APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Jiaxing Yu,Zeyu Gong,Shaohan Wang,Huajie Zhong,Yuan Tao,Yu Hou,Qi Fu,Huangsheng Yang,Jianqiang Li,Junhui Wang,Zhengping Hao,Gangfeng Ouyang
Carbon-based advanced oxidation processes through electron-transfer pathway are regarded as a green technology for efficient and selective oxidation of the emerging pollutants in complex water matrixes. Despite achievements in the superior activity and selectivity for organic degradation of carbocatalysts, their stabilities remain unsatisfactory, primarily because of the underexplored deactivation mechanisms. This study identifies two distinct deactivation mechanisms. The first is Oxidant Deactivation, due to overoxidation by the oxidant and predominantly affected by the concentration of oxidant. The other is Organic Deactivation, primarily caused by attachment of organic byproducts on catalyst surface, which reduces the overall oxidation potential of carbon/persulfate complex, instead of covering the surface “active sites”. Furthermore, the deactivation mechanisms mainly depend on intrinsic catalytic pathways: Oxidant Deactivation originates from the adjacent transfer pathway and Organic Deactivation from the electron shuttle pathway. Finally, the relationship between the deactivation mechanisms and carbon configuration (sp 2 /sp 3 ) is revealed, and a catalyst with optimal activity and stability can be achieved through properly regulating the sp 2 /sp 3 ratio. Results indicate that different protective strategies and application scenarios should be adopted for different systems to extend their lifespan in real wastewater treatment. This work sheds light on rational catalyst design toward advanced water purification systems with high efficiency and stability.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
MOLECULES
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2023
·Vol. 28
·期 13
·5176
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IF 4.6
Dongrong Cheng,Xiaofeng Wei,Yanting Zhang,Qian Zhang,Jianwei Xu,Jiaxin Yang,Junjie Yu,Antony Stalin,Huan Liu,Jintao Wang,Dian Zhong,Lanying Pan,Wei Zhao,Yuan Chen
Erythromycin is one of the few compounds that remarkably increase ether-a-go-go-related gene (hERG) inhibition from room temperature (RT) to physiological temperature (PT). Understanding how erythromycin inhibits the hERG could help us to decide which compounds are needed for further studies. The whole-cell patch clamp technique was used to investigate the effects of erythromycin on hERG channels at different temperatures. While erythromycin caused a concentration-dependent inhibition of cardiac hERG channels, it also shifted the steady-state activation and steady-state inactivation of the channel to the left and significantly accelerated the onset of inactivation at both temperatures, although temperature itself caused a profound change in the dynamics of hERG channels. Our data also suggest that the binding pattern to S6 of the channels changes at PT. In contrast, cisapride, a well-known hERG blocker whose inhibition is not affected by temperature, does not change its critical binding sites after the temperature is raised to PT. Our data suggest that erythromycin is unique and that the shift in hERG inhibition may not apply to other compounds.Keywords:erythromycin;temperature;hERG;steady-state activation;steady-state inactivation
研究领域:
药理学
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心脏病学
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生物物理学
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DOI
PubMed
高影响因子
Nature Communications
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2023
·Vol. 14
·期 1
·1-20
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IF 16.6
Xu Tao,Ji Haifeng,Xu Lin,Cheng Shengjun,Liu Xianda,Li Yupei,Zhong Rui,Zhao Weifeng,Kizhakkedathu Jayachandran N.,Zhao Changsheng
Clinical use of intraoperative auto-transfusion requires the removal of platelets and plasma proteins due to pump-based suction and water-soluble anticoagulant administration, which causes dilutional coagulopathy. Herein, we develop a carboxylated and sulfonated heparin-mimetic polymer-modified sponge with spontaneous blood adsorption and instantaneous anticoagulation. We find that intrinsic coagulation factors, especially XI, are inactivated by adsorption to the sponge surface, while inactivation of thrombin in the sponge-treated plasma effectively inhibits the common coagulation pathway. We show whole blood auto-transfusion in trauma-induced hemorrhage, benefiting from the multiple inhibitory effects of the sponge on coagulation enzymes and calcium depletion. We demonstrate that the transfusion of collected blood favors faster recovery of hemostasis compared to traditional heparinized blood in a rabbit model. Our work not only develops a safe and convenient approach for whole blood auto-transfusion, but also provides the mechanism of action of self-anticoagulant heparin-mimetic polymer-modified surfaces.
研究领域:
血液学
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外科技术
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材料科学
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生物医学工程
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DOI
PubMed
高影响因子
JOURNAL OF FOOD ENGINEERING
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2024
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IF 5.3
Xiaodan Guo,Lei Zhang,Xinian Li,Xiaojing Ren,Jian Yu,Tianli Yue,Fangyu Long
High hydrostatic pressure (HHP) is widely used to inactivate microorganisms in food, but achieving effective spore inactivation by conventional HHP remains challenging due to their resistance. The present study compared the effectiveness of continuous, intermittent and induced inactivation HHP techniques for inactivation of Alicyclobacillus acidoterrestris spores. Under optimal induced inactivation conditions (200 MPa/4 cycles, 600 MPa/2 cycles), reductions of 0.79 log CFU/mL for the highly resistant DSM3922 spores and 1.94 log CFU/mL for the less resistant DSM3924 spores were achieved. Mechanistic investigations revealed that: (Ⅰ) structural damage, including breakage, wrinkling, and concavity, was induced in spores post-HHP treatment; (Ⅱ) pulsation forces generated by repeated pressurization and depressurization during induced inactivation HHP reduced the D90 values of the spore aggregates to 99.37 μm for DSM3922 and 76.49 μm for DSM3924, enhancing the inactivation efficacy; (Ⅲ) the inner membrane (IM) and cortex were severely impaired, while nucleic acid and protein leakage from spores significantly increased after HHPs. To further enhance spore inactivation, Tea Tree, Nutmeg, Eucalyptus, and Litsea cubeba essential oils (EOs) were selected from twelve EOs as safe and effective antimicrobial substances that synergize with HHP. Combining 5% Litsea cubeba EO with HHP (200 MPa/4 cycles, 600 MPa/2 cycles) resulted in reductions of 2.57 log CFU/mL for DSM3922 and 5.08 log CFU/mL for DSM3924. These findings suggest that the combination of HHP and EOs could be a promising approach for inactivating A. acidoterrestris spores.
研究领域:
食品科学
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微生物学
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DOI
高影响因子
ENERGY & FUELS
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2022
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IF 4.654
Nini Zhang,Sheng-Li Chen,Ruyue Zhu,Wei Sun
In this work, we found that besides formaldehyde, an important intermediate in methanol-to-olefins (MTO) conversion, acetaldehyde and acetone were also formed in the MTO reaction and accurately quantified their contents in the reaction system with time on stream. The formation of formaldehyde, acetaldehyde, and acetone follows a sequential reaction. Acetaldehyde could induce the formation of aromatic species, promoting the conversion of lighter aromatic species across cages to polycyclic aromatics and further promoting the formation of insoluble coke, resulting in rapid catalyst deactivation. In addition, acetaldehyde enhances the propagation of the aromatic-based cycle, which leads to the formation of ethylene, thus resulting in the high ethylene selectivity. In contrast, acetone has little effect on the working lifetime of the catalyst and the product distribution of the MTO reaction, although it can be converted to light hydrocarbons similar to that of MTO under the circumstance of the MTO reaction.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
ENERGY & FUELS
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2025
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IF 5.3
Jinsong Luo,Tianci Xiao,Xiang Li,Qingyu Wang,Xusheng Zheng,Jiuzhong Yang,Chengyuan Liu,Yang Pan
The methanol-to-hydrocarbon (MTH) reaction offers a promising non-fossil fuel pathway for the production of olefins and aromatics. A formaldehyde (HCHO) intermediate has attracted great attention due to its critical role in the aromatization and coking process of the MTH reaction. However, because of the difficulty in the direct detection of HCHO, details on the impact of reaction condition on its formation and conversion were seldom studied. Here, synchrotron radiation photoionization mass spectrometry (SR-PIMS) was applied to thoroughly study the changes in HCHO and other relevant species under different reaction conditions, including contact time, temperature, zeolite acidity, and methanol concentration. It is revealed that higher temperature and acidity promoted the formation of HCHO and its transformation to aromatics and coke, whereas higher methanol concentration mainly enhanced hydrogen transfer reactions, resulting in a higher yield of polyunsaturated species and, consequently, more aromatics. Combining the results from SR-PIMS and soft X-ray absorption spectroscopy of the spent catalyst, it is verified that HCHO formation promoted coke formation, but the presence of olefinic species can shift the methanol conversion pathway toward methylation reactions and then limit the level of HCHO yield. Therefore, we proposed a butanol cofeeding strategy that can limit the contribution of HCHO-induced coke formation and extend the catalyst lifetime by up to ∼60%.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jiayou Liu,Xiaoxiang Huang,Lizhen Hu,Penglei Liu,Liuhu Jia,Keiko Sasaki,Zhongchao Tan,Hesheng Yu
Simultaneous avoidance of secondary air pollution and catalyst deactivation remains a challenge for existing photocatalytic removal of nitric oxide (NO). Herein, a photocatalysis-adsorption (P-A) heterojunction is synthesized for eco-friendly NO removal by facilely grinding Pd single atoms (Pd 1 ) anchored g-C 3 N 4 (48CN/Pd) with UiO-66-NH 2 (UION). Under visible-light irradiation, the 40UION-CN/Pd composite shows 93.91 % of NO removal efficiency with only 2.73 % of NO 2 emissions and negligible catalyst deactivation. The DeNO x index increases remarkably from −0.66 for 48CN/Pd to 0.86 for 40UION-CN/Pd. Furthermore, the synthesized P-A heterojunction efficiently removes NO from real flue gases produced by a domestic coal-fired stove and from SO 2 -rich flue gases. The mechanism exploration based on experimental investigations and density functional theory (DFT) calculations reveals that UION captures the NO 2 selectively produced by 48CN/Pd, simultaneously suppressing NO 2 emissions and refreshing active sites for NO photooxidation. Moreover, the results of X-ray photoelectron spectroscopy (XPS), charge density difference calculation, energy-resolved distribution of electron traps (ERDT) and in-situ Kelvin probe force microscopy (KPFM) reveal that the built-in electric field and Type-II heterojunction formed between 48CN/Pd and UION promote the separation of photogenerated carriers, enhancing the catalytic activity of the composite. This work provides an innovative strategy to avoid NO 2 emission and catalyst deactivation during photocatalytic NO removal.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Tianyu Ren,Shengping You,Muyuan Zhang,Yuefei Wang,Wei Qi,Rongxin Su,Zhimin He
Herein, the lignin-to-fuel conversion process was studied using real lignin as feedstock. Unlike model compounds, real lignin poisons the catalyst, causing rapid deactivation. The problem of catalyst deactivation was analyzed in detail for improving the conversion efficiency. We found that heavy carbonaceous deposits on the inner surface of the catalyst were responsible for the fast deactivation encountered in the conventional one-step reaction process. Moreover, the ester structures in lignin, which have previously been neglected in research, were confirmed to considerably worsen catalyst deactivation because they induce easier polymerization and hinder lignin conversion. Based on these points, we developed a three-step method that eliminates serious catalyst deactivation in the lignin-to-fuel conversion process, involving depolymerization of lignin, extraction of lignin monomers and hydrodeoxygenation of lignin monomers. The fuel production was 8.1–17.6-times more efficient using this three-step method than using the one-step batch reaction.
研究领域:
化学工程
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能源科学
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DOI
高影响因子
Catalysts
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2024
·Vol. 14
·期 5
·288
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IF 3.8
Tianyun Wang,Yingjie Guan,Haidan Wu,Zhaojie Su,Jianguo Zhuang,Siyan Yan,Xuedong Zhu,Fan Yang
Utilizing carbon dioxide as a carbon source for the synthesis of olefins and aromatics has emerged as one of the most practical methods for CO2reduction. In this study, an improved selectivity of 85% for targeting products (ethylbenzene and propylbenzene) is achieved with a benzene conversion of 16.8% by coupling the hydrogenation of carbon dioxide to olefins over the bifunctional catalyst “Oxide-Zeolite” (OX-ZEO) and the alkylation of benzene with olefins over ZSM-5. In addition to investigating the influence of SAPO-34 and ZSM-5 zeolite acidity on product distribution, catalyst deactivation due to coke formation is addressed by modifying both molecular sieves to be hierarchical to extend the catalyst lifespan. Even after 100 h of operation at 400 °C, the catalysts maintained over 80% selectivity towards the target products, with benzene conversion over 14.2%. Furthermore, the pathway of propylbenzene formation is demonstrated through simple experimental design, revealing that the surface Brønsted acid sites of SAPO-34 serve as its primary formation sites. This provides a novel perspective for further investigation of the reaction network.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
Journal of Environmental Sciences
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2021
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IF 5.565
Chang Cui,Yan Zhang,Wenpo Shan,Yunbo Yu,Hong He
Alumina supported Pd catalyst (Pd/Al 2 O 3 ) is active for complete oxidation of methane, while often suffers transient deactivation during the cold down process. Herein, heating and cooling cycle tests between 200 and 900°C and isothermal experiments at 650°C were conducted to investigate the influence of NO x on transient deactivation of Pd/θ-Al 2 O 3 catalyst during the methane oxidation. It was found that the co-fed of NO alleviated transient deactivation in the cooling ramp from 800 to 500°C, which was resulted from the in situ formation of NO 2 during the process of methane oxidation. Over the Pd/θ-Al 2 O 3 , thermogravimetric analysis and O 2 temperature programmed oxidation measurements confirmed that transient deactivation was due to the decomposition of PdO particles and the hysteresis of Pd reoxidation, while the metal Pd entities were less active for methane oxidation than the PdO ones. CO pulse chemisorption and scanning transmission electron microscopy characterizations rule out the NO 2 effect on Pd size change. Powder X-ray diffraction and X-ray photoelectron spectroscopy characterizations were used to obtain palladium status of Pd/θ-Al 2 O 3 before and after reactions, indicating that in lean conditions at 650°C, the presence of NO 2 increases the content of active PdO on the catalyst surface, thus benefits methane oxidation. Homogeneous reaction between CH 4 , O 2 , and NO x may be partially responsible for the alleviation above 650°C. The interesting research of alleviation in transient deactivation by NO x , the components co-existing in exhausts, are of great significance for the application.
研究领域:
催化化学
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环境科学
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DOI
高影响因子
RENEWABLE ENERGY
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2019
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IF 5.439
Qing Zhou,Xinyan Zhong,Xingyue Xie,Xuanyi Jia,Baiquan Chen,Ning Wang,Lihong Huang
Biomass-derived acetic acid (HAc), as a hydrogen storage medium, can be transformed to hydrogen via on-board reformer for fuel cells. Steam reforming (SR) of HAc is a traditional hydrogen production process, but endothermicity of SR is a concern for heat management in dynamic on-board application. Auto-thermal reforming (ATR) of HAc is a promising route, while catalyst deactivation in harsh ATR atmosphere should be addressed. Samarium-promoted ordered mesoporous Ni-xSm-Al-O catalysts were synthesized via improved evaporation-induced self-assembly (EISA) method, and tested in ATR of HAc for hydrogen production. The Ni-2Sm-Al-O catalyst produced a stable HAc conversion near 100.0% and a hydrogen yield at 2.6 mol-H 2 /mol-HAc in a 30-h test. Meanwhile, the Ni-2Sm-Al-O catalyst shows resistance to oxidation , sintering and coking; this improved reactivity and durability can be attributed to basic Sm oxides and ordered mesoporous framework with confinement effect : the basic sites are beneficial to adsorption and activation of HAc, and the ordered mesoporous framework constrains the thermal agglutination of Ni metal and formation of coking, while intermediate carbonous species of *CH x (x = 0–3) can be gasified via the Sm 2 O 3 -Sm 2 O 2 CO 3 cycle. These Sm-promoted Ni-based catalysts are also tested with different temperatures and O/C, and show potentials in ATR of HAc for hydrogen production.
研究领域:
能源化学
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催化科学
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产品关联
DOI
高影响因子
Carbon Capture Science & Technology
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2025
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IF 10.5
Haoyu Xiao,Guocheng Wang,Shengwei Feng,Shuaishuai Lei,Yang Yang,Yingquan Chen,Haiping Yang,Hanping Chen
Understanding the influence of polyvinyl chloride (PVC) on carbon nanotube (CNT) production from waste plastics is essential for enhancing the high-value utilization of real plastic waste. Hence, the influence of chlorine (Cl) on plastic catalytic pyrolysis for CNT formation was investigated from the perspective of Cl in the volatile phase and the catalyst phase, aiming to find the potential strategy to mitigate the impact of Cl. The results showed that catalyst reduction effectively converts Fe 2 O 3 into a more stable Fe 2 AlO 4 spinel structure, thereby safeguarding the active Fe site from deactivation. The carbon yield increased from 17 wt% to 25 wt%, in the instance of real plastic with roughly 10 wt% PVC content. And, at a lower catalytic temperature (600 °C), the catalyst also displays increased resistance to hydrogen chloride (HCl) volatiles. Optimal adjustment of pyrolysis and catalytic temperatures can significantly mitigate catalyst deactivation by Cl and produce CNT with a maximum carbon yield of 28 wt%. This work proposes a pioneering anti-chlorine process designed to recover high-value products from plastic waste, advancing carbon sequestration strategies.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
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