JOURNAL OF POLYMER SCIENCE
·
2023
·Vol. 61
·期 6
·472-481
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IF 3.4
Xiang-Yue Cheng,Fu-Sheng Du,Zi-Chen Li
1,3-Disubstituted bicyclo[1.1.1]pentane (BCP) is a rigid, linear, non-conjugated hydrocarbon unit that is usually transformed from [1.1.1]propellane. This unit has been introduced into drugs as mimics of 1,4-disubstituted benzene moieties and used as rigid linkers in small-molecule materials. However, the influence of this unique structure on the polymer properties has only been scarcely investigated. In this work, three symmetrical α,ω -diene monomers containing one and two BCP units were synthesized for the first time from [1.1.1]propellane. Three types of precise poly(1,3-bicyclo[1.1.1]pentane alkylene)s with BCPs located on every 11th and 21st chain carbons were obtained via acyclic diene metathesis (ADMET) polymerization and subsequent hydrogenation. All these polymers show higher thermal stability than linear polyethylene. For polymers containing one BCP moiety in their repeating unit, BCP acts as a defect to distort the PE crystals and decrease the melting temperature of PE. However, the polymer that containing a [2]staffane moiety (two jointed BCP units) in the polymer backbone forms a new crystalline morphology. This work elucidates the impact of BCP units on the thermal and crystallization behavior of PE, providing new insights of utilizing BCP unit to construct new polymer backbone, regulate the packing order of polymers and their properties. Graphical
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Chong Wang,Gaoyu Chen,Juanrong Kou,Xianju Zhang,Xiangxing Xu,Jianchun Bao,Zihan Shen,Xin Jin,Huigang Zhang,Li Liu,Kehan Yu
Antimony (Sb) is a competitive candidate for lithium ion batteries (LIBs) as anode material because of its high theoretical discharge capacity (660 mAh/g). However, it remains a challenge caused by the volume change in the process of charge and discharge, which would damage the Sb anode that lead to poor rate performance and low cycle stability. Herein, we report the synthesis of Sb@S–N–C nanocomposite as the anode material to solve the problem. First, SbSI nanowires with diameter of ∼10 nm were synthesized. Then the SbSI nanowires were coated with polypyrrole (PPy) to form SbSI@PPy core-shell nanowires. By thermal reduction of SbSI@PPy, Sb@S–N–C nanocomposite was formed. Using the Sb@S–N–C nanocomposite as the anode material, a capacity of 536 mAh/g was obtained in 100 cycles at 0.5 A/g. Excitingly, it also exhibited superior reversible and long-cycle non-decay stability with the capacity of 342 mAh/g in 2000 cycles at a high current density of 1A/g.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yong Lu,Gaohong Wu,Xiaohui Zhao,Xiaoxu Wang,Wenming Zhang,Zhanyu Li
Due to their high reactivity and theoretical capacity, chalcogen elements have been favored and applied in many battery studies. However, the high surface charge density and high solubility of these elements as electrode materials have hindered their deeper exploration due to the shuttle effect. In this article, organic structural triphenylphosphine is used as a molecular main chain structure, and chalcogen elements O, S, and Se are introduced to combine with P as active sites. This approach not only takes advantage of the beneficial effects of the aromatic ring on the physical and chemical properties of the chalcogen element but also allows for the optimization of its advantages. By utilizing Triphenylphosphine selenide (TP-Se) as the cathode material in aluminum-ion batteries(AIBs), a high-performance Al-organic battery was fabricated, which exhibited a high initial capacity of 180.6 mAh g −1 and stable cycling for up to 1000 cycles. Based on density functional theory (DFT) calculations, TP-Se exhibits a smaller energy gap, which renders it favorable for chemical reactions. Moreover, the calculated results suggest that TP-Se tends to undergo redox reactions with AlCl 2 + . The molecular structure of triphenylphosphine and its combination with Se offers an enticing pathway for designing cathode materials in aluminum-organic batteries.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Liping Wu,Chuyue Cai,Xi Yu,Zihe Chen,Yuxin Hu,Fang Yu,Shengjun Zhai,Tao Mei,Li Yu,Xianbao Wang
Lithium sulfur batteries (LSBs) are regarded as one of the most promising energy storage devices due to the high theoretical capacity and energy density. However, the shuttling lithium polysulfides (LiPSs) from the cathode and the growing lithium dendrites on the anode limit the practical application of LSBs. To overcome these challenges, a novel three-dimensional (3D) honeycombed architecture consisting of a local interconnected Co3O4 successfully assembled into a scalable modified layer through mutual support, which is coated on commercial separators for high-performance LSBs. On the basis of the 3D honeycombed architecture, the modified separators not only suppress effectively the “shuttle effects” but also allow for fast lithium-ions transportation. Moreover, the theoretical calculations results exhibit that the collaboration of the exposed (111) and (220) crystal planes of Co3O4 is able to effectively anchor LiPSs. As expected, LSBs with 3D honeycombed Co3O4 modified separators present a reversible specific capacity with 1007 mAh g–1 over 100 cycles at 0.1 C. More importantly, a high reversible capacity of 808 mAh g–1 over 300 cycles even at 1 C is also acquired with the modified separators. Therefore, this proposed strategy of 3D honeycombed architecture Co3O4 modified separators will give a new route to rationally devise durable and efficient LSBs.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2022
·Vol. 24
·期 18
·10838-10850
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IF 3.945
Wei Deng,Yuping Gai,Haitao Duan,Zhide Chen,Xiaojun Hu,Sheng Han,Niwei Xu,Shanlin Qiao,Zijian Yao,Fei Jiang
Although reasonably specified and adjustable preparation of nanostructures with specific morphologies, ordered chemical compositions and electronic structures involving advanced energy chemistries is an important research area, high-efficiency, stable, and low-cost electrocatalysts for water splitting are greatly desirable and challenging. In this study, partially delocalized Co–S–Se ultra-thin nanosheets are obtained via a liquid–liquid interface-mediated strategy at an oil–water interface. These Co–S–Se ultra-thin nanosheets exhibit different-sized lamellar structures and have an average thickness of 0.83 nm. The ternary ultra-thin Co0.45S0.38Se0.17 nanosheets demonstrate excellent performance for the OER, accompanied by an overpotential of 290 mV (1.52 V vs. RHE) at 10 mA cm−2, and a Tafel slope of 74.5 mV dec−1. In the meantime, the catalyst recombined with a stoichiometry NiOx catalyst to form a composite interface, which also exhibited a good OER performance, with an overpotential of 260 mV at 10 mA cm−2 and a smaller Tafel slope of 53.9 mV dec−1. The nanosheets can rearrange the electronic density near the metal catalytic centers and increase the electron transfer. DFT calculations indicate that the partially delocalized charges can improve electrocatalytic performances, demonstrating modulated electroreduction properties. Due to the special atomic and electronic structure of the ternary transition metal alloy chalcogenide, the compound has great potential for energy storage, which will help in the rational design and synthesis of high-efficiency electrocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Yafei Sang,Jianhan Huang
Porous materials with high Brunauer-Emmett-Teller (BET) surface area ( S BET ) and abundant ionic active sites facilitate efficient CO 2 capture and conversion. Herein, a kind of novel benzimidazole-based hyper-cross-linked poly(ionic liquid)s (HPILs) were developed via the hyper-cross-linking strategy and the as-prepared HPILs possessed high S BET (485–780 m 2 /g), plentiful micro/mesoporosity, and abundant ionic active sites. The HPILs showed noteworthy CO 2 uptake (79–143 mg/g at 273 K and 1.0 bar), moderate isosteric heats (32–45 kJ/mol), and acceptable CO 2 /N 2 selectivity (IAST: 23–46). Intriguingly, HPILs-Cl-2 exhibited excellent catalytic activity for CO 2 cycloaddition and 99% of propylene oxide was successfully converted to cyclic carbonates under mild conditions (70 °C, 0.1 MPa CO 2 , 9 h). This synthetic strategy is of great importance for the functionalized hyper-cross-linked polymers and the synthesized HPILs are promising for efficient CO 2 capture and conversion under mild conditions.
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ACS Omega
·
2024
·
IF 3.7
Dandan Jiang,Yingzhen Zhang,Xin Qiao,Jun Xiao,Kunming Liu,Juanhua Li,Jinbiao Liu
An iron-catalyzed selective N═S coupling of N-methoxy amides and sulfoxides has been developed and was found to be a highly efficient method for the synthesis of N-acyl sulfoximines. Electron-donating as well as electron-withdrawing groups on the phenyl ring are tolerated, and even sensitive substituents are compatible. The current catalytic transformation was conducted under an air atmosphere and can be easily scaled up to a gram scale with a catalyst loading of only 1 mol %. In this case, both coupling partners are used in their native forms, thus obviating prior functionalization and activation.
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PubMed
高影响因子
Materials Today Energy
·
2022
·
IF 9.257
ZhiLong Han,Han Zhang,Qiang Wu,ShuPing Li,Wei Zhong,RenJie He,ShiJie Cheng,Jia Xie
Silicon-sulfur (Si-S) full cells show significant potential in energy storage due to their high theoretical energy density compared to commercial lithium-ion batteries. Nevertheless, a majority of electrolytes reported for Si-S full cells still cannot meet the requirements of stable long-duration cycling. Herein, we report a high-areal-capacity Si-S full cell consisted with prelithiated SiO, thick Li 2 S-Se 0.05 S 0.95 @pPAN electrode and a trifluorobenzene (F 3 B) modified and diluted high-concentration electrolytes. This novel electrolyte can effectively mitigate the volume expansion of the prelithiated SiO anode and enhance the utilization of active S in the cathode, showing excellent compatibility with electrodes. The assembled Si-S full cell using modified electrolyte displays remarkable cyclability over 100 cycles at 0.1C, exhibiting higher capacity retention (54.0% vs . 17.5%) than the pristine electrolyte without F 3 B. More importantly, a full cell with a thick sulfur cathode (16 mg/cm 2 ) exhibits a superior initial areal capacity of 8.34 mAh/cm 2 and high-capacity retention of 52% after 80 cycles, even at a lean electrolyte condition (2 μL/mg). This work provides guidance for the achievement of high-performance Si-S full cells under lean electrolytes.
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Desalination and Water Treatment
·
2024
·
IF 1
Yang Liu,Yuanyuan Wang,Jie Ma,Runping Han
ABSTRACT In this study, peanut shell was modified using β-cyclodextrin (β-CD) and citric acid to improve the adsorption capacity for removal of lead ion (Pb 2+ ) and bisphenol S (BPS) from solution in batch mode. Scanning electron microscopy, Fourier-transform infrared spectroscopy, elemental analysis, X-ray fluorescence analysis, specific surface area analysis, thermogravimetric analysis, etc were used to characterize the adsorbent before and after modification. The results showed that the adsorbent was successfully modified. The adsorption results of Pb 2+ and BPS on β-CD-PS indicated that acidic conditions were not conducive to the adsorption of Pb 2+ , the adsorption of BPS basically remained unchanged at pH 2~7, and alkaline conditions were not conducive to the adsorption. The presence of salt had a negative effect on Pb 2+ , but had no effect on the adsorption of BPS. The Langmuir and Koble–Corrigan models could predict the equilibrium adsorption process of Pb 2+ while Temkin and Koble–Corrigan models could describe the equilibrium adsorption process of BPS. The adsorption quantity from experiments is 89.6 mg·g –1 for Pb 2+ and 16.2 mg·g –1 for BPS at 293 K, respectively. The adsorption process of Pb 2+ was consistent with the pseudo-first-order and Elovich models, indicating the presence of ion-exchange in the adsorption process; the adsorption of BPS was consistent with the pseudo-second-order model, indicating that chemisorption was the main rate-controlling step. Thermodynamic studies indicated that the adsorption of Pb 2+ was a spontaneous and endothermic reaction with increasing entropy, while the adsorption of BPS was a spontaneous and exothermic reaction with decreasing entropy. 0.1 mol·L –1 HNO 3 could desorb and regenerate the β-CD-PS adsorbed Pb 2+ for three times, and 75% C 2 H 5 OH had a better desorption and regeneration effect for BPS loaded β-CD-PS. β-CD-PS can effectively remove the lead ion and BPS from mixtures and the study can provide the basis for the effective utilization of peanut shell in environmental remediation.
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Journal of Energy Chemistry
·
2024
·
IF 14
Xuejun Xu,Rutao Meng,Yue Liu,Han Xu,Jianpeng Li,Yi Zhang
Solution-processed chalcopyrite solar cells are widely regarded as a promising alternative method in reducing the cost compared with vacuum-based techniques. It is noted that the absorber layer usually needs to be prepared under a high insert pressure (∼1.6 atm) to suppress element loss or under a mild pressure but additional surface etching is needed for fabricating high efficient solar cell. Herein, a copper gradient structured precursor is proposed to prepare CuIn(S,Se) 2 (CISSe) film under a mild pressure (1.1 atm). The designed gradient Cu not only promotes crystal grain growth and tailors the defects, but also avoids the surface etching of the formed CISSe film for the fabrication of high efficient solar cells. Further, Cu gradient design decreases the conduction band offset of heterojunction, boosting the carriers transport across the p-n heterojunction. Accordingly, a 13.35% efficient CISSe solar cell, comparable to the high efficient CISSe solar cell prepared by this method under high pressure or with film surface etching, is fabricated. This work provides a facile pathway to fabricate high efficient solution-processed chalcopyrite solar cell, avoiding high selenization pressure and film etching, and shows huge potential for solution-processed copper-based solar cells.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Qian Yu,Jingshu Wang,Haibo Li,Ruiqing Li,Suyuan Zeng,Rui Li,Qingxia Yao,Hongyan Chen,Konggang Qu,Yao Zheng
In the electrocatalytic oxygen reduction and hydrogen evolution reactions (ORR/HER), metal-free carbon-based materials presented great potentials as alternatives to Pt because of their flexible adjustability of electronic and geometric properties. The pursuit of high-performance carbons demand for high-level doping, large surface area and high graphitization, but the improvement of the former two aspects would inevitably impair the third one, which seems a contradictive proposition. Herein, by a facile “mix-and-pyrolyze” method, natural DNA was first developed to synthesize N, P, S-tridoped carbons (NPSC) with porous sheet structures, high graphitization, large surface areas and abundant high-quality dopants simultaneously. Thus, the newly-prepared NPSC displays superior alkaline ORR performance comparable to Pt/C together with excellent acidic activity and better stability. Meanwhile, NPSC is one of most active acidic HER catalysts and the best alkaline HER catalyst among carbon counterparts. Density function theory computation reveled the origins of superior performance are attributed to positively charged C sites neighboring to S for ORR and P sites for HER because of DNA-derived advantaged structural features. The as-fabricated rechargeable zinc–air battery based on current tridoped carbon has closed peak power density and specific capacity but much better charge–discharge stability compared with Pt/C.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2024
·
IF 4.1
Shuhan Jiang,Yujie Jia,Xiaoxia Yang,Qianchen Ou,Yanan Liu,Siqian Zhang,Dianwu Huang,Hongmei Wang
FeCo-LDH/g-C 3 N 4 S-type heterojunction photocatalysts were successfully prepared by thermal polymerization and electrostatic self-assembly methods. The structure, morphology, light absorption and photoelectrochemical properties of the prepared samples were characterized. The photocatalytic properties of the photocatalysts were evaluated by the degradation of tetracycline (TC) and photocatalytic hydrogen evolution from water splitting under visible light irradiation. The experimental results showed that the photocatalytic properties of FeCo-LDH/g-C 3 N 4 nanocomposites were superior to those of pristine g-C 3 N 4 . In addition, when the mass ratio of FeCo-LDH to g-C 3 N 4 was 7:100, the photocatalytic performance of the as-prepared FeCo-LDH(7 %)/g-C 3 N 4 is the optimal. The TC degradation rate of FeCo-LDH(7 %)/g-C 3 N 4 reached 78.0 % within 120 min, which was 2.63 times of that of pure g-C 3 N 4 . And the photocatalytic hydrogen evolution of FeCo-LDH(7 %)/g-C 3 N 4 was 107.28 μmol for 4 h, which was 12.68 times that of g-C 3 N 4 . The results showed that the as-prepared FeCo-LDH/g-C 3 N 4 nanocomposite photocatalysts have excellent performance in the degradation of TC and the photocatalytic H 2 evolution. Meanwhile, the EPR and trapping experiments revealed that OH and O 2 − played a main role in the photocatalytic TC degradation. The mechanism of photocatalytic TC degradation and hydrogen production of FeCo-LDH/g-C 3 N 4 nanocomposite photocatalysts was also discussed.
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