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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Rational reconfiguration of a gradient redox mediator with in-situ fabricated gel electrolyte for Li–air batteries

Yinwei Fu,Xiaofeng Lei,Huiming Yin,Xizheng Liu

Flexible lithium–air batteries (LABs) with a redox mediator (RM) in the electrolyte demonstrate enhanced round-trip efficiency. However, their cycle performance is unsatisfactory due to severe corrosion of the Li metal anode. Herein, we propose a two step gelatinization strategy to fabricate a gradient RMs (including LiI, TMPD, and DMPZ) gel electrolyte, in which the bare electrolyte gelatinization on the Li surface and then the electrolyte contained RMs sequentially gelled on the formed gel. The RMs mainly distributed at the surface and anchored at the cathode side. By suppressing the shuttle of RMs in the electrolyte and alleviating the passivation of the Li anode, the mid-charging potentials can reach 3.44 and 4.08 V at the 15th cycle with and without the LiI mediator, respectively. The energy efficiency is 63% even at the 150th cycle, whereas the corresponding energy efficiency are only 47% and 51% for the LABs with liquid and normal gel electrolytes, respectively. Moreover, the cycle life of the battery containing the gradient gel electrolyte is three times longer than that with the liquid electrolyte. The gel electrolyte further offers the flexibility of the device, and the laminated cells thus fabricated can readily operate under harsh bending conditions.

研究领域: 电化学 · 能源材料 · 纳米材料 · 界面化学 · 储能技术 · 先进电池 · 功能高分子 · 柔性电子
✓ 已验证 DOI 高影响因子
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Small · 2024 ·Vol. 20 ·期 24 ·2308304 · IF 13

Fracture Resistant CrSi2-Doped Silicon Nanoparticle Anodes for Fast-Charge Lithium–Ion Batteries

Weiqun Li,Chucheng Luo,Jimin Fu,Juan Yang,Xiangyang Zhou,Jingjing Tang,B. Layla Mehdi

Lithium–ion batteries (LIBs) has been developed over the last three decades. Increased amount of silicon (Si) is added into graphite anode to increase the energy density of LIBs. However, the amount of Si is limited, due to its structural instability and poor electronic conductivity so a novel approach is needed to overcome these issues. In this work, the synthesized chromium silicide (CrSi 2 ) doped Si nanoparticle anode material achieves an initial capacity of 1729.3 mAh g −1 at 0.2C and retains 1085 mAh g −1 after 500 cycles. The new anode also shows fast charge capability due to the enhanced electronic conductivity provided by CrSi 2 dopant, delivering a capacity of 815.9 mAh g −1 at 1C after 1000 cycles with a capacity degradation rate of <0.05% per cycle. An in situ transmission electron microscopy is used to study the structural stability of the CrSi 2 -doped Si, indicating that the high control of CrSi 2 dopant prevents the fracture of Si during lithiation and results in long cycle life. Molecular dynamics simulation shows that CrSi 2 doping optimizes the crack propagation path and dissipates the fracture energy. In this work a comprehensive information is provided to study the function of metal ion doping in electrode materials.

研究领域: 材料科学 · 电化学 · 纳米科技 · 能源存储 · 固体物理 · 计算材料学
✓ 已验证 DOI 高影响因子
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Advanced Electronic Materials · 2021 ·Vol. 8 ·期 4 ·2101125 · IF 7.295

In-Situ Loading Bridgman Growth of Mg3Bi1.49Sb0.5Te0.01 Bulk Crystals for Thermoelectric Applications

Qi-Qi Wang,Fan Li,Sheng-Qing Xia,Jian Liu,Xiao-Cun Liu,Ling Chen,Cheng-Qian Zhang

The single crystal growth of Mg 3 Bi 2 -based thermoelectric materials is of great significance for their applications near room temperature. So far, it is still a big challenge to grow such bulk single crystals and attempts are primarily focused on the metal flux methods. For the first time, bulk single crystals of n-type Mg 3 Bi 1.49 Sb 0.5 Te 0.01 are directly grown by applying an In-situ Loading Bridgman method. The as-grown single crystal features an excellent carrier mobility of 220 cm 2 V −1 s −1 , which is among the best compared to other Mg 3 Bi 2 -based bulk materials. Besides, this method is successfully developed to fast grow uniform polycrystalline materials with high thermoelectric and mechanic performance. As demonstrated by the single-leg device, a large temperature difference of 10.5 K is achieved at the supplied electric current of 0.6 A, much superior to other room temperature state-of-the-art thermoelectric materials. With the single crystalline and polycrystalline materials prepared reliably and conveniently, in-depth investigations on the Mg 3 Bi 2 thermoelectric system can be greatly benefited, which should as well significantly facilitate their practical applications at room temperature.

研究领域: 材料科学 · 热电学 · 凝聚态物理 · 晶体生长 · 功能材料 · 能源材料
✓ 已验证 DOI 高影响因子
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APPLIED SURFACE SCIENCE · 2018 · IF 4.439

Phase inversion, formation and stability mechanism of poly(urethane-acrylate) nanoemulsions based on block-copolymer surfmer

Haihua Wang,Bei Li,Guiqiang Fei,Yiding Shen,Ke Zhu

We reported herein the synthesis of block copolymers and their application in the in-situ emulsion polymerization of waterborne poly (urethane-acrylate) (WPUA) nanoemulsions based on phase inversion process. The polymerizable surfmers containing terminal unsaturated double bonds (MSA-r) were successfully synthesized via catalytic chain transfer polymerization (CCTP). Random copolymer (MSA-t) prepared through radical polymerization was utilized as control. The structure, surface tension and aggregation behavior of surfmers were characterized. The phase inversion, formation and stability of WPUA nanoemulsions were systematically investigated. Effects of MSA-r surfmer content and BMA/MMA ratio on the water resistance and thermal stability of the corresponding films were also discussed. It was found that the phase inversion mechanism of PUA prepolymer in the presence of MSA-r surfmers is different from conventional polyurethane prepolymer. The addition of MSA-r and MSA-t surfmers alters the rheological behaviors of PUA prepolymer via PUA-surfmer interactions, as well as the phase inversion process. Compared with WPUA/MSA-t emulsion, WPUA/MSA-r nanoemulsion displayed improved stability at higher solid content. The minimum particle size of WPUA/MSA-r nanoemulsion was 88.7 nm and kept almost constant after 12-month storage, while the particle size of WPUA/MSA-t emulsion was 131.3 nm and increased to 178.9 nm. Moreover, the WPUA/MSA-r film possessed improved water resistance and thermal stability.

研究领域: 高分子化学 · 胶体与界面科学 · 材料化学 · 纳米材料 · 功能高分子 · 水性涂料 · 聚合物乳液
✓ 已验证 DOI 高影响因子
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Small · 2024 ·Vol. 20 ·期 29 ·2310092 · IF 13

Supported Ionic Liquid Membrane with Highly-permeable Polyamide Armor by In Situ Interfacial Polymerization for Durable CO2 Separation

Yu-Ren Xue,Chang Liu,Hao-Cheng Yang,Hong-Qing Liang,Chao Zhang,Zhi-Kang Xu

Supported ionic liquid membranes (SILMs), owing to their capacities in harnessing physicochemical properties of ionic liquid for exceptional CO 2 solubility, have emerged as a promising platform for CO 2 extraction. Despite great achievements, existing SILMs suffer from poor structural and performance stability under high-pressure or long-term operations, significantly limiting their applications. Herein, a one-step and in situ interfacial polymerization strategy is proposed to elaborate a thin, mechanically-robust, and highly-permeable polyamide armor on the SILMs to effectively protect ionic liquid within porous supports, allowing for intensifying the overall stability of SILMs without compromising CO 2 separation performance. The armored SILMs have a profound increase of breakthrough pressure by 105% compared to conventional counterparts without armor, and display high and stable operating pressure exceeding that of most SILMs previously reported. It is further demonstrated that the armored SILMs exhibit ultrahigh ideal CO 2 /N 2 selectivity of about 200 and excellent CO 2 permeation of 78 barrers upon over 150 h operation, as opposed to the full failure of CO 2 separation performance within 36 h using conventional SILMs. The design concept of armor provides a flexible and additional dimension in developing high-performance and durable SILMs, pushing the practical application of ionic liquids in separation processes.

研究领域: 膜科学与技术 · 气体分离 · 环境化学 · 材料化学 · 化学工程 · 可持续能源技术
✓ 已验证 DOI 高影响因子
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Advanced Energy Materials · 2016 ·Vol. 7 ·期 8 ·1602149 · IF 15.23

Unveiling the Unique Phase Transformation Behavior and Sodiation Kinetics of 1D van der Waals Sb2S3 Anodes for Sodium Ion Batteries

Shanshan Yao,Jiang Cui,Ziheng Lu,Zheng-Long Xu,Lei Qin,Jiaqiang Huang,Zoya Sadighi,Francesco Ciucci,Jang-Kyo Kim

Carbon-coated van der Waals stacked Sb 2 S 3 nanorods (SSNR/C) are synthesized by facile hydrothermal growth as anodes for sodium ion batteries (SIBs). The sodiation kinetics and phase evolution behavior of the SSNR/C anode during the first and subsequent cycles are unraveled by coupling in situ transmission electron microscopy analysis with first-principles calculations. During the first sodiation process, Na + ions intercalate into the Sb 2 S 3 crystals with an ultrafast speed of 146 nm s −1 . The resulting amorphous Na x Sb 2 S 3 intermediate phases undergo sequential conversion and alloying reactions to form crystalline Na 2 S, Na 3 Sb, and minor metallic Sb. Upon desodiation, Na + ions extract from the nanocrystalline phases to leave behind the fully desodiated Sb 2 S 3 in an amorphous state. Such unique phase evolution behavior gives rise to superb electrochemical performance and leads to an unexpectedly small volume expansion of ≈54%. The first-principles calculations reveal distinctive phase evolution arising from the synergy between the extremely low Na + ion diffusion barrier of 190 meV and the sharply increased electronic conductivity upon the formation of amorphous Na x Sb 2 S 3 intermediate phases. These findings highlight an anomalous Na + ion storage mechanism and shed new light on the development of high performance SIB anodes based on van der Waals crystals.

研究领域: 材料科学 · 电化学 · 纳米科技 · 能源存储 · 固态物理 · 计算材料学
✓ 已验证 DOI 高影响因子
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Acta Biomaterialia · 2021 · IF 8.947

Biodegradable Zn−3Mg−0.7Mg2Si composite fabricated by high-pressure solidification for bone implant applications

Xian Tong,Wenhao Cai,Jixing Lin,Kun Wang,Lufan Jin,Zimu Shi,Dechuang Zhang,Jianguo Lin,Yuncang Li,Matthew Dargusch,Cuie Wen

Zinc (Zn)-based alloys have been considered potential biodegradable materials for medical applications due to their good biodegradability and biocompatibility. However, the insufficient mechanical properties of pure Zn do not meet the requirements of biodegradable implants. In this study, we have developed a biodegradable Zn−3Mg−0.7Mg 2 Si composite fabricated by high-pressure solidification. Microstructural characterization revealed that the high-pressure solidified (HPS) composite exhibited uniformly distributed fine MgZn 2 granules in an α-Zn matrix. Comprehensive tests indicated that the HPS composite exhibited exceptionally high compression properties including a compressive yield strength of 406.2 MPa, an ultimate compressive strength of 1181.2 MPa, and plastic deformation up to 60% strain without cracking or fracturing. Potentiodynamic polarization tests revealed that the HPS composite showed a corrosion potential of −0.930 V, a corrosion current density of 3.5 μA/cm 2 , and a corrosion rate of 46.2 μm/y. Immersion tests revealed that the degradation rate of the HPS composite after immersion in Hanks’ solution for 1 month and 3 months was 42.8 μm/y and 37.8 μm/y, respectively. Furthermore, an extract of the HPS composite exhibited good cytocompatibility compared with as-cast (AC) pure Zn and an AC composite at a concentration of ≤25%. These results suggest that the HPS Zn−3Mg−0.7Mg 2 Si composite can be anticipated as a promising biodegradable material for orthopedic applications .

研究领域: 生物医学工程 · 材料科学 · 生物材料 · 骨科 · 可降解金属 · 组织工程 · 腐蚀科学
✓ 已验证 DOI 高影响因子
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Journal of CO2 Utilization · 2017 · IF 4.292

A green process for production of p-aminophenol from nitrobenzene hydrogenation in CO2/H2O: The promoting effects of CO2 and H2O

Lijun Zhao,Haiyang Cheng,Tong Liu,Yan Li,Zhong Ying,Wenjing Yang,Weiwei Lin,Xiangchun Meng,Chengxue Wang,Fengyu Zhao

An efficient green process was developed for production of p -aminophenol (PAP) from hydrogenation of nitrobenzene (NB) over a traditional Pt/Al 2 O 3 catalyst in a reaction medium of supercritical CO 2 (scCO 2 ) and H 2 O without any additional acid catalyst involved. The combination of scCO 2 and H 2 O was confirmed to be effective for the production of PAP. The acidity, aroused by the in situ formed carbonic acid, increased with CO 2 pressure, which acted as acid catalysis during the reaction, and it can easily self-neutralize by depressurization of CO 2 , resulting in a green and a intensive process for it removed the final neutralization and salts disposal of the traditional liquid acids. Under the optimal reaction conditions, a high yield to PAP (68.9%) was achieved at the high conversion of NB (98.5%). Moreover, the results of in situ diffuse reflectance FTIR spectra revealed that CO was generated by the reverse water-gas shift reaction (CO 2   +   H 2   →   CO   +   H 2 O), it can adsorbed on the surface of Pt/Al 2 O 3 to suppress the undesired deep hydrogenation of N -phenylhydroxylamine (PHA) to aniline (AN), which also contributed to the obtained high selectivity of PAP. Therefore, the present green and efficient catalysis process will arouse the interest of researchers in the fields of the green and sustainable organic synthesis.

研究领域: 绿色化学 · 有机合成 · 催化化学 · 环境友好工艺 · 工业化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF MATERIALS SCIENCE · 2023 ·Vol. 58 ·期 17 ·7456-7468 · IF 4.5

Butterfly metamorphosis inspired injectable in situ forming scaffolds with time-dependent pore formation for bone regeneration

Zhang Ning,Wang Zongliang,Zeng Yuqi,Guo Yueming,Wang Liqiang,Liu Jianguo,Wang Yu,Zhang Peibiao

Preformed three-dimensional scaffolds with insufficient mechanical properties, poor surgical performance, and morphological mismatch to defects with irregular shape have shown drawbacks in animal evaluations and clinical applications. This motivates the development of novel injectable systems to ideally fill bone defects, allowing in situ solidification within the host tissues while retaining high initial mechanical strength and appropriate porosity. In this study, an in situ forming scaffold with time-dependent pore formation inspired by the metamorphosis of a butterfly was fabricated by incorporating gelatin microspheres (GMs) into a poly(lactic-co-glycolic acid) (PLGA)-based injectable implant. After optimizing solvent, molecular weight and solution concentration of PLGA matrix, the injectable mixture could be easily injected into both aqueous solution and random-shaped grooves while in situ solidified instantaneously. The injectability enabled an in situ morphological match within an irregular bone defect, providing high initial strength in the early period. The toughness of the injectable implant also allowed them to be easily bent into a ring without breaking. Time-dependent pore formation was accomplished by gradual degradation of GMs, generating appropriate space for tissue ingrowth in the scaffold. It is expected that the injectable in situ forming implant would aid the bone healing process by maintaining initial mechanical support and creating a spatiotemporally evolutionary microstructure during bone tissue regeneration.

研究领域: 生物材料学 · 组织工程 · 骨科学 · 再生医学 · 高分子科学 · 药物递送系统
✓ 已验证 DOI 高影响因子
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Enhanced atomic-oxygen resistance of surface-siliconized polyimide film via an in-situ precursor network at the interface

Ruihan Wang,Nanxi Dong,Guofeng Tian,Gang Liu,Bo Zhou,Shengli Qi,Dezhen Wu

In order to allow polyimide (PI) to resist the erosion of atomic oxygen (AO) in Low Earth Orbit to extend the life of the aircraft, an in-situ precursor network approach was proposed to manufacture the inorganic gradient microstructure across the organic/inorganic transition interface and simplify the process, which create a three-tier microstructure film and lead the dense SiO 2 protective layer firmly grasps the PI film. Benefiting from the integrated structure, SiO 2 -coated PI film shows remarkable surface and interface state after 3000 times mechanical bending, which able to delay the initial AO corrosion caused by the defect of the protective layer, resistance to AO reported as AO erosion yield of 2.39 × 10 −26 cm 3 O atom −1 under 7 × 10 21 O atoms cm −2 AO fluence. This work proposes a novel approach for the fabrication of high-performance and AO resistant PI to enable the aircraft to complete more efficient and highly integrated flight missions and shows great potential in the general preparation of organic-inorganic interface.

研究领域: 高分子材料科学 · 航天材料工程 · 表面与界面化学 · 空间环境效应 · 功能涂层技术
✓ 已验证 DOI 高影响因子
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

An engineering approach for active and stable dry methane reforming within solid oxide fuel cell stacks using La0.6Sr0.2Cr0.85Ni0.15O3-δ as a catalyst

Cheng Li,Guangyu Li,Yongtao Zhan,Chenzhao Liu,Yujie Tang,Dong Yan,Jian Li,Lichao Jia

A strategy of in-stack dry reforming of methane (DRM) is proposed by using La 0.6 Sr 0.2 Cr 0.85 Ni 0.15 O 3-δ -loaded Ni foam (LSCrN@NF) as a CH 4 –CO 2 reformer, fuel gas distributor, and anode current collector in a SOFC stack. The prepared LSCrN exists as a single phase in a perovskite structure ; its reduced form contains exsolved Ni nanoparticles embedded on the surface of the LSCrN substrate. Introduced into an NF, the reduced LSCrN@NF demonstrates high DRM activity that increases with the increase of LSCrN amount to an optimum of about 42%. With the LSCrN@NF in-stack DRM, the conversions of CH 4 and CO 2 into CO and H 2 increase. Thus, the electrode polarization resistance, including the cathode and anode , decreases to 0.62, 1.07, and 3.93 Ω cm 2 at 800 °C, 750 °C, and 700 °C, respectively. Consequently, the peak power density (PPD) of the cell using 45% CH 4 -45% CO 2 –10% N 2 as fuel is 1.17, 0.94, and 0.47 W cm −2 , significantly higher than that of the cell without LSCrN@NF in-stack DRM. In addition, the voltage of the cell with LSCrN@NF in-stack DRM is stable on a level between 0.81 and 0.82 V at 400 mA cm −2 and 750 °C for 270 h without detected carbon deposition in the Ni–Y 2 O 3 stabilized ZrO 2 anode. This LSCrN@NF in-stack DRM strategy is also adopted with a large-scale (13 × 13 cm 2 ) single cell, which shows an extrapolated PPD of 428.3 mW cm −2 at 750 °C and is operated for 40 h at 400 mA cm −2 without noticeable performance degradation .

研究领域: 能源材料 · 电化学工程 · 催化化学 · 燃料电池技术 · 高温材料科学 · 化学反应工程 · 清洁能源转化
✓ 已验证 DOI 高影响因子
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POLYMER · 2022 · IF 4.432

Straightforward preparation of Ca-bentonite/polymer nanocomposite by confining salt-resistant copolymers into montmorillonite interlayers

Hui Wang,Chongrui Zhang,Lusha Jiang,Shan Tong,Yu-Chao Li,Hefu Pu,Qiang Zhao

Calcium bentonites (CaB), rich in European and Asian countries, are potential barrier materials for landfill leachate containment. However, CaB has to be converted into sodium bentonite (NaB) by Na-activation so as to facilitate intercalation modification. In this study, salt-resistant poly(acrylic acid-N, N-diethyl acrylamide) [P(AA-DEA)] was designed to intercalate and graft CaB by in situ polymerization without prior Na-activation. By this design, acrylic acid monomers were first adsorbed into interlayers of Ca-montmorillonite (Ca-MT) through the electrostatic complexation with Ca 2+ , dislodging Ca 2+ from montmorillonite surfaces. Then, ammonium ions of N, N-diethyl acrylamide were adsorbed into Ca-MT interlayers. Swelling index of the obtained CaB/P(AA-DEA) nanocomposite in aggressive coal combustion product (CCP) leachate is 15.8 mL/2g, which is as high as 3.4 times that of CaB. CaB/P(AA-DEA)-based geosynthetic clay liners (GCLs) exhibit very low hydraulic conductivity (1.6✕10 −12  m/s) to CCP leachate, which is as low as 3.3% that of the U.S. standard requirement and ∼4 orders of magnitude lower than that of CaB-based GCL. Polymer elution of CaB/P(AA-DEA)-8% in CCP leachate is as low as 1.9% that of the dry mixed samples.

研究领域: 环境工程 · 材料科学 · 土木工程 · 高分子化学 · 地质屏障材料
✓ 已验证 DOI 高影响因子
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