PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2021
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IF 6.158
Shichun Weng,Wenqian Wu,Zichao Guo,Fuqing Meng,Ying Chen,Wanghua Chen
2,4,6-Trinitroresorcinol (TNR), one main by-product in the dinitrobenzene (DNB) production process, is self-reactive substance and has led to tragic explosion incidents in China. In this article, the formation mechanism of TNR during the DNB production process was studied employing HPLC and HPLC-MS technique. Thermal decomposition behavior of TNR was also systematically studied by differential scanning calorimeter (DSC). The decomposition kinetics of TNR were investigated employing both iso-conversional (Friedman and Ozawa method) and model-fitting method. The formation mechanism of TNR during the dinitrobenzene (DNB) production is confirmed: The two by-products of dinitrophenol (DNP) and trinitrophenol (TNP) produced in the benzene mononitration stage are further nitrated to form tetranitrophenol (TTNP) in the mononitrobenzene (MNB) nitration stage. Then most of TTNP will be hydrolyzed to form the TNR during the water washing process. The decomposition process of TNR has been proven to follow three consecutive steps (A→B1→B2→B). The former two steps present autocatalytic behavior while the last step obeys N-order reaction model. The accuracy of the developed decomposition model and the obtained model parameters have been demonstrated by the comparison of the simulated and experimental DSC data and the activation energy obtained by both the iso-conversional method and model-fitting method. The same trend of experimental and simulated results about isothermal reaction further verify the building model.
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高影响因子
OPTICAL MATERIALS
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2021
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IF 3.08
Weisai Liu,Dapeng Li,Fei Wang,Xiaoyi Chen,Xuquan Wang,Yang Tian
A lanthanide metal-organic framework, {[Tb(FDA) 1.5 (DMF)]·DMF} n (Tb-FDA) was designed and prepared by mixing Tb 3+ and 2,5-furandicarboxylic acid (H 2 FDA) under solvothermal condition. The crystal structure of the complex was determined by single-crystal X-ray diffraction. The thermal stability and the luminescence properties of Tb-FDA were studied. The detection of organic molecules and cations and the interference of other analytes were considered and investigated in detail, revealing the excellent performance of Tb-FDA for sensing nitrobenzene (NB) and Fe 3+ with high efficiency, sensitivity and chemical stability. In addition, the sensing function possesses selectivity even with the existence of other analogous interfering substances. The mechanism of fluorescence quenching with NB and Fe 3+ was also given in this work.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Peizhen Yang,Songrong Li,Liang Xiaofu,An Xiaojing,Dongfang Liu,Wenli Huang
The degradation of organic contaminants via traditional radical-dominated advanced oxidation processes (AOPs) under high salinity conditions was limited due to side reactions between coexisting inorganic anions and radicals. Herein, a nonradical oxidation process via peroxymonosulfate (PMS) activation by CuO/MXene for treating high-salinity organic wastewater was developed. Rapid removal efficiency of target pollutant carbamazepine (CBZ) was significantly enhanced to 95.88% within 20 min by CuO/MXene under high salinity conditions (NaCl, 200 mM), compared to the efficiency of 4.30% exhibited by PMS alone. Besides, CBZ maintained a higher removal efficiency of > 81.04% in complex highly saline wastewater composed of eight common inorganic anions. Radical quenching experiments and electron paramagnetic resonance (EPR) analysis confirmed that radical and nonradical oxidation processes were involved in the catalytic process. However, singlet oxygen ( 1 O 2 ) was identified as the primary reactive species, and its contribution rate to CBZ degradation was > 73.58% in a wide pH range (3.0-9.0). The oxygenated functional groups and the interaction between CuO/MXene and PMS facilitated the production of 1 O 2 . The degradation pathway was proposed based on the detection of intermediates. This work provided a new inspiration for the decontamination of organic contaminants under high salinity conditions via a nonradical oxidation process.
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高影响因子
Journal of Experimental Nanoscience
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2021
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IF 3.075
Zhiwei Pan,Xinru Zhu,Hong Jiang,Yefei Liu,Rizhi Chen
Flexible and hierarchical nanostructured Pd/SiO2-TiO2 nanofibrous catalytic membranes were fabricated via combining electrospinning technique and a two-step hydrothermal method. The size and distribution of TiO2 nanorods immobilised on SiO2 nanofibrous membranes can be regulated via adjusting the dosage of TiCl3 solution in the first step hydrothermal process. When using an optimal TiCl3 solution dosage of 0.2 mL, a hierarchical structured Pd/SiO2-TiO2-0.2 nanofibrous catalytic membrane with uniformly dense TiO2 nanorods loaded on SiO2 nanofibers is obtained, and still shows good tensile strength and flexibility. The catalytic activity of Pd/SiO2-TiO2-0.2 increases 5 times as compared to Pd/SiO2-TiO2-0 in the reduction of p-nitrophenol (PNP) to p-aminophenol (PAP). The modification with TiO2 nanorods can provide more surface areas for loading the Pd nanoparticles, thereby increased active sites. The three-dimensional open-cell network stacked and assembled by thousands of SiO2 nanofibers and TiO2 nanorods enhances the contact between the reactants and Pd nanoparticles. Both aspects contribute the superior catalytic activity of Pd/SiO2-TiO2-0.2. Furthermore, a continuous and complete conversion of PNP to PAP can be stably operated over 240 min in a gravity-driven catalytic membrane reactor constructed by Pd/SiO2-TiO2-0.2.
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ACS Applied Nano Materials
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2021
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IF 5.097
Dajiao Cheng,Rong Liu,Limei Tian,Quan Zhou,Fushuang Niu,Yinghong Yue,Ke Hu
Photocatalytic activation of prodrugs for killing cancer cells is an attractive alternative phototherapy to photodynamic therapy that typically relies on the supply of oxygen. Although prodrugs are widely developed, few other than Pt(IV) complexes are studied for photocatalytic activation. Herein, we report the photocatalytic reduction of nitrobenzene to aniline, an important chemical conversion for a large class of nitroaromatic prodrugs in cancer therapy that was previously limited to only enzyme-catalyzed activation. The carefully designed photocatalyst is a photosensitizer (PS)-functionalized gold nanocluster (Au NC) (abbreviated as Au-PS) in which a ruthenium coordination compound as the PS is covalently linked to the glutathione-ligated Au NC surface. Visible light excitation of the photocatalyst reduces nitrobenzene to aniline with 100% selectivity. The remarkably high selectivity is attributed to the specific catalytic nature of the reduced Au NC from photoinduced charge separation within the Au-PS analyzed by time-resolved absorption spectroscopy. In vitro experiments show that the nitroaromatic prodrug 5-(aziridin-1-yl)-2,4-dinitrobenzamide (CB1954) induces significant cytotoxicity in the presence of the Au-PS and light under hypoxia. The photocatalytic nitroaromatic prodrug activation by the Au-PS provides an alternative approach in the category of photochemotherapy to confront hypoxic cancer cells.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Tong Liu,Zhican Xie,Peng Zhou,Zhaokun Xiong,Heng Zhang,Zhicheng Pan,Yang Liu,Bo Lai
Transition metal activation of sulfite (S(IV)) is a promising wastewater treatment technology . In this study, the activation of potassium pyrosulfite (PPS) with ferric iron (Fe 3+ ) is proposed firstly to degrade carbamazepine (CBZ). PPS has the advantages of low cost, non-toxicity and acidic solution, which makes it unnecessary to adjust the pH. The results showed that the Fe 3+ cycle was realized during the reaction process, and the degradation trend of CBZ was consistent with the formation rate of Fe 2+ and the decay rate of S(IV). Moreover, oxygen (O 2 ) plays a decisive role in the system and was the initiator of free radical chain reactions. The existence of sulfite radical (SO 3 •− ), sulfate radical (SO 4 •− ) and hydroxyl radicals (HO • ) in Fe 3+ /PPS system was proved by electron paramagnetic resonance (EPR), quenching experiments and terephthalic acid (TA) photoluminescence probing technique. The contribution of SO 4 •− and OH • to the removal of CBZ in Fe 3+ /PPS system is 64% and 35%, respectively. In addition, intermediates of CBZ were identified by Liquid Chromatography–Tandem Mass Spectrometry (LC–MS/MS) and possible removal pathways were also proposed. Finally, the effects of PPS concentration, Fe 3+ concentration, initial pH, anions and humic acid (HA) were also investigated.
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Materials Today Chemistry
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2021
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IF 8.301
X. Jiao,H. Li,X. Cheng
This article deals with three cellulose-based fluorescent macromolecular sensors by introducing 1,8-naphthalimide fluorophore to cellulose . First, through the etherification reaction of cellulose with BrCH 2 CH 2 NH 2 , –NH 2 group–bearing cellulose CS 1 was obtained. Then, the –NH 2 group reacts with 4-bromo-1,8-naphthalic anhydride to synthesize a naphthalimide cellulose derivative ( CS 2 ). Finally, the recognition group was introduced by substituting Br atoms, and three cellulose fluorescent probes ( CS 3 , CS 4 , and CS 5 ) were obtained eventually. Structure and fluorescence properties of the macromolecular sensors were characterized and confirmed. Fluorescence detection measurements show that these probes can be used as selective and sensitive fluorescent sensors to 2,4,6-trinitrophenol (TNP). The detection limits are 0.52 μM, 0.76 μM, and 0.81 μM, indicating good detection performance. This work provides a new method for the selective detection of TNP and also a method to enlarge the application scope of cellulose.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Hongbin Shi,Xiaofeng Dai,Qing Liu,Teng Zhang,Yabing Zhang,Yuling Shi,Tao Wang
Magnetic CuNi alloy nanoparticles (CuNi NPs) for the catalytic transfer hydrogenation (CTH) of nitroarene were successfully prepared by the facile thermal decomposition of copper formate (Cuf) and nickel formate (Nif) simultaneously. Liquid paraffin served as solvent, and oleylamine (OAM) acted as both complexing agent and stabilizer. The particle size and Cu/Ni composition of CuNi NPs could be controlled by adjusting the amount of OAM and the Cu/Ni ratio of the precursor. The average diameter of the prepared CuNi NPs ranged from 10.2 to 56.9 nm. It had been confirmed that CuNi NPs were an alloy of Cu and Ni and effectively resistant to oxidation. The prepared CuNi NPs could be separated under an external magnetic field without any energy consumption since they were superparamagnetic. Among the prepared CuNi NPs with different compositions, the Cu3Ni7 NPs were the best catalyst for catalytic transfer hydrogenation of nitrobenzene with ethylene glycol (EG) as the hydrogen donor, giving a nitrobenzene conversion of 99% and an aniline yield of >97%. The conversion and yield remained above 95% and 80% respectively after 10 cycles of NOBF4-treated Cu3Ni7 NPs, demonstrating good reusability for the CTH reaction. This work reported a novel method for preparing magnetic CuNi NPs and also provided a new approach for the hydrogenation of nitroarene catalyzed by non-noble metals in a green environment.
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Journal of Energy Chemistry
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2023
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IF 13.1
Bing Ma,Jingqing Tian,Xueling Lang,Shutao Lei,Bolong Li,Chen Zhao
Ultra-long n -alkanes are highly valuable in both scientific research and as major constituents of specialty high-melting-point waxes. Unlike conventional methods (e.g., Fischer–Tropsch (FT), ethylene oligomerization, and polyethylene cracking) typically resulting in wide n -alkane distributions, the elaborate design strategy presented herein allows the direct synthesis of pure, long n -alkanes using a modular splicing method with acetone, furfural, and fatty acid anhydrides or acyl chlorides as bio-blocks. The herein approach is based on a simple four-step catalytic reaction scheme involving C–C chain elongation and C–O bond activation. The synthesized pure n -alkanes had a carbon chain length as high as C 49 (total yield of 49%). The synthesis approach also allows to selectively prepare n -alkanes with even and odd carbon numbers ranging from C 15 to C 49 . This process represents a great breakthrough in the synthesis of long-chain pure n -alkanes, surpassing the carbon number limitations reported in previous methodologies.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2023
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IF 5.8
Li Yang,Ma Hairun,Li Qianwei,Yan Guangxu,Guo Shaohui
Ti/SnO 2 -Sb electrodes possess high catalytic activity and efficiently degrade nitrobenzene (NB); however, their low service life limits their wide application. In this study, we used one-step hydrothermal synthesis to successfully prepare Pt-Nd co-doped Ti/SnO 2 -Sb nanosphere electrodes. Scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy were applied to characterize the surface morphology, microstructure, and chemical composition of the electrodes, respectively. The electrochemical activity and stability of the electrodes were characterized via linear sweep and cyclic voltammetry, electrochemical impedance spectroscopy, and an accelerated service life test; their performance for NB degradation was also studied. An appropriate amount of Pt-Nd co-doping refined the average grain size of SnO 2 and formed a uniform and compact coating on the electrode surface. The oxygen evolution potential, total voltammetric charge, and electron transfer resistance of the Ti/SnO 2 -Sb-Nd-Pt electrodes were 1.88 V, 3.77 mC/cm 2 , and 11.50 Ω, respectively. Hydroxy radical was the main active radical species during the electrolytic degradation of nitrobenzene with Ti/SnO 2 -Sb-Nd-Pt. After Pt-Nd co-doping, the accelerated service life of the electrodes was extended from 8.0 min to 78.2 h (500 mA/cm 2 ); although the NB degradation rate decreased from 94.1 to 80.6%, the total amount of theoretical catalytic degradation of NB in the effective working time increased from 17.4 to 8754.1 mg/cm 2 . These findings reveal good application potential for the electrodes and provide a reference for developing efficient and stable electrode materials.
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PubMed
高影响因子
Engineering
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2023
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IF 12.8
Ning Li,Haoxi Dai,Mengting He,Jun Wang,Zhanjun Cheng,Beibei Yan,Wenchao Peng,Guanyi Chen
The distribution pattern of metals as active centers on a substrate can influence the peroxymonosulfate (PMS) activation and contaminants degradation. Herein, atomic layer deposition is applied to prepare Cu single atom (SA-Cu), cluster (C-Cu), and film (F-Cu) decorated MXene catalysts by regulating the number of deposition cycles. In comparison with SA-Cu-MXene (adsorption energy ( E ads ) = −4.236 eV) and F-Cu-MXene ( E ads = −3.548 eV), PMS is shown to adsorb preferably on the C-Cu-MXene surface for activation ( E ads = −5.435 eV), realizing higher utilization efficiency. More SO 4 − · are generated in C-Cu-MXene/PMS system with steady-state concentration and 1–3 orders of magnitude higher than those in the SA-Cu-MXene and F-Cu-MXene activated PMS systems. Particularly, the contribution of SO 4 − · oxidation to sulfamethoxazole (SMX) degradation followed the order, C-Cu-MXene (97.3%) > SA-Cu-MXene (90.4%) > F-Cu-MXene (71.9%), realizing the larger SMX degradation rate in the C-Cu-MXene/PMS system with the degradation rate constants ( k ) at 0.0485 min −1 . Additionally, SMX degradation routes in C-Cu-MXene/PMS system are found with fewer toxic intermediates. Through this work, we highlighted the importance of guided design of heterogeneous catalysts in the PMS system. Appropriate metal distribution patterns need to be selected according to the actual water treatment demand. Metal sites could be then fully utilized to produce specific active species to improve the utilization efficiency of the oxidants.
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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Tingting Liu,Zizhu Wang,Mingxi Liu,Tao Hu,Shenghu Zhou
In this study, we report a facile templating method to construct hollow silica nanotubes. In particular, bis-terpyridine is used to coordinate metal ions to form polymeric bis-terpyridine–metal complexes that further self-assemble into tubular organogels in the presence of cetyltrimethylammonium bromide. The following silica deposition on organogels and subsequent calcination give metal oxide-doped hollow silica nanotubes (MxOy-HSNs). Facilitated by the high coordination stability constants of bis-terpyridine with metal ions, a series of metal ions, such as Fe, Ni, Cu, and Zn, could be used to form polymeric bis-terpyridine–metal complexes. The supported Pt/FexOy-HSNs exhibit good catalytic performance for hydrogenation of a series of substituted nitrobenzenes, showing that the obtained MxOy-HSNs could be used as catalyst supports due to their good textural properties.
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