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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY · 2024 · IF 4.1

Efficient hydrogen peroxide photogeneration over GaOOH/In(OH)3 composites via the half-reaction of tetracycline oxidation

Ting Yu,Ying Liang,Zejun Zhou,Fengjie Chen,Yingjun Wang,Yunjun Mei,Mengxi Cao,Bolei Chen,Pu Wang,Yawei Wang

The photocatalytic generation of hydrogen peroxide (H 2 O 2 ) using artificial synthetic methods is promising. However, the sluggish hole-induced water oxidation half-reaction that hinders charge separation severely limits H 2 O 2 generation efficiency. This study used the oxidation half-reaction of tetracycline (C 22 H 24 N 2 O 8 , TC) to accelerate charge separation over GaOOH/In(OH) 3 composites with Type II heterojunctions under sunlight irradiation to increase the H 2 O 2 generation efficiency. The results demonstrated that the H 2 O 2 generation efficiency significantly increased from 74.7 to 389.8 µmol L −1 h −1 as the TC degradation efficiency increased from 0.02 to 0.37 mg L −1 h −1 . Radical quenching experiments further indicated that TC degradation consumed holes, increasing the electron formation rate and enhancing H 2 O 2 generation. A comparison with density functional theory calculations revealed that H 2 O 2 generation was a one-step 2-electron route (O 2  + 2e − + 2H + → H 2 O 2 ). These findings are expected to provide new strategies for promoting photocatalytic synthesis of H 2 O 2 .

研究领域: 环境科学 · 化学 · 材料科学 · 光催化
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RSC Advances · 2018 ·Vol. 8 ·期 56 ·32358-32367 · IF 2.936

Facile preparation of UiO-66 /PAM monoliths via CO2-in-water HIPEs and their applications

Yong Dong,Liqin Cao,Jing Li,Yongxia Yang,Jide Wang

A novel clean method to synthesis a composite monolith was developed. Given its amphiphilic property, UiO-66 can emulsify water and CO2 to format a high internal phase emulsion (HIPE) under certain conditions. These UiO-66-emulsified Pickering HIPEs can be used as templates to prepare interconnected macroporous MOF/polymer composite monoliths. The effects of UiO-66 amount, cross-linking agent concentration, and CO2–water ratio on UiO-66/PAM structures were investigated. Then, the as-synthesized MOF/PAM composites were characterized by TGA, XRD, SEM, and FT-IR analyses, as well as rheological and DMA measurements. The results indicated that the composites are interconnected with hierarchical pores, and the diameter of the voids is 10–50 μm. The directly prepared monoliths exhibited relatively high stresses at 82% strain and recovered their shape quickly. The adsorption capacity of the composites for methylene blue (MB) is 50 mg g−1 at a faster adsorption rate. The monoliths also exhibit underlying applications in edible oil–water separation.

研究领域: 材料科学 · 化学工程 · 环境科学
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JOURNAL OF BIOLOGICAL CHEMISTRY · 2020 ·Vol. 295 ·期 20 ·6958-6971 · IF 4.238

Activation of JNK signaling promotes all-trans-retinal–induced photoreceptor apoptosis in mice

Chunyan Liao,Binxiang Cai,Yufeng Feng,Jingmeng Chen,Yiping Wu,Jingbin Zhuang,Zuguo Liu,Yalin Wu

Disrupted clearance of all-trans-retinal (atRAL), a component of the visual (retinoid) cycle in the retina, may cause photoreceptor atrophy in autosomal recessive Stargardt disease (STGD1) and dry age-related macular degeneration (AMD). However, the mechanisms underlying atRAL-induced photoreceptor loss remain elusive. Here, we report that atRAL activates c-Jun N-terminal kinase (JNK) signaling at least partially through reactive oxygen species production, which promoted mitochondria-mediated caspase- and DNA damage-dependent apoptosis in photoreceptor cells. Damage to mitochondria in atRAL-exposed photoreceptor cells resulted from JNK activation, leading to decreased expression of Bcl2 apoptosis regulator (Bcl2), increased Bcl2 antagonist/killer (Bak) levels, and cytochrome c (Cyt c) release into the cytosol. Cytosolic Cyt c specifically provoked caspase-9 and caspase-3 activation and thereby initiated apoptosis. Phosphorylation of JNK in atRAL-loaded photoreceptor cells induced the appearance of γH2AX, a sensitive marker for DNA damage, and was also associated with apoptosis onset. Suppression of JNK signaling protected photoreceptor cells against atRAL-induced apoptosis. Moreover, photoreceptor cells lacking Jnk1 and Jnk2 genes were more resistant to atRAL-associated cytotoxicity. The Abca4−/− Rdh8−/− mouse model displays defects in atRAL clearance that are characteristic of STGD1 and dry AMD. We found that JNK signaling was activated in the neural retina of light-exposed Abca4−/−Rdh8−/− mice. Of note, intraperitoneal administration of JNK–IN-8, which inhibits JNK signaling, effectively ameliorated photoreceptor degeneration and apoptosis in light-exposed Abca4−/−Rdh8−/− mice. We propose that pharmacological inhibition of JNK signaling may represent a therapeutic strategy for preventing photoreceptor loss in retinopathies arising from atRAL overload.

CAS / MDL: 127-09-3
研究领域: 眼科学 · 细胞生物学 · 分子生物学 · 神经科学
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Environmental Science-Nano · 2024 · IF 5.8

High-performance TiO2 catalyst composited with In–1,1,2,2-tetra(4-carboxylbiphenyl)ethylene for the efficient degradation of organic pollutants

Xinyu Liu,Chenchen Li,Jian Nan,Ruike Liang,Huabin Wang,Rui Xu,Yong Zhang

A combination of metal–organic frameworks (MOFs) with TiO2 can improve the performance of TiO2 in the photocatalytic degradation of organic pollutants. The selection of organic ligands for MOF preparation is a key factor for designing MOF–TiO2 composites with excellent photocatalytic properties. However, the photocatalytic performance of such composites has rarely been examined. In this study, a series of TiO2 nanoflowers (NFs) modified with In-based MOFs were prepared via a hydrothermal method using 1,1,2,2-tetra(4-carboxylbiphenyl)ethylene (TCBPE) as the organic ligand. The fabricated TiO2@In–TCBPE (TIT) heterojunctions exhibited enhanced light absorption, charge separation, and electron transfer characteristics owing to the transport of ·O2− free radicals through the charge transfer pathway between heterostructures. Rhodamine B (RhB) was chosen as a typical representative of organic pollutants under simulated sunlight and is used to evaluate the photocatalytic performance of TIT composites. The optimized TIT composite exhibited a strong photocatalytic effect, and the complete degradation of RhB was achieved in 13 min. In addition, the prepared TIT composite demonstrated excellent photocatalytic activity during the degradation of organic pollutants in different aqueous environments (tap water, lake water, and river water). This study provides a reference for the selection of ligands for the subsequent construction of high-performance MOF photocatalysts.

CAS / MDL: 68-12-2 81-88-9
研究领域: 材料科学 · 环境科学 · 化学
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POLYMERS FOR ADVANCED TECHNOLOGIES · 2020 ·Vol. 31 ·期 7 ·1591-1601 · IF 2.578

Preparation of porous monoliths via CO2-in-water HIPEs template and the in situ growth of metal organic frameworks on it for multiple applications

Yongxia Yang,Jing Li,Yong Dong,Jide Wang,Liqin Cao

Monolithic porous copolymers with 3D structure were prepared via CO 2 -in-water high internal phase emulsions template by graft copolymerization of sodium methacrylate (MAANa) on to methyl cellulose (MC) backbone. The yielded copolymer monoliths are characterized by Fourier transform infrared spectra, scanning electron microscopy (SEM), and mechanical instrument, the swelling degree of MC- g -PMAANa monoliths with different crosslinker in diverse pH were investigated. The adsorption performance of monolith to Cu(II) were conducted to explore its adsorption capacity to heavy metal ions from the wastewater. Then, a strategy of in situ growth of metal-organic frameworks (MOFs) on MC- g -PMAANa that adsorbed with metal ions was proposed first. The X-ray powder diffraction, SEM, and Brunauer-Emmett-Teller (BET) surface area result of MC- g -PMAANa/MOFs composites indicated that the MOFs nanoparticles were grown uniformly on the monolith wall without destroying its original 3D porous structure. Compared with MOFs nanoparticle, MC- g -PMAANa/MOFs composites have advantages of easy operation and handle, which more conform to practical application. Furthermore, the antibacterial activity of MC- g -PMAANa/MOFs was evaluated by disk agar diffusion and optical density methods. In addition, MC- g -PMAANa/Cu-BTC composite was applied to dye adsorption, which has proved the underlying application of such composites in dye removal.

研究领域: 材料科学 · 化学工程 · 环境科学 · 纳米技术
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2022 · IF 4.326

Origin of the High Conductivity of the LiI-Doped Li3PS4 Electrolytes for All-Solid-State Lithium–Sulfur Batteries Working in Wide Temperature Ranges

Zhongkai Wu,Ru Wang,Chuang Yu,Chaochao Wei,Shuai Chen,Cong Liao,Shijie Cheng,Jia Xie

Sulfide electrolytes show great potential as solid electrolytes for all-solid-state batteries due to their high ionic conductivity and low interfacial resistance toward electrode materials. The structure of the P–S framework in the composition of sulfides plays a crucial role in the conductivity. Introducing LiI in the Li3PS4 structure can tailor the P–S frameworks and thus achieve high ionic conductivities. Herein, the dopant of LiI is optimized by high-rotation milling, followed by a sintering route to achieve the highest Li-ion conductivity of 2.3 mS cm–1 for the Li3PS4-50% LiI electrolyte (also denoted as Li7P2S8I) among different compositions. The phase variations and structure evolution of the P–S frameworks in the LiI-doped Li3PS4 electrolytes are carefully investigated in a combination of X-ray diffraction and Raman spectra. All-solid-state Li–S batteries using the prepared Li7P2S8I electrolyte combined with a nano Li2S cathode and a Li–In anode deliver a high initial discharge capacity of 739.7 mA h g–1 and sustain a discharge capacity of 517.7 mA h g–1 after 60 cycles with a capacity retention of 70.0% at 0.13 mA cm–2 at room temperature. When the operating temperature rises to 60 °C, it shows a higher discharge capacity of 862.8 mA h g–1 with fast capacity decay. However, it exhibits stable capacities and superior cycling performance under 0 °C over 70 cycles. Electrochemical impedance spectroscopy and in situ stack-pressure results find that the electrochemical performance differences of the assembled battery at different operating temperatures are associated with the interfacial resistance caused by volume changes. This work provides the strategy to obtain highly conductive sulfide electrolytes for SSBs and unravels the temperature effects on the electrochemical performance of all-solid-state Li–S batteries.

研究领域: 材料科学 · 电化学 · 能源存储
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MICROCHIMICA ACTA · 2020 ·Vol. 187 ·期 4 ·1-9 · IF 6.232

“French fries”-like luminescent metal organic frameworks for the fluorescence determination of cytochrome c released by apoptotic cells and screening of anticancer drug activity

Xie Ruirui,Liu Yanyan,Yang Peipei,Huang Lan,Zou Xun,Liu Jiamin,Ren Qingfan,Tao Jia,Zhao Peng

A luminescent metal organic framework was prepared by encapsulating Zn–Ag–In–S quantum dots into “French fries”-like MIL-68(In) metal organic frameworks (ZAISQDs@MIL-68(In)). The ZAISQDs@MIL-68(In) had a maximum excitation wavelength at 370 nm and maximum emission wavelength at 620 nm. It was found that the ZAISQDs@MIL-68(In) was efficiently quenched by cytochrome c (Cyt c), which is an important biomarker of early cell apoptosis. The quenching mechanism was ascribed to be an inner filter effect and dynamic quenching of Cyt c towards the ZAISQDs@MIL-68(In), and the enrichment effect of MIL-68(In). Benefiting from the multiple advantages, ZAISQDs@MIL-68(In) was developed as an assay strategy of Cyt c with logarithmic relation between signal quenching and concentration in the range 0.02 to 3.5 μM. The linear equation was (F 0 –F)/F 0  = 0.5043 + 0.2678 × logc Cyt c with a detection limit of 8 nM. Cyt c released by drug induced apoptotic cells was determined by ZAISQDs@MIL-68(In), and this strategy has been utilized for the screening of anticancer drug activity. Schematic representation of the synthesis of ZAISQDs@MIL-68(In) and its application for Cyt c and screening anticancer drug activity

研究领域: 分析化学 · 生物化学 · 癌症研究 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

A flexible indium-based metal-organic framework with ultrahigh adsorption capacity for iodine removal from seawater

Yu-Zhen Shi,Qing-Hua Hu,Xin Gao,Li Zhang,Ru-Ping Liang,Jian-Ding Qiu

The highly efficient removal of radioactive iodine from nuclear accident-polluted seawater is of great significance for the purpose of environmental protection. Herein, we report an indium-based metal–organic framework, named In-MOF, for highly efficient removing iodine from seawater. In-MOF is constructed by In 3+ ions coordinated with tris (4-(1H-imidazol-1-yl) phenyl) amine and exhibits high chemical stability even under seawater for 30 days. Due to the flexible one-dimensional linear structure and high-density charged imidazolium groups, In-MOF possesses a high adsorption capacity (1138 mg/g) for iodine in water. Furthermore, it exhibits high selectivity in the presence of competitive ions, due to forming the unique I-π interactions between iodine and the In-MOF. Notably, these excellent adsorption features endowed In-MOF successfully remove iodine from seawater with a high removal rate of 93.86%. These results are of fundamental importance to understanding iodine uptake and designing materials with high adsorption capacity.

CAS / MDL: 22519-64-8
研究领域: 材料科学 · 环境科学 · 核工程
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Journal of Materials Chemistry A · 2022 ·Vol. 10 ·期 38 ·20545-20551 · IF 14.511

Suppressing water clusters by using “hydrotropic” ionic liquids for highly stable aqueous lithium-ion batteries

Canfu Zhang,Binbin Chen,Ziyang Cai,Fenglin Zhang,Renzhi Huang,Mengdie Yan,Yingchun Liu,Huilin Pan

The state-of-the-art water-in-salt electrolytes exhibit a wider electrochemical window than conventional dilute aqueous electrolytes. However, the extended electrochemical stability window via increasing the salt concentration has reached a bottleneck. An alternative approach is to effectively suppress H2O activity using multi-functional components. Here, we design an isolated water-in-salt solvation structure in aqueous electrolytes with the “hydrotropic” ionic liquid 1-methyl-1-propylpiperidinium bis(fluorosulfonyl)imide (PP13FSI). The addition of PP13FSI suppresses H2O clusters via the hydrophobic PP13+ cations and lithium-philic FSI− anions, showing a greatly extended electrochemical stability window up to 4.9 V. A robust alkaline-based organic–inorganic hybrid solid electrolyte interface is achieved on a low-voltage Li4Ti5O12 anode, which further extends kinetics stability of aqueous electrolytes. Aqueous Li4Ti5O12‖LiMn2O4 full cells demonstrate stable cycling over 1000 cycles at 2C rate and a capacity retention of 70% with an average coulombic efficiency of 99.7%. This work provides new avenues to explore effective approaches for the development of next-generation highly stable aqueous lithium-ion batteries.

研究领域: 电化学 · 材料科学 · 能源存储
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Molecular Catalysis · 2021 · IF 5.062

Preparation of supported In2O3/Pd nanocatalysts using natural pollen as bio-templates for CO2 hydrogenation to methanol: Effect of acid-etching on template

Pan Tian,Zhongjie Cai,Guowu Zhan,Jiale Huang,Qingbiao Li

The conversion of CO 2 into value-added chemicals is an effective way to mitigate the environmental problems caused by huge anthropogenic CO 2 emissions. Although In 2 O 3 /Pd catalyst possesses excellent catalytic performance in CO 2 hydrogenation to methanol, the formation of Pd-In alloy on the catalyst surface greatly reduces the yield of methanol. Herein, we adopt a natural biomaterial ( viz. , rape pollen) as a template to synthesize hierarchically structured bio-In 2 O 3 and bio-In 2 O 3 /Pd catalysts. In particular, we found that the pretreatment of pollen using hydrochloric acid (HCl) played a critical role in determining catalytic performance. A series of bio-In 2 O 3 were prepared by using the pollen templates with different etching degrees, and then the bio-In 2 O 3 -x/Pd catalysts (x denoted as the amount of HCl, mL) were prepared using an impregnation-reduction method. It was surprising that the CO 2 conversion of bio-In 2 O 3 –15/Pd catalyst was 8.2% with methanol selectivity of 74.7%, which was much better than the bio-In 2 O 3 –0/Pd (2.6% and 54.6%, respectively). The dramatic enhancement was due to that the acid-etched pollen template owns a hollow cage-like structure and abundant surface functional groups (-NH 2 and -COOH), which is beneficial to the growth of In 2 O 3 with a high amount of surface oxygen vacancies. Also, the bio-In 2 O 3 /Pd catalyst (prepared with untreated pollen template) was more prone to form Pd-In alloys as a result of the strong interaction between Pd with In 2 O 3 . In contrast, the In 2 O 3 spatial distribution of bio-In 2 O 3 –15/Pd was more uniform with an appropriate interaction of Pd with In 2 O 3 that inhibited the formation of Pd-In alloys. Even Pd loaded on commercial In 2 O 3 exhibited inferior performance (3.4% CO 2 conversion and 81% methanol selectivity) to bio-In 2 O 3 –15/Pd catalyst. Accordingly, the present work offers a green and efficient method to prepare supported In 2 O 3 /Pd catalysts by using the acid-etched pollen as a template.

CAS / MDL: 25249-54-1 9003-39-8
研究领域: 催化 · 环境科学 · 材料科学 · 化学工程
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Journal of Energy Chemistry · 2023 · IF 13.1

Li-richening strategy in Li2ZrCl6 lattice towards enhanced ionic conductivity

Haochang Zhang,Zhaozhe Yu,Hannan Chen,Yongjian Zhou,Xiao Huang,Bingbing Tian

All-solid-state Li batteries (ASSLBs) with solid-state electrolytes (SSEs) are exciting candidates for next-generation energy storage and receive considerable attention owing to their reliability. Halide SSEs are promising candidates due to their excellent stability against 4 V-class layered cathodes. Compared with Li 3 InCl 6 or Li 3 ScCl 6 , the low ionic conductivity of Li 2 ZrCl 6 (LZC) is a challenge despite its low raw-material cost. Herein, we report a family of Li-Richened chloride, Li 2+2 x Zr 1– x M x Cl 6 , which can be used in high-performance ASSLBs owing to its high ionic conductivity (up to 0.62 mS cm −1 ). The theoretical (ab initio molecular dynamics simulations) and experimental results prove that the strategy of aliovalent substitution with divalent metals to obtain Li-Richened LZC is effective in improving Li + conductivity in SSEs. By combining Li 2.1 Zr 0.95 Mg 0.05 Cl 6 (Mg5-LZC) with a Li–In anode and a LiCoO 2 cathode, a room-temperature ASSLBs with excellent long-term cycling stability (88% capacity retention at 0.3C for 100 cycles) and high-rate capability (121 mA h g −1 at 1C) is reported. This exploratory work sheds light on improving the Li + conductivity of low-cost LZC-family SSEs for constructing high performance ASSLBs.

研究领域: 材料科学 · 电化学 · 能量存储
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POLYMERS FOR ADVANCED TECHNOLOGIES · 2021 ·Vol. 32 ·期 8 ·3194-3204 · IF 3.665

In situ growth of the ZIF-8 on the polymer monolith via CO2-in-water HIPEs stabilized using metal oxide nanoparticles and its photocatalytic activity

Hong-yan Niu,Li-qin Cao,Xu-le Yang,Kai-nan Liu,Lu Liu,Ji-de Wang

Here, the ZnO/polyacrylamide (ZnO/PAM) macroporous composite monolith was first prepared through the radical polymerization of acrylamide in ZnO-costabilized CO 2 -in-water Pickering high internal phase emulsions (HIPEs). An efficient and green synthesis method was used to prepare the ZnO/PAM porous precursor materials, and ZnO nanoparticles (NPs) were used as a metal ion source to grow the metal organic frameworks (MOF) phase through secondary recrystallization, thereby synthesizing the target MOF/PAM porous monolith. The effects of the contents of ZnO NPs on the formation of HIPEs and properties of the target MOF/PAM composites for the photocatalytic degradation of cationic dye were studied. As the content of ZnO NPs increased to 3.75 wt%, the composite monolith had high mechanical stress (0.24 MPa) at 80% strain and recovered their shape. The as-synthesized ZIF-8/PAM composites were characterized using X-ray diffraction, scanning electron microscope (SEM), Brunauer Emmett Teller (BET), energy dispersive X-ray spectrometer (EDS) mapping, and TG methods. SEM images showed that the hybrid materials were interconnected, and the sizes of the open macropore and interconnected pore throats were 30–125 and about 2–20 μm, respectively. In addition, the ZIF-8/PAM material could be used as a high-efficiency photocatalyst to remove the cationic dye at a fast rate (88.6%).

CAS / MDL: 693-98-1 1314-13-2
研究领域: 材料科学 · 化学 · 环境科学
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