Publications by authors named "Jinyun Liu"

67 Publications

Engineering a novel microcapsule of CuS core and SnS quantum dot/carbon nanotube shell as a Li-ion battery anode.

Chem Commun (Camb) 2021 Nov 26. Epub 2021 Nov 26.

Department of Modern Mechanics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.

A novel microcapsule composed of CuS and SnS quantum dots (QDs)/carbon nanotubes (CNTs) prepared through a microfluidic approach was developed for a Li-ion battery anode. CNTs enhance the conductivity, while pores in the shell facilitate electrolyte penetration, and void in the microcapsule buffers the volume change. The microcapsule-based anode displayed stable capacity, a Coulombic efficiency of 99.9%, and reversible rate-performance at temperatures of -10 °C and 45 °C, which are significant for developing high-performance energy-storage materials and battery systems.
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http://dx.doi.org/10.1039/d1cc05657cDOI Listing
November 2021

A novel free-standing metal organic frameworks-derived cobalt sulfide polyhedron array for shuttle effect suppressive lithium-sulfur batteries.

Nanotechnology 2021 Nov 24. Epub 2021 Nov 24.

Chinese Academy of Sciences - Intelligent Machines Institute, Science Island 1130 M B, Hefei 230026, Hefei, 230031, CHINA.

Metal-organic-foams (MOFs)-derived nanostructures have received broad attention for secondary batteries. However, common strategies are focusing on the preparation of dispersive materials, which need complicated steps and some additives for making electrodes of batteries. Here, we develop a novel free-standing Co9S8 polyhedron array derived from ZIF-67, which grows on a three-dimensional carbon cloth for lithium-sulfur (Li-S) battery. The polar Co9S8 provides strong chemical binding to immobilize polysulfides, which enables efficiently suppressing of the shuttle effect. The free-standing [email protected] polyhedron array-based cathode exhibits ultrahigh capacity of 1079 mAh g-1 after cycling 100 times at 0.1C, and long cycling life of 500 cycles at 1C, recoverable rate-performance and good temperature tolerance. Furthermore, the adsorption energies towards polysulfides are investigated by using density functional theory (DFT) calculations, which display a strong binding with polysulfides.
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http://dx.doi.org/10.1088/1361-6528/ac3ce5DOI Listing
November 2021

A transparent low intensity pulsed ultrasound (LIPUS) chip for high-throughput cell stimulation.

Lab Chip 2021 Nov 5. Epub 2021 Nov 5.

Department of Biomedical Engineering, The Pennsylvania State University, University Park, PA 16802, USA.

We report an on-chip platform for low-intensity pulsed ultrasound (LIPUS) stimulation of cells directly cultured on a biocompatible surface of a transparent ultrasound transducer (TUT) fabricated using lithium niobate. The high light transmittance (>80%) and compact size (3 mm × 3 mm × 2 mm) of TUTs allowed easy integration with powerful optical microscopy techniques with no additional acoustic coupling and risk for contamination. TUTs were excited with varying acoustic excitation parameters (voltage amplitude and duty cycle) and resulting live cell calcium signaling was simultaneously imaged using time-lapse confocal microscopy, while the temperature change was measured by a thermocouple. Quantitative single-cell fluorescence analysis revealed the dynamic calcium signaling responses and together with the temperature measurements elucidated the optimal stimulation parameters for non-thermal and thermal effects. The fluorescence change profile was distinct from the recorded temperature change (<1 degree Celsius) profile under LIPUS treatment conditions. Cell dead assay results confirmed cells remain viable after the LIPUS treatment. These results confirmed that the TUT platform enables controllable, safe, high-throughput, and uniform mechanical stimulation of all plated cells. The on-chip LIPUS stimulation using TUTs has the potential to attract several and biomedical applications such as controlling stem cell differentiation and proliferation, studying biomechanical properties of cancer cells, and gaining fundamental insights into mechanotransduction pathways when integrated with state-of-the-art high-speed and high-resolution microscopy techniques.
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http://dx.doi.org/10.1039/d1lc00667cDOI Listing
November 2021

A novel nanosphere-in-nanotube iron phosphide Li-ion battery anode displaying a long cycle life, recoverable rate-performance, and temperature tolerance.

Nanoscale 2021 Oct 1;13(37):15624-15630. Epub 2021 Oct 1.

National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Nanjing University, Nanjing, Jiangsu 210093, P. R. China.

Currently, non-ideal anodes restricts the development of long-term stable Li-ion batteries. Several currently available high-capacity anode candidates are suffering from a large volumetric change during charge and discharge and non-stable solid interphase formation. Here, we develop a novel nanosphere-confined one-dimensional yolk-shell anode taking iron phosphide (FeP) as a demonstrating case study. Multiple FeP nanospheres are encapsulated inside an FeP nanotube through a magnetic field-assisted and templated approach, forming a nanosphere-in-nanotube yolk-shell (NNYS) structure. After long-term 1000 cycles at 2 A g, the NNYS FeP anode shows a good capacity of 560 mA h g, and a coulombic efficiency of 99.8%. A recoverable rate-performance is also obtained after three rounds of tests. Furthermore, the capacities and coulombic efficiency remain stable at temperatures of -10 °C and 45 °C, respectively, indicating good potential for use under different conditions.
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http://dx.doi.org/10.1039/d1nr05294bDOI Listing
October 2021

A Polysulfides-Confined All-in-One Porous Microcapsule Lithium-Sulfur Battery Cathode.

Small 2021 Oct 12;17(41):e2103051. Epub 2021 Sep 12.

National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Nanjing University, Nanjing, Jiangsu, 210093, P. R. China.

Developing emerging materials for high energy-density lithium-sulfur (Li-S) batteries is of great significance to suppress the shuttle effect of polysulfides and to accommodate the volumetric change of sulfur. Here, a novel porous microcapsule system containing a carbon nanotubes/tin dioxide quantum dots/S (CNTs/QDs/S) composite core and a porous shell prepared through a liquid-driven coaxial microfluidic method as Li-S battery cathode is developed. The encapsulated CNTs in the microcapsules provide pathways for electron transport; SnO QDs on CNTs immobilize the polysulfides by strong adsorption, which is verified by using density functional theory calculations on binding energies. The porous shell of the microcapsule is beneficial for ion diffusion and electrolyte penetration. The void inside the microcapsule accommodates the volumetric change of sulfur. The Li-S battery based on the porous CNTs/QDs/S microcapsules displays a high capacity of 1025 mAh g after 100 cycles at 0.1 C. When the sulfur loading is 2.03 mg cm , the battery shows a stable cycling life of 700 cycles, a Coulombic efficiency exceeding 99.9%, a recoverable rate-performance during repeated tests, and a good temperature tolerance at both -5 and 45 °C, which indicates a potential for applications at different conditions.
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http://dx.doi.org/10.1002/smll.202103051DOI Listing
October 2021

Mevalonate Blockade in Cancer Cells Triggers CLEC9A Dendritic Cell-Mediated Antitumor Immunity.

Cancer Res 2021 Sep 15;81(17):4514-4528. Epub 2021 Jul 15.

State Key Laboratory of Oncology in South China, Collaborative Innovation Center for Cancer Medicine, Sun Yat-sen University Cancer Center, Guangzhou, China.

Hyperactive mevalonate (MVA) metabolic activity is often observed in cancer cells, and blockade of this pathway inhibits tumor cell lipid synthesis and cell growth and enhances tumor immunogenicity. How tumor cell MVA metabolic blockade promotes antitumor immune responses, however, remains unclear. Here we show that inhibition of the MVA metabolic pathway in tumor cells elicits type 1 classical dendritic cells (cDC1)-mediated tumor recognition and antigen cross-presentation for antitumor immunity. Mechanistically, MVA blockade disrupted prenylation of the small GTPase Rac1 and induced cancer cell actin filament exposure, which was recognized by CLEC9A, a C-lectin receptor specifically expressed on cDC1s, in turn activating antitumor T cells. MVA pathway blockade or Rac1 knockdown in tumor cells induced CD8 T-cell-mediated antitumor immunity in immunocompetent mice but not in mice lacking CLEC9A dendritic cells. These findings demonstrate tumor MVA metabolic blockade stimulates a cDC1 response through CLEC9A-mediated immune recognition of tumor cell cytoskeleton, illustrating a new immune surveillance mechanism by which dendritic cells monitor tumor metabolic dysregulation and providing insight into how MVA pathway inhibition may potentiate anticancer immunity. SIGNIFICANCE: These findings suggest that mevalonate blockade in cancer cells disrupts Rac1 prenylation to increase recognition and cross-presentation by conventional dendritic cells, suggesting this axis as a potential target for cancer immunotherapy.
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http://dx.doi.org/10.1158/0008-5472.CAN-20-3977DOI Listing
September 2021

Machine learning builds full-QM precision protein force fields in seconds.

Brief Bioinform 2021 Nov;22(6)

Key Laboratory for Thin Film and Microfabrication of Ministry of Education, Department of Micro/Nano Electronics, Shanghai Jiao Tong University, China.

Full-quantum mechanics (QM) calculations are extraordinarily precise but difficult to apply to large systems, such as biomolecules. Motivated by the massive demand for efficient calculations for large systems at the full-QM level and by the significant advances in machine learning, we have designed a neural network-based two-body molecular fractionation with conjugate caps (NN-TMFCC) approach to accelerate the energy and atomic force calculations of proteins. The results show very high precision for the proposed NN potential energy surface models of residue-based fragments, with energy root-mean-squared errors (RMSEs) less than 1.0 kcal/mol and force RMSEs less than 1.3 kcal/mol/Å for both training and testing sets. The proposed NN-TMFCC method calculates the energies and atomic forces of 15 representative proteins with full-QM precision in 10-100 s, which is thousands of times faster than the full-QM calculations. The computational complexity of the NN-TMFCC method is independent of the protein size and only depends on the number of residue species, which makes this method particularly suitable for rapid prediction of large systems with tens of thousands or even hundreds of thousands of times acceleration. This highly precise and efficient NN-TMFCC approach exhibits considerable potential for performing energy and force calculations, structure predictions and molecular dynamics simulations of proteins with full-QM precision.
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http://dx.doi.org/10.1093/bib/bbab158DOI Listing
November 2021

Modulation of lactate-lysosome axis in dendritic cells by clotrimazole potentiates antitumor immunity.

J Immunother Cancer 2021 05;9(5)

State Key Laboratory of Oncology in South China, Collaborative Innovation Center for Cancer Medicine, Sun Yat-sen University Cancer Center, Guangzhou, China

Background: Dendritic cells (DCs) play a critical role in antitumor immunity, but the therapeutic efficacy of DC-mediated cancer vaccine remains low, partly due to unsustainable DC function in tumor antigen presentation. Thus, identifying drugs that could enhance DC-based antitumor immunity and uncovering the underlying mechanism may provide new therapeutic options for cancer immunotherapy.

Methods: In vitro antigen presentation assay was used for DC-modulating drug screening. The function of DC and T cells was measured by flow cytometry, ELISA, or qPCR. B16, MC38, CT26 tumor models and C57BL/6, Balb/c, nude, and mice were used to analyze the in vivo therapy efficacy and impact on tumor immune microenvironment by clotrimazole treatment.

Results: By screening a group of small molecule inhibitors and the US Food and Drug Administration (FDA)-approved drugs, we identified that clotrimazole, an antifungal drug, could promote DC-mediated antigen presentation and enhance T cell response. Mechanistically, clotrimazole acted on hexokinase 2 to regulate lactate metabolic production and enhanced the lysosome pathway and expression in DCs subsequently induced DC maturation and T cell activation. Importantly, in vivo clotrimazole administration induced intratumor immune infiltration and inhibited tumor growth depending on both DCs and CD8+ T cells and potentiated the antitumor efficacy of anti-PD1 antibody.

Conclusions: Our findings showed that clotrimazole could trigger DC activation via the lactate-lysosome axis to promote antigen cross-presentation and could be used as a potential combination therapy approach to improving the therapeutic efficacy of anti-PD1 immunotherapy.
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http://dx.doi.org/10.1136/jitc-2020-002155DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8141455PMC
May 2021

A yolk-shell [email protected]@carbon nanochain as shuttle effect suppressive and volume-change accommodating sulfur host for long-life lithium-sulfur batteries.

Nanoscale 2021 Apr;13(16):7744-7750

Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Provincial Engineering Laboratory for New-Energy Vehicle Battery Energy-Storage Materials, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, Anhui 241002, P.R. China.

A lithium-sulfur (Li-S) battery is considered a promising next-generation secondary battery owing to its high theoretical capacity and energy density. However, the volume change and poor conductivity of sulfur, and the shuttle effect, restrict its practical applications. Herein, we develop a yolk-shell [email protected]@C nanochain as the Li-S battery cathode in which sulfur is encapsulated between the Fe3O4 core and the carbon shell. After cycling 500 times at 0.2C, the [email protected]@C nanochains exhibit a stable capacity of 625 mA h g-1 and a coulombic efficiency exceeding 99.8%. When measuring at temperatures of -5 and 45 °C, the capacities remain stable, and a well-reversible rate performance under repeated testing for three rounds is also achieved. Furthermore, density functional theory (DFT) calculations show large adsorption energies of Fe3O4 towards polysulfides, indicating the capability of suppressing the shuttle effect during long-term charge and discharge.
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http://dx.doi.org/10.1039/d1nr00658dDOI Listing
April 2021

A Self-Healing Flexible Quasi-Solid Zinc-Ion Battery Using All-In-One Electrodes.

Adv Sci (Weinh) 2021 Apr 14;8(8):2004689. Epub 2021 Feb 14.

National Laboratory of Solid State Microstructures College of Engineering and Applied Sciences Nanjing University Nanjing Jiangsu 210093 P. R. China.

Self-healing and flexibility are significant for many emerging applications of secondary batteries, which have attracted broad attention. Herein, a self-healing flexible quasi-solid Zn-ion battery composing of flexible all-in-one cathode (VS nanosheets growing on carbon cloth) and anode (electrochemically deposited Zn nanowires), and a self-healing hydrogel electrolyte, is presented. The free-standing all-in-one electrodes enable a high capacity and robust structure during flexible transformation of the battery, and the hydrogel electrolyte possesses a good self-healing performance. The presented battery remains as a high retention potential even after healing from being cut into six pieces. When bending at 60°, 90°, and 180°, the battery capacities remain 124, 125, and 114 mAh g, respectively, cycling at a current density of 50 mA g. Moreover, after cutting and healing twice, the battery still delivers a stable capacity, indicating a potential use of self-healing and wearable electronics.
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http://dx.doi.org/10.1002/advs.202004689DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8061350PMC
April 2021

Ab initio determination of crystal stability of di-p-tolyl disulfide.

Sci Rep 2021 Mar 29;11(1):7076. Epub 2021 Mar 29.

Key Laboratory for Thin Film and Microfabrication of Ministry of Education, Department of Micro/Nano-Electronics, Shanghai Jiao Tong University, Shanghai, 200240, China.

With the rapid growth of energy demand and the depletion of existing energy resources, the new materials with superior performances, low costs and environmental friendliness for energy production and storage are explored. Di-p-tolyl disulfide (p-TolS) is a typical lubricating material, which has been applied in the field of energy storage. The conformational properties and phase transformations of p-TolS have been studied by pioneers, but their polymorphs and the polymorphism induced crystal structure changes require further analysis. In this study, we perform the crystal structural screening, prediction and optimization of p-TolS crystal with quantum mechanical calculations, i.e., density functional theory (DFT) and second-order Møller-Plesset perturbation (MP2) methods. A series of crystal structures with different molecular arrangements are generated based on the crystal structure screening. As compared to long-established lattice energy calculation, we take an advantage of using more accurate technique, which is Gibbs free energy calculation. It considers the effects of entropy and temperature to predict the crystal structures and energy landscape. By comparing the Gibbs free energies between predicted and experimental structures, we found that phase α is the most stable structure for p-TolS crystal at ambient temperature and standard atmospheric pressure. Furthermore, we provide an efficient method to discriminate different polymorphs that are otherwise difficult to be identified based on the Raman/IR spectra. The proposed work enable us to evaluate the quality of various crystal polymorphs rapidly.
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http://dx.doi.org/10.1038/s41598-021-86519-1DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8007795PMC
March 2021

Delivery of mRNA vaccine with a lipid-like material potentiates antitumor efficacy through Toll-like receptor 4 signaling.

Proc Natl Acad Sci U S A 2021 02;118(6)

State Key Laboratory of Oncology in South China, Collaborative Innovation Center for Cancer Medicine, Sun Yat-sen University Cancer Center, Guangzhou 510060, China;

Intracellular delivery of messenger RNA (mRNA)-based cancer vaccine has shown great potential to elicit antitumor immunity. To achieve robust antitumor efficacy, mRNA encoding tumor antigens needs to be efficiently delivered and translated in dendritic cells with concurrent innate immune stimulation to promote antigen presentation. Here, by screening a group of cationic lipid-like materials, we developed a minimalist nanovaccine with C1 lipid nanoparticle (LNP) that could efficiently deliver mRNA in antigen presenting cells with simultaneous Toll-like receptor 4 (TLR4) activation and induced robust T cell activation. The C1 nanovaccine entered cells via phagocytosis and showed efficient mRNA-encoded antigen expression and presentation. Furthermore, the C1 lipid nanoparticle itself induced the expression of inflammatory cytokines such as IL-12 via stimulating TLR4 signal pathway in dendritic cells. Importantly, the C1 mRNA nanovaccine exhibited significant antitumor efficacy in both tumor prevention and therapeutic vaccine settings. Overall, our work presents a C1 LNP-based mRNA cancer nanovaccine with efficient antigen expression as well as self-adjuvant property, which may provide a platform for developing cancer immunotherapy for a wide range of tumor types.
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http://dx.doi.org/10.1073/pnas.2005191118DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8017939PMC
February 2021

General Liquid-Driven Coaxial Flow Focusing Preparation of Novel Microcapsules for Rechargeable Magnesium Batteries.

Adv Sci (Weinh) 2021 Jan 27;8(2):2002298. Epub 2020 Nov 27.

National Key Laboratory of Science and Technology on Micro/Nano Fabrication Key Laboratory for Thin Film and Microfabrication of Ministry of Education Department of Micro/Nano-electronics Shanghai Jiao Tong University Shanghai 200240 P. R. China.

Magnesium batteries have been considered promising candidates for next-generation energy storage systems owing to their high energy density, good safety without dendrite formation, and low cost of magnesium resources. However, high-performance cathodes with stable capacity, good conductivity, and fast ions transport are needed, since many conventional cathodes possess a low performance and poor preparation controllability. Herein, a liquid-driven coaxial flow focusing (LDCFF) approach for preparing a novel microcapsule system with controllable size, high loading, and stable magnesium-storage performance is presented. Taking the MoS-infilled microcapsule as a case study, the magnesium battery cathode based on the microcapsules displays a capacity of 100 mAh g after 100 cycles. High capacity retention is achieved at both low and high temperatures of -10, ‒5, and 45 °C, and a stable rate-performance is also obtained. The influences of the liquid flow rates on the size and shell thickness of the microcapsules are investigated; and electron and ion diffusion properties are also studied by first-principle calculations. The presented LDCFF method is quite general, and the high performance of the microcapsules enables them to find broad applications for making emerging energy-storage materials and secondary battery systems.
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http://dx.doi.org/10.1002/advs.202002298DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7816708PMC
January 2021

xCT: A Critical Molecule That Links Cancer Metabolism to Redox Signaling.

Mol Ther 2020 11 2;28(11):2358-2366. Epub 2020 Sep 2.

Sun Yat-sen University Cancer Center, State Key Laboratory of Oncology in South China, Collaborative Innovation Center for Cancer Medicine, 651 Dongfeng East Road, Guangzhou 510060, China; Metabolic Innovation Center, Sun Yat-sen University Zhongshan School of Medicine, 74 Zhongshan 2nd Road, Guangzhou 510080, China. Electronic address:

System x cystine/glutamate antiporter, composed of a light-chain subunit (xCT, SLC7A11) and a heavy-chain subunit (CD98hc, SLC3A2), is mainly responsible for the cellular uptake of cystine in exchange for intracellular glutamate. In recent years, the xCT molecule has been found to play an important role in tumor growth, progression, metastasis, and multidrug resistance in various types of cancer. Interestingly, xCT also exhibits an essential function in regulating tumor-associated ferroptosis. Despite significant progress in targeting the system x transporter in cancer treatment, the underlying mechanisms still remain elusive. It is also unclear why solid tumors are more sensitive to xCT inhibitors such as sulfasalazine, as compared to hematological malignancies. This review mainly focuses on the role of xCT cystine/glutamate transporter in regard to tumor growth, chemoresistance, tumor-selective ferroptosis, and the mechanisms regulating xCT gene expression. The potential therapeutic implications of targeting the system x and its combination with chemotherapeutic agents or immunotherapy to suppress tumor growth and overcome drug resistance are also discussed.
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http://dx.doi.org/10.1016/j.ymthe.2020.08.021DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7647670PMC
November 2020

NRIP3 upregulation confers resistance to chemoradiotherapy in ESCC via RTF2 removal by accelerating ubiquitination and degradation of RTF2.

Oncogenesis 2020 Aug 24;9(8):75. Epub 2020 Aug 24.

State Key Laboratory of Oncology in South China, Collaborative Innovation Center for Cancer Medicine, Sun Yat-sen University Cancer Center, Guangzhou, China.

Esophageal squamous cell carcinoma (ESCC) is a common malignant cancer worldwide. Despite recent improvements in surgical techniques and adjuvant therapies, the prognosis of patients with advanced ESCC remains poor. Resistance to chemoradiotherapy (CRT) remains a major cause of treatment failure for advanced ESCC patients. Here, we report that NRIP3 (nuclear receptor interacting protein 3) promotes ESCC tumor cell growth and resistance to CRT in ESCC cells by increasing and binding to DDI1 (DNA-damage inducible 1 homolog 1) and RTF2 (homologous to Schizosaccharomyces pombe Rtf2), and accelerating the removal of RTF2, which is a key determinant for the ability of cells to manage replication stress. In addition, we found that NRIP3 could increase DDI1 expression via PPARα. The NRIP3-PPARα-DDI1-RTF2 axis represents a protective molecular pathway in ESCC cells that mediates resistance to replication stress signals induced by chemoradiotherapy. In addition, elevated NRIP3 is associated with the poor clinical outcome of ESCC patients receiving radiotherapy and/or cisplatin-based chemotherapy. Our study therefore reveals that NRIP3 is a prognostic factor in ESCC and could have some predictive value to select patients who benefit from CRT treatment. A common mechanism that protects ESCC tumor cells from DNA damage induced by CRT is also revealed in this study.
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http://dx.doi.org/10.1038/s41389-020-00260-4DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7445249PMC
August 2020

A novel [email protected]@hydrogel yolk-shell particle with a high sulfur content for volume-accommodable and polysulfide-adsorptive lithium-sulfur battery cathodes.

Nanotechnology 2020 Nov 18;31(45):455402. Epub 2020 Aug 18.

Key Laboratory of Functional Molecular Solids of the Ministry of Education, Anhui Laboratory of Molecule-Based Materials, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, Anhui 241000, People's Republic of China.

High-energy-density secondary batteries are required for many applications such as electric vehicles. Lithium-sulfur (Li-S) batteries are receiving broad attention because of their high theoretical energy density. However, the large volume change of sulfur during cycling, poor conductivity, and the shuttle effect of sulfides severely restrict the Li-storage performance of Li-S batteries. Herein, we present a novel core-shell nanocomposite consisting of a sulfur core and a hydrogel polypyrrole (PPy) shell, enabling an ultra-high sulfur content of about 98.4% within the composite, which greatly exceeds many other conventional composites obtained by coating sulfur onto some hosts. In addition, the void inside the core-shell structure effectively accommodates the volume change; the conductive PPy shell improves the conductivity of the composite; and PPy is able to adsorb polysulfides, suppressing the shuttle effect. After cycling for 200 cycles, the prepared [email protected]@PPy composite retains a stable capacity of 650 mAh g, which is higher than the bare sulfur particles. The composite also exhibits a fast Li ion diffusion coefficient. Furthermore, the density functional theory calculations show the PPy shell is able to adsorb polysulfides efficiently, with a large adsorption energy and charge density transfer.
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http://dx.doi.org/10.1088/1361-6528/abaa72DOI Listing
November 2020

Seasonal variation and secondary formation of size-segregated aerosol water-soluble inorganic ions in a coast megacity of North China Plain.

Environ Sci Pollut Res Int 2020 Jul 7;27(21):26750-26762. Epub 2020 May 7.

State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC), Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, 100029, China.

The aerosol samples of water-soluble inorganic ions (WSIs), including SO, NO, NH, Cl, K, Na, Ca, and Mg in size-segregated particulate matter (PM), were collected by an Anderson sampler (with 8 nominal cut-sizes ranged from 0.43 to 9.0 μm) in urban Tianjin during 2013-2014. The results showed that particulate matters in the fine mode (PM, Dp < 2.1 μm) comprised large part of mass concentrations of aerosols, and the water-soluble ionic species in the fine mode were 47.07 ± 14.29 μg m (spring), 67.87 ± 28.74 μg m (summer), 86.60 ± 48.53 μg m (autumn), and 104.16 ± 51.76 μg m (winter), respectively, which accounted for 59.5%, 63.3%, 71.9%, and 71.4% of the PM mass concentrations. Secondary pollutants of SO, NO, and NH (SNA) were the dominant contributors of WSIs, which showed a bimodal size distribution in each season, with the larger peak appeared in the size fraction of 0.65-1.1 μm and the smaller one in 3.3-5.8 μm fraction. SNA concentrations in lightly polluted days (LPD) and heavily polluted days (HPD) were observably higher than non-polluted days (NPD), especially in the fine mode, with the peak diameter moving from 0.43-0.65 μm on NPD to 0.65-1.1 μm on LPD and HPD. The correlation analysis between NH, NO, and SO suggested that almost all SO and NO for fine particles had been completely neutralized by NH, and primarily existed in the forms of (NH)SO and NHNO. The sulfur oxidation ratio (SOR) and nitrogen oxidation ratio (NOR) on LPD and HPD in fine mode were observably higher than those on NPD, especially in the range of 0.65-1.1 μm and 1.1-2.1 μm. Furthermore, SOR and NOR values in the size fraction of 0.43-3.3 μm increase as the RH elevated, especially in 0.43-2.1 μm, where RH was significantly positive correlated with SOR and NOR, indicating the significant contributions of heterogeneous processes to the secondary formation of SO and NO. These results suggested an enhanced formation ability of secondary pollutants under high RH in the coast city. Therefore, controlling the precursors of SNA, such as SO and NOx, would be more effective to reduce the fine particulate pollution in the coast megacity of Tianjin.
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http://dx.doi.org/10.1007/s11356-020-09052-0DOI Listing
July 2020

A novel silicon nanoparticles-infilled capsule prepared by an oil-in-water emulsion strategy for high-performance Li-ion battery anodes.

Nanotechnology 2020 Aug 6;31(33):335403. Epub 2020 May 6.

Key Laboratory of Functional Molecular Solids of the Ministry of Education, Anhui Laboratory of Molecule-Based Materials, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, Anhui 241000 People's Republic of China.

Conventional approaches for preparing yolk-shell nanostructures require complicated procedures such as multi-step coatings and template removal. Herein, we present a new and general strategy for making yolk-shell nanocomposites based on an oil-in-water emulsion system. As a demonstrating case, silicon nanoparticles were dispersed in an oil phase which was in an oil-in-water emulsion; then the oil/water interface was in-situ polymerized to form microcapsules. After carbonization, the shell of microcapsules was formed. The Li-ion battery anodes based on the microcapsules exhibit a good electrochemical performance including stable capacity and high rate-performance. The capacity remains 1100 mAh g after 500 cycles at a current density of 1.9 A g, along with a Coulombic efficiency of ≈ 99.9%. In addition, the method presented here is general, which is applicable for the synthesis of many yolk shell-structured nanocomposites.
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http://dx.doi.org/10.1088/1361-6528/ab90b9DOI Listing
August 2020

Ab Initio Prediction of the Phase Transition for Solid Ammonia at High Pressures.

Sci Rep 2020 May 5;10(1):7546. Epub 2020 May 5.

Key laboratory for Thin Film and Microfabrication of the Ministry of Education, Department of Micro/Nano-electronics, Shanghai Jiao Tong University, Shanghai, 200240, China.

Ammonia is one of the most basic components on the planet and its high-pressure characteristics play an important role in planetary science. Solid ammonia crystals frequently adopt multiple distinct polymorphs exhibiting different properties. Predicting the crystal structure of these polymorphs and under what thermodynamic conditions these polymorphs are stable would be of great value to environmental industry and other fields. Theoretical calculations based on the classical force fields and density-functional theory (DFT) are versatile methods but lack of accurate description of weak intermolecular interactions for molecular crystals. In this study, we employ an ab initio computational study on the solid ammonia at high pressures, using the second-order Møller-Plesset perturbation (MP2) theory and the coupled cluster singles, doubles, and perturbative triples (CCSD(T)) theory along with the embedded fragmentation method. The proposed algorithm is capable of performing large-scale calculations using high-level wavefunction theories, and accurately describing covalent, ionic, hydrogen bonding, and dispersion interactions within molecular crystals, and therefore can predict the crystal structures, Raman spectra and phase transition of solid ammonia phases I and IV accurately. We confirm the crystal structures of solid ammonia phases I and IV that have been controversial for a long time and predict their phase transition that occurs at 1.17 GPa and 210 K with small temperature dependence, which is in line with experiment.
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http://dx.doi.org/10.1038/s41598-020-64030-3DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7200730PMC
May 2020

An oriented laterally-growing NiCoO nanowire array on a FeO microdisc as a high-capacity and excellent rate-performance secondary battery anode.

Chem Commun (Camb) 2020 Feb;56(17):2618-2621

Key Laboratory for Thin Film and Micro Fabrication of the Ministry of Education, Department of Micro/Nano Electronics, Shanghai Jiao Tong University, Shanghai 200240, P. R. China and Center for High-Performance Computing, Shanghai Jiao Tong University, Shanghai 200240, P. R. China.

A novel hierarchical composite consisting of an ordered NiCo2O4 nanowire array growing on the lateral side of a Fe2O3 microdisc is presented, which was confirmed by X-ray holography technology on a synchrotron radiation station. The composite-based Li-ion battery anode exhibits a high capacity of 1528 mA h g-1 after 200 cycles at 0.2C, a recoverable rate-performance after repeated tests, and robust mechanical properties.
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http://dx.doi.org/10.1039/d0cc00553cDOI Listing
February 2020

Phase Transition of Ice at High Pressures and Low Temperatures.

Molecules 2020 Jan 23;25(3). Epub 2020 Jan 23.

National Key Laboratory of Science and Technology on Micro/Nano Fabrication, Key laboratory for Thin Film and Microfabrication of the Ministry of Education, Department of Micro/Nano-electronics, Shanghai Jiao Tong University, Shanghai 200240, China.

The behavior of ice under extreme conditions undergoes the change of intermolecular binding patterns and leads to the structural phase transitions, which are needed for modeling the convection and internal structure of the giant planets and moons of the solar system as well as H2O-rich exoplanets. Such extreme conditions limit the structural explorations in laboratory but open a door for the theoretical study. The ice phases IX and XIII are located in the high pressure and low temperature region of the phase diagram. However, to the best of our knowledge, the phase transition boundary between these two phases is still not clear. In this work, based on the second-order Møller-Plesset perturbation (MP2) theory, we theoretically investigate the ice phases IX and XIII and predict their structures, vibrational spectra and Gibbs free energies at various extreme conditions, and for the first time confirm that the phase transition from ice IX to XIII can occur around 0.30 GPa and 154 K. The proposed work, taking into account the many-body electrostatic effect and the dispersion interactions from the first principles, opens up the possibility of completing the ice phase diagram and provides an efficient method to explore new phases of molecular crystals.
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http://dx.doi.org/10.3390/molecules25030486DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7037513PMC
January 2020

An artificial sea urchin with hollow spines: improved mechanical and electrochemical stability in high-capacity Li-Ge batteries.

Nanoscale 2020 Mar 24;12(10):5812-5816. Epub 2020 Jan 24.

Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Laboratory of Molecule-Based Materials, Key Laboratory of Electrochemical Clean Energy of Anhui Higher Education Institutes, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, Anhui 241000, P.R. China.

Metallic germanium (Ge) as the anode can deliver a high specific capacity and high rate capability in lithium ion batteries. However, the large volume expansion largely restrains its further application. Herein, we constructed a three-dimensional sea urchin structure consisting of double layered Ge/TiO nanotubes as the spines via a ZnO template-removing method, which displays a capacity as high as 1060 mA h g over 130 cycles. The robust, hollow oxide backbone serves as a strong support to accommodate the morphological change of Ge while the enhanced electron-transfer kinetics is attributed to the Ge content and the intimate contact between Ge and TiO during charging/discharging, which were confirmed using in situ transmission electronic microscopy observations and first-principles simulations. In addition, a high capacity retention of batteries using this hybrid composite as the anode was also achieved at low temperature.
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http://dx.doi.org/10.1039/c9nr09107fDOI Listing
March 2020

Electrodeposition Technologies for Li-Based Batteries: New Frontiers of Energy Storage.

Adv Mater 2020 Jul 30;32(27):e1903808. Epub 2019 Sep 30.

National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Collaborative Innovation Center of Advanced Microstructures, Institute of Materials Engineering, Nanjing University, Nanjing, 210093, Jiangsu, China.

Electrodeposition induces material syntheses on conductive surfaces, distinguishing it from the widely used solid-state technologies in Li-based batteries. Electrodeposition drives uphill reactions by applying electric energy instead of heating. These features may enable electrodeposition to meet some needs for battery fabrication that conventional technologies can rarely achieve. The latest progress of electrodeposition technologies in Li-based batteries is summarized. Each component of Li-based batteries can be electrodeposited or synthesized with multiple methods. The advantages of electrodeposition are the main focus, and they are discussed in comparison with traditional technologies with the expectation to inspire innovations to build better Li-based batteries. Electrodeposition coats conformal films on surfaces and can control the film thickness, providing an effective approach to enhancing battery performance. Engineering interfaces by electrodeposition can stabilize the solid electrolyte interphase (SEI) and strengthen the adhesion of active materials to substrates, thereby prolonging the battery longevity. Lastly, a perspective of future studies on electrodepositing batteries is provided. The significant merits of electrodeposition should greatly advance the development of Li-based batteries.
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http://dx.doi.org/10.1002/adma.201903808DOI Listing
July 2020

A novel spring-structured coaxial hierarchical [email protected] nanowire as a lithium-ion battery anode and its in situ real-time lithiation.

Nanotechnology 2020 Jan 26;31(3):035401. Epub 2019 Sep 26.

Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Laboratory of Molecule-Based Materials, Key Laboratory of Electrochemical Clean Energy of Anhui Higher Education Institutes, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, Anhui 241000, People's Republic of China.

High capacity and stable anodes are demanded since the current graphite-based anode does not meet the high-performance requirements of emerging Li-ion battery systems. Herein, we present a novel spring-shaped hierarchical [email protected] nanowire composite, which exhibits good Li-storage performance. The special structure is able to effectively accommodate the change in structure during charge-discharge, and the coaxial hierarchical morphology enables rapid Li ion and electron transfer. The spring-shaped [email protected] anode exhibits a capacity of 770 mAh g, along with a high Coulombic efficiency of 99.8% after 400 cycles. A stable rate performance even after three rounds of measurements is also achievable. In addition, the real-time lithiation of the [email protected] composite is investigated through an in situ transmission electron microscopy technology, which demonstrates the stable structure of the spring-shaped [email protected] composite during the rapid lithiation process.
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http://dx.doi.org/10.1088/1361-6528/ab4848DOI Listing
January 2020

Synthesis of Uniform Alkane-Filled Capsules with a High Under-Cooling Performance and Their Real-Time Optical Properties.

Polymers (Basel) 2019 Jan 24;11(2). Epub 2019 Jan 24.

Beckman Institute for Advanced Science and Technology, University of Illinois at Urbana-Champaign, Urbana, IL 61801, USA.

Encapsulating under-cooling materials has been a promising strategy to address the compatibility issue with a surrounding matrix. Herein, we present the synthesis of a uniform alkane-infilled capsule system that shows obvious under-cooling properties. As demonstrating examples, -hexadecane was selected as a liquid alkane and -eicosane as a solid in our systems as core materials via in-situ polymerization, respectively. The under-cooling properties of capsules were investigated using differential scanning calorimetry, real-time optical observations with two polarizers, and molecular modeling. The -hexadecane encapsulated capsules exhibited a large under-cooling temperature range of 20 °C between melt and crystallization, indicating potential applications for structure-transformation energy storage. In addition, molecular modeling calculations confirmed that the solid forms of -hexadecane and -eicosane are more stable than their liquid forms. From liquid to solid form, the -hexadecane and -eicosane release energies were 4.63 × 10³ and 4.95 × 10³ J·g, respectively.
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http://dx.doi.org/10.3390/polym11020199DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6418806PMC
January 2019

Three-Dimensionally Porous Li-Ion and Li-S Battery Cathodes: A Mini Review for Preparation Methods and Energy-Storage Performance.

Nanomaterials (Basel) 2019 Mar 15;9(3). Epub 2019 Mar 15.

Key Laboratory for Thin Film and Micro Fabrication, Ministry of Education, Department of Micro/Nano Electronics, Shanghai Jiao Tong University, Shanghai 200240, China.

Among many types of batteries, Li-ion and Li-S batteries have been of great interest because of their high energy density, low self-discharge, and non-memory effect, among other aspects. Emerging applications require batteries with higher performance factors, such as capacity and cycling life, which have motivated many research efforts on constructing high-performance anode and cathode materials. Herein, recent research about cathode materials are particularly focused on. Low electron and ion conductivities and poor electrode stability remain great challenges. Three-dimensional (3D) porous nanostructures commonly exhibit unique properties, such as good Li⁺ ion diffusion, short electron transfer pathway, robust mechanical strength, and sufficient space for volume change accommodation during charge/discharge, which make them promising for high-performance cathodes in batteries. A comprehensive summary about some cutting-edge investigations of Li-ion and Li-S battery cathodes is presented. As demonstrative examples, LiCoO₂, LiMn₂O₄, LiFePO₄, V₂O₅, and LiNiCoMnO₂ in pristine and modified forms with a 3D porous structure for Li-ion batteries are introduced, with a particular focus on their preparation methods. Additionally, S loaded on 3D scaffolds for Li-S batteries is discussed. In addition, the main challenges and potential directions for next generation cathodes have been indicated, which would be beneficial to researchers and engineers developing high-performance electrodes for advanced secondary batteries.
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http://dx.doi.org/10.3390/nano9030441DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6474075PMC
March 2019

A bee pupa-infilled honeycomb structure-inspired LiMnSiO cathode for high volumetric energy density secondary batteries.

Chem Commun (Camb) 2019 Mar;55(25):3582-3585

Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, Anhui 241002, P. R. China.

Emerging power batteries with both high volumetric energy density and fast charge/discharge kinetics are required for electric vehicles. The rapid ion/electron transport of mesostructured electrodes enables a high electrochemical activity in secondary batteries. However, the typical low fraction of active materials leads to a low volumetric energy density. Herein, we report a novel biomimetic "bee pupa infilled honeycomb"-structured 3D mesoporous cathode. We found previously the maximum active material filing fraction of an opal template before pinch-off was about 25%, whereas it could be increased to ∼90% with the bee pupa-infilled honeycomb-like architecture. Importantly, even with a high infilling fraction, fast Li+/e- transport kinetics and robust mechanical property were achievable. As the demonstration, a bee pupa infilled honeycomb-shaped Li2MnSiO4/C cathode was constructed, which delivered a high volumetric energy density of 2443 W h L-1. The presented biomimetic bee pupa infilled honeycomb configuration is applicable for a broad set of both cathodes and anodes in high energy density batteries.
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http://dx.doi.org/10.1039/c9cc00729fDOI Listing
March 2019

A novel biomimetic dandelion structure-inspired carbon nanotube coating with sulfur as a lithium-sulfur battery cathode.

Nanotechnology 2019 Apr 14;30(15):155401. Epub 2019 Jan 14.

Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, Anhui 241002, People's Republic of China.

Lithium-sulfur (Li-S) batteries have attracted considerable attention because of their high theoretical energy density. However, poor conductivity and a large volume change in S during cycling, together with a shuttle effect of polysulfides, severely restrict the battery performance, and remain a great challenge. Herein, inspired by a natural dandelion structure, we present a novel biomimetic S-coated carbon nanotube composite consisting of dandelion-like three-dimensional carbon nanotubes coated with S particles on the surface. Carbon nanotubes provide high-speed electron transfer pathways for S during cycling, while the special dandelion-like morphology provides a suitable environment for accommodating the volume change in S upon charge-discharge. The dandelion-like S-coated carbon nanotube-based Li-S batteries exhibit a stable capacity exceeding 760 mAh g after 500 cycles at 0.1 C, along with a Coulombic efficiency as high as 99.9%. Even under repeated rounds of rate-performance measurements, and cycling at different charge versus discharge rates, the batteries retain high capacities and good recovery capabilities. In addition, the proportion of capacitive contribution in the overall capacity is high, indicating a good reversible capacity provided by the composite.
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http://dx.doi.org/10.1088/1361-6528/aafe46DOI Listing
April 2019

An all-in-one Sn-Co alloy as a binder-free anode for high-capacity batteries and its dynamic lithiation in situ.

Chem Commun (Camb) 2019 Jan;55(4):529-532

Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, Anhui 241002, P. R. China.

A three-dimensional all-in-one Sn-Co alloy anode is reported for the first time, which delivers a high capacity along with a stable coulombic efficiency as well as good temperature tolerance. The binder-free electrode eliminates the complexity of conventional slurry preparation while maintaining an integrated scaffold, which provides space to accommodate volume expansion, as confirmed by an in situ transmission electron microscopy study.
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http://dx.doi.org/10.1039/c8cc07868hDOI Listing
January 2019

Low Interface Energies Tune the Electrochemical Reversibility of Tin Oxide Composite Nanoframes as Lithium-Ion Battery Anodes.

ACS Appl Mater Interfaces 2018 Oct 19;10(43):36892-36901. Epub 2018 Oct 19.

National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Collaborative Innovation Center of Advanced Microstructures, Institute of Materials Engineering , Nanjing University , Nanjing 210093 , Jiangsu , China.

The conversion reaction of lithia can push up the capacity limit of tin oxide-based anodes. However, the poor reversibility limits the practical applications of lithia in lithium-ion batteries. The latest reports indicate that the reversibility of lithia has been appropriately promoted by compositing tin oxide with transition metals. The underlying mechanism is not revealed. To design better anodes, we studied the nanostructured metal/LiO interfaces through atomic-scale modeling and proposed a porous nanoframe structure of Mn/Sn binary oxides. The first-principles calculation implied that because of a low interface energy of metal/LiO, Mn forms smaller particles in lithia than Sn. Ultrafine Mn nanoparticles surround Sn and suppress the coarsening of Sn particles. Such a composite design and the resultant interfaces significantly enhance the reversible Li-ion storage capabilities of tin oxides. The synthesized nanoframes of manganese tin oxides exhibit an initial capacity of 1620.6 mA h g at 0.05 A g. Even after 1000 cycles, the nanoframe anode could deliver a capacity of 547.3 mA h g at 2 A g. In general, we demonstrated a strategy of nanostructuring interfaces with low interface energy to enhance the Li-ion storage capability of binary tin oxides and revealed the mechanism of property enhancement, which might be applied to analyze other tin oxide composites.
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http://dx.doi.org/10.1021/acsami.8b11062DOI Listing
October 2018
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