ACS Applied Energy Materials
·
2022
·
IF 6.959
Yang Chen,Shujian Liu,Shaokai Cheng,Shuyu Gao,Jingchao Chai,Qiuyue Jiang,Zhihong Liu,Xueqing Liu,Jiyan Liu,Ming Xie,Wubin Dai
The polyvinylidene fluoride (PVdF) binder is the classic binder for cathodes because of its excellent electrochemical stability and superior adhesion property. However, PVdF is very expensive and sensitive to moisture. Therefore, pursuit of a cost-effective binder is highly desirable, especially for high-voltage cathode application. Polyacrylonitrile (PAN) possesses strong polar C≡N groups, endowing it with oxidation resistance and strong binding properties. Herein, the PAN binder was systematically investigated for the electrochemical performance of the 4.5 V high-voltage LiCoO2 (HV-LCO) electrode. The results showed that the HV-LCO-PAN electrode delivered superior rate capability and cycling stability to the corresponding HV-LCO-PVdF. The PAN binder was highly tolerant of moisture and was capable of forming uniform coating on the cathode materials. Moreover, the PAN binder had ultrahigh mechanical modulus (8.01 GPa) and hardness (381.45 MPa) in a liquid electrolyte, thereby improving cycling stability and rate capability. X-ray photoelectron spectroscopy analysis further demonstrated that PAN formed uniform coating on the surface of LiCoO2 and played a role of an artificial cathode–electrolyte interphase layer, suppressing decomposition of the liquid electrolyte under high cutoff voltage.
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Small Structures
·
2022
·Vol. 4
·期 1
·2200161
·
IF 11.343
Lu Chen,Youbing Li,Ke Chen,Xiaojing Bai,Mian Li,Shiyu Du,Zhifang Chai,Qing Huang
Entropy stabilization is an effective method to design and explore MAX phases with outstanding properties via tuning constituent elements and crystal structures, which have received considerable critical attention. Currently, some medium-/high-entropy (ME/HE) MAX phases, whose A layers are composed of Al, S, and magnetic elements, are reported, while few discussions about ME/HE-MAX phases with other A elements (e.g., Sn) are conducted. Herein, fully dense ME/HE-MAX phase bulks ((TiVNb) 2 SnC, (TiVNbZr) 2 SnC, and (TiVNbZrHf) 2 SnC) are designed and synthesized because of the chemical diversity of MAX phases. The results of Rietveld refinement of X-ray diffraction, scanning electron microscopy, and high-resolution scanning transmission electron microscopy-affiliated energy-dispersive spectrometer analysis comprehensively verify the crystal structure of ME/HE-MAX phases. Both the electrical conductivity and the charge carrier mobility are significantly lower than the reported correlation ternary MAX phases, due to the electron scattering and structural defects in ME/HE-MAX phase crystal structures. Similarly, the electron contribution of thermal conductivity is gradually declining; on the contrary, the phonon plays an increasingly dominant role as temperature increases. Owing to the richness in composition of MAX phases, herein, a composition design route for discovering new MAX phases and tuning their properties is indicated.
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CRYSTENGCOMM
·
2021
·Vol. 23
·期 38
·6668-6674
·
IF 3.545
Xianpei Ren,Qingbo Wei,Fei Wu,Yonghua Wang,Qiang Li
Transition metal sulfides, such as molybdenum sulfide and vanadium sulfide, have recently attracted substantial attention due to their potential application to the catalysis of the hydrogen evolution reaction (HER). Alloying is one of the powerful methods to exceed the intrinsic properties of pure metals. In this study, we report a simple one-step sintering method to synthesize MoS2, V1.5S2 and V–Mo–S alloys on carbon nanotubes (CNT/VMoS). Due to its compositional, morphological and electrical superiorities, the CNT/VMoS-2 catalyst recorded the optimal HER activity with a low overpotential of −146 mV at 10 mA cm−2, a low Tafel slope of 61 mV dec−1 and a very small Rct value of 8.8 Ω, which were superior to CNT/MoS2, CNT/V1.5S2 and other CNT/VMoS catalysts in acidic media, holding a great promise for practical water-splitting applications. We believe that the present work could broaden our horizon about the preparation of other transition metal sulfide alloys and provide a platform to understand the fundamental catalytic mechanism for improving HER performance.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Chunkai Huang,Zhiquan Xiang,Jincan Huang,Guangbing Liu,Xuemin Yu,Weijing Liu,Haijin Cao
Significant amounts of Sb(III) and Sb(V) are present in printing and dyeing wastewater (PDW), which leads to the detrimental effects on the environment if not treated properly. In this paper, the adsorptive removal of Sb(III) and Sb(V) by TiCl 4 derived flocs and the oxidation process were investigated. The results showed that TiCl 4 conducted superior coagulation performance on Sb(III) removal than Sb(V) in terms of dosage, pH range and immunity to interference. When the dosage was 50 mg/L and the final pH was 5.0, the concentration of Sb(III) and Sb(V) was reduced from 2000 μg/L to 100 μg/L and 180 μg/L, respectively. According to the Langmuir model, The adsorption for Sb(III) (74.27 mg/g) by TiCl 4 derived flocs was higher than Sb(V) (68.45 mg/g). The Sb(III) in the solution could partially inhibit the adsorption of Sb(V). It was also observed that the Sb(III) was oxidized to Sb(V), which was owing to the molecular oxygen during the coagulation and the flocs might act as catalyst. The actual printing and dyeing wastewater treatment experiments results showed that pre-reduction of Sb(V) to Sb(Ⅲ) could considerably improve the total Sb removal from 83 % to 98.8 %. The characterization results, such as zeta potential and x-ray photoelectron spectroscopy (XPS), indicated that the Sb(Ⅲ) removal was mainly achieved by chemisorption. The Sb(V) removal was mainly dependent on chemisorption and electrostatic adsorption, while the latter contributed more than former. The results of DFT calculations explained the reason for higher removal efficiencies of Sb(III) than Sb(V) in the TiCl 4 coagulation system. This study provides a new idea for the efficient removal of Sb(III) and Sb(V) using TiCl 4 in PDW to save the cost in engineering practice.
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Nano-Micro Letters
·
2025
·Vol. 17
·期 1
·1-20
·
IF 36.3
Mu Yongbiao,Liao Zifan,Chu Youqi,Zhang Qing,Zou Lingfeng,Yang Lin,Feng Yitian,Ren Haixiang,Han Meisheng,Zeng Lin
High-voltage lithium (Li) metal batteries (LMBs) face substantial challenges, including Li dendrite growth and instability in high-voltage cathodes such as LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NCM811), which impede their practical applications and long-term stability. To address these challenges, tris(pentafluorophenyl)borane additive as an electron acceptor is introduced into an ethyl methyl carbonate/fluoroethylene carbonate-based electrolyte. This approach effectively engineers robust dual interfaces on the Li metal anode and the NCM811 cathode, thereby mitigating dendritic growth of Li and enhancing the stability of the cathode. This additive-driven strategy enables LMBs to operate at ultra-high voltages up to 4.7 V. Consequently, Li||Cu cells achieve a coulombic efficiency of 98.96%, and Li||Li symmetric cells extend their cycle life to an impressive 4000 h. Li||NCM811 full cells maintain a high capacity retention of 87.8% after 100 cycles at 4.7 V. Additionally, Li||LNMO full cells exhibit exceptional rate capability, delivering 132.2 mAh g −1 at 10 C and retaining 95.0% capacity after 250 cycles at 1 C and 5 V. As a result, NCM811||graphite pouch cells maintain a 93.4% capacity retention after 1100 cycles at 1 C. These findings underscore the efficacy of additive engineering in addressing Li dendrite formation and instability of cathode under high voltage, thereby paving the road for durable, high-performance LMBs.
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高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Jinping Mu,Aijia Wei,Xiaohui Li,Rui He,Lijing Sun,Peizhao Liu,Xue Bai,Lihui Zhang,Xi Zhang,Zhenfa Liu,Jing Gao
Tris (trimethylsilyl) phosphate (TMSP) and tris(2,2,2-trifluoroethyl) phosphate (TTFP) was added to carbonate solvent-based electrolytes as dual-additives to enhance the performance of LiNi 0·5 Mn 1·5 O 4 (LNMO). The X-ray photoelectron spectroscopy results revealed that both TMSP with high oxidation ability and TTFP with high oxidation resistance participated in the formation of cathode–electrolyte interphase (CEI) films. Electrochemical impedance spectroscopy confirmed that the constructed CEI films had excellent electronic insulation and ionic conductivity , reducing the interfacial impedance of the LNMO electrode, and improving the electrochemical performance of LNMO/Li half-cells and LNMO/Li 4 Ti 5 O 12 full-cells. As measured by the nuclear magnetic resonance , the incorporation of TMSP and TTFP significantly reduced the HF content in the electrolytes. Therefore, both LNMO/Li half-cells (500 cycles with 95.7% capacity retention) and LNMO/Li 4 Ti 5 O 12 full-cells (200 cycles with 79.9% capacity retention) displayed higher cycling stabilities at 5 C owing to the synergistic effect of TMSP and TTFP. In comparison, capacity retentions of ∼76.5% after 500 cycles and ∼37.2% after 200 cycles were respectively achieved for the LNMO/Li half-cells and LNMO/Li 4 Ti 5 O 12 full-cells with the standard electrolyte at 5 C. This study provides strong evidence that additive combinations can improve the electrochemical performance of high-energy and high-voltage cathode materials .
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FUEL
·
2024
·
IF 6.7
Lingrui Cui,Xu Liu,Mannian Ren,Jun Xu,Fahai Cao
Nickel and vanadium in crude oil adversely affects the quality of petroleum coke and refining process. Polymer brushes bearing high-density ligands have shown promising nickel removal ability. In this work, submicron polybutadiene (PB) grafted by aminodithio- carbamate acrylamide (PAMDTC@PB) was prepared and characterized by the infrared spectroscopy, dynamic light scattering, and elemental analysis. Based on results of molecular simulation, PAMDTC was selected as ligand molecule at first. Then the nickel and vanadium removal rates by PAMDTC@PB and traditional polyacrylic acid brushes (PAA@PB) were evaluated through the electric desalination process, both in the model and real oil samples. The result shows that S atom in AMDTC is most likely to chelate with metal porphyrin compounds and AMDTC molecule presents highest chelating activity. Compared with PAA@PB, the removal rate of Ni and V porphyrin compounds with the aid of PAMDTC@PB increases significantly, with an optimized removal rate of 46.91 % and 56.81 %. To achieve better metal removal efficiency and higher utilization rate of prepared polymer brushes, sodium dimethyl dithiocarbamate (SDD) is introduced into the electric desalination process as a adjuvant. The results indicate that the addition of SDD leads to a increment of 10–30 % to the removal rate of Ni and V and a reduction of brush dosage by 200–400 ppm in the electric desalination process, exhibiting great potential of industrial applications of novel desalination process with adjuvant.
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Advanced Energy Materials
·
2024
·
IF 24.4
Yu Chen,Jiajun He,Chengwei Ye,Shaochun Tang
Evaporative hydrovoltaic generators hold significant potential for alleviating water-energy crisis, but low output voltage configurations due to the slow phase transition rate of water molecules and the intricate nature of integration limit their applications. Herein, a lotus-inspired interfacial evaporation-driven hydrovoltaic generators (IEHVG) is developed for efficient generation of water vapor and electricity from seawater instead of freshwater and achieves an ultrahigh voltage output higher than 100-volt level through forested IEHVG integration. The biomimetic hydrogel is developed with specific liquid transport channels, graphene quantum dots/MXene nanocomposites, and gradient hydrophobic interface for highly enhanced photothermal evaporation and electricity generation by mimicking the transpiration process of a “stems-leaves of lotus”. The synergistic thermodiffusion effect leads to the output power density of IEHVG reaches up to 45.6 µW cm −2 and can power electronic devices or charge commercial supercapacitors. The freshwater-electricity cogeneration integrated system consisting of 192 IEHVG units can harvest a record-breaking voltage reaching 105 V and a high freshwater harvesting rate up to 2.0 L m −2 h −1 from seawater in a well-lit outdoor area. This work demonstrates that IEHVG offers a novel concept for modular freshwater and high-voltage power sources access on offshore work platforms.
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ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Zhengping Ding,Ran Song,Yu Shen,Huahui Lin,Peng Wei,Xiangqun Zhuge,Ke Qu,Zhenzhong Yang,Yurong Ren
Combining a high cut-off voltage cathode with a high specific-capacity lithium metal anode offers a promising path toward ultra-high-energy-density batteries (> 400 Wh kg -1 ). However, the practical application of LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811)||Li batteries with a 4.5 V cut-off voltage is challenged by severe interface deterioration. This study introduces a novel bifunctional electrolyte additive called 2,2,2-Trifluoroethyl Nonafluorobutanesulfonate (TNS), designed to form a thin, robust electrolyte interface layer on both cathode and anode surfaces. Detailed analysis reveals that TNS decomposes and modifies the solid-electrolyte-interface layer. Through the synergistic effects of fluoride and sulfonate functional groups, the resulting cathode-electrolyte-interface (CEI) enhances the structural stability of NCM811 while providing a high-efficiency lithium-ion transport channel to accelerate Li + insertion and extraction. At a cut-off voltage of 4.5 V, NCM811||Li batteries with 1 % TNS (by weight) exhibit high discharge capacity retention of 74.2 % after 150 cycles at a 1C rate and 60.1 % after 150 cycles at a 2C rate. This study offers valuable insights for designing high-voltage electrolyte additives in ultra-high-energy-density lithium metal batteries.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2024
·
IF 8
Na Liu,Ruili Gao,Jingjing Guo,Longwei Fu,Bin Xue,Kun Ma,Chen Lin
The environmental impact of arsenic (As) pollution has been a focal point within environmental science. In arsenic-polluted saline-alkali environment, the addition of exogenous biochar can affect the morphological transformation of As both through direct and indirect mechanisms, with calcium ions (Ca(II)) playing a crucial role. This study investigates the immobilization mechanisms of undissolved biochar (UOB) and dissolved biochar (DOB) on As(V) in the absence and presence of Ca(II) under alkaline conditions and aerobic atmosphere. While UOB and DOB alone are insufficient for As(V) immobilization, their combined action in the presence of Ca(II) achieves remarkable immobilization rates of 91.9% and 98.1%, respectively. Precipitation of calcium arsenate is identified as the primary immobilization pathway in both the UOB-Ca(II)-As(V) and DOB-Ca(II)-As(V) systems. Furthermore, Ca(II) acts as a mediator for As(V) immobilization through the formation of ternary UOB/DOB-Ca-As complexes, which are corroborated by Density Functional Theory (DFT) analysis from a microscopic perspective. Notably, the synergistic immobilization of As by DOB and newly generated CaCO 3 in DOB-Ca(II)-As(V) system is highlighted. Additionally, the increase in Ca(II) concentration (0–100 mM) and solution pH (9.0–12.0) both significantly enhance the immobilization of As(V). An increase in the dosage of UOB (0.4–4 g/L) reduces the immobilization of As(V), while effect of the DOB concentration is insignificant. This study provides new insights into how the release of two biochar fractions into a typical Ca(II)-rich saline-alkali environment may alter the fate and transport of As species.
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高影响因子
Inorganic Chemistry Frontiers
·
2024
·
IF 6.1
Qixian Ren,Wangfei Che,Mengmeng Chen,Chen Cui,Yabo Wu,Zhi Su
Thioantimonates containing high oxidation state Sb5+ have been proven to exhibit excellent performance in the design of new materials such as infrared optical crystals and lithium-ion batteries. However, as described by the “inert pair effect”, the preparation of P-block elements containing high oxidation states in sealed systems has been a challenge. In this study, an aliovalent cation substitution strategy was used to design and synthesize three novel thioantimonates(V), A4BaSb2Se8 (A = Cs, Rb) and Rb2BaSbS4Cl (RBSSC), respectively, all of which contain rare [SbS4] tetrahedral units. The introduction of Ba2+ ions leads to the distortion and high-density arrangement of [SbSe4] units, which is manifested as a significant 3.7 times enhancement of the birefringence compared to that of the parent compound Cs3SbSe4 (0.041 → Cs4BaSb2Se8 0.150@1064 nm). By further introducing highly electronegative halogen atoms, the first antimony-based thiohalide(V) RBSSC was synthesized. Theoretical calculations show that the band gap of RBSSC is up to 3.674 eV, larger than those of all known antimony-based thiohalides(III). This work provides strong evidence that the aliovalent cation substitution strategy is an effective way to find new thioantimonate(V) families, and also indicates that the cation size effect introduced by elemental substitution may lead to surprising performance improvements.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Kaige Dong,Yuhang Cheng,Mengmeng Jia,Sakil Mahmud,Manyu Deng,Zhuoran Yi,Weiting Wang,Yimeng Feng,Dahao Lian,Gaosheng Zhang,Zhu Xiong
As (V) poses significant environmental and health risks due to its toxicity, making efficient wastewater treatment technologies essential. In this study, we introduce a novel composite material: MOF-like zirconium (Zr)-doped Prussian blue (PB) analogs decorated on polytetrafluoroethylene microporous membranes (Zr-PBAs x -PDA/PEI-M) for As (V) adsorption. Comprehensive characterization techniques, confirmed the successful incorporation of Zr into PB crystals and its growth on the membrane surface through PDA/PEI interlayers. We systematically explored the effects of varying Fe-Zr modification ratios, finding that Zr-PBAs 3 -PDA/PEI-M (Fe: Zr = 2:3) exhibited the optimal performance for As (V) removal and adsorption capacity, with a more intact and densely distributed crystal structure. It demonstrated that Zr-O bonding plays a crucial role in the adsorption mechanism, forming a double-dentate mononuclear structure with As (V). Moreover, the Zr-PBAs 3 -PDA/PEI-M’s adsorption capacity of As (V) was comprehensively assessed by key factors such as temperature, pH, operating pressure, natural organic matter (NOM), and initial As (V) concentration during wastewater treatment, which exhibited the excellent resistance to interference in removing As (V). Remarkably, Zr-PBAs 3 -PDA/PEI-M retained its high adsorption capacity across three cycles of reuse, highlighting its excellent stability and reusability. When tested on simulated Pearl River water samples containing As (V), the material achieved filtrate concentrations well below 0.5 mg/L, in compliance with China’s Comprehensive Wastewater Discharge Standard. This study presents a promising solution for efficient As (V) removal in wastewater, offering practical insights into its potential application for real-world water treatment challenges.
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