LANGMUIR
·
2021
·
IF 3.882
Qingyu Liao,Dong Chen,Xianhong Zhang,Yuhong Ma,Changwen Zhao,Wantai Yang
A facile synthetic route was developed to prepare a surface-grafted brush layer of poly(vinyl ethers) (PVEs) directly by a radical mechanism, with the “naked” Li+ acting as a catalyst. Density functional theory calculations suggested that complexation of naked Li+ to VEs significantly reduced the highest unoccupied molecular orbital–lowest unoccupied molecular orbital (HOMO–LUMO) energy gap from 5.08 to 0.68 eV, providing a better prospect for electron transfer. The structure, morphology, and surface properties of grafted polymer layers were characterized using attenuated total reflection Fourier transform infrared spectroscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, atomic force microscopy, and dynamic water contact angle (DCA). Moreover, ellipsometry data indicated that the thickness of the polymer brushes was in the range of 20–60 nm, which corresponds to the grafting densities of 0.65–1.15 chain/nm2, and DCA decreased from 84.4 to 45.3°. Most importantly, no hydrolysis was observed for the modified surface after 30 days of exposure to phosphate-buffered saline solution, 0.1 mol/L NaOH(eq) and 0.1 mol/L HCl(eq), demonstrating excellent hydrolysis resistance with long service life. In addition, as a proof of concept, the side hydroxyl groups of grafted PVEs provide active sites for efficient fixation of bioactive molecules, e.g., glycosaminoglycan and serum protein.
研究领域:
高分子化学
·
材料科学
·
表面工程
✓ 已验证
DOI
高影响因子
Analytical Methods
·
2017
·Vol. 9
·期 22
·3296-3301
·
IF 1.9
Lei Wang,Yuan Ji,Yuezhen He,Lun Wang,Hongqi Chen
Li+-Doped NaYF4:Yb,Er upconversion luminescent nanoparticles (UCLNPs) were synthesized and modified with poly(acrylic acid) (PAA). The luminescence of the carboxyl-functionalized UCLNPs at 664 nm was quenched in the presence of cupric ions (Cu2+) due to the coordination of Cu2+ with the carboxyl group of PAA. When pyrophosphate ions (PPi) were added, the luminescence of the UCLNPs was restored due to the competitive binding of PPi with Cu2+. However, pyrophosphatase (PPase) could promote the hydrolysis of PPi, thus releasing Cu2+, leading to requenching of the luminescence. Under optimal conditions, the luminescence response was virtually proportional to the activity of the PPase between 0.500 and 50.0 mU mL−1, and the limit of detection was 0.441 mU mL−1. Based on the competition assay approach, a new highly sensitive method in the red region for real-time detection of PPase activity was developed.
研究领域:
分析化学
·
生物化学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Yuwen Gao,Shougui Wang,Fei Gao,Changqing Guo,Jipeng Dong,Guanghui Chen
The Li 1.6 Mn 1.6 O 4 driven lithium ion-sieve (LIS) is considered as a potential adsorbents for recovering Li + ions from brines owing to their good theoretical adsorption performance and excellent adsorption selectivity. However, the poor cycle stability and the decrease of adsorption capacity resulting from the manganese dissolution loss limit its practical applications. In this work, to mitigate this issue, several novel Al and Cr co-doped manganese LISs were prepared by a facile hydrothermal synthesis method, followed by the acid treatment. The characterization results show that Al and Cr ions are uniformly doped into the spinel crystal structure of LIS, and the introduction of Al and Cr ions can cause the crystal shrinkage, decrease the Mn 3+ content, and raise the mean valence of manganese in the co-doped samples, effectively improving their structural stability. Compared with un-doped ion-sieve H 1.6 Mn 1.6 O 4 , the optimal co-doped ion-sieve H 1.6 Mn 1.54 Al 0.02 Cr 0.04 O 4 with 2% Al doping and 4% Cr doping possesses a higher lithium adsorption capacity, lower manganese dissolution loss, and stronger cyclic stability. Additionally, the H 1.6 Mn 1.54 Al 0.02 Cr 0.04 O 4 possesses a high adsorption selectivity of Li + over Mg 2+ , Ca 2+ , K + and Na + . Furthermore, the lithium adsorption is determined to be a chemical and monolayer adsorption process on the prepared LIS. The good lithium adsorption capacity and adsorption selectivity as well as the good recyclability make the prepared Al and Cr co-doped LIS a promising adsorbent for the efficient lithium recovery form brines.
研究领域:
材料科学
·
环境工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jiaqi Li,Long Chen,Fengling Wang,Zuoyu Qin,Ying Zhang,Ning Zhang,Xiaohe Liu,Gen Chen
Low lithium ion (Li + ) mobility and thermal stability of polyolefin separator are crucial obstacles that limit the utilization of Li metal electrodes in the age of rapid acceleration toward high-energy-density rechargeable batteries. Herein, we report anionic metal-organic frameworks (MOFs) modified separator to overcome the barriers. By grafting –SO 3 − group onto the Universitetet i Oslo (UIO) structure, the anionic MOFs nanoparticles are synthesized (noted as UIO-SOLi). The UIO-SOLi is adhered on the surface of Celgard 2400 via polyacrylic acid (PAA) to fabricate the modified separator (UIOSOL@PP). The MOFs coating optimizes the wettability and thermal stability of the pristine separator. Negatively charged moieties –SO 3 − within the pore surface electrostatically repel anions while facilitate the transport of Li + , thus achieving a high Li + transference number ( t Li + ) of 0.82. The effective Li + transport relieves the concentration polarization, regulates the Li + flow and realizes the uniform deposition of lithium. By implementing the UIOSOL@PP separator, the LiFePO 4 |Li cells deliver superior rate performance and cycling lifespan that renders a high discharge capacity retention of 155 mAh g −1 over 600 cycles at 1C. These results indicate that anionic MOFs modified separator is a promising strategy to modulate Li + flow and assist with efficient long-term operation of lithium metal batteries.
研究领域:
材料科学
·
电化学
·
电池技术
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2023
·
IF 13.1
Haochang Zhang,Zhaozhe Yu,Hannan Chen,Yongjian Zhou,Xiao Huang,Bingbing Tian
All-solid-state Li batteries (ASSLBs) with solid-state electrolytes (SSEs) are exciting candidates for next-generation energy storage and receive considerable attention owing to their reliability. Halide SSEs are promising candidates due to their excellent stability against 4 V-class layered cathodes. Compared with Li 3 InCl 6 or Li 3 ScCl 6 , the low ionic conductivity of Li 2 ZrCl 6 (LZC) is a challenge despite its low raw-material cost. Herein, we report a family of Li-Richened chloride, Li 2+2 x Zr 1– x M x Cl 6 , which can be used in high-performance ASSLBs owing to its high ionic conductivity (up to 0.62 mS cm −1 ). The theoretical (ab initio molecular dynamics simulations) and experimental results prove that the strategy of aliovalent substitution with divalent metals to obtain Li-Richened LZC is effective in improving Li + conductivity in SSEs. By combining Li 2.1 Zr 0.95 Mg 0.05 Cl 6 (Mg5-LZC) with a Li–In anode and a LiCoO 2 cathode, a room-temperature ASSLBs with excellent long-term cycling stability (88% capacity retention at 0.3C for 100 cycles) and high-rate capability (121 mA h g −1 at 1C) is reported. This exploratory work sheds light on improving the Li + conductivity of low-cost LZC-family SSEs for constructing high performance ASSLBs.
研究领域:
材料科学
·
电化学
·
能量存储
✓ 已验证
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Feng Yangyang,Li Yong,Lin Jing,Wu Huyue,Zhu Lei,Zhang Xiang,Zhang Linlin,Sun Chuan-Fu,Wu Maoxiang,Wang Yaobing
Stable lithium metal negative electrodes are desirable to produce high-energy batteries. However, when practical testing conditions are applied, lithium metal is unstable during battery cycling. Here, we propose poly(2-hydroxyethyl acrylate-co-sodium benzenesulfonate) (PHS) as negative electrode protective layer. The PHS contains soft poly (2-hydroxyethyl acrylate) and poly(sodium p-styrene sulfonate), which improve electrode flexibility, connection with the Cu current collector and transport of Li ions. Transmission electron cryomicroscopy measurements reveal that PHS induces the formation of a solid electrolyte interphase with a fluorinated rigid and crystalline internal structure. Furthermore, theoretical calculations suggest that the -SO 3 - group of poly(sodium p-styrene sulfonate) promotes Li-ion motion towards interchain migration through cation-dipole interaction, thus, enabling uniform Li-ion diffusion. Electrochemical measurements of Li | |PHS-coated-Cu coin cells demonstrate an average Coulombic efficiency of 99.46% at 1 mA/cm 2 , 6 mAh/cm 2 and 25 °C. Moreover, when the PHS-coated Li metal negative electrode is paired with a high-areal-capacity LiNi 0.83 Co 0.11 Mn 0.06 O 2 -based positive electrode in multi-layer pouch cell configuration, the battery delivers an initial capacity of 6.86 Ah (corresponding to a specific energy of 489.7 Wh/kg) and, a 91.1% discharge capacity retention after 150 cycles at 2.5 mA/cm 2 , 25 °C and 172 kPa.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
PubMed
高影响因子
Materials Today Communications
·
2023
·
IF 3.8
Shi Qiu,Fengdong Sun,Chen You,Chaokun Tang,Baoli Zhou,Shuquan Zhang,Jiangtao Feng,Aixian Tian,Minfang Chen
Through preparing the porous Zn-0.8Li scaffolds with 50–70 % porosity by using NaCl particles as pore-forming agents in the range of 150–350 µm and 350–550 µm with the infiltration casting method, the present study investigated the pore structure , mechanical properties and weight loss in simulated body fluids (SBF), and conducted the cellular activity and in vivo degradation experiments on porous Zn-0.8Li scaffolds before and after chitosan coating treatment. The results showed that the porous samples with small pore size had higher mechanical properties and lower degradation rate. However, with relatively higher average porosity and through-porosity, the porous samples with large pore size showed better pore connectivity, which provided channels for nutrient transport and promoted the lateral growth of internal tissues. In terms of cell experiments, chitosan coated Zn-0.8Li scaffolds with large pore size had better cell activity and adhesion. Since the coating of chitosan inhibited the release of Zn 2+ during the implantation of porous Zn-0.8Li scaffolds in vivo, it effectively promoted the growth of new bone tissue around the porous scaffolds, which provided an ideal microenvironment for the adhesion, proliferation and differentiation of MSCS. The results of this study demonstrated the great potential of chitosan coated porous biodegradable Zn-based scaffolds for bone tissue engineering.
研究领域:
生物医学工程
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材料科学
·
组织工程
·
生物材料
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Minhui Liao,Yang Zhou,Xunchang Jiang,Renjie Wan
High safety, high ion conductivity, and stable interface contacts are of significant importance for the application of solid-state electrolytes (SSEs) in solid-state lithium metal batteries (SSLMBs). In this study, SSEs with high ion conductivity and safety were constructed by in-situ polymerization of poly butyl acrylate (PBA) based electrolytes in the three-dimensional (3D) pores of a polyvinylidene fluoride (PVDF) nanofiber membrane, and embedded with ion conductor succinonitrile (SN), fluorinated ethylene carbonate (FEC), and imidazolium-based ionic liquid (IL). The test results and microscopic structural analysis indicate that SN is uniformly dispersed in PVDF, effectively reducing the crystallinity of solid polymer electrolytes (SPEs) and constructing a 3D interconnected lithium-ion conduction network. Consequently, an ion conductivity of 4.89 mS cm −1 was achieved at 25°C. Meanwhile, density functional theory (DFT) calculations demonstrated that imidazolium-based ionic liquid can adjust the dissolution characteristics of Li + through weak interactions with the polymer framework and strong coordination with TFSI - . X-ray photoelectron spectroscopy (XPS) characterization revealed that the imidazolium-based ionic liquid can form a stable solid electrolyte interface enriched with Li 3 N on the lithium-metal surface. The resulting SPEs demonstrated excellent ion conductivity, a high Li + transfer number (t Li + = 0.739), and a nanofiber-reinforced interpenetrating framework with a tensile strength of 17.15 MPa. Furthermore, the LiFePO 4 (LFP)||Li battery equipped with PBA-PVDF-SN (modified with IL) exhibited excellent electrochemical performance at room temperature with a capacity retention of 87.4 % after 800 cycles at 0.5C.
研究领域:
材料科学
·
电化学
·
电池技术
·
聚合物化学
✓ 已验证
DOI
高影响因子
Small
·
2023
·Vol. 19
·期 33
·2301391
·
IF 13.3
Wenjing Zhang,Jian Zheng,Ruoyu Wang,Li Huang,Junkai Wang,Tianran Zhang,Xiangfeng Liu
Lithium–oxygen (Li–O 2 ) batteries have received extensive attention owing to ultrahigh theoretical energy density. Compared to typical discharge product Li 2 O 2 , LiOH has attracted much attention for its better chemical and electrochemical stability. Large-scale applications of Li–O 2 batteries with LiOH chemistry are hampered by the serious internal shuttling of the water additives with the desired 4e − electrochemical reactions. Here, a metal organic framework-derived “water-trapping” single-atom-Co-N 4 /graphene catalyst (Co-SA-rGO) is provided that successfully mitigates the water shuttling and enables the direct 4e − catalytic reaction of LiOH in the aprotic Li–O 2 battery. The Co-N 4 center is more active toward proton-coupled electron transfer, benefiting - direction 4e − formation of LiOH. 3D interlinked networks also provide large surface area and mesoporous structures to trap ≈12 wt% H 2 O molecules and offer rapid tunnels for O 2 diffusion and Li + transportation. With these unique features, the Co-SA-rGO based Li–O 2 battery delivers a high discharge platform of 2.83 V and a large discharge capacity of 12 760.8 mAh g −1 . Also, the battery can withstand corrosion in the air and maintain a stable discharge platform for 220 cycles. This work points out the direction of enhanced electron/proton transfer for the single-atom catalyst design in Li–O 2 batteries.
研究领域:
材料科学
·
电化学
·
能源存储
·
电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2024
·
IF 15.8
Yuqing Dai,Jiaxu Tan,Zihan Hou,Bianzheng You,Gui Luo,Duo Deng,Wenjie Peng,Zhixing Wang,Huajun Guo,Xinhai Li,Guochun Yan,Hui Duan,Ying Wang,Feixiang Wu,Jiexi Wang
The matching of poly(ethylene oxide) (PEO)-based electrolytes with ultrahigh-nickel cathode materials is crucial for designing new-generation high-energy-density solid-state lithium metal batteries (SLMBs), but it is limited by serious interfacial side reactions between PEO and ultrahigh-nickel materials. Here, a high-concentration electrolyte (HCE) interface with a customized Li+ solvation sheath is constructed between the cathode and the electrolyte. It induces the formation of an anion-regulated robust cathode/electrolyte interface (CEI), reduces the unstable free-state solvent, and finally achieves the compatibility of PEO-based electrolytes with ultrahigh-nickel cathode materials. Meanwhile, the corrosion of the Al current collector caused by lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) ions is prevented by lithium difluoro(oxalato)borate (LiDFOB) ions. The synergistic effect of the double lithium salt is achieved by a well-tailored ratio of TFSI– and DFOB– in the first solvation sheath of Li+. Compared with reported PEO-based SLMBs matched with ultrahigh-nickel (Ni ≥ 90%) cathodes, the SLMB in this work delivers a high discharge specific capacity of 216.4 mAh g–1 (0.1C) even at room temperature. This work points out a direction to optimize the cathode/electrolyte interface.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Dexuan Pei,Ziying Liu,Rui Ma,Shuo Huang,Shuen Hou,Min Liu,Guozhong Cao,Hongyun Jin
Composite polymer electrolytes (CPEs) have shown extraordinary promise for use in all-solid-state lithium metal batteries (LMBs) because of their tunable merits in ionic conductivity and mechanical flexibility. Their practical application is however hindered by the poor interface stability and the uncontrollable Li dendrite formation. Addressing these two issues, we report an in-situ formed Li-Al-O interface layer between CPEs and Li metal anode by introducing Al 2 O 3 nanoparticles in CPEs. X-ray photoelectron spectroscopy results indicated that the CPE-Al 2 O 3 could slowly release Al atoms which react with Li metal to form the current Li-Al-O interface layer. We highlight that the Li-Al-O interface layer can stabilize lithium deposition/stripping over 1400 h in lithium symmetric batteries, and afford an impressive cycle life of 300 cycles in LiFePO 4 -Li batteries with almost no capacity loss. The present findings demonstrate that in-situ constructing a slow-release Li-Al-O interface layer is an easy and effective approach to stabilize the solid electrolyte interface and suppress the Li dendrites growth. Furthermore, the obtained batteries show excellent cycling stability, indicating the strategy with in-situ formed CPEs shed light on improving the processability of fabrication of high-performance electrolytes.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
Energy Storage Materials
·
2024
·
IF 18.9
Xinyang Li,Jie Feng,Yanan Li,Na Li,Xin Jia,Yinshui Wang,Shujiang Ding
The inability to effectively inhibit the lithium (Li) dendrite growth is identified as the real culprit hindering the practical application of polyethylene oxide (PEO)-based electrolytes. Herein, a novel PEO composite electrolyte with ion rectifier is developed based on the cross-scale synergistic rectification strategy. At the micro-scale, the array structure of the ion rectifier suppresses the growth of PEO crystals and their distribution in the non-ionic conduction direction through space confinement, alleviating ion-migration crosstalk and enabling polymer chain rectification. Furthermore, the matrix contains abundant copper ions and oxygen-containing groups that inhibit anion conduction and accelerate Li + migration at the nanoscale, respectively, to achieve ion flow rectification. Implementing this strategy results in a uniform, fast, and stable Li + migration/diffusion behavior from the electrolyte to anode interface. The critical current density of the PEO electrolyte is increased to 2.5 mA cm −2 , indicating a significant improvement in dendrite growth inhibition. Impressively, the composite electrolytes exhibit long-term stability (>4000 h at 0.2 mA cm −2 ) and ultra-high current-density tolerance (>200 h at 1 mA cm −2 ). Moreover, the composite electrolytes enable stable cycling of high-area-capacity (3.11 mAh cm −2 , 20 mg cm −2 ) LiFePO 4 /Li pouch cells, highlighting the importance of this strategy for the practical application of PEO electrolytes.
研究领域:
材料科学
·
电化学
·
能源存储
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）