JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Lei Hou,Baolin Xing,Huihui Zeng,Weiwei Kang,Hui Guo,Song Cheng,Guangxu Huang,Yijun Cao,Zhengfei Chen,Chuanxiang Zhang
The utilization of mining wastes for value-added energy applications is vitally important in a clean and sustainable society. In this work, we report the preparation of nanostructured Si/C composites from a vermiculite waste via an aluminothermic reduction reaction. During the preparation process, chitosan is employed as the carbon source which can intercalate into the interspacing between the layers of vermiculate through cation exchange, which is the key to form a layered Si/C composite. Such obtained Si/C composites exhibit layered structure, large specific surface area, abundant nanopores , and minor SiO x and N components, thus having the merits of buffering volume expansion, good structure stability and high electrical conductivity . Finally, the Si/C composites are applied as anode for lithium-ion batteries and shows excellent specific capacity of ~948 mAh g −1 after 350 cycles at 1.0 A g −1 with a capacity retention of 85%, proving the applicability of such Si/C composite as an alternative to commercial graphite anode. This work not only provides a mild route for designing nanostructured Si/C composite anode materials , but also paves an innovative way for the reutilization of waste tailings for high value-added materials applications .
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Lingyi Zhao,Ruiqin Yang,Yi Wei,Yujing Guo,Qian Zhao,Hongwen Zhang,Weiping Cai
Rapid and flexible detection or accurate recognition of trace drugs is of great importance in cracking down on drug crimes, but it remains to be expected. Here, a solid chip is presented for the efficient detection and recognition of trace opioids (typically morphine) in aqueous solutions based on surface-enhanced Raman spectroscopy (SERS). Firstly, a Au-coated Si nano-cone array (Au-SNCA) is designed and fabricated via Si-based organic colloidal template etching and Au deposition. This Au-SNCA shows three-dimensional nanostructure with high densities of nanotips and deep nanogaps as well as high structural consistency, which exhibits strong SERS activity to morphine and outstanding stability. Then, such Au-SNCA is used as solid SERS chip to detect morphine in aqueous solutions. It has been demonstrated that using such solid chip, trace morphine in solutions could be recognized and detected within 1 min, and the detection limit is 10 -5 mg/mL (∼10 ppb), showing rapid and sensitive detection , which is much better than the previous reports. Meanwhile, the Au-SNCA chip also can be utilized to detect trace morphine in tap water and reservoir water, the recoveries range from 90.4% to 102.4%. Such excellent SERS performance of this Au-SNCA chip is attributed to its special structure which enhances not only local electromagnetic field but also molecular adsorption . The experimental results about the effects of immersion time and concentration show that the adsorption behavior of morphine molecules on such Au-SNCA chip can be explained by the pseudo-second-order kinetic model and Freundlich adsorption mode. Moreover, the Au-SNCA chip is also suitable for the identification of morphine homologues and the broad-spectrum detection of various common drugs. This study presents a practical solid chip and a simple approach for the efficient SERS detection and recognition of trace drugs in solutions. This is of significance to on-site detect drugs in forensic science.
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高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Enyou Zhao,Shiqiang Luo,Zhengxi Zhang,Nagahiro Saito,Li Yang,Shin-ichi Hirano
Silicon-based material have been considered as the most competitive candidate for next-generation anode in lithium-ion batteries (LIBs) due to its high specific energy density, natural abundance and attractive operating voltage. However, silicon-based anodes generally undergo significant volume changes and structural collapse during cycling, resulting in limited battery lifespan. Herein, a multi-strategy optimized in-situ gel electrolyte-binder system (GEBS) is rationally constructed, and electrochemical performances of the LIBs with Silicon-Graphite (Si-Gr) anodes are systematically evaluated by half-cell and full-cells. The in-situ generated polymer skeleton and improved interfacial compatibility of the GEBS effectively preserve the electrode structural integrity. Compared with the commercial liquid electrolyte , the volume change of the anode cycled with GEBS is suppressed from 208 % to 126 %. Benefiting from these merits, the full-cell with LiFePO 4 cathode displays stable cycling stability with the capacity retention of 96.8 % after 260 cycles. Besides, the reversible capacity of the LiNi 0.6 Co 0.2 Mn 0.2 O 2 ║Si-Gr full-cell is as high as 121.7 mAh g −1 after 200 cycles (capacity retention of 85.1 %), and the GEBS also exhibits obvious dominance at 55°C. This contribution effectively integrates multiple optimization strategies for Si-based anode and provides a feasible solution to address the challenge of its practical application in LIBs.
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Materials Today Communications
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2021
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IF 3.383
Jinzhao Guan,Kaiyu Xie,Aimin Liu,Zhongning Shi,Gong Chen,Miroslav Boca
In this study, Al–Si alloy, a precursor of the solar-grade silicon , was prepared via the aluminothermic reduction–molten salt electrolysis of SiO 2 in KF–AlF 3 molten salt by employing liquid aluminum as the working cathode. The reaction mechanism of the aluminothermic reduction of SiO 2 in KF–AlF 3 molten salt at 750 °C was determined by thermogravimetry–differential scanning calorimetry. The reaction rate equation for the aluminothermic reduction of SiO 2 in KF–AlF 3 molten salt was: d α dt = 7.156 × 10 24 e − 4.688 × 10 5 RT ( 1 − α ) 1.734 . In 49.4 wt% KF–47.6 wt% AlF 3 –3 wt% SiO 2 molten salt at 750 °C, the Si content in the Al–Si alloy obtained by the aluminothermic reduction–molten salt electrolysis of SiO 2 was 24.53 wt%. Compared with solely aluminothermic reduction of SiO 2 , the current efficiency in the process of the aluminothermic reduction–molten salt electrolysis of SiO 2 was evaluated. The results reveal that the Al–Si alloy is predominantly prepared in the aluminothermic reduction step, while supplemented by electrolysis. The calculated Faradic current efficiency of the proposed aluminothermic reduction–molten salt electrolysis process was 28.4%.
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Journal of Cleaner Production
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2021
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IF 9.297
Fengjiao Lai,Feng Yan,Pengju Wang,Fan Qu,Xuehua Shen,Zuotai Zhang
Efficient conversion of biomass-derived carbohydrates to alkyl levulinates is an important goal of biorefinery process, but is still challenging on applicable catalyst. Ce–Si pillared montmorillonite (CeSiM) clay heterostructures , incorporated with Wells-Dawson tungstophosphoric acid (H 6 P 2 W 18 O 64 , DPW), were prepared for the first time and used as the multifunctional catalyst for direct production of ethyl levulinate (EL) from various biomass-derived sugars. The DPW introduced by sol-gel method (DPW-CeSiM) has been effectively incorporated into the framework of porous CeSiM, while part of DPW was just absorbed on the surface of CeSiM by impregnation method (DPW-CeSiM-I). The DPW-CeSiM catalyst has large specific surface area owing to the insertion of Ce–Si pillars, and possesses strong Brønsted acidity and moderate Lewis acidity originated from the incorporated DPW and the Ce-doping, respectively. Due to the well synergistic effect of porous structure and dual acid, the DPW-CeSiM catalyst efficiently catalyzed the conversion of glucose into EL with 56.2% yield and nearly 100% conversion at 170 °C for 4 h. The recyclability studies certified that DPW-CeSiM catalyst showed higher stability than DPW-CeSiM-I over cycles and could be easily recovered from consecutive alcoholysis of biomass-derived sugars. The DPW-CeSiM catalyst also displayed high activity toward the conversion of other biomass-derived carbohydrates (fructose, sucrose, cellobiose and cellulose) into EL. Therefore, this work provides an instructive strategy for the design of efficient and stable DPW-based catalysts with dual acid sites uniformly distributed over the porous structure, which is obviously potential for industrial production of alkyl levulinates from carbohydrates and biomass.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
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2021
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IF 5.302
Chong He,Xinger Liu,Cong Ma,Yueqi Cao,Feng Hou,Liwen Yan,Anran Guo,Jiachen Liu
Nowadays, 3D polymer-derived silicon oxycarbide ceramics (SiOC) can be fabricated by the stereolithography method successfully. However, due to their intrinsically poor ceramic content and the large thermal shrinkage during the pyrolysis, it is difficult for the bulk 3D polysiloxane precursors to be pyrolyzed into dense 3D-ceramics. Herein, the ceramic content of the photocurable polysiloxane precursors was increased by adding a large amount of SiO 2 powders into the low solid content epoxy-acrylic siloxane. After being added with proper dispersant, the viscosity of the high solid loading polysiloxane/SiO 2 slurry can reach a proper level. Bulk 3D-silica ceramics with the wall-thickness around 8 mm can be conveniently fabricated from the polysiloxane/SiO 2 slurry by stereolithography and a two-step sintering process. The addition of a proper sintering aid NaF can promote the 3D-PSO/SiO 2 precursor to be converted into dense and crack-free 3D-silica ceramics with good mechanical proprieties.
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ACS Applied Materials & Interfaces
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2021
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IF 9.229
Hui Wang,Mouren Miao,Hui Li,Yuliang Cao,Hanxi Yang,Xinping Ai
Si is being actively developed as one of the most promising high-capacity anodes for next-generation lithium-ion batteries (LIBs). However, low cycling coulombic efficiency (CE) due to the repetitive growth of the solid electrolyte interphase (SEI) film is still an issue for its application in full batteries. Here, we propose a strategy to in situ form an artificial solid electrolyte interphase (ASEI) on the ferrosilicon/carbon (FeSi/C) anode surface by a purposely designed nucleophilic reaction of polysulfides with vinylene carbonate (VC) and fluoroethylene carbonate (FEC) molecules. The as-formed ASEI layer is mechanically dense and ionically conducting and therefore can effectively prevent the electrolyte infiltration and decomposition while allowing Li+ transport across, thus stabilizing the interface of the FeSi/C anode. As a result, the ASEI-modified FeSi/C anode exhibits a large reversible capacity of 1409.4 mA h g–1, an excellent cycling stability over 650 cycles, and a greatly elevated cycling CE of 99.8%, possibly serving as a high-capacity anode of LIBs.
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高影响因子
POLYMER INTERNATIONAL
·
2021
·Vol. 70
·期 12
·1668-1679
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IF 2.99
Jiarong He,Lingzhi Zhang,Haoxiang Zhong
Gum arabic grafted poly(acrylic acid) (GA- g -PAA) is synthesized as a mechanically robust water-soluble binder for silicon (Si) anodes in lithium-ion batteries by graft polymerization of acrylic acid onto GA backbone via a free radical reaction. 1 H NMR and Fourier transform infrared spectroscopies and thermogravimetric analysis are systematically conducted to confirm the grafting polymerization process. GA- g -PAA with different grafting length of PAA shows enhanced adhesion strength and excellent flexibility after grafting. Optimal Si-GA- g -8PAA electrode displays better cyclic stability, higher Coulombic efficiency and superior rate properties compared with a Si electrode with linear PAA binder. The Si-GA- g -8PAA electrode exhibits a high electrical conductivity, low interfacial/charge transfer resistance and high lithium-ion diffusion coefficient. GA- g -8PAA binder with grafted structure not only can maintain the mechanical and electrical integrity of the electrode, facilitating favorable electrochemical kinetics, but also assists in preserving a stable solid electrolyte interphase on Si surface upon long-term cycling. Such a facile strategy for designing a novel grafted binder shows potential for practical application on high-capacity anode materials with large volume change. © 2021 Society of Industrial Chemistry.
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ChemElectroChem
·
2020
·Vol. 7
·期 21
·4423-4430
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IF 4.154
Chao Yuan,Dujiang Lu,Yongling An,Xiufang Bian
Graphical Grind and coat : A novel nanocomposite of amorphous carbon-coated Si nanosphere and ZIF-67 derived hollow porous cobalt sulfide/carbon polyhedron is fabricated by a simple grinding process. ZIF-67 derived Co 9 S 8 /C can serve as a buffer to alleviate the volume expansion of Si. The vast conductive carbon layer originated from Co 9 S 8 /C and Si@C plays a key role in facilitating the electron transfer and lithium ion transport kinetics. Si@C−Co 9 S 8 /C anodes deliver improved electrochemical performance. Silicon (Si) is regarded as one of the most promising anode materials for lithium-ion batteries (LIBs) due to its high capacity and low working voltage. However, dramatic volume expansion and inferior electrical conductivity greatly impede the commercial use of Si anodes. Herein, we design and synthesize a novel nanocomposite of Si nanosphere coated by carbon (Si@C) and hollow porous Co 9 S 8 /C polyhedron (Si@C−Co 9 S 8 /C). The hollow porous Co 9 S 8 /C derived from Co-based zeolitic imidazolate framework can serve as a buffering matrix to accommodate the volume expansion of Si, which is beneficial to improve the cycle performance. The vast conductive carbon layer originated from Co 9 S 8 /C and Si@C plays a key role in accelerating the electron transfer and lithium ion transport kinetics, which can significantly enhance the rate performance. As a result, the Si@C−Co 9 S 8 /C anodes deliver stable cycle performance with a reversible capacity of 1399 mA h g −1 after 200 cycles at 100 mA g −1 , improved rate performance and high Coulombic efficiency. This simple route sheds light on designing Si-based composites for LIBs anodes.
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POLYMER
·
2021
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IF 4.43
Haoxiang Zhong,Jiarong He,Lingzhi Zhang
s Arabic gum grafted poly (acrylic acid) (GA- g -PAA) is prepared through a free radical graft polymerization of acrylic acid onto Arabic gum. Crosslinkable aqueous binder is developed by combining GA-g-PAA and branched polyols (pentaerythrotol, PER; triethanolamine , TEOA) as crosslinking agent for Si anodes of lithium-ion batteries. The aqueous composite binder undergoes crosslinking at about 110 °C to form robust crosslinked networks, matching well with the processing temperature of the electrode sheet in industry. GA-g-PAA/PER binder displays higher adhesion strength than GA-g-PAA and GA-g-PAA/TEOA. The Si electrode with GA-g-PAA/PER exhibits a slightly better cycling stability at 0.2C for 100 cycles, better rate capability than GA-g-PAA and GA-g-PAA/TEOA. At a high rate of 1C, Si electrode with GA-g-PAA/P delivers a higher specific capacity of 1968.1 mAhg −1 with a better capacity retention of 57.5% when compared with those with GA-g-PAA and GA-g-PAA/T binder.
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SOLAR ENERGY
·
2020
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IF 4.608
Yu Zhang,Ping Su,Linqing Liu,Pengfei Qiu,Li Su,Guangsheng Fu,Wei Yu
Achieving large Fermi energy splitting under illumination is critical for improving the performance of photovoltaic devices. In this work, we conducted the energy band structure modulation of MoS 2 thin films via MoO x doping scheme to realize its photovoltaic operation on n-type c-Si by magnetron sputtering. It is found that, by capping a MoO x overlayer, the MoS 2 electrons density decreased and the Fermi level shifted ~0.4 eV towards valence band, consequently the MoS 2 conductive type changing. With this doped MoS 2 layer, the built-in electric field of fabricated MoS 2 /n-Si heterojunction devices greatly improved and exceeded 400 mV owing to the larger interface energy-level differences. Meanwhile, the defects recombination losses reduced benefiting from the holes-selective behavior of O-deficiencies in MoO x , so that the photo-generated carriers extraction process were promoted. As a result, the doped MoS 2 /n-Si devices showed excellent rectification behavior with rectifying ratio to 10 5 and ideality of 1.12. The TRPL spectrums corroborated the enhanced carrier transport mechanism at MoS 2 /n-Si interface by MoO x modulation doping effect. Correspondingly, the significant improvement of doped MoS 2 /n-Si solar cells performance (V oc of 289 mV, FF of 60.72% and J sc of 31.25 mA/cm 2 ) was achieved, exhibiting an optimized conversion efficiency of 5.47%. The UPS analysis revealed that the doping mechanism of MoO x /MoS 2 stacks lies in energy band overlap and electrons contact transfer between these two materials. This observation of MoO x modulation doping effect on large-area sputtering MoS 2 could help in building a better interface carrier transport in photovoltaic and optoelectronic applications of 2D materials.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2020
·Vol. 34
·期 6
·e5612
·
IF 3.14
Na Zhang,Jiaqi Bu,Yong Meng,Jia Wan,Lu Yuan,Xin Peng
In this study, Ti-Si-Sn-Sb/GAC particle electrodes were prepared by sol–gel method. The particle electrodes were characterized by SEM, XRD, EDX, and BET then used to carry out three-dimensional (3D) electrocatalytic oxidation degradation on simulated refractory p-aminophenol (PAP) wastewater. The effects of initial pH, cell voltage, aeration flow rate and initial PAP concentration on degradation experiments were investigated. Under the optimal conditions, the PAP and COD removal rates were 89.45% and 75.17% respectively. In addition, the possible degradation mechanism of PAP was further investigated by UV–Vis and HPLC. Finally, it was found that the Ti-Si-Sn-Sb/GAC particle electrodes with high catalytic activity and excellent stability could significantly improve the PAP wastewater removal efficiency.
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