APPLIED ENERGY
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2022
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IF 11.446
Wenshuo Hu,Yu Zhang,Xiaoxiang Wang,Weihong Wu,Hao Song,Yang Yang,Shaojun Liu,Chenghang Zheng,Xiang Gao
Ceria has absorbed extensive interests in functioning as catalysts for low-temperature (LT) selective catalytic reduction (SCR) of NOx due to its abundant surface oxygen species and salient redox property. The mechanistic interpretations of how such redox property contributes to its LT-SCR activity, however, still remain debated. Here, we use a model tungsten-promoted ceria catalyst (WO 3 /CeO 2 ), known as preeminent in LT-SCR reactions, and combine steady-state kinetic, structural characteristic and in situ spectroscopic experiments with theoretical treatments to reveal the mechanistic connections between NO oxidative activation and LT-SCR turnovers. We show that, compared with NO oxidation to NO 2 , NO oxidative activation to nitrite intermediates is both kinetically and thermodynamically more favorable; surface nitrate species are not detected in the present case, indicating their more difficult formation than nitrites. All these results thus suggest the prevalence of NO activation to nitrites over NO to nitrates or oxidation to NO 2 and subsequent occurrence of fast SCR in the WO 3 /CeO 2 -catalyzed LT-SCR reaction. These findings progress the understanding of LT-SCR reaction mechanism on CeO 2 -based catalysts and convey a detailed perspective of different reaction intermediates and their consequences for LT-SCR turnovers, which may contribute to the rational design of catalysts towards further improved LT-SCR activity.
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CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Yingnan Zhao,Xing Qin,Xinyu Zhao,Xin Wang,Huaqiao Tan,Huiying Sun,Gang Yan,Haiwei Li,Wingkei Ho,Shun-cheng Lee
Bismuth-based photocatalysts are a class of excellent visible-light photocatalysts; however, their redox activity is relatively poor and the efficiency of photogenerated carrier separation is low, limiting their development and application in the field of photocatalysis . To address these issues, a series of polyoxometalate PW 12 O 40 3– -doped Bi 2 O 3– x /Bi Schottky photocatalysts PW 12 @Bi 2 O 3– x /Bi- n (PBOB- n , where n is the amount of NaBH 4 , i.e., 6, 12, 18, 24, and 48 mg) were prepared by a simple electrospinning/calcination/in-situ NaBH 4 reduction method. In this composite photocatalyst, the doping of PW 12 could effectively adjust the electronic structure of Bi 2 O 3– x and improve its redox properties. As a shallow electron trap, PW 12 promoted the separation of the photogenerated carriers. Furthermore, desirable Schottky junction between the metal Bi nanoparticles and PW 12 @Bi 2 O 3– x further accelerated the separation of the photogenerated carriers. The synergistic effect of the aforementioned factors endowed PBOB- n with excellent photocatalytic activity. Among the samples, PBOB-18 exhibited superior photocatalytic activity. Under visible-light irradiation, 93.7% (20 mg catalyst) of 20 ppm tetrabromobisphenol A (TBBPA, 20 mL) was degraded in 60 min. Its activity was 4.4 times higher than that of Bi 2 O 3 . PBOB-18 also exhibited an ultrahigh photocatalytic performance for the removal of NO. Its removal rate (600 ppb) reached 83.3% in 30 min, making it one of the most active Bi-based photocatalysts. Furthermore, the photocatalytic mechanisms of PBOB-18 for TBBPA and NO have been proposed. This work provides a new direction and reference for the design of low-cost, efficient, stable, and versatile photocatalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
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IF 9.136
Ying Zhang,Xu Li,Zhi Wang,Jixiao Wang
The fabrication of anti-biofouling nanofiltration (NF) membrane is one of the effective methods to improve the vulnerability of membranes to bacteria in the feed solution. The prevalent approach to prepare anti-biofouling NF membranes is to graft biotoxic substances onto the NF membrane surface to kill the attached bacteria, inducing antimicrobial resistance in bacteria and water safety problem. In this study, non-biotoxic methyl 2-aminobenzoate (MA) was employed to prepare the anti-biofouling NF membranes. Instead of killing bacteria, the modified NF membrane could effectively prevent proliferation of bacteria on the membrane surface by blocking the quorum sensing in bacteria, thereby avoiding the generation of antimicrobial resistance. On the condition that the bacteria are alive, the biofilm formed by Escherichia coli ( E. coli ) and Bacillus subtilis ( B. subtilis ) on the modified NF membrane were significantly reduced by 94.5% and 65.1%, respectively. Additionally, the modified membrane showed superior anti-adhesion property for proteins and polysaccharides, attributing from the improved hydrophilicity of membrane surface. The optimally modified membrane exhibited the enhanced water permeability (from 6.72 L m -2 h −1 bar −1 to 12.12 L m -2 h −1 bar −1 ) and un-degraded divalent salt rejection (98.4% of Na 2 SO 4 ). This work provided an efficient and non-biotoxic approach for the fabrication of environmental friendly anti-biofouling NF membranes, which would eliminate the worries about the water safety and the development of antimicrobial resistance in bacteria.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2023
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IF 4.3
Li-Zhi Zhang,Hong-Bin Ju,Tao Geng,De-Bao Li,Ya-Jie Jiang,Ya-Kui Wang
Graphical A novel phase transfer catalyst comprising phosphotungstic acid and biquaternary ammonium cation salt is synthesized for the epoxidation of long carbon chain olefins under solvent-free conditions, which exhibits high selectivity for epoxides. Different methods are used to characterize the fundamental structure and catalytic mechanism of this catalyst. In this study, we have developed a novel catalyst synthesized by phosphotungstic acid and a gemini quaternary ammonium cation salt. This quaternary ammonium salt not only reduces the interfacial tension between olefins and hydrogen peroxide but also forms a notably stable structure with phosphotungstic acid. Dodecene was successfully epoxidized to epoxy dodecane with a selectivity of 82.9 %. The impact of initial conditions was systematically investigated such as molar ratio, temperature, reaction time, and catalyst dosage on the catalytic performance. Characterization of the catalyst morphology was performed by SEM, TEM and SAXS. Raman spectra, FT-IR and XPS spectra were employed to perform the catalyst transformation during the epoxidation reaction. This catalytic mechanism study could provide the industrial application in the epoxidation of long-chain olefins.
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PubMed
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Nanoscale
·
2023
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IF 6.7
Yingyi Zhang,Lin Zhang,Yuhan Zhang,Rong Ju,Guoqing Wei
Antimicrobial sonodynamic therapy (SDT) has broad application potential in the eradication of multidrug-resistant (MDR) bacterial infections due to its non-invasiveness, absence of resistance concern, and high cytotoxicity. However, the hypoxic infection microenvironment and the rapid depletion of O2 during SDT severely limit the therapeutic efficacy of SDT. Herein, an ultrasound-controllable ROS-responsive nanoplatform (FOT/Fe3O4@Lipo-ICG) was constructed and prepared by encapsulating FOT and Fe3O4 nanoparticles (Fe3O4 NPs) within sonosensitiser ICG-modified liposomes. Both in vitro and in vivo, we observed that the ICG conjugation on the surface of liposomes could effectively maintain a good dispersion and prevent ICG aggregates in complex biological matrices. In addition, the liposomes could significantly block the catalytic activity of the Fe3O4 NPs, as well as the release of FOT, whereas upon US irradiation, the catalytic activity of Fe3O4 NPs was recovered to catalyse the decomposition of endogenous H2O2 into O2 and •OH. Meanwhile, the FOT was successfully released to react with endogenous glutathione to sequentially produce NO. Based on the aforementioned advantages, the FOT/Fe3O4@Lipo-ICG demonstrated potent efficacy in eradicating methicillin-resistant Staphylococcus aureus-induced local infection and sepsis resulting from local infection. Thus, the developed US-controllable nanoplatform offers a promising strategy for enhancing SDT for eradicating MDR bacterial infections.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Fei Wang,Zhe Wang,Junjian Yu,Shuai Han,Xiangwei Li,Yan Wang
Mixed matrix membranes (MMMs) based on metal–organic frameworks (MOFs) are expected to realize efficient separation of CO 2 . However, interfacial compatibility issues between MOFs and polymer matrices limit their performance. In this work, a post-synthesis modification (PSM) strategy was adopted to convert UiO-66 into porous liquids (PLs). MMMs were prepared by incorporating PLs into PIM-1 matrix. The PLs have a liquid-like behavior and can be evenly scattered in PIM-1 matrix to form an interface without defect. The SEM morphology analysis further certified that MMMs had no interface defect and PLs had brilliant compatibility with the polymer film . In addition, the CO 2 -philic ether bonds of the EO fragments enable the MMMs to have superior CO 2 selective separation. Compared with pure PIM-1, the highest CO 2 permeability was improved by 158.0 % and 62.5 % was the increase in CO 2 /N 2 selectivity, arriving at 7211.7 Barrer and 26.0, respectively. Meanwhile, the overall separation performance of MMMs for CO 2 /N 2 exceeds the 2008 Robson upper limit, showing outstanding gas separation performance.
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Asian Journal of Pharmaceutical Sciences
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2023
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IF 10.2
Min Zhong,Peiqin Liang,Zhenzhen Feng,Xin Yang,Guang Li,Rui Sun,Lijuan He,Jinxiu Tan,Yangpengcheng Xiao,Zhiqiang Yu,Muhua Yi,Xuefeng Wang
Ovarian cancer (OC) is one of the most common and recurring malignancies in gynecology. Patients with relapsed OC always develop "cascade drug resistance" (CDR) under repeated chemotherapy, leading to subsequent failure of chemotherapy. To overcome this challenge, amphiphiles (P1) carrying a nitric oxide (NO) donor (Isosorbide 5-mononitrate, ISMN) and high-density disulfide are synthesized for encapsulating mitochondria-targeted tetravalent platinum prodrug (TPt) to construct a nanocomposite (INP@TPt). Mechanism studies indicated that INP@TPt significantly inhibited drug-resistant cells by increasing cellular uptake and mitochondrial accumulation of platinum, depleting glutathione, and preventing apoptosis escape through generating highly toxic peroxynitrite anion (ONOO − ). To better replicate the microenvironmental and histological characteristics of the drug resistant primary tumor, an OC patient-derived tumor xenograft (PDX OC ) model in BALB/c nude mice was established. INP@TPt showed the best therapeutic effects in the PDX OC model. The corresponding tumor tissues contained high ONOO − levels, which were attributed to the simultaneous release of O 2 •− and NO in tumor tissues. Taken together, INP@TPt-based systematic strategy showed considerable potential and satisfactory biocompatibility in overcoming platinum CDR, providing practical applications for ovarian therapy.
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Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Liu Yang,Jing Li,Guoqiang Cao,Yiyan Yang,Wen Luo,Zhiqi Zhang,Lizhi Feng,Xinglai Zhang,Baodan Liu
This study reports on the development of highly-efficient Pt/CuO-Fe 2 O 3 /TiO 2 monolithic catalysts for the low-temperature conversion of NO to N 2 via CO-SCR. In this case, ultrathin TiO 2 nanosheet arrays are designed to in situ grow on flexible Ti mesh to provide more spaces/areas for the loading of highly-dispersed Fe 2 O 3 and CuO active components. Furthermore, Pt nanoparticles with an average size of 1.30 nm are effectively decorated on the surface of CuO-Fe 2 O 3 /TiO 2 . The H 2 -TPR and NO-TPD results demonstrate that the excellent synergistic effect between TiO 2 , CuO, Fe 2 O 3 and trace amounts of Pt is conducive to enhance the adsorption of NO and finally promote the CO-SCR. The obtained Pt/CuO-Fe 2 O 3 /TiO 2 catalysts exhibit excellent CO-SCR performance with 100 % NO conversion, and 100 % N 2 selectivity at 250 °C, showing great potential of de-NO x application by using toxic CO as reductant in industry.
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FOOD CHEMISTRY
·
2021
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IF 7.514
Wenji Zhang,Junxi Cao,Zhigang Li,Qiuhua Li,Xingfei Lai,Lingli Sun,Ruohong Chen,Shuai Wen,Shili Sun,Zhaoxiang Lai
Each type of tea has a unique volatile profile due to its variety, processing technologies and origin. Using HS-SPME and GC/MS, we analyzed the changes of volatile components in cultivar Yinghong No. 9 during pile-fermentation every 10 days. A total of 94 compounds showed significant differences during a total of 60 days mainly including alkanes, ketones, esters, terpenes, aromatics and heterocyclic compounds. Interestingly, 13 metabolites were progressively reduced during the first 20 days and remained unchanged in subsequent procedures, while 17 metabolites remained unchanged in the early stage and progressively increased during the last 20 days of pile fermentation, indicating that they are characteristic volatile compounds of raw material sun-dried green tea and dark tea, respectively. β-ionone, phenylethyl alcohol, and a-ionone could be the top three contributed aroma compounds in the final dark tea. Our study provides a theoretical basis for process and quality improvement of Yinghong No. 9.
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CATALYSIS LETTERS
·
2020
·Vol. 151
·期 6
·1755-1765
·
IF 2.482
Meng Fanyu,Zhang Mingjia,Zhou Fayang,Zou Haocheng,Zhu Boming,Zeng Yiqing,Zhang Shule,Zhong Qin
Abstract CrO x /black-TiO 2 catalysts were prepared by ligand-assisted (citric acid, oxalic acid and ethylenediaminetetraacetic acid) impregnation method. These catalysts were characterized in detail by means of X-ray diffraction, Raman, BET, X-ray photoelectron spectroscopy, H 2 and O 2 (NO) temperature programmed reduction or desorption and in-suit DFTIR spectra. The results indicated that ligands assistance was beneficial for CrO x interacted with oxygen vacancies and O–Ti–O structures. Among all the catalysts, CrO x /black-TiO 2 /CA (modified by citric acid) revealed excellent catalytic activity and stability for NO oxidation in the temperature range of 200–450 °C. The characterization results exhibited that the interaction existed between CrO x and oxygen vacancies resulting in more Cr 6+ . Moreover, the strong interaction between CrO x and O–Ti–O was attributed to the modification of carboxylic acid, which increased the content of Cr 3+ and chemical adsorption oxygen. High content of chemical adsorption oxygen promoted the adsorption ability of O 2 , and Cr 6+ enhanced the adsorption capacity of NO. Hence, chemical adsorption oxygen and Cr 6+ synergistically promoted the NO oxidation. Graphic Abstract
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CATALYSIS LETTERS
·
2020
·Vol. 151
·期 4
·966-979
·
IF 2.482
Liu Qinglong,Yang Jingchao,Luo Mingsheng,Yang Zhi,Zhao Qiuna
Abstract A series of Mn–Ti oxide catalysts were synthesized by the sol–gel method and the effects of different synthesis conditions were investigated in sequence. The microstructures and properties of the catalysts were characterized by using N 2 adsorption–desorption, XRD, SEM, H 2 -TPR, NH 3 -TPD, Raman and XPS. The catalytic performance over Mn–Ti oxide catalysts prepared under different synthesis conditions for the low-temperature SCR of NO with NH 3 were also comparatively evaluated. The results reveal that the calcination temperature and metal source play a significant role in the characteristics and the SCR activities of the catalysts. A relatively low calcination temperature is beneficial to low-temperature SCR activity. Manganese nitrate or manganese acetate as the Mn source combining with tetrabutyl titanate as Ti source can achieve high SCR activities. The excellent low-temperature NH 3 -SCR activity can be ascribed to the appropriate textural properties, amorphous Mn-oxides with equal ratio of Mn 3+ /Mn 4+ , good low-temperature reducibility and abundant surface B-acid sites. Graphic Abstract
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2020
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IF 3.99
Xuecheng Liu,Lin Liu,Zurun Yao,Zhehan Yang,Hui Xu
The nitrogen-rich ZnO/g-C 3 N 4 composites were prepared and exhibited excellent photocatalytic performance for hydrogen evolution and NO photo-oxidation under visible-light illumination. The obtained nitrogen-rich ZnO/g-C 3 N 4 composite has efficient visible-light utilization and effective separation of photogenerated electron-hole pairs. Experimental data verifies that the photocatalytic activity of ZnO/g-C 3 N 4 composite could be improved by N dopant. NZnOCN1 composite exhibits the highest photocatalytic activity for H 2 evolution and NO removal. The results show that the possible mechanism of the photocatalytic H 2 evolution reaction is the type II mechanism, while the Z-scheme mechanism of nitrogen-rich ZnO/g-C 3 N 4 composite is conducive to NO photo-oxidation.
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