SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yiling Ran,Man Yang,Jian Li,Jinlei Song,Yi Wang,Zhanguo Li,Liyong Yuan
Developing versatile sorption materials for radionuclide capture (e.g. iodine) is critical for nuclear energy and environmental science. Covalent organic frameworks (COFs) have recently become a new platform for developing sorption materials because of their high surface area and functionalised skeleton structure. Herein, two types of COF materials containing thiophene were designed as iodine sorbents and synthesised via a Schiff base reaction of benzo[1,2-b:3,4-b’:5,6-b’’]trithiophene-2,5,8-tricarbaldehyde, benzidine (DADP) and p-phenylenediamine (DAB): DADP-COF and DAB-COF. DAB-COF exhibits a unique granular-rod-like morphology and has a higher surface area (1775 m 2 /g) than DADP-COF (1140 m 2 /g), which is clearly beneficial for the physical adsorption of iodine. Meanwhile, the COF backbone is rich in N and S sites, which are advantageous for the chemical adsorption of iodine. These two features make the two prepared COFs ideal iodine sorption materials. DAB-COF demonstrates an excellent gaseous iodine adsorption capacity of 4.2 g/g, ranking it as one of the most effective iodine sorption materials, while DADP-COF exhibits a good adsorption capacity of over 235 mg/g for iodine in cyclohexane solutions. Density functional theory calculations prove that imine N and thiophene S serve as active sites during the iodine adsorption. DAB-COF exposes more active sites because of its higher surface area, leading to a higher iodine adsorption capacity than DADP-COF. The results of this study indicate that introducing thiophene to COFs improves sorption efficacy for sorption applications in general and particularly paves the way for developing stable and effective COF sorbents for iodine capture from various environments.
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JOURNAL OF MATERIALS SCIENCE
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2017
·Vol. 53
·期 2
·1286-1296
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IF 2.599
Cao Sheng,Zheng Jinju,Dai Chencheng,Wang Lin,Li Chengming,Yang Weiyou,Shang Minghui
In this report, doping concentration-dependent photoluminescence (PL) properties of Mn-doped ternary Zn–In–S quantum dots (QDs) were studied by using steady-state and time-resolved PL spectroscopy. The QDs PL was firstly significantly intensified with the increasing Mn doping concentration and then decreased after the doping concentration increased up to 7.5 at.%. However, their decay lifetimes exhibit a monotone decrease with Mn doping concentration ranged from 0 to 10 at.%. It can be concluded that the PL intensity was mainly determined by two factors: one was the increased efficiency of energy transfer from host excitons to Mn 2+ ion accepter, and the other was the decreased efficiency of the emission from a Mn 2+ ion, which was caused by the increased component of exposed Mn 2+ ions on QDs surface and the accelerated interaction between adjacent dopants. The competition of above two exciton relaxation dynamics processes determined the trend of the PL intensity, while the latter was responsible for the monotonously decreased lifetime of the Mn 2+ ion emission with the increasing Mn doping concentration.
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CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Baolong Zhang,Fangxuan Liu,Bin Sun,Tingting Gao,Guowei Zhou
ABSTRACT Photocatalytic water splitting to produce H 2 using semiconductor photocatalysts is a reliable approach to alleviating energy shortages and environmental pollution. However, the inadequate light-harvesting ability, rapid photogenerated carrier recombination, and inferior redox capacity of the individual photocatalysts restrict their photocatalytic activity . To address these limitations, a hierarchical S-scheme heterojunction of ZnIn 2 S 4 -nanosheet-decorated flower-like TiO 2 microspheres for enhancing photocatalytic H 2 evolution, purposely constructed through in situ chemical bath deposition, has been reported. The as-synthesized TiO 2 /ZnIn 2 S 4 heterojunctions exhibited ZnIn 2 S 4 -content-dependent photocatalytic activity for solar-driven H 2 evolution. As a result, the optimized TiO 2 /ZnIn 2 S 4 heterojunction exhibited a superior photocatalytic H 2 evolution rate of 6.85 mmol g –1 h –1 , approximately 171.2- and 3.9-fold with respect to that obtained on pure TiO 2 and ZnIn 2 S 4 , respectively, mainly attributed to the unique hierarchical structure, extended light-harvesting ability, enhanced redox capacity, and improved separation and transfer efficiencies of the photogenerated carriers induced by the S-scheme heterojunctions. Simultaneously, a detailed analysis of the S-scheme electron transfer pathway in the TiO 2 /ZnIn 2 S 4 heterojunction was performed using in situ irradiated X-ray photoelectron spectroscopy and electron paramagnetic resonance spectroscopy . This study provides insights into the design of highly active heterojunction photocatalysts for sustainable solar-to-fuel energy conversion.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Xiu Huang,Yong Li,Zhao Shu,Li Huang,Qian Liu,Guibin Jiang
Plastic pollution is a significant environmental concern globally. Plastics are normally considered chemically inert and resistant to biodegradation. Although many papers have reported enzyme-induced biodegradation of plastics, these studies are primarily limited to enzymes of microbial origin or engineered enzymes. This study reveals that poly(ethylene terephthalate) (PET, ∼6000 Da and 100 kDa) particles and plastic bottle debris (PBD, 24.9 kDa) can be efficiently degraded by a mammal-origin natural phase II metabolic isozyme, glutathione S-transferase (GST), under mild conditions. The degradation efficiency of PET plastics reached 98.9%, with a degradation rate of 2.6 g·L–1·h–1 under ambient or physiological conditions at 1 atm. PET plastics can be degraded by GST with varying environmental or biological factors (i.e., temperature, light irradiation, pH, and presence of humic acid or protein). We suggest a novel mechanism for PET degradation other than hydrolysis, i.e., the mechanism of cleavage and release of PET plastic monomers via nitridation and oxidation. This finding also reveals a novel function of GST, previously thought to only degrade small molecules (<1000 Da). This method has been successfully applied in real human serum samples. Additionally, we have tested and confirmed the ability to degrade PET of a mammal-origin natural digestive enzyme (trypsin) and a human-derived natural metabolic enzyme (CYP450). Overall, our findings provide a potential new route to plastic pollution control and contribute to our understanding of the metabolism and fate of plastics in organisms.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
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IF 8.3
Yanze Wang,Zhenyu Liu,Wenxuan Wang,Junxiao Tang,Rongjie Wang,Jingjing Xie,Zhengyi Fu
Accelerating charge transport and avoiding recombination are promising strategies for establishing highly efficient artificial photosystems. Herein, an S-scheme heterostructure consisting of Zn x Cd 1− x S and TiO 2 is fabricated via the in situ crystal growth method. The refined structure significantly enhances the transport of photogenerated charges, thereby improving photocatalytic hydrogen production efficiency. The optimized TiO 2 −Zn x Cd 1− x S composite, incorporating 60% TiO 2 with Zn 0.4 Cd 0.6 S, exhibits a robust H 2 evolution rate of 50.96 mmol g −1 h −1 with continuous release of H 2 bubbles. It is worth noting that the hydrogen production rate in seawater is as high as 26.22 mmol g −1 h −1 . The strong interfacial interaction and staggered band alignment between TiO 2 and Zn x Cd 1− x S result in the formation of a built-in electric field and high-content oxygen vacancies, which can drive the directional migration of photoelectrons with high redox ability and high speed. The designed photocatalyst with S-scheme and rich Oxygen vacancies at the interface provides a new approach for fabricating high-efficiency photocatalysts.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Hongxu Zhou,Weichen Han,Hongquan Chai,Hao Huang,Jingang Zheng,Han Zhang,Lixiang Li,Weimin Zhou,Baigang An,Chengguo Sun
Sluggish reaction kinetics in lithium–sulfur (Li–S) batteries has seriously hindered their practical application. Herein, a three-dimensional (3D) granular carbon skeleton decorated with nickel-rich NCM materials (NCM@3D-SP) is prepared as a cathode host for Li–S batteries, where the carbon matrix is rich in pore channels, can provide good conductivity and electrolyte diffusion, and NCM811 particles contribute abundant metal sulfides active sites through metal-ion exsolution. The different metal sulfides (NiS, Ni3S2, Ni7S6, and CoS) in heterogeneous structures exhibit outstanding catalytic and adsorption effects on polysulfides during cycling, where the ion diffusion coefficient is increased by approximately 2.5 times compared to the cathode without catalytic active sites (3D-SP). A Li metal battery using NCM@3D-SP/S as the cathode exhibits a capacity decay of only 0.051% per cycle at 2C after 500 cycles. Even at an ultra-high current density of 10C and a sulfur-loading of 6 mg cm−2, the cells maintain a stable reversible discharge capacity of 453.1 mA h g−1 after 500 cycles and 4 mA h cm−2. The incorporation of nickel-rich cathode materials and 3D sulfur host structure presents a novel strategy for high-catalytic activity cathodes of Li–S batteries.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Alamgir,Raza Ullah,Khalid Talha,Hongye Yang,Nouraiz Mushtaq,Abrar Ahmad,Linkun Fan,Lan Li,Guixia Zhao,Xusheng Wang,Junkuo Gao
It is challenging to engineer a photocatalyst that can degrade antibiotics efficiently. We have successfully developed a series of photocatalysts by annealing In-MOF (BUT-205) with TiO 2 , namely (a) In 2 O 3 /TiO 2 -I, (b) In 2 O 3 /TiO 2 -II, and (c) In 2 O 3 /TiO 2 -III. These catalysts, particularly In 2 O 3 /TiO 2 -III, exhibited superior efficiency in degrading tetracycline (TC) under visible light. The enhanced photocatalytic performance of In 2 O 3 /TiO 2 -III can be attributed to the formed S-scheme heterojunction, which promoting the separation of electron-hole pairs. The S-scheme heterojunction was confirmed by XPS , in-situ XPS, UV–vis diffuse reflectance spectroscopy, and Mott-Schottky plot, etc. Compared to pure TiO 2 and In 2 O 3 , the In 2 O 3 /TiO 2 -III demonstrated an 18-fold and 3-fold higher degradation rate constant (k). Various factors affecting the degradation of TC were investigated, including pollutant concentration, catalyst type, solution pH, catalyst dosage, inorganic anions , inorganic cations , and radical species. Photoluminescence (PL) and transient photocurrent density evaluate the separation rate of electron-hole pairs, and EPR experiments (active species trapping) studies confirmed •O 2 − and h + as the primary entities in TC photodegradation by In 2 O 3 /TiO 2 -III. HPLC/MS analysis revealed the photocatalytic degradation pathway. The MOF-derived photocatalysts efficiency in TC photoreduction results from the formed S-scheme heterojunction, making it a promising candidate for environmental remediation.
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JOURNAL OF POWER SOURCES
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2017
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IF 6.395
Xiao Huang,Cai Liu,Yang Lu,Tongping Xiu,Jun Jin,Michael E. Badding,Zhaoyin Wen
A high strength Li-Garnet solid electrolyte composite ceramic is successfully prepared via conventional solid state method with Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 and nano MgO powders. Well sintered ceramic pellets and bars are obtained with 0–9 wt.% MgO. Fracture strength is approximately 135 MPa for composite ceramics with 5–9 wt.% MgO, which is ∼50% higher than that of pure Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (90 MPa). Lithium-ion conductivity of the composite is above 5 × 10 −4 S cm −1 at room temperature ; comparable to the pure Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 material. SEM cross-sections of the composite ceramic shows a much more uniform microstructure comparing with pure ones, owing to the grain growth inhibition effect of the MgO second phase. A battery cell consisting of Li/composite ceramics/Sulfur-Carbon at 25 °C exhibits a capacity of 685 mAh g −1 at 0.2 C at the 200 th cycle, while maintaining a coulombic efficiency of 100%. These results indicate that the composite ceramic Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 -MgO is promising for the production of electrolyte membrane and fabrication of Li-Sulfur batteries.
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CHEMICAL ENGINEERING JOURNAL
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2018
·
IF 6.735
Qian Zhang,Wan Huang,Jun-ming Hong,Bor-Yann Chen
As the efficiency of electrocatalysis is depended on the characteristics of anode materials, heteroatom doping was applied to improve the physicochemical, electromagnetic, and structure properties of grapheme considering that the efficiency of electrocatalysis depends on the characteristics of anode materials. However, the mechanism underlying efficiency promotion remains unclear due to the complicated doping species of heteroatom. Single-form S loaded S/graphene/Pt/TiO 2 (S-GN/Pt/TiO 2 ) was prepared for the first time by using radical as precursor to clarify the function of S doping. The catalytic center for direct (pollution oxide on anode) and indirect electro-oxidation (pollution oxide by radicals) was then confirmed by density functional theory (DFT) calculation. Results indicated that C atom besides SOx is the active site for direct oxidation of acetaminophen (APAP), and SOx is the active site for indirect oxidation for the generation of HO . Furthermore, the effect of some parameters (such as S content, pH, applied current, temperature) and oxidants generated through different electrolytes were also completely deciphered in this study. GC–MS analysis was implemented to identify intermediates of APAP after electro-oxidation (i.e., eight types of intermediates identified) and the possible pathway of degradation was proposed. The single form S doping approach and S function discussion could provide the in-depth understanding to the mechanism of electrocatalysis and suggesting performance of related materials with practical values for applications.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2017
·Vol. 135
·期 16
·46187
·
IF 1.86
Xinqi Lin,Xuesong Li,Jinmeng Hao,Xuan Zhao,Yanfeng Wei,Jianxin Mu
A series of novel poly(arylene ether)s were synthesized with diphenol liner polydimethysiloxanes with different silicon numbers (2OH-PDMS- P ; P = 2, 6, 10, 12, 16) and decafluorobiphenyl via a two-step nucleophilic substitution polymerization. The chemical structures of the polymers were confirmed by Fourier transform infrared spectrometer, 19 F-NMR and 1 H-NMR spectra. All the polymers provided outstanding hydrophobic properties, high thermal stability and good solubility. The water contact angle (WCA) first increased and then suddenly decreased with the increasing of silicon numbers in PDMS. The highest WCA about 112° was obtained when silicon numbers was ten. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135 , 46187.
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FUEL
·
2025
·
IF 7.5
Honglin Li,Xin Zhang,Yuanyuan Wen,Jingyuan Li,Yu Liu,Hongjun Mao,Hongman Sun,Jingbin Zeng,Zifeng Yan
Sulfur-doped copper (S-doped Cu) was regarded as an efficient catalyst for formate in CO 2 electrochemical reduction reaction (CO 2 RR), but the selectivity and current density are still unsatisfied due to the hydrogen evolution reaction (HER) and CO generation pathway. Herein, S-doped Cu nanoparticles were synthesized by in-situ reduction of the constructed Cu-thioamide coordination polymers, exhibiting impressive performance for formate production in the CO 2 RR process. Particularly, the CuBr-thiobenzamide (TBA) coordination polymers derived S-doped Cu nanoparticles (CuBr-TBA-R) achieve a formate Faradaic efficiency of 84.4 % with current density of formate to 6.7 mA cm −2 . The characterization results indicate these generated S-doped Cu nanoparticles are uniform with the particle size of 20–30 nm exposed a large amount of Cu (100) facets due to the coordination of thioamide molecules and presence of Br - and I - in electrolyte. The morphological characteristics and strong affinity for oxygen is the reason of higher formate selectivity and current density. This finding reveals the characterizations of efficient S-doped Cu catalysts for formate and provide a controllable approach to prepare these catalysts.
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INTERNATIONAL IMMUNOPHARMACOLOGY
·
2024
·
IF 4.8
Yuxin Zhang,Lixuan Yang,Yonghui Gan,Chenchen Zhao,Chao Zhou,Jian Chen,Yanping Yin,Shengnan Xia,Haiyan Yang,Xinyu Bao,Meijuan Zhang,Yun Xu,Jingwei Li
Microglia, the primary immune cells of the central nervous system, play a crucial role in the neuroinflammatory processes following ischemic stroke. Targeting neuroinflammation is a promising strategy to enhance the outcomes of ischemic stroke. Benzydamine (BA), a well-known non-steroidal anti-inflammatory drug, has demonstrated potential in inhibiting pro-inflammatory cytokines across various disease models. However, the potential role of BA in microglial activation and post-stroke neuroinflammation remains unclear. Our study reveals that BA effectively suppresses the lipopolysaccharide (LPS)-stimulated pro-inflammatory responses of primary microglia, with high-dose BA (10 μM) suppressing LPS-induced inflammatory markers by up to 59.1 % in the mRNA levels of IL-1β. Furthermore, BA mitigated ischemic brain injury in experimental stroke mice. BA treatment also significantly attenuated neuroinflammatory responses and attenuates ischemic brain injury in experimental stroke mice. Further investigation revealed that BA reduces the release of the LPS-stimulated pro-inflammatory factors and activation of primary microglia by directly binding to and inhibiting the activity of cathepsin S (CTSS). In conclusion, our study identifies BA as a promising CTSS inhibitor with potential to suppress neuroinflammation following ischemic stroke. Our findings provide a theoretical basis for developing new neuroprotective strategies.
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