APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Liming Yang,Guangzhen Liu,Zhenglin Chen,Zhiyan Guo,Tian Liu,Hui Shi,Penghui Shao,Xianchuan Xie,Wenwei Li,Xubiao Luo
Transition metal sulfides have demonstrated excellent heavy metal detoxification in previous studies. However, the activity of their S-functional sites is usually not maximized because they are not precisely regulated. Herein, we report a new short-term cathodic tuned CuS crystals (C-tuned CuS) distortion strategy, ultrafast detoxicating over 95% Cr(VI) in 1 min,its detoxification rate was elevated by five orders of magnitude times compared to the untuned one. The high Cr(VI) detoxification performance is mainly attributed to the layered sulfur atoms tuning within series of cathodic potential shown by In-situ Raman. Besides, the four-tuning stages of C-tuned CuS lattice distortion based on the variation of Raman peak height and redshift changes was investigated by density functional theory (DFT) calculations, showing that the S-S bonds was stretched under cathodic tuning, extending from 2.106 to 2.345 Å. The stretched S-S bonds with enhanced polarity and electron activity prevailed the formation of transient Cr-S bonds with Cr(VI), favoring the direct electron transfer without O mediation, thus reducing the Cr(VI) reduction energy barrier. Cathodic tuning CuS crystal distortion, a “Plug and Play” strategy, show a new electron-level microscopic insights into wastewater reduction techniques development.
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MOLECULES
·
2013
·Vol. 18
·期 4
·4158-4169
·
IF 2.428
Luhui Ren,Xue Du,Mengnan Hu,Chaoqun Yan,Taigang Liang,Qingshan Li
An asymmetric synthesis of a series of novel 4-methyl-(3'S,4'S)-cis-khellactone derivatives3a–ois reported for the first time. Their structures were confirmed by1H-NMR,13C-NMR and MS. Their cytotoxic activity was evaluated by the MTT assay against three selected human cancer cell lines: HEPG-2 (human liver carcinoma), SGC-7901 (human gastric carcinoma), LS174T (human colon carcinoma). Some compounds showed high inhibitory activity against these human cancer cell lines. Among them, compound3aexhibited strong cytotoxicity, with IC50values ranging from 8.51 to 29.65 μM. The results showed that 4-methyl-cis-khellactone derivatives withS,Sconfiguration could be a potential antitumor agents.Keywords:4-methyl-(3'S,4'S)-cis-khellactone derivatives;asymmetric synthesis;antitumor activity
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
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2020
·Vol. 24
·期 4
·997-1006
·
IF 2.646
Song Haishen,Yuan Hailiang,Chen Hezhang,Tang Anping,Xu Guorong,Liu Lihua,Zhang Zhian,Kuang Qiujuan
The commercial application of lithium-sulfur (Li-S) battery is hampered by the insulating characteristic and dissolution problem of sulfur and lithium polysulfides. Herein, a mesoporous TiO 2 @PPy material has been fabricated to act as the chemical immobilizer for sulfur species in Li-S battery. In the structure, PPy layer is covered uniformly on surface of the mesoprous TiO 2 , forming a core-shell structure. The well-developed mesopores act as the reservoir for sulfur, while the PPy layer improves the conductivity of material and further prevents diffusion of soluble polysulfides. The synthesized TiO 2 /S@PPy composite delivers an improved rate capability and cycling stability, with an initial discharge specific capacity of 1013.7 mAh g −1 at 0.1 C. In addition, the composite reserves a high capacity of 567.0 mAh g −1 after 300 cycles at 0.5 C, with a decreasing rate of 0.103% per cycle.
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Research
·
2020
·
IF 0
Changping Wang,Chongyi Liu,Qiyao Wei,Lei Yang,Peng Yang,Yiwen Li,Yiyun Cheng
Photocleavable hydrogels are of great importance in the field of controlled drug delivery, stem cell fate regulation, surface patterning, and intelligent devices. However, the development of novel photocleavable gel systems by visible light is usually met with challenges such as the lack of efficient and tunable photocleavable groups and reactions. Herein, we reported the facile fabrication of a new type of photocleavable hydrogels by the direct gelation of 4-arm thiol-terminated polyethylene glycol with 3,6-dichloro-1,2,4,5-tetrazine via the formation of S,S-tetrazine linkages. The prepared hydrogels underwent efficient degradation upon irradiation by ultraviolet or green light, and the degradation kinetics could be significantly promoted by hydrogen peroxide. Correspondingly, the hydrogels loaded with calcium peroxide microparticles or glucose oxidase/catalase enzymes enabled the precise and efficient in vivo photocontrol of gel degradation and drug release for cancer treatment. This work offers a promising and facile strategy towards the fabrication of visible light cleavable hydrogels with tunable and on-demand drug release properties.
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Polymer Chemistry
·
2020
·Vol. 11
·期 21
·3605-3614
·
IF 5.342
Guiting Chen,Dan Cheng,Wenyan Zou,Ziyan Cai,Yufeng Xie,Yaqi Chen,Baitian He,Hongqing Hao,Wei Yang,Yong Cao
Herein, a novel electron-deficient conjugated water/alcohol-soluble polyelectrolyte (WSPE) named PFSOPyCl-E, consisting of dibenzothiophene-S,S-dioxide, bispyridinium salts and fluorene with ethylene oxide side chains, was presented. Previously we have synthesized another WSPE (PFSOPyCl) composed of the same backbone as that of PFSOPyCl-E but with octyl side chains. PFSOPyCl and PFSOPyCl-E were applied as cathode buffer materials (CBMs) to inverted polymer solar cells (PSCs) of poly[4,8-bis(2-ethylhexyloxyl)benzo[1,2-b:4,5-b′]dithiophene-2,6-diyl-alt-ethylhexyl-3-fluorothithieno[3,4-b]thiophene-2-carboxylate-4,6-diyl] (PTB7):[6,6]-phenyl-C71 butyric acid methyl ester (PC71BM) systems, and simultaneous enhancements in open-circuit voltage (Voc), short-circuit current density (Jsc) and fill factor (FF) could be achieved when inserting these cathode buffer layers (CBLs). It was found that these CBLs could build directed dipoles at the indium tin oxide (ITO)/active layer interfaces, leading to the reductions in the ITO work function (WF) and improvements in Voc for the modified devices. The Jsc and FFs of PSCs were increased by several mechanisms. Firstly, the energy level alignments between the reduced ITO WFs (4.30–4.32 eV), deep LUMO energy levels (ELUMO) of these CBLs (4.04–4.10 eV) and ELUMO of PC71BM (∼3.90 eV) could generate good ohmic contacts, facilitating electron extractions and transportations. Secondly, these CBLs were able to n-dope PC71BM at the interfaces, inducing efficient electron-transporting pathways in the devices. Moreover, these polar polymeric CBLs could improve the compatibilities between ITO and the active layers, thus decreasing the interfacial resistances. It is worth noting that PFSOPyCl-E showed better cathode-modifying performance than PFSOPyCl, probably since PFSOPyCl-E with ethylene oxide side chains of high polarity and flexibility possessed better wettability with ITO and smoother films than PFSOPyCl. Hence, the devices modified by PFSOPyCl-E displayed lower contact resistances and higher FFs and Jsc than the PFSOPyCl-modified ones. Therefore, this class of electron-deficient conjugated WSPEs are promising CBMs for high-performance PSCs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Ni Luo,Cheng Chen,Dingming Yang,Wenyuan Hu,Faqin Dong
In the field of photocatalysis , one focus is on high-performance visible light catalysis. For this study, which follows the defect engineering strategy, ultrathin two-dimensional (2D) S defect-rich MoS 2 nanosheets were created in situ by ball-milling MoS 2 nanosheets with ascorbic acid and then used for the removal of Cr(VI) from wastewater. The results show that ascorbic acid increases both the specific surface area of MoS 2 nanosheets and the concentration of S stripping-defects significantly. Of the samples, D-MoS 2 -3 (i.e., S defect-rich ultrathin 2D MoS 2 nanosheets) exhibited the best Cr(VI) adsorption capacity and photocatalytic activity thanks to its large specific surface area and a high concentration of total S defects (18.5%), 311.1% better than for P-MoS 2 (i.e., pristine MoS 2 nanosheets) (4.5%). The concentration of S point-defects in D-MoS 2 -3 is only a little greater than in P-MoS 2 , but the concentration of S stripping-defects is significantly greater. S point-defects at such a high concentration readily act as recombination centers for photogenerated carriers. By contrast, S stripping-defects that lack dangling Mo-S bonds trap photogenerated holes and add to the separation efficiency of photogenerated electron-hole pairs. As a consequence, the photocatalytic performance of D-MoS 2 -3 in removing Cr(VI) is significantly better. Given this finding, the present study offers a new design pathway and a reference for the practical application of defect engineering to ultrathin 2D materials.
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Journal of Materials Chemistry C
·
2021
·Vol. 9
·期 27
·8537-8544
·
IF 7.393
Zhongyuan Guan,Haihang Ye,Peiwen Lv,Lijin Wang,Jing Zhang,Bin Zou,Aiwei Tang
Multinary Cu-based chalcogenide nanocrystals (NCs) are excellent candidates for optoelectronic applications, but their growth mechanism and its impacts on the NCs’ optical properties remain controversial. Herein, we employed a simple colloidal chemistry method for the growth of multinary Cu-based NCs including ternary Cu–In–S NCs, quaternary Cu–In–Se–S NCs, and five-component Cu–In–Zn–Se–S NCs, to explore their growth mechanism and investigate their optical properties. It is found that the ternary Cu–In–S NCs contain a large number of copper vacancies, which affect the major acceptor level for the exciton recombination. With the high reaction activity of Se, the quaternary Cu–In–Se–S NCs form at low reaction temperature and have a red-shift of the photoluminescence (PL) maximum due to the recombination from the conduction band to the acceptor level. The formation process of five-component Cu–In–Zn–Se–S NCs highly depends on the Zn amount, which shows a competitive relationship between the NCs’ growth and diffusion of Zn, leading to the red- and blue-shift of PL maximum, respectively. Our study provides a clear map for the growth of multinary Cu-based NCs and shows their impacts on optical properties.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Shijun Zhang,Qinjun Shao,Yan Su,Lei Xu,Qike Jiang,Jian Chen
Lithium-sulfur (Li-S) battery possess the advantage of high specific energy but suffer from unstable cyclic performance due to the sluggish liquid-solid conversion kinetics causing severe lithium polysulfides (LiPS) shuttling. Designing multifunctional electrocatalysts with improved activity and abundant active sites to regulate the dynamics for sulfur electrochemistry is still a significant challenge. Herein, we proposed a thiourea assisted pyrolysis combined with hard template method to synthesize cobalt single atoms co-coordinated by N and S atoms embedded hollow carbon spheres (Co-NS-HCS) as a novel sulfur host. The Co-NS-HCS mainly consists of well-dispersed Co-N 3 S-C center sites where Co is co-bonded by N and S atoms. Systematical characterizations revealed that the Co-NS-HCS exhibit improved SRR electrocatalytic properties with higher exchange current density and larger electron transfer number than that of Co-N-HCS. When equipped in sulfur cathodes, the S@Co-NS-HCS exhibits superior rate performance (925 mAh g −1 at 2 C), long cycle stability (69.1% of capacity retention after 500 cycles at 1 C). Moreover, the assembled Li-S pouch type cell also exhibits competitive cyclic performance that work stably for 100 cycles at 0.1 C with a high capacity retention of 84.7%. This work furnishes a feasible scheme for the rational design of single atoms catalysts with improved electrocatalytic activity for sulfur cathodes based on the coordination environment regulation strategy.
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Materials
·
2020
·Vol. 13
·期 6
·1279
·
IF 3.057
Yanqin Xu,Liyue Xiao,Yating Chang,Yuan Cao,Changguo Chen,Dan Wang
In order to achieve a controlled release drug delivery system (DDS) for cancer therapy, a pH and redox dual-responsive mesoporous silica nanoparticles (MSN)-sulfur (S)-S- chitosan (CS) DDS was prepared via an amide reaction of dithiodipropionic acid with amino groups on the surface of MSN and amino groups on the surface of CS. Using salicylic acid (SA) as a model drug, SA@MSN-S-S-CS was prepared by an impregnation method. Subsequently, the stability, swelling properties and drug release properties of the DDS were studied by x-ray diffraction, scanning electron microscopy, Fourier transform infrared microspectroscopy, size and zeta potential as well as Brunauer–Emmett–Teller surface area. Pore size and volume of the composites decreased after drug loading but maintained a stable structure. The calculated drug loading rate and encapsulation efficiency were 8.17% and 55.64%, respectively. The in vitro drug release rate was 21.54% in response to glutathione, and the release rate showed a marked increase as the pH decreased. Overall, double response functions of MSN-S-S-CS had unique advantages in controlled drug delivery, and may be a new clinical application of DDS in cancer therapy.Keywords:mesoporous silica nanoparticles;double response;drug delivery;drug release
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DESIGNED MONOMERS AND POLYMERS
·
2017
·
IF 1.139
Kun Zhang,Kai Yang,Shiyun Ai,Jing Xu
A blue-fluorescence 2,4,6-tris(4-fluorophenyl)-1,3,5-triazine (TFPT) monomer was synthesized with high yield and high purity under mild reaction conditions. The TFPT, which had three active fluoric groups, was facilely incorporated into stable cross-linked fluorescent polymeric nanoparticles (FCPNs) via precipitation polymerization with 6-(4-hydroxyphenyl)pyridazin-3(2H)-one (HPZ). The FCPNs were highly dispersible in water and showed uniform size, intense blue fluorescence, and excellent biocompatibility, making them promising for live cell imaging label applications. This work has the potential to promote the exploitation of novel s-triazine monomers, and to provide a new view of functional crossing-linked polymers based on such monomers.
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CONSTRUCTION AND BUILDING MATERIALS
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2014
·
IF 2.265
Xiaolu Guo,Wenpei Hu,Huisheng Shi
Nano-modified composite geopolymers were successfully prepared from municipal solid waste incineration fly ash (MSWIFA) and class C fly ash (CFA). The results indicate that both nano-SiO 2 and nano-γ-Al 2 O 3 have a good modification effect on geopolymer, of which nano-SiO 2 has a better performance than nano-γ-Al 2 O 3 . The optimum content of nano-SiO 2 and nano-γ-Al 2 O 3 are 1.5% and 2.0%, respectively. XRD shows that there is no new phase emerging after adding a small amount of nanomaterials. By FT-IR and SEM, it means that nanomaterials facilitate the reaction of geopolymer, making the modified geopolymer more compact. BET shows nano-SiO 2 especially modifies the pore distribution and pore structure of geopolymers. Additionally, nanomaterials have an improvement to the solidification/stabilization (S/S) of heavy metals.
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ADVANCED MATERIALS
·
2025
·
IF 26.8
Bo Shao,Tianyun Liu,Deng-Bing Li,Linxing Meng,Jianyuan Wang,Wei Zhai,Liang Li
Solar-driven hydrogen production is significant for achieving carbon neutrality but is limited by unsatisfactory surface catalytic reaction kinetics. Layer regulation can impact carrier transmission or catalytic behavior, but the specific effects on the oxygen or hydrogen evolution reaction (OER or HER) remain unclear, and atomic layer level modulation for maxing HER is challenging. Here the distinct roles of modulated Zn–S or In–S surface layers in ZnIn 2 S 4 (ZIS) for the OER and HER, respectively, are disentangled. Moreover, the extensive characterizations and computational results demonstrate that stressful environments enable individual modulation and introduce Ni into the surface In–S layer rather than the easily alterable Zn–S layer, creating deeper hybridized electronic states of Ni 3 d –S 3 p , optimizing H * adsorption/desorption, and maximizing surface catalytic benefits for the HER. Consequently, the optimized ZIS exhibited a photocatalytic hydrogen production rate of up to 18.19 mmol g −1 h −1 , ≈32 times higher than pristine ZIS. This investigation expands the application scenarios of ultrasonic technology and inspires other precise control types, such as defects and crystal plane engineering, etc.
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