INORGANIC CHEMISTRY
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2024
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IF 4.3
Xiaoxiao Zheng,Xiaoping Chen,Xiaoqing Li,Jide Zhu,Jipeng Chen,Fengcai Lin,Lijuan Shen,Yanlian Xu,Lilong Jiang
The development of stable and effective catalysts to convert toxic H2S into high value-added sulfur is essential for production safety and environmental protection. However, the inherent defects of traditional iron- and zirconium-based catalysts, such as poor activity, high oxygen consumption, and low sulfur selectivity, limit their further developments and applications. Herein, the Fe–Zr bimetallic organic framework FeUIO-66(x) with different cubic morphologies was synthesized via a facile solvothermal method. The results indicate that the introduction of Fe not only increases the specific surface area and weak L-sites of the catalyst without changing its crystal structure, which provides enough reaction space and more active sites for the adsorption and activation of H2S, but also reduces the activation energy of the reaction, significantly promoting the selective oxidation of H2S. As a result, the as-obtained FeUIO-66(1) catalyst exhibits the highest desulfurization activity and superior durability and water resistance stability, and its H2S conversion and sulfur selectivity within 50 h are 100 and 88%, respectively. More importantly, the structure of the catalyst after the desulfurization reaction is consistent with that of the fresh counterpart. The study offers new insights into the development of effective and stable bimetallic catalysts to eliminate H2S and recycle sulfur.
研究领域:
催化化学
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环境科学
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材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Jingran Zhang,Zihan Yuan,Chao Wang,Lele Liu,Yanan Wang,Yurong Guo,Guangjiu Zhao
Perovskite nanocrystals (PNCs) have attracted extensive attention for their potential applications in biology. However, only a handful of PNCs have been scrutinized in the biological domain due to issues such as instability, poor dispersion, and size inhomogeneity in polar solvents. The development of dual-functional perovskite nanomaterials with hydrogen sulfide (H 2 S) sensing and antibacterial capabilities is particularly intriguing. In this study, we prepared chiral quasi-two-dimensional (quasi-2D) perovskite nanomaterials, Bio(S-PEA) 2 CsPb 2 Br 7 and Bio(R-PEA) 2 CsPb 2 Br 7 , that were uniformly dispersed in aqueous media. The effective encapsulation of methoxypolyethylene glycol amine (mPEG-NH 2 ) improved water stability and uniformity of particle size. Circular dichroism (CD) signals were created by the successful insertion of chiral cations. These perovskites as probes showed a rapid and sensitive fluorescence quenching response to H 2 S, and the effect of imaging detection was observed at the Escherichia coli (E. coli) level. As antibacterial agents, their pronounced positive charge properties facilitated membrane lysis and subsequent E. coli death, indicating a significant antibacterial effect. This work has preliminary explored the application of chiral perovskites in biology and provides insight into the development of bifunctional perovskite nanomaterials for biological applications.
研究领域:
生物化学
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材料科学
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微生物学
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jun Tao,Hui Deng,Zhengnan Li,Liping Cao,Yanfei Rao,Zhanhai Yin
The progression and severity of osteoarthritis (OA) are significantly associated with intra-articular synovitis, with the imbalance of M1/M2 macrophages serving as a critical driving factor in the pathogenesis of synovitis. In this study, we developed macrophage-targeted nanomicelles capable of scavenging reactive oxygen species (ROS) and releasing hydrogen sulfide (H 2 S). These nanomicelles were encapsulated within injectable methacrylate gelatin (GelMA) porous hydrogel microspheres, thereby creating a new H 2 S gas therapy platform for the treatment of osteoarthritis. In vitro experiments demonstrated that GelMA@FPLBD actively targeted macrophages, efficiently removed ROS, and gradually released H 2 S. This process inhibited the expression of phosphorylated extracellular signal-regulated kinase (p-ERK) and phosphorylated signal transducer and activator of transcription 3 (p-STAT3) in activated macrophages, thereby suppressing M1 polarization and promoting M2 polarization, resulting in significant anti-inflammatory effects. In vivo experiments utilizing a destabilization of the medial meniscus (DMM)-induced osteoarthritis (OA) rat model further revealed the anti-inflammatory and cartilage-protective properties of GelMA@FPLBD, effectively mitigating the progression of OA. Therefore, this study indicates that GelMA@FPLBD, functioning as a H 2 S gas therapy platform, holds significant promise for the treatment of osteoarthritis (OA).
研究领域:
药理学
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纳米技术
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骨科
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炎症研究
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SENSORS AND ACTUATORS B-CHEMICAL
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2019
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IF 6.393
JunPing Wang,Ying Wen,FangJun Huo,CaiXia Yin
The research of endogenous hydrogen sulfide (H 2 S) biology function, pathological and pharmacological effects has been active in the field of chemists and biologists in recent years. Especially, consequent H 2 S detection mechanisms and biological applications based on fluorescence probe emerged in endlessly, competing ideas, each had its advantage. In facts, the reaction mechanism and luminescence properties play a decisive role in the biology application of H 2 S fluorescence probe. In this despite booming season, in the process of research we still skillfully conceived, in view of H 2 S with small structure being able to do successive nucleophilic substitution in the same molecules, high selective H 2 S subcellular detection was realized. Specifically, we take the cyanine (Cy7) with positive charge as a red fluorophore, through the introduction of disulfide bond and carbonate to build the specific reaction sites of H 2 S, thus avoiding the interference of other sulfur-containing substances in biological systems. After reaction with H 2 S, the Probe released red fluorophore, realizing mitochondria target H 2 S detection. Because the advantages of red fluorescence emission probe, the Probe successfully was applied imaging in mice.
研究领域:
生物化学
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医学影像
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分子生物学
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yinhong Xie,Mengchen Chi,Ruichen Dong,Sui Wu,Jinming Yang,Qin Wang,Junying Chen,Yajun Weng
Atherosclerosis, a chronic inflammatory disease characterized by the formation of atherosclerotic plaques in the arterial walls. The pathological process of atherosclerosis mainly contains lipid metabolism disorder, endothelial dysfunction, and progressive inflammation. Given the complexity of pathological process, treatments based on a single target might have very limited therapeutic efficacy. Thus, developing a nanoplatform to obtain an enhanced multi-target therapy is promising. Hydrogen sulfide (H 2 S) has various functions including anti-inflammation, anti-oxidation and endothelial protection. In this study, a responsive multi-target nanoplatform (MM/ZnS/ATV) combining the functions of H 2 S and atorvastatin was developed. The acidic microenvironment of the plaque can accelerate ZnS hydrolysis to trigger H 2 S and atorvastatin release. The responsive H 2 S release from ZnS can overcome the shortcomings of rapid H 2 S release from H 2 S donors in vivo. Furthermore, the ZnS hydrolysis-mediated H + consumption in the microenvironment can reduce acidity to some extent. Results showed macrophage membranes (MM) coating reduced the phagocytosis of nanoparticles and increased the bioavailability. In vitro studies demonstrated that H 2 S release from MM/ZnS/ATV inhibited ROS-induced endothelial cell apoptosis and repaired the damaged endothelium. Moreover, atorvastatin released from MM/ZnS/ATV regulated lipid metabolism and reduced the blood lipid content. Both in vitro and in vivo studies confirmed MM/ZnS/ATV exhibited excellent therapeutic efficacy. Specifically, in vivo results showed that H 2 S combined with atorvastatin effectively reduced inflammatory infiltration, and promoted plaque regression and stabilization. Our study provides a promising strategy for atherosclerosis therapy.
研究领域:
纳米技术
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药学
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心血管疾病
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Advanced Healthcare Materials
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2023
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IF 10
Abdullkhaleg Ali Albashari,Yan He,Yu Luo,Xingxiang Duan,Jihea Ali,Mingchang Li,Dehao Fu,Yangfan Xiang,Youjian Peng,Song Li,Lihua Luo,Xingjie Zan,Tushar Kumeria,Qingsong Ye
Spinal cord injury (SCI) commonly induces nerve damage and nerve cell degeneration. In this work, a novel dental pulp stem cells (DPSCs) encapsulated thermoresponsive injectable hydrogel with sustained hydrogen sulfide (H 2 S) delivery is demonstrated for SCI repair. For controlled and sustained H 2 S gas therapy, a clinically tested H 2 S donor (JK) loaded octysilane functionalized mesoporous silica nanoparticles (OMSNs) are incorporated into the thermosensitive hydrogel made from Pluronic F127 (PF-127). The JK-loaded functionalized MSNs (OMSF@JK) promote preferential M2-like polarization of macrophages and neuronal differentiation of DPSCs in vitro. OMSF@JK incorporated PF-127 injectable hydrogel (PF-OMSF@JK) has a soft consistency similar to that of the human spinal cord and thus, shows a high cytocompatibility with DPSCs. The cross-sectional micromorphology of the hydrogel shows a continuous porous structure. Last, the PF-OMSF@JK composite hydrogel considerably improves the in vivo SCI regeneration in Sprague–Dawley rats through a reduction in inflammation and neuronal differentiation of the incorporated stem cells as confirmed using western blotting and immunohistochemistry. The highly encouraging in vivo results prove that this novel design on hydrogel is a promising therapy for SCI regeneration with the potential for clinical translation.
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FUEL PROCESSING TECHNOLOGY
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2023
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IF 7.5
Yi Yuan,Lijia Huang,Tian C. Zhang,Yuan Wang,Shaojun Yuan
Metal oxide loaded carbon-based materials have attracted extensive attention as promising desulfurizers to solve the problem of H 2 S emission at room temperature . However, low desulfurization capacity, difficult regeneration and high economic cost are the main problems of metal oxide loaded carbon-based desulfurizers, which limit their industrial application. Herein, a novel and low-cost CaCO 3 -ZnO loaded biochar (RCZ) was synthesized by one-step pyrolysis of scrap rice and metal salts for highly efficient H 2 S removal at room-temperature. The optimized RCZ-1-1-1-800 sample showed an excellent H 2 S removal ability of 834.48 mg/g at the reaction temperature of 25 °C, oxygen content of 10%, and relative humidity of 70% as compared to 29.31 mg/g achieved by the inactivated biochar (prepared without activator). Such an RCZ-1-1-1-800 desulfurizer also delivered a high H 2 S removal ability under different desulfurization conditions. The associated desulfurization mechanism of RCZ was the coupling of reactive adsorption and catalytic oxidation with sulfur being the main desulfurization product. Moreover, the as-fabricated RCZ also exhibited a high reusability , retaining about 95% of the initial H 2 S removal capacity after five adsorption/regeneration cycles. This work provides a promising idea for the preparation of low-cost and high-capacity metal oxide- and carbonate-loaded carbon-based desulfurizers.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2023
·Vol. 30
·期 27
·70884-70896
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IF 5.8
Li Ke,Zhu Yuqiu,Wang Zixuan,Chen Dingkai,Wu Wenwei,Luo Yongming,He Dedong
High concentration of H 2 S in acidic natural gas will lead to poisoning of catalysts for hydrogen production by methane steam reforming, thus limiting the further use of natural gas. Reforming CH 4 by H 2 S can be considered as an alternative route to hydrogen production from methane. This process not only achieves the removal of H 2 S but also obtains chemical raw material CS 2 and clean energy H 2 . By impregnating the Mo source on SiO 2 treated with hydrogen peroxide and then using the catalyst in the CH 4 /H 2 S reforming reaction, we surprisingly found that the conversion rate of CH 4 and H 2 S increased from 28 and 32% to 34% and 43%, respectively, after hydrogen peroxide treatment. The H 2 production rate and the yield of CS 2 increased from 20 mmolH 2 /(g Mo *min) and 52% to 30 mmolH 2 /(g Mo *min) and 65%, respectively. Combining with characterization methods such as X-ray diffraction (XRD), hydrogen temperature programmed reduction (H 2 -TPR), 1 H-based solid-state nuclear magnetic resonance ( 1 H MAS NMR), X-ray photoelectron spectroscopy (XPS), Raman spectra (RS), and transmission electron microscopy (TEM), we found that the hydroxyl concentration of the support increased after hydrogen peroxide treatment, which led to the strengthening of the force between the metal and the support, which was easy to form low-level and small-size MoS 2 , exposing more active sites, and further improving the catalytic activity. This method provides a new idea for hydrogen production by CH 4 /H 2 S reforming and the development of high-performance MoS 2 -based catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Anqiang Jiang,Heng Guo,Shan Yu,Fengying Zhang,Tingyu Shuai,Yubin Ke,Peng Yang,Ying Zhou
Low charge carrier separation and transfer efficiency continues to be the major obstacle to harvest solar energy to split hydrogen sulfide (H 2 S) as hydrogen source for H 2 production with value-added utilization for waste by-products. Herein, we designed a Type-II core/shell AgIn 5 S 8 /CdS (AIS/CdS) quantum dots (QDs) photocatalyst capped with short-chain inorganic sulfide ion (S 2− ) ligand with dual charge-accepting engineering to promote charge carrier extraction and faster photogenerated electron transfer. Transient absorption spectroscopy analysis demonstrates that the excited electrons are fast injected into CdS shell from AIS core within 1.7 ps, instead of transferring to sub-bandgap states. Consequently, the highest photocatalytic hydrogen evolution rate of AIS/CdS QDs with S 2- ligand is 12.74 mmol g −1 h −1 that is more than four times of pristine AIS core. This work offers insightful guidance on the rational design of charge-accepting engineering QDs-based photocatalysts, thereby stimulating solar to hydrogen generation and resource utilization of pollutants.
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FUEL
·
2023
·
IF 7.4
Yi Yuan,Lijia Huang,Murat Yılmaz,Tian C. Zhang,Yuan Wang,Shaojun Yuan
To improve their low-temperature desulfurization performance, the activated carbon-based materials have typically been modified by either metal oxide loading or nitrogen doping. However, most of the aforementioned materials are limited to only one of the above modification methods, resulting in relatively poor desulfurization performance. Herein, a novel MgFe 2 O 4 -loaded N -doped biochar (MgFe 2 O 4 @NBC) was fabricated by one-pot pyrolysis of a nitrogen containing precursor of g-C 3 N 4 , cooked rice waste, and metal salts for efficient low-temperature desulfurization of H 2 S. Different fabrication conditions such as pyrolysis temperature and the nitrogen mixing ratio (i.e., the mass ratio of cooked rice waste to g-C 3 N 4 ) have been extensively studied. The optimized MgFe 2 O 4 @NBC-500–2 sample delivered a superior breakthrough capacity of 1052.83 mg/g in an atmosphere of O 2 content of 20% and relative humidity of 80% at 25 °C, and demonstrated high tolerance and stability of desulfurization performance to harsh environmental conditions with 80% relative humidity and no oxygen. The desulfurization mechanism of H 2 S on the surfaces of the MgFe 2 O 4 @NBC composites was attributed to the synergistic effects of reactive adsorption and catalytic oxidation process. The composite also demonstrated excellent reusability, retaining 85% of the initial breakthrough capacity after 5 recycled uses. Therefore, the as-prepared MgFe 2 O 4 @NBC composite offers a potentially promising carbon-based desulfurizers for practical applications in the low-temperature desulfurization field.
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ENERGY & FUELS
·
2018
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IF 3.024
XiangFeng Tian,LeMeng Wang,Dong Fu,Chao Li
The absorption performance of low-partial-pressure H2S in a monoethanolamine (MEA)-activated N-methyldiethanolamine (MDEA) aqueous solution was investigated. The absorption amount (in mass, g H2S/g solutions) and H2S loadings (mol H2S/(mol MEA + mol MDEA)) were measured, and the apparent absorption rate was determined from the time-dependent absorption capacity. Experimentally, the temperature and partial pressure of H2S (PH2S) ranged from 303.2 to 323.2 K and from 300 to 500 Pa, respectively. The mass fractions of MDEA (wMDEA) and MEA (wMEA) ranged from 0.30 to 0.50 and from 0 to 0.075, respectively. The temperature, wMDEA, wMEA, and PH2S dependencies of the absorption performance were analyzed. It is impressive that the addition of MEA significantly enhanced the absorption amount of H2S yet slightly influenced the apparent absorption rate. In addition, a tray column consisting of six plates was used to verify the removal efficiency of low-partial-pressure H2S (PH2S = 500 Pa) and the results showed that in the case of wMDEA = 0.5, wMEA = 0.075, and T = 313.2 K, the removal efficiency achieved 95% when the ratio of gas to liquid was 40, indicating that MEA-activated MDEA aqueous solutions are promising in the removal process of low-partial-pressure H2S.
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INORGANICA CHIMICA ACTA
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2019
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IF 2.433
Lixia Liu,Xuefang Shang,Ruiqi He,Jie Li,Yanmei Chen,Hongli Chen,Tianyun Wang
A zinc(II) complex–based selective colorimetric chemosensor for H 2 S was synthesized. The ligand and complex crystals were obtained, and the molecular structures were confirmed by single-crystal X-ray diffraction analysis in addition to electrospray ionization high resolution mass spectrometer, as well as elemental analysis . The photo-physical and recognition properties toward HS – were examined. The complex indicated the presence of HS – with an obvious color change from yellow to red, based on zinc ion displacement mechanism. However no obvious changes were observed in the presence of other anions (AcO − , H 2 PO 4 − , F − , Cl − , Br − , I − and SO 3 2− ). In addition, the chemosensor was applied to assess HeLa cell cytotoxicity. Our inorganic-reaction based sensor for HS – is simple, easily prepared and efficient. The complex has many potential chemical and analytical applications for the sensing of H 2 S.
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