process was suggested by the electrostatic interaction and coordination between the carboxyl group and metal ions with the aid of FTIR and XPS measurements. Finally, recycling experiments were performed to demonstrate the recyclability and stability of PIL@MOF composites undergoes at least five adsorption–desorption runs. The current research presented a series of poly(ionic liquid)s@MOF composites as a universal adsorption platform that demonstrated great potential for removing metal ions with remarkable efficiency.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Yulai Zhao,Zhongzheng Zhu,Anjun Wang,Longqiang Xiao,Linxi Hou
Porous carbon materials have been widely used as electrode materials for supercapacitors . However, low specific capacitance severely hinders the practical application. To further improve the capacitance, this work reports a facile approach to prepare N, S co-doped hierarchical porous carbon/MnO 2 composites (NSPC/MnO 2 ). Acidified thiourea, acting as N and S source, is used to crosslink sodium alginate (SA) to give SA-based composite gels which are pyrolyzed to produce NSPC/MnO 2 . X-ray diffraction and X-ray photoelectron spectra proved that manganese exists in the porous carbon in the form of MnO 2 . The obtained NSPC/MnO 2 exhibit hierarchical porous structure, remarkable mesoporous feature (the proportion of mesopores and macropores reached 32.69%), and high specific surface area of 1701 m 2 g −1 . Meanwhile, NSPC/MnO 2 show abundant heteroatom doping, i.e. Mn (2.05 at%), N (6.76 at%), and S (2.16 at%), which provided plenty of pseudocapacitance. The electrochemical tests show that NSPC/MnO 2 as electrode material can reach a high specific capacity of 281.1 F g −1 at 1 A g −1 (which is almost 1.85 times higher than the comparative sample), with good cycling stability (86.02% after 5000 cycles at 10 A g −1 ).
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ELECTROCHIMICA ACTA
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2022
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IF 7.336
Xiaoqing Liu,Guangshe Li,Jinjiang Wu,Lingshen Meng,Dan Zhang,Xin Zhang,Liping Li
Transition metal nitrides have attracted extensive attention due to their high electronic conductivity and considerable theoretical capacity. However, large volume change and sluggish reaction kinetics during electrochemical reaction process impede their further application. Herein, we report a topochemical self-nitridation approach in-situ to synthesize VN nanocrystals embedded in N, S co-doped porous carbon framework and prove that the as-obtained composite nanocrystals are good anode for Li ion battery (LIB). The composite nanocrystals deliver a high reversible capacity of 294 mA h g −1 at 10 A g −1 after 1000 cycles for LIBs. Systematic characterizations coupled with the kinetic analysis manifest that VN nanocrystals exhibit short ions diffusion path and N, S co-doped porous carbon framework improves electronic conductivity as well as buffers volume change during electrochemical process. Furthermore, when using the composite nanocrystals as an anode and commercial LiFePO 4 as a cathode to package a full cell, three red LEDs are easily lightened up, indicating a huge potential of VN nanocrystals as electrode materials for practical application.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Yuanyuan Yang,Xiaofei Tan,Eydhah Almatrafi,Shujing Ye,Biao Song,Qiang Chen,Hailan Yang,Qianmin Fu,Yuanyuan Deng,Zhuotong Zeng,Guangming Zeng
Polluted stormwater (PSW) treatment is becoming increasingly important because of the existence of multiple pollutants from non-point pollution sources. Alfalfa biochar loaded with Mg/Fe layered double hydroxide (AF-LDH) was successfully synthesized to remove trace metal(loid)s from stormwater. The adsorption kinetics and isotherms of metal(loid)s in a mono-component system and the reusability of the composite materials was investigated in this study. The result showed that the maximum removal efficiency for Pb(II), Cu(II), Zn(II), Cd(II), As(V), and Cr(VI) were 98.98 %, 98.11 %, 97.88 %, 97.71 %, 98.81 %, and 50.89 %, respectively, when added calcined AF-LDH (AF-LDO) composite material to the multi-component solution. The AF-LDH and AF-LDO could efficiently remove trace pollutants (10‐100 μg/L) from multi-component solution, especially for AF-LDO, which could completely remove the tested six trace metal(loid)s. Furthermore, Fourier transform infrared spectra and X-ray diffraction characterizations supported the Mg/Fe layered double hydroxide reconstruction. The main mechanisms of Pb(II), Cu(II), Zn(II), and Cd(II) (cationic metals) removal were ion exchange and surface precipitation, whereas As(V) and Cr(VI) (anionic metals) were mainly dislodged through the formation of surface complexation, electrostatic attraction, and interlayer anion exchange, concerning the –OH and –COOH of AF-LDH. Importantly, the results of the column experiment demonstrated that AF-LDO was superior to AF-LDH for anionic metal removal from stormwater. In this study, we synthesized AF-LDH and AF-LDO for trace metal(loid) removal and proposed a new and practical approach for stormwater purification.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Jiangli Sun,Jinhang Yang,Jiaxiang Liang,Lingli Tu,Yuejing Bin,Yanping Hou
It is crucial to design efficient photocatalysts for elimination of combined pollutants in wastewater. Herein, the S-scheme Zn 3 In 2 S 6 -BGQDs/AgBr (ZBA) heterojunction was synthesized through co-modification of Zn 3 In 2 S 6 with B-doped graphene quantum dots (BGQDs) and AgBr nanoparticles using solvothermal method for synchronous removals of nitrofurazone (NFZ) and Cr (VI). Characterization results revealed that ZBA showed superior photocatalytic activity than the counterparts. In NFZ-Cr (VI) coexistence environment, removal efficiencies towards NFZ and Cr (VI) were 95.23% and 99.39% using the ZBA photocatalyst within 2 h of visible light irradiation. Results demonstrated that ∙OH, h + and ∙O 2 − played major role for NFZ removal, while mainly e - and ∙O 2 − contributed to Cr (VI) reduction. The S-scheme heterojunction mechanism of ZBA was confirmed by energy band structure analysis, ESR and calculated work function. Possible pathways and mechanisms of NFZ degradation were proposed according the identified intermediates. Besides, the ecotoxicity of intermediates was analyzed. This study advances the development of photocatalytic treatment of combined-polluted wastewater.
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