ELECTROCHIMICA ACTA
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2021
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IF 6.901
Hongcheng Gao,Shihao Miao,Mengqin Shi,Xiaoxia Mao,Xiaojing Zhu
Low redox kinetics and shuttle effect of polysulfides (PSs) is a grand challenge for practical applications of lithium-sulfur (Li-S) batteries. Herein, cobalt (Co) nanoparticles embedded inside nitrogen (N)-doped hierarchical porous carbon (MgCo-HC) are prepared via one-pot approach. As a result, MgCo-HC unique structure with the large surface area and Co, N-doping is proposed for the strong physical/chemical adsorption of PSs, high conductivity, fast redox reaction kinetics and the high S utilization. The resultant S cathode delivers a high specific capacity of 1086.4 mA h/g at 0.1 C, low-capacity fading rate of 0.041% per cycle over 880 cycles at 2 C, and superior rate performance up to 5 C. More intriguingly, the S/MgCo-HC electrode delivers reversible area capacities of 5.1 and 5.5 mA h/cm 2 at 0.1 C under high S loading and learn electrolyte condition, respectively. Furthermore, the assembled Li-S soft-packaged battery is also readily assembled, which highlights stable electrochemical properties under folding conditions. This work provides a simple strategy to design advanced S hosts for the practical application of Li-S batteries with excellent electrochemical performance.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Long Huang,Linzhi Zuo,Tao Yu,Haoquan Wang,Zeyang He,Hu Zhou,Shichuan Su,Ting Bian
Substituting costly Pt-based oxygen reduction reaction (ORR) catalysts with highly active and stable non-precious metal catalysts is a great challenge in zinc-air batteries. Herein, we fabricated Co/Co 9 S 8 nanoparticles decorated nitrogen, sulfur dual-doped carbon leaves (Co/Co 9 S 8 -NCL) with outstanding ORR performance by pyrolysis of dithiooxamide (DTO) molecule modified two-dimensional (2D) leaf-shaped zeolitic imidazolate framework (ZIF-L). The functionality of DTO simultaneously optimizes 2D nanostructure and component (S doping) by the confinement effect due to the coordination interaction between S atoms of DTO and Co 2+ in ZIF-L. Benefiting from the synergistic effect between Co-N x sites and Co/Co 9 S 8 species coupled with unique two-dimensional N, S-codoped carbon leaves, the resulting Co/Co 9 S 8 -NCL-30 exhibits a remarkable ORR activity with a half-wave potential of 0.852 V comparable to Pt/C (0.843 V) and outstanding long-term stability. Impressively, the Zn-air battery with Co/Co 9 S 8 -NCL-30 achieves high power density of 112 mW cm −2 and specific capacity of 799 mAh g −1 Zn . This work will present a new pathway to prepare highly active and durable 2D transition metal-based carbon nanomaterials in zinc-air batteries.
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NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 46
·期 5
·2309-2319
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IF 3.591
Yichen Jiang,Yifei Zhao,Lin Liang,Xiao Zhang,Jianmin Sun
Imidazolium-based ionic liquid 1,n-dialkyl-3,3′-bis-1-vinyl imidazolium dibromide (n = 2, 4 and 6) monomers were synthesized and further polymerized inside a MIL-101 framework to afford poly(ionic liquid)@MIL-101 composites (PIL-n@MIL-101, n = 2, 4 and 6). Furthermore, the ratio of poly(ionic liquid) to MIL-101 affected the structures of the composites. Different molar ratios of PIL-4/MIL-101 were prepared and characterized using elemental analysis, powder X-ray diffractometry, thermogravimetric measurements, N2 adsorption/desorption and CO2 adsorption measurements. Thanks to the high Brunauer–Emmett–Teller surface area and porous structure of MIL-101 together with the incorporated poly(ionic liquid), PIL-4@MIL-101-0.5 exhibited good CO2 uptake capacity (42.7 cm3 g−1 at 100 kPa, 273 K). Additionally, due to the synergistic effects of the unsaturated coordinated Lewis acidic Cr sites and nucleophilic Br− in the PIL-4@MIL-101 composites, the developed composites exhibited efficient catalytic performance in the CO2 and epichlorohydrin cycloaddition reaction, with 99.6% conversion obtained at 90 °C and 1.0 MPa for 2.5 h without an additional cocatalyst or solvent. The composites also showed easy separation and better recycling stability. Combining the advantages of facile synthesis, excellent performance for CO2 adsorption and conversion, good thermal stability and recycling stabilities, the poly(ionic liquid)@MIL-101 composites are appealing candidates for application in CO2 capture and utilization.
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BIOMASS & BIOENERGY
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2021
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IF 5.061
Jingyue Wang,Yuelong Xu,Meifang Yan,Bin Ren,Xiaoxi Dong,Junfeng Miao,Lihui Zhang,Xinqiang Zhao,Zhenfa Liu
Porous biomass-carbon materials for supercapacitor applications have recently attracted attention. Chitin , which has abundant amides and hydroxyl groups, was used as an ideal precursor for carbon in this work. The chitin was treated with a one-step method to produce a heteroatom-loaded porous carbon material, and its electrochemical properties were significantly improved through the introduction of loaded elements. A mixture of chitin, zinc chloride , and heteroatoms was carbonized to obtain heteroatoms (N and S) and the bimetallic sulfide loaded hierarchical porous carbon. Then, the porous carbon with S, N, Zn, and Fe heteroatoms loading was used to prepare a supercapacitor with a specific capacitance of 277.4 F g −1 at 1 A g −1 . In addition, the supercapacitor had a specific capacitance retention rate of 90% at 5 A g −1 after 10,000 cycles. Therefore, hierarchical porous carbon materials loaded with heteroatoms and bimetallic sulfide were prepared by carbonization activation with chitin as the precursor. The resulting supercapacitor showed that the as-prepared porous biomass materials possessed ideal charging-discharging performance. Moreover, this work provides strategies for obtaining metal sulfides and heteroatom co-loading of carbon materials with excellent properties using a simple and efficient one-step method for renewable energy storage device applications.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Yang Chen,Huijing Cui,Mao Wang,Xudong Yang,Shujie Pang
Cr(VI) is a toxic heavy metal, which is not readily decomposed and ingested by bacteria. Therefore, there is an urgent need for a sensing method with high selectivity and high sensitivity to detect Cr(VI) in other widely distributed metal ions . Here, a fluorescent probe based on carbon dots (CDs) was developed, with the characteristics of low cost, low environmental impact, high stability, and good water solubility. Although many sensors have been reported for the detection of Cr(VI), most of them are based on the quenching fluorescence method , whereas the one reported here is based on fluorescence enhancement, for which o-phenylenediamine and dl -Thioctic acid were used as raw materials. The transmission electron microscopy , Fourier infrared spectroscopy , X-ray photoelectron spectroscopy, X-ray diffraction, and ultraviolet-visible spectroscopy measurements showed that Cr(VI) can significantly enhance the fluorescence of the probe compared to previous sensors, as the obtained CDs have excellent fluorescence properties (quantum yield up to 21.82%) and high light stability. The detection limit of the probe for Cr(VI) is as low as 0.64 μM, indicating that the developed probe can detect Cr(VI) quickly, sensitively, and selectively, and has broad application prospects in environmental analysis applications. To facilitate rapid detection of Cr(VI), the CDs were also incorporated into a fluorescent composite film suitable for visual inspection.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Zhenzong Zhang,Yuxin Cao,Fenghao Zhang,Wenjie Li,Yuanling Li,Han Yu,Meiyang Wang,Hongbing Yu
A novel S-scheme photocatalytic heterojunction composite nanomaterial is developed by integrating zero-dimensional WO 3 quantum dots (WQDs) on two-dimensional ultrathin CdIn 2 S 4 (CIS) nanosheets with the aim of fostering carrier separation, enhancing the performance of carrier interface transport, minimizing carrier distance transport, and achieving effective photocatalytic CO 2 reduction. The composite photocatalyst WQDs/CdIn 2 S 4 (WCIS) allows for the efficient photocatalytic reduction of CO 2 to CO and CH 4 , as shown by product analysis and isotopic measurement. The photogenerated electrons in WQDs recombine with the holes in CIS nanosheets, and the left electrons in CIS have stronger CO 2 reduction abilities. The highest yields of CO and CH 4 achieved with the WCIS photocatalyst are 8.2 and 1.6 μmol g -1 h −1 ––2.6 and 8 times higher than those for CIS, respectively. Moreover, the S-scheme WCIS possesses a stable crystal structure and recycling ability. Finally, the S-scheme charge transfer path on the WCIS composite is proposed according to theoretical calculation, in-situ irradiated X-ray photoelectron spectroscopy, and electron paramagnetic resonance (ESR) analyses.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Lin Zhang,Lei Xing,Jie Liu,Tieyue Qi,Meng Li,Lidong Wang
Cobalt-based catalysts can promote sulfite oxidation to recover the valuable byproducts formed during wet magnesia desulfurization. However, Hg(II) in the desulfurization slurry degrades the quality of reclaimed products and poses considerable environmental risk. Here, a bifunctional sulfur-doped catalyst/adsorbent, Co-TUD-1/S, is prepared through one-pot synthesis, in which the sulfur site is designed for trapping aqueous Hg 2+ . The catalytic rate of Co-TUD-1/S for MgSO 3 is 0.083 mmol/L/S, which is 10.4 times of that under non-catalytic condition, the removal efficiency of Hg 2+ is higher than 90%. The isothermal models and kinetic models for the adsorption of Hg 2+ are well-fitted to the Langmuir model and pseudo-second-order model, respectively, and the maximum adsorption capacity of experimental data is 96 mg/g. The characterization results confirm that Co 3 O 4 is functioned as the active catalysis site, and the formation of S–Hg bonds plays a crucial role in Hg 2+ capture. Density functional theory calculations reveal that the Co site is more likely to combine with sulfite rather than Hg 2+ , which reduces the interference of absorbed Hg 2+ on the catalytic activity of Co. Specialization and cooperation between the catalysis site of –Co and adsorption site of –S are realized. The results reveal that the use of Co-TUD-1/S is a feasible strategy for improving wet desulfurization efficiency.
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EUROPEAN POLYMER JOURNAL
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2021
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IF 4.598
Zhenghui Yang,Pingchuan Ma,Furong Li,Haiquan Guo,Chuanqing Kang,Lianxun Gao
The flexibility of organic light-emitting diode (OLED) displays highly depends on the properties of the flexible substrates. In this paper, a series of aromatic polyimides have been fabricated via the copolycondensation of pyromellitic dianhydride (PMDA), the two different rigid heterocyclic diamines, 2,5-bis(4-aminophenyl)pyrimidine (PRM) or 2,5-bis(4-aminophenyl)pyridine (PRD), and another flexible diamine, 4,4′-oxydianiline (ODA). The performance of the polyimide films could be systematically tailored by means of adjusting the main-chain rigidity, as well as the close packing and orientation of polymer chains by the formation of the intermolecular hydrogen bonds between poly(amic acid)s. The optimal results (PIb-4, PIb-5, PIc-2) showed that the polyimides were endowed with ultra-high glass transition temperature (T g ) exceeding 450 °C, low coefficient of thermal expansion (CTE) at 0–5 ppm K −1 and excellent thermal stability (T d5% = 570–590 °C). Meanwhile, all of them exhibited sufficient flexibility, the elongation at break at of 40–60%, extremely high tensile strength of 250–380 MPa and modulus of 4.1–6.1 GPa. Hence, the polyimide films should be the promising candidates for application as the polymer substrates for flexible OLED displays.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Hongbo Wang,Wangfeng Cai,Leqiu He,Manlin Zhu,Yan Wang
Successful synthesis of novel multi-component metal composites with a unique structure can effectively promote the electrochemical performance improvement of supercapacitors . Herein, three-dimensional (3D) ZnCo 2 O 4 @NiCoMn-S(denoted as ZnCo 2 O 4 @NxCyMzS-X, x, y and z refer to the element content ratio, X refers to the number of cycles) arrays growing on nickel foam (NF) were synthesized with facile hydrothermal and electrodeposition processes. The structure of samples is regulated with the molar content of Ni/Mn ions and deposition time in electrodeposition . ZnCo 2 O 4 @N1C2M1S-4 with optimal hierarchical structure shows a high area capacity of 7.04 C·cm −2 under 2 mA·cm −2 (1671 C·g −1 at 1.1 A·g −1 ) and cycle retention rate of 76.48% after 3000 cycles under 50 mA·cm −2 . Furthermore, a ZnCo 2 O 4 @N1C2M1S-4//Active Carbon (AC) hybrid supercapacitor (HSC) was assembled to test the practical application of ZnCo 2 O 4 @N1C2M1S. It is shown the voltage window of HSC achieves as high as 1.9 V, and it reveals a high energy density of 64.36 Wh·kg −1 under a power density of 0.95 kW·kg −1 along with great stability with 75% retention at 5 A·g −1 after 5000 cycles, showing a broad prospect in the field of energy storage. At the time, this study provides a reference for material structure design.
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ACS Applied Materials & Interfaces
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2021
·
IF 9.229
Yu Wang,Haifeng Ji,Xiaojie Zhang,Jingjing Shi,Xiaona Li,Xiaoxia Jiang,Xiongwei Qu
Cyclopropenium cationic-based covalent organic polymer (iCP@TFSI) was successfully prepared through the SN2 reaction and ion replacement process, which can be incorporated into the PEO/LiTFSI matrix as a filler. The obtained solid-state polymer electrolytes were utilized for an all-solid-state lithium–sulfur (Li–S) battery. Padding iCP@TFSI into the PEO matrix not only has a positive influence on both the ionic conductivity and the mechanical capacity of solid-state polymer electrolytes but also increases the stability of the lithium metal anode, which essentially improves the overall cycling ability of all-solid-state Li–S batteries. Among the membranes attained, the PEO-10%iCP@TFSI electrolyte displays the best ionic conductivity up to 1.2 × 10–3 S·cm–1 at 80 °C. The symmetrical lithium battery exhibits higher cycle stability (600 h) due to the higher mechanical properties related to more stable lithium metal interfaces. The Li–S battery based on the PEO-10%iCP@TFSI electrolyte exhibits excellent electrochemical performance with better Coulombic efficiency and outstanding cycling stability. Its capacity is maintained at 490 mAh·g–1 after 500 cycles at 1 C with a 0.032% decay rate each cycle, and the Coulombic efficiency is close to 100% during the whole cycling.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
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IF 7.312
Ping Sun,Hui Liu,Mingbao Feng,Xuesheng Zhang,Yingsen Fang,Zhicai Zhai,Virender K. Sharma
This work demonstrates for the first time the potential application of a novel nonradical oxidation system consisting of N/S co-doped ordered mesoporous carbon (NS-CMK-3) and peroxymonosulfate (PMS). The results showed that the NS-CMK-3 catalyst effectively activated PMS to completely degrade pharmaceutical acetaminophen (ACT). The catalytic performance of NS-CMK-3 was ~20 and 10 times better than that of pristine CMK-3 and single N-doped one (N-CMK-3), respectively. The oxidative system could also remove other pollutants (i.e., sulfathiazole, trans -ferulic acid, orange G, and phenol). A higher content of N (5.3 at.%) and a distribution of graphite-N (28.1%) were determined in NS-CMK-3 than in N-CMK-3. The synergistic effect of N/S co-doping (i.e., graphite-N and thiophene-S) resulted in the enhanced catalytic performance. The activation of PMS by NS-CMK-3 primarily followed two nonradical pathways (i.e., singlet oxygen and catalyst surface-bound reactive PMS complexes), supported by quenching experiments and electron paramagnetic resonance measurements. The p -benzoquinone ( p -BQ) and ACTdimer were main degradation products. The removal of total organic carbon (TOC) was ≈27%, suggesting nonradicals could mineralize ACT. The NS-CMK-3 not only demonstrated superior stability owing to a removal efficiency that was still as high as 98% in the fifth recycle run, but also significantly decreased the potential effects of water constituents (e.g., Cl − , NO 3 − , HCO 3 − , and humic acid) on the removal process. The NS-CMK-3/PMS oxidative system offers a novel strategy to carry out environmental remediation via nonradical processes.
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INTERNATIONAL JOURNAL OF PHARMACEUTICS
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2021
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IF 5.875
Liping Wang,Xuhui She,Zhi Chen,Sisi Quan,Yingtao Liu,Xiaoman Mai,Tiefeng Yuan,Huajun Fan
A novel molecularly imprinted polymer (MIP) with chiral recognition affinity to S-sulpiride (S-SUL) enantiomer was prepared by using newly synthesized N-acryloyl-tryptophan (ATrp) as function monomer , S-SUL as the template molecule, and ethyleneglycol dimethacrylate (EGDMA) as the cross linker. Under the optimized synthesis conditions, the MIP was synthesized by bulk polymerization according to the molar ratio of 1:4 of S-SUL to ATrp, and structurally characterized by Fourier transform infrared spectroscopy (FT-IR), scanning electron microscope (SEM) and laser particle analysis. The results illustrated that the MIP offered uniform, loose and porous structure. The adsorption performance of the MIP was evaluated by the isotherm and kinetic models, and the adsorption isotherm conformed to the Freundlich model. The maximum adsorption capacity, selectivity factor and enantioselectivity coefficient to S-SUL were respectively 226.2389 µmol/g, 2.34 and 11.66. Based on the chiral recognition specificity, the drug release experiments demonstrated that the MIP as controlled and sustained release carrier could inhibit the release rate of S-enantiomer compared to the tablet without the MIP, exhibiting the potential of the MIP synthesized in chiral drug delivery.
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