JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 5
·050548
·
IF 4.316
Chengjun Zhang,Sha Chen,Guangying Zhou,Qiong Hou,Suilian Luo,Yuhai Wang,Guang Shi
Two poly(arylamine-imide)s, poly(N,N,N',N'-tetraphenyl-1,4-benzenediamine naphthalenediimide) (PDDP-NI) and poly(N,N,N',N'-tetraphenyl-1,4-benzenediamine perylenediimide) (PDDP-PI), were successfully prepared by condensation polymerization of an amine monomer N,N,N',N'-tetraphenyl-1,4-benzenediamine (DDP) with dianhydride monomer 1,4,5,8-naphthalenetetracarboxylic dianhydride (NTCDA) or 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA). The DDP units in the polymer can reversibly dope/dedope the PF6− anion, while the naphthalenediimide (NI) unit or perylene diimide (PI) unit can reversibly insert/extract the lithium cation. The lithium ion half-cells based on the polymer cathode and the lithium anode are assembled and the electrochemical properties are tested. Due to the high voltage of the DDP unit in the polymer backbone, lithium-ion half-cells based on PDDP-NI and PDDP-PI cathodes provide a high average discharge voltage of about 3.2 V. Moreover, the as-prepared polymer materials exhibit long-cycle performance, PDDP-NI remains 89% capacity after 500 cycles at 10 C and PDDP-PI maintains 98% capacity after 1000 cycles at 10 C, furthermore, their coulombic efficiency close to 100% at all current rates tested, which shows that these organic cathode materials have potential applications in long-cycle lithium-ion batteries.
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INORGANIC CHEMISTRY
·
2020
·
IF 4.825
Ji Wu,Ke Cao,Cai-Yan Zhang,Tao-Tao Xu,Xin-Yu Wen,Bo Li,Junxiao Yang
A palladium catalyzed selective B(3)–H activation/oxidative dehydrogenative coupling for the synthesis of bis(o-carborane)s connected with B(3)–B(3′) and B(3)–B(6′) bonds has been developed for the first time. A plausible mechanism involving stepwise activation of B(3)–H and B(3′/6′)–H bonds by PdII and PdIV was proposed. This work is the first example and the most efficient protocol for synthesis of bis(o-carborane)s connected with B(3)–B(3′) and B(3)–B(6′) bonds, which has important reference for design, synthesis, and application of bis(o-carborane)s in related fields.
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CHINESE JOURNAL OF POLYMER SCIENCE
·
2020
·Vol. 39
·期 1
·51-59
·
IF 3.154
Song Bo,Qin An-Jun,Tang Ben Zhong
Green monomers, such as carbon dioxide (CO 2 ), are closely related to our daily life and highly desirable to be transferred to functional polymers with diverse structures and versatile properties because they are abundant, cheap, nontoxic, renewable, and sustainable. However, the polymerizations based on these green monomers are to be further developed. In this work, a facile CO 2 and alkyne-based one-pot, two-step, four-component tandem polymerization was successfully established. The polymerization of CO 2 , diynes, alkyl dihalides, and primary/secondary amines can proceed under mild reaction conditions and regio- and stereoregular poly(aminoacrylate)s with good solubility and thermal stability were obtained in high yields (up to 95%). Notably, distinctly different stereoregularity of resultant poly(aminoacrylate)s was realized via using primary or secondary amines. Using the former would readily generate polymers with 100% Z -isomers, whereas the latter furnished products with over 95% E -isomers. Through different monomer combination, the polymers with tunable structures and properties were obtained. Moreover, the tetraphenylethene units containing poly(aminoacrylate)s, showing the unique aggregation-induced emission characteristics, could function as a fluorescent probe for sensitive explosive detection. Thus, this work not only develops a facile CO 2 and alkyne-based multicomponent tandem polymerization but also provides a valuable strategy to fine-tune the polymer structures and properties, which could be potentially applied in diverse areas.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zewen Yang,Dandan Jia,Yue Wu,Depeng Song,Xiaolin Sun,Cheng Wang,Li Yang,Yuan Zhang,Jing Gao,Takeo Ohsaka,Futoshi Matsumoto,Jianfei Wu,Qiang Shen
Lithium-sulfur (Li-S) batteries exhibit a high specific capacity (1675 mAh g −1 ) but poor S conductivity and severe shuttle effects. Selenium (Se) can greatly mitigate these disadvantages, but its theoretical capacity is relatively low (675 mAh g −1 ). A series of S x -Se y compounds supported by chitosan-derived carbon with intertwined carbon nanotube (CC + CNT) carriers exhibit the high capacity of S, the stability of Se, and the excellent conductivity of C, complementing their individual defects. S 2 Se 1 /CC + CNT shows the best electrochemical performance (833.2 mAh g −1 after 500 cycles). Characterization results reveal the structure–activity relationships and complex reaction mechanisms of the prepared electrode materials. The overall reactions are a combination of basic Li-S and Li-Se reactions. The discharge steps are clearly identifiable, while the reaction sequences are slightly adjusted and fully integrated when charging. This work provides a foundation for future research and for the practical application of chalcogenides in lithium-metal batteries.
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JOURNAL OF BIOMATERIALS APPLICATIONS
·
2024
·
IF 2.3
Yang Sheng,Danni Qing,Naijun Li,Peng Zhang,Yixin Sun,Rong Zhang
Zn-Ag-In-S (ZAIS) quantum dots (QDs) were synthesized with various Ag-to-In ratios and used as novel photosensitizers for photodynamic therapy (PDT) on cancer cell inhibition and bacterial sterilization, and their structural, optical, and photodynamic properties were investigated. The alloyed QDs displayed a photoluminescence quantum yield of 72% with a long fluorescence lifetime of 5.3 μs when the Ag-to-In ratio was 1:3, suggesting a good opportunity as a dual functional platform for fluorescence imaging and PDT. The ZAIS QDs were then coated with amphiphilic brush copolymer poly(maleic anhydride-alt-1-octadecene) (PMAO) before application. The 1O2 quantum yield of the ZAIS/PMAO was measured to be 8%, which was higher than previously reported CdSe QDs and comparable to some organic photosensitizers. Moreover, the ZAIS QDs showed excellent stability in aqueous and biological media, unlike organic photosensitizers that tend to degrade over time. The in vitro PDT against human melanoma cell line (A2058) and Staphylococcus aureus shows about 30% inhibition rate upon 20 min light irradiation. Cell staining images clearly demonstrated that co-treatment with ZAIS QDs and light irradiation effectively killed A2058 cells, demonstrating the potential of ZAIS QDs as novel and versatile photosensitizers for PDT in cancer and bacterial treatment, and provides useful information for future designing of QD-based photosensitizers.
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PubMed
高影响因子
Advanced Powder Materials
·
2021
·
IF 0
Mengqin Gao,Wan-Ying Zhou,Yu-Xue Mo,Tian Sheng,Yanhong Deng,Liezun Chen,Kai Wang,Yanliang Tan,Haiqing Zhou
Here we proposed a novel approach to greatly enhance the electrochemical performance of Li–S batteries by designing a composite electrode material composed of a core-shell structure of S@Pt composite (sulfur content, 85%) grown on the S surface. The platinum (Pt) nanosheets provide physical barrier and strong chemical binding to anchor LiPSs and improve the electronic conductivity of S. Significantly, by introducing carbon nanofibers (CNFs) as the interlayer, we achieved outstanding Li–S battery with a high initial discharge capacity of 1040 mAh g −1 at 1.0 C and a reversible capacity of 742 mAh g −1 after 350 cycles, demonstrating its excellent long-term cycling stability with a low capacity decay rate of 0.08% per cycle. According to the density functional theory (DFT) calculations, we proposed that the superior performance is attributed to the cooperative effects of the strong interfacial interaction between Pt (111) surface and the S 8 molecule, and very low reaction energy of decomposition, −6.4 eV.
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MACROMOLECULES
·
2019
·
IF 5.997
Bingjie Zhao,Kun Wei,Lei Wang,Sixun Zheng
3,13-Di(cyclic carbonate) double decker silsesquioxane, a new difunctional polyhedral oligomeric silsesquioxane (POSS), was successfully synthesized. By using this POSS macromer, the organic–inorganic poly(hydroxyl urethanes) (PHUs) were synthesized with POSS cages in the main chains. Compared to the neat PHU, the organic–inorganic PHUs displayed improved thermomechanical properties. The organic–inorganic PHUs were microphase-separated, and the main-chain POSS cages were self-assembled into the nanodomains in the size of 10–30 nm. It was found that the POSS nanodomains acted as the nano-cross-linking points of physically cross-linked networks. Although the linear organic–inorganic PHUs were soluble in common organic solvents, they were capable of displaying the thermomechanical properties similar to cross-linked PHU elastomers. Owing to the physical cross-linking, the organic–inorganic PHUs were endowed with shape memory properties. In the meantime, the organic–inorganic PHUs can be reprocessed at elevated temperature; the tensile mechanical strength can be recovered up to 90%. The reprocessing properties resulted from the transcarbamoylation reaction of hydroxyurethane structural units other than the disintegration of POSS nanodomains at elevated temperature. The reprocessing properties can be utilized to program the original shapes of shape memory polymers.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-7
·
IF 16.6
Li Peihui,Hou Songjun,Wu Qingqing,Chen Yijian,Wang Boyu,Ren Haiyang,Wang Jinying,Zhai Zhaoyi,Yu Zhongbo,Lambert Colin J.,Jia Chuancheng,Guo Xuefeng
The transformation from one compound to another involves the breaking and formation of chemical bonds at the single-bond level, especially during catalytic reactions that are of great significance in broad fields such as energy conversion, environmental science, life science and chemical synthesis. The study of the reaction process at the single-bond limit is the key to understanding the catalytic reaction mechanism and further rationally designing catalysts. Here, we develop a method to monitor the catalytic process from the perspective of the single-bond energy using high-resolution scanning tunneling microscopy single-molecule junctions. Experimental and theoretical studies consistently reveal that the attack of a halogen atom on an Au atom can reduce the breaking energy of Au−S bonds, thereby accelerating the bond cleavage reaction and shortening the plateau length during the single-molecule junction breaking. Furthermore, the distinction in catalytic activity between different halogen atoms can be compared as well. This study establishes the intrinsic relationship among the reaction activation energy, the chemical bond breaking energy and the single-molecule junction breaking process, strengthening our mastery of catalytic reactions towards precise chemistry.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Lanlan Guo,Wei Zhao,Linlin Dong,Xin Shi,Guodong Wang,Rui Li,Jianliang Cao,Xueli Yang,Xiaolian Liu,Yan Wang
The construction of high-performance sensitive materials is a basis for excellent sensors. Among prior SnS 2 -based sensors, high sensing performance often accompanies high operating temperatures or expensive costs, which limits their practical use. Herein, we employed Sr doping and NaBH 4 treatment strategies to increase the S-vacancies content in the SnS 2 microflowers. Particularly, this composite sensitive material shows large specific surface area, low crystallinity and rich S-vacancies content, which enables this sensor excellent sensing properties toward NO 2 , with a response of 4.7 toward 5 ppm NO 2 at 100 °C. In addition, this sensor has a low detection limit for NO 2 as low as 0.2 ppm, which is a lower value compared to many SnS 2 -based NO 2 sensors as reported. XRD, SEM, TEM, EPR and BET characterization combined with density functional theory (DFT) calculations are adopted to illustrate the enhancement mechanism toward NO 2 of the composite sensitive materials fabricated in this work. This study provides new ideas and scientific basis for the construction of metal sulfide based NO 2 sensors, which has important theoretical significance and application value.
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高影响因子
ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Yan Jia,Peng Li,Wei Song,Guangjiu Zhao,Daoyuan Zheng,Dongmei Li,Yanni Wang,Jiayue Wang,Chunyan Li,Keli Han
S-Adenosylhomocysteine hydrolase (SAHase) is a cellular enzyme that plays a key role in the methylation process, and a potential drug target in the discovery of antiviral and anticancer agents. There is increasing interest in determining its activity in the biological and clinical fields with chemosensors but with limited success so far. Herein, we designed and developed for the first time an off/on-type of fluorogenic substrate (NADE) that is directly responsive to SAHase activity. NADE used 1,8-naphthalimide as the signal reporter and adenosine (Ade) as the reaction center; removal of the Ade moiety enhanced the fluorescence by >10-fold. Kinetic study showed that NADE followed a non-Michaelis–Menten pattern that corresponded to the allosteric behavior of SAHase. NADE showed excellent selectivity and functioned efficiently in cells, allowing the microscopic imaging of SAHase activity. NADE can also be used to identify and measure the effectiveness of inhibitors in a markedly superior way. In a word, NADE would be broadly useful in clinical applications and academic studies.
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POLYMER
·
2022
·
IF 4.432
Jie Huan,Jing Li,Yinjia Lan,Sheng Wang,Xiaohong Li,Xiaoming Yang,Huanjun Lu,Yingfeng Tu
We present here the effect of oligo(ethylene glycol) (OEG) segmental length on properties of cyclic oligo(oligoethylene glycol terephthalate)s (COEGTs) and their corresponding polymer counterparts, poly(oligoethylene glycol terephthalate)s (POEGTs). COEGT monomers were synthesized from terephthaloyl chloride with corresponding diethylene glycol , triethylene glycol , and tetraethylene glycol under pseudo-high-dilution conditions. As those large ring cyclic monomers are hard to be polymerized via traditional ring-opening polymerization, a cascade polycondensation-coupling ring-opening polymerization method is utilized to obtain high molecular weight POEGTs. The cascade polymerization mechanism is confirmed by the kinetics study . The structures of COEGTs and POEGTs were well characterized and their properties were studied to reveal the structure-property relationship. With the increment of OEG length in repeating units, the chain flexibility of POEGT and COEGTs is enhanced. As a result, the melting temperatures of COEGTs and glass transition temperatures of POEGTs decrease. On the other hand, the thermal degradation temperature of POEGTs and COEGTs increases due to the enhanced ether fraction and reduced ring strain. Solid-state polymer electrolytes based on POEGTs was prepared by blending with lithium bis(trifluoromethanesulfonyl)imide. The measured ionic conductivity increased with the OEG length in POEGT repeating units. Our results revealed the effect of OEG length on the structure-property relationship in cyclic oligo(ether ester)s and copoly(ether ester)s, providing a facile way to tune their properties.
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高影响因子
IONICS
·
2022
·Vol. 28
·期 3
·1157-1166
·
IF 2.961
Jin Zhengfei,Ma Xiangyu,Qiu Linlin,Liu Yang,Yuan Yongfeng,Song Lixin,Du Pingfan,Xiong Jie
Compared to conventional lithium batteries, lithium-sulfur (Li–S) batteries are not only low-cost and environmentally friendly but also have a high theoretical energy density. However, the insulating nature of sulfur materials and the poor cycle stability of Li–S batteries inhibit their commercialization. Herein, porous carbon nanofibers (PCNFs) were fabricated by a facile electrospinning method and used as a cathode hosting sulfur for Li–S batteries. The porous structure effectively restrained soluble polysulfides from migrating due to shuttle effect of lithium-sulfur batteries. With the PCNFs as the sulfur host, the PCNFs/S cathode exhibited excellent cycling stability. An initial specific capacity of 835 mAh g −1 at 0.1C and a reversible capacity of 98.6% after 100 cycles were achieved. This outstanding performance can be ascribed to the rational design of the electrode structure, which can increase the interfacial contact and provide a large number of electrochemically active sites for polysulfide storage.
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