Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Zhuoyue Liu,Ke Wang,Danyang Li,Zhenxin Wang,Shengjiong Yang,Heliang Pang,Gen Wang,Dahu Ding,Delu Miao
Mesoporous carbon materials are promising catalysts for peroxydisulfate (PDS) activation for degrading aqueous organic pollutants but limited by the intrinsic inertness. Herein, co-doping of iron and nitrogen into the mesoporous carbon framework was performed via thermal conversion of metal-polyphenol coordination polymers (Fe-TA) to synthesize Fe/N co-doped mesoporous carbon for efficient PDS activation. Owing to the large surface area, high graphitization degree and defective configurations, the Fe/N co-doped mesoporous carbon (Fe/N-MCs) exhibited superior catalytic performance toward the degradation of organic pollutants . Electron paramagnetic resonance tests, chemical quenching experiments, electrochemical analysis and spectra measurements revealed that the degradation of organic pollutants over the Fe/N-MCs followed a nonradical oxidation pathway based on electron transfer process. Graphite nitrogen and hydroxyl (C-OH) groups on the defective edges of Fe/N-MCs were proved to be possible active sites for PDS activation. PDS catalyzed by the Fe/N-MCs exhibited strong anti-interference capability to surrounding inorganic ions (such as Cl – , CO 3 2– , NO 3 – and SO 4 2– ) and natural organic matters, making it a promising candidate for the degradation of organic pollutants. This work provides a new prospect for developing highly active mesoporous carbon materials via heteroatom doping for PDS activation for wastewater decontamination .
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Bin Wang,Pei-ya Li,Qian Dong,Li-qin Chen,Hai-qiang Wang,Pei-long Han,Tao Fang
Liquid organic hydrogen carrier technology (LOHC) is considered to be the most promising solution for hydrogen storage and transport, but its development is limited by the high cost of noble metal catalysts. In this paper, four kinds of Ni/Co bimetallic catalysts with different proportions were prepared by the impregnation method. The effects of the Ni/Co molar ratio and the reduction temperature on the hydrogenation performance of N-ethylcarbazole (NEC) were studied. The relationship between the structure and the properties of the catalyst was discussed by combining various characterization methods. The results show that when cobalt is added to 50%, the hydrogenation activity is the most significant. Meanwhile, 100% of NEC conversion and 98.99% of 12H-NEC selectivity were achieved. The hydrogenation capacity is 5.77 wt %, when the catalyst reduction temperature is 450 °C. The characterizations show that the two metals are uniformly doped and highly dispersed with a good pore structure, and the metal particles have good alloy morphology. The synergistic interaction between Ni/Co metals is the key factor for the remarkable catalytic activity of the catalyst. The design and application of highly efficient nonprecious metal hydrogenation catalysts provide more feasibility to promote the commercial development of liquid organic hydrogen carrier technology.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Baowei Cao,Dachuan He,Fei Rao,Qadeer Ul Hassan,Xiaolong Cai,Lingna Liu,Fan Xue,Gangqiang Zhu
BiOI-loaded flower-like CeO 2 (BiOI/CeO 2 ) p-n heterojunction was synthesized via a simple two-step chemical route. The phase structure and chemical states of the heterojunction were analyzed by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS), respectively. The transmission electron microscopic (TEM) and the scanning electron microscope (SEM) reveal the close contact between BiOI and CeO 2 . The formation of the p-n heterojunction is verified by the Mott-Schottky curves. The p-type BiOI with a narrow band-gap when loaded on CeO 2 can not only improve the separation of photogenerated electron-hole pairs but also facilitate the absorption of visible light. The photo-oxidative removal efficiency of 9%BiOI/CeO 2 among other heterojunctions for NO reaches 45.49% and remains highly stable with an efficiency of 40.40% after the five cycles. Trapping experiments and ESR measurements were conducted to explore the contribution of charge carriers and the reactive oxygen species during the photocatalytic NO removal. This work highlights that constructing such p-n heterojunction by loading BiOI on CeO 2 microstructures can significantly enhance photocatalytic NO removal.
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Journal of Food Measurement and Characterization
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2022
·Vol. 17
·期 2
·1662-1670
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IF 3.006
Yang Zhengfei,Zhang Weijia,Zhu Jiangyu,Yin Yongqi,Xue Huaiguo,Fang Weiming
Detection and control of nitrite are major concerns in recent years for ensuring food and environmental safety. In this study, Mn, N co-doped Co-Carbons (CoMnN-Cs) were synthesized by calcination of bimetallic Co-Mn zeolite-imidazolate framework (CoMnZIF-67) materials at different temperatures (600–900 °C) in nitrogen atmosphere. Many characterizations, such as scanning electron microscope (SEM), elemental mapping, and, N 2 adsorption–desorption were performed to analyze the morphology, structure, and composition of the CoMnN-Cs. SEM revealed the generation of rich carbon nanotubes (CNTs). Mn-doping was obtained, which could be seen from the elemental mapping. The characterization also revealed that the pyrolysis temperature has an important effect to catalytic activities. From obtained results, it was found that the CoMnN-Cs prepared at 800 °C (CoMnN-Cs-800), showed better detection performance compared with CoMnN-Cs developed at other temperatures. As a result, the CoMnN-Cs-800-based sensor manifested an extended linear range (from 0.2 to 7000 μM), a low detection limit of 0.16 μM, and high sensitivity. Meanwhile, the developed sensor exhibited good selectivity, reproducibility, and long-term stability. Moreover, the sensor achieved satisfactory recoveries for the quantification of nitrite in tap water and sausage samples. This study implies CoMnN-Cs-800 is a promising material for the measurement of nitrite. Graphical abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Meng Cheng,Junhao Liu,Hao Jiang,Chunling Li,Shuangqing Sun,Songqing Hu
In view of the critical importance of oxygen to corrosion evolution, to starve corrosion via depleting oxygen in coatings is a promising strategy. In this work, a novel nanocatalytic anticorrosion concept is proposed to design new coating with outstanding corrosion resistance . Different from the passive barrier of traditional coatings and self-repair after corrosion of current stimuli-feedback coatings, such coating could spontaneously eliminate internal diffused oxygen and greatly suppress the corrosion process. As a proof of concept, single-atom Fe-N-C electrocatalyst with isolated FeN 4 active sites is synthesized by a simple confined carbonization method, exhibiting excellent oxygen reduction performance (E 1/2 = 0.902 V). In composite coating , the evenly dispersed Fe-N-C compensates for the coating defects and serves as oxygen scavengers, which could actively adsorb and consume ambient oxygen, thereby preventing oxygen penetration to the metal substrate surface, eliminating the oxygen contribution to corrosion and significantly boosting the anticorrosion performance of epoxy coating. This in-situ mediation for oxygen in coating prevents metal substrate from receiving new supply of oxygen, while imparting active anticorrosion property to the coating.
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高影响因子
APPLIED CATALYSIS A-GENERAL
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2022
·
IF 5.723
Chencheng Dong,Yan Bao,Mingyang Xing,Masakazu Anpo,Jinlong Zhang
Advanced oxidation processes (AOPs) are reckoned effective for removing persistent and recalcitrant pollutants by reactive oxygen species (ROSs), including hydroxyl radicals (•OH), sulfate radicals (SO 4 • - ), and superoxide radicals (•O 2 - ), as well as singlet oxygen ( 1 O 2 ). In this work, the Mo 2 C quantum dots enriched N-doped graphitic carbon layers (Mo 2 C QDs/NGCLs) were constructed via a facile two-step methodology. Interestingly, the Mo 2 C QDs/NGCLs acted as a highly efficient cocatalyst and/or catalyst simultaneously in AOPs, in particular visible-light-driven (VLD) Fenton and VLD PMS activation. In the hydroxyl radical-based AOPs (•OH-AOPs), it exhibited a remarkable removal efficiency for a range of aromatic organic pollutants , including rhodamine B (RhB) (99.9 %), phenol (90 %), benzophenone-3 (BZP) (83 %), methyl orange (MO) (58 %), methyl blue (MB) (89 %), ibuprofen (IBU) (100 %), and carbamazepine (CBZ) (50 %). Sulfate radicals-based AOPs (SR-AOPs) effectively degrade RhB (72 %), MO (83 %), IBU (70 %), and BZP (100 %). Thus, the present findings confirmed the potential of transition metal carbides for AOP applications and established a solid theoretical and technical basis for further research.
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Catalysts
·
2022
·Vol. 12
·期 12
·1658
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IF 4.501
Rong-Kuan Jiang,Yue Pan,Li-Hua Du,Ling-Yan Zheng,Zhi-Kai Sheng,Shi-Yi Zhang,Hang Lin,Ao-Ying Zhang,Han-Jia Xie,Zhi-Kai Yang,Xi-Ping Luo
Benzimidazole scaffolds became an attractive subject due to their broad spectrum of pharmacological activities. In this work, a methodology was developed for the synthesis of N-substituted benzimidazole derivatives from benzimidazoles and α, β-unsaturated compounds (acrylonitriles, acrylate esters, phenyl vinyl sulfone) catalyzed by lipase TL IM fromThermomyces lanuginosusin continuous-flow microreactors. Investigations were conducted on reaction parameters such as solvent, substrate ratio, reaction temperature, reactant donor/acceptor structures, and reaction time. The transformation is promoted by inexpensive and readily available lipase in methanol at 45 °C for 35 min. A wide range of β-amino sulfone, β-amino nitrile, and β-amino carbonyl compounds were efficiently and selectively synthesized in high yields (76–97%). All in all, a microfluidic biocatalysis system was applied to the synthesis of N-substituted benzimidazole derivatives, and could serve as a promising fast synthesis strategy for further research to develop novel and highly potent active drugs.Keywords:enzymatic synthesis;benzimidazole derivatives;continuous-flow reaction technology;continuous-flow microreactor;aza-Michael addition
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 30
·期 8
·20790-20803
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IF 5.19
Huang Hua,Tao Xin,Niu Zhirui,Shan Baoqin,Liu Yu,Ren Jingyu
To improve the photocatalytic performance of Mn 0.6 Zn 0.4 Fe 2 O 4 (MZFO) and ZnIn 2 S 4 (ZIS) for organic pollutants, the p-n MZFO@ZIS heterojunctions with different weight percentage (10 ~ 40%) of MZFO are constructed from spent batteries and added indium ion via a green bioleaching and hydrothermal method. Structural, optical, and photocatalytic properties for the heterojunctions are investigated systematically by XRD, FT-IR, SEM–EDX, TEM, BET, VB-XPS, UV–vis DRS, PL, etc. The results confirm that p–n junction significantly improves the visible light adsorption and the separation efficiency of photogenerated carriers. Specifically, MZFO-25%@ZIS shows the highest photodegradation performance toward Congo red (CR), and its reactive kinetic constant is about 9.6, 7.8, and 7.0 times higher than that of P25 TiO 2 , MZFO, and ZIS, respectively, and MZFO-25%@ZIS still possesses a high reusability and simple magnetic separation after 5 cycles of reuse. The radical trapping experiments and electronic paramagnetic resonance (EPR) tests show that · O 2 − , · OH, and h + are the most important active substance for degrading CR. The pathways for the CR degradation are further proposed based on the intermediate analysis. DFT + U calculations confirm that the high charge density of Zn–O, Fe–O, and Zn–S bonds in the MZFO and ZIS molecules provides the electrons for the sufficient production of free radicals. This work also provides a novel high value-added strategy for the green utilization of spent batteries.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Linli Dai,Yi Xie,Yongkui Zhang,Yabo Wang
In this work, microorganism of Phanerochaete chrysosporium with iron-tolerating and accumulating abilities was cultivated and harvested as mycelial pellets, which could serve as a sustainable and environmental-friendly precursor for iron phosphide/N-doped biocarbon composite preparation. Through one-step pyrolysis process , the inherent Fe and P elements in mycelial pellet enabled the formation of well crystallized Fe 2 P particles, loading on N-doped biocarbon matrix. Benefiting from the porous structure, high specific surface area, N doping-induced defects and C O groups of biocarbon, as well as the good electron-donating property of Fe 2 P, the as-obtained Fe 2 P/BC composite performed well for bisphenol pollutant (e.g., BPAF) removal through peroxymonosulfate (PMS) activation. Specifically, almost complete BPAF removal was achieved within 30 min adsorption and 10 min catalysis process with an apparent reaction rate constant of 0.486 min −1 . The good crystallinity and protective carbon layer wrapping on Fe 2 P enabled the wide pH adaptability and low iron leaching of Fe 2 P/BC in catalytic reaction . Inorganic anions and humic acid brought only slight inhibition for BPAF removal, which could be overcome by prolonging reaction time to 30 min. Further mechanism studies indicated that reactive oxygen species , e.g., SO 4 - •, •OH and 1 O 2 were generated through both radical and non-radical pathways and contributed to BPAF degradation. After treatment by Fe 2 P/BC-PMS system, the total organic carbon (TOC) of original BPAF solution (20 mg L −1 ) was reduced by 51.6%. Fortunately, the residual degradation intermediate products showed much reduced ecotoxicity in both predicted (ECOSAR program) and experimental results (growth inhibition test using Raphidocelis subcapitata as ecological indicator).
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Polymers
·
2022
·Vol. 14
·期 23
·5080
·
IF 4.967
Leixuan Li,Yan Xin,Fengze Wu,Xiangrong Lyu,Qiyuan Yao,Xiaoting Yin,Qiang Zhang,Wenjuan Shan,Yong Chen,Qiuxia Han
CyclicN-halamines are highly antimicrobial, very stable, and not susceptible to bacterial resistance. A polysiloxane delivery vehicle was synthesized to deliver cyclic imideN-halamine onto cellulose via a benign and universal procedure that does not require a harmful solvent or chemical bonding. In brief, Knoevenagel condensation between barbituric acid and 4-hydroxybenzaldehyde furnished 5-(4-hydroxybenzylidene)pyrimidine-2,4,6-trione, whose phenolic O−H was subsequently reacted with the Si−H of poly(methylhydrosiloxane) (PMHS) via silane alcoholysis. The product of silane alcoholysis was interpenetrated into cellulose in supercritical CO2(scCO2) at 50 °C, to form a continuous modification layer. The thickness of the modification layer positively correlated with interpenetration pressure in the experimental range of 10 to 28 MPa and reached a maximum value of 76.5 nm, which demonstrates the ability for tunable delivery, to control the loading of the imide N−H bond originating from barbituric acid unit. The imide N−H bonds on cellulose with the thickest modifier were then chlorinated into N−Cl counterparts usingtert-butyl hypochlorite, to exert a powerful biocidability, providing ~7 log reductions of bothS. aureusandE. coliin 20 min. The stability and rechargeability of the biocidability were both very promising, suggesting that the polysiloxane modifier has a satisfactory chemical structure and interlocks firmly with cellulose via scCO2interpenetration.Keywords:cyclic imideN-halamines;polysiloxane;delivery vehicle;antibacterial surface;cellulose;scCO2interpenetration
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CATALYSIS LETTERS
·
2022
·Vol. 153
·期 10
·3074-3091
·
IF 2.936
Faizan Muhammad,Saeed Aamir,Song Piao,Zhang Ruirui,Liu Ruixia,Chang Zhi,Wu Liuzhu,Zhang Manyuan
Vanadium phosphorous oxide (VPO) catalysts have been recognized as heterogeneous catalyst for selective oxidation of low-carbon alkanes i.e., n -butane toward maleic anhydride. This process has widely gained attention globally due to its highly selective and cost-effective process. Herein, we employed Cd 0 . 2 Zn 0 . 8 S as a support for the VPO catalyst and evaluated its n -butane catalytic performance. Compared to the unpromoted catalyst (Blank-VPO), a higher n -butane conversion and MA yield were successfully obtained from the promoted catalyst (Cd 0 . 2 Zn 0 . 8 S@VPO). Interestingly, it reduces the byproducts, i.e., CO 2 and CO emission. Characterization methods such as TGA, XRD, EDS, SEM, FTIR, NH 3 -TPD, XPS, TEM, and Raman spectroscopy were used to characterize the Cd 0 . 2 Zn 0 . 8 S, VPO precursor and catalyst. Graphical Abstract
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Xiaoming Liu,Yinchu Zhang,Hongwei Wang,Jiajun Yan,Liushui Yan,Kexin Li,Huiqin Guo,Wang Gong,Jun Lin
In this work, a series of Zn x Cd 1-x S solid solutions are firstly prepared by a solvothermal process. The optimized composition of Zn x Cd 1-x S solid solution is determined to be Zn 0·2 Cd 0.8 S. On this basis, the Cu 7 S 4 /Zn 0·2 Cd 0·8 S composite photocatalyst with a binary p-n heterojunction has been synthesized by a co-precipitation process followed by a solvothermal method . Owning to the synergistic effect of the heterojunction structure in the interface of Cu 7 S 4 (p-type) and Zn 0·2 Cd 0·8 S (n-type) and the built-in electric field in binary p-n heterojunction, the as-prepared Cu 7 S 4 /Zn 0·2 Cd 0·8 S composite photocatalyst exhibits a significantly improved photocatalytic activity toward hydrogen production from water with visible light response, which is approximately 5.0 times and 16.5 times higher than of pristine Zn 0·2 Cd 0·8 S and CdS, respectively. The possible photocatalytic mechanism has been proposed basing on a series of experimental results. The current work might be valuable inspirations for designing highly efficient heterojunction composite photocatalyst for solar hydrogen evolution .
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