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1.
Adv Sci (Weinh) ; : e2400829, 2024 May 05.
Article in English | MEDLINE | ID: mdl-38704695

ABSTRACT

Self-assembling peptides have numerous applications in medicine, food chemistry, and nanotechnology. However, their discovery has traditionally been serendipitous rather than driven by rational design. Here, HydrogelFinder, a foundation model is developed for the rational design of self-assembling peptides from scratch. This model explores the self-assembly properties by molecular structure, leveraging 1,377 self-assembling non-peptidal small molecules to navigate chemical space and improve structural diversity. Utilizing HydrogelFinder, 111 peptide candidates are generated and synthesized 17 peptides, subsequently experimentally validating the self-assembly and biophysical characteristics of nine peptides ranging from 1-10 amino acids-all achieved within a 19-day workflow. Notably, the two de novo-designed self-assembling peptides demonstrated low cytotoxicity and biocompatibility, as confirmed by live/dead assays. This work highlights the capacity of HydrogelFinder to diversify the design of self-assembling peptides through non-peptidal small molecules, offering a powerful toolkit and paradigm for future peptide discovery endeavors.

2.
Cell Death Dis ; 15(5): 319, 2024 May 06.
Article in English | MEDLINE | ID: mdl-38710705

ABSTRACT

Argininosuccinate synthase (ASS1), a critical enzyme in the urea cycle, acts as a tumor suppressor in many cancers. To date, the anticancer mechanism of ASS1 has not been fully elucidated. Here, we found that phosphoglycerate dehydrogenase (PHGDH), a key rate-limiting enzyme in serine synthesis, is a pivotal protein that interacts with ASS1. Our results showed that ASS1 directly binds to PHGDH and promotes its ubiquitination-mediated degradation to inhibit serine synthesis, consequently suppressing tumorigenesis. Importantly, the tumor suppressive effects of ASS1 were strongly abrogated by PHGDH knockout. In addition, ASS1 knockout and knockdown partially rescued cell proliferation when serine and glycine were depleted, while the inhibitory effect of ASS1 overexpression on cell proliferation was restored by the addition of serine and glycine. These findings unveil a novel role of ASS1 and suggest that the ASS1/PHGDH serine synthesis pathway is a promising target for cancer therapy.


Subject(s)
Argininosuccinate Synthase , Cell Proliferation , Phosphoglycerate Dehydrogenase , Serine , Triple Negative Breast Neoplasms , Phosphoglycerate Dehydrogenase/metabolism , Phosphoglycerate Dehydrogenase/genetics , Serine/metabolism , Serine/biosynthesis , Humans , Female , Triple Negative Breast Neoplasms/metabolism , Triple Negative Breast Neoplasms/pathology , Triple Negative Breast Neoplasms/genetics , Animals , Argininosuccinate Synthase/metabolism , Argininosuccinate Synthase/genetics , Cell Line, Tumor , Mice, Nude , Ubiquitination , Mice , Glycine/metabolism
3.
BMC Musculoskelet Disord ; 25(1): 291, 2024 Apr 15.
Article in English | MEDLINE | ID: mdl-38622662

ABSTRACT

OBJECTIVES: The aim of this study was to explore the long non-coding RNA (lncRNA) expression profiles in serum of patients with ankylosing spondylitis (AS). The role of these lncRNAs in this complex autoimmune situation needs to be evaluated. METHODS: We used high-throughput whole-transcriptome sequencing to generate sequencing data from three patients with AS and three normal controls (NC). Then, we performed bioinformatics analyses to identify the functional and biological processes associated with differentially expressed lncRNAs (DElncRNAs). We confirmed the validity of our RNA-seq data by assessing the expression of eight lncRNAs via quantitative reverse transcription polymerase chain reaction (qRT-PCR) in 20 AS and 20 NC samples. We measured the correlation between the expression levels of lncRNAs and patient clinical index values using the Spearman correlation test. RESULTS: We identified 72 significantly upregulated and 73 significantly downregulated lncRNAs in AS patients compared to NC. qRT-PCR was performed to validate the expression of selected DElncRNAs; the results demonstrated that the expression levels of MALAT1:24, NBR2:9, lnc-DLK1-35:13, lnc-LARP1-1:1, lnc-AIPL1-1:7, and lnc-SLC12A7-1:16 were consistent with the sequencing analysis results. Enrichment analysis showed that DElncRNAs mainly participated in the immune and inflammatory responses pathways, such as regulation of protein ubiquitination, major histocompatibility complex class I-mediated antigen processing and presentation, MAPkinase activation, and interleukin-17 signaling pathways. In addition, a competing endogenous RNA network was constructed to determine the interaction among the lncRNAs, microRNAs, and mRNAs based on the confirmed lncRNAs (MALAT1:24 and NBR2:9). We further found the expression of MALAT1:24 and NBR2:9 to be positively correlated with disease severity. CONCLUSION: Taken together, our study presents a comprehensive overview of lncRNAs in the serum of AS patients, thereby contributing novel perspectives on the underlying pathogenic mechanisms of this condition. In addition, our study predicted MALAT1 has the potential to be deeply involved in the pathogenesis of AS.


Subject(s)
MicroRNAs , RNA, Long Noncoding , Spondylitis, Ankylosing , Humans , RNA, Long Noncoding/genetics , Gene Expression Profiling/methods , Spondylitis, Ankylosing/genetics , MicroRNAs/metabolism , Computational Biology/methods , Gene Regulatory Networks , Adaptor Proteins, Signal Transducing/genetics , K Cl- Cotransporters
4.
ACS Appl Mater Interfaces ; 16(2): 2397-2407, 2024 Jan 17.
Article in English | MEDLINE | ID: mdl-38178364

ABSTRACT

Hard carbons (HCs), while a leading candidate for sodium-ion battery (SIB) anode materials, face challenges in their unfavorable sodiation kinetics since the intricate microstructure of HCs complicates the Na+ diffusion channel. Herein, a Hovenia dulcis-derived HC realizes a markedly enhanced high-rate performance in virtue of dual-functionalized Ca. The interlayer doped Ca2+ effectively enlarges the interlayer spacing, while the in situ-formed CaSe templates induce the formation of hierarchical pore structures and intrinsic defects, significantly providing fast Na+ diffusion channels and abundant active sites and thus enhancing the sodium storage kinetics. Achieved by the synergistic effect of regulation of intrinsic microcrystalline and pore structures, the optimized HC shows remarkable performance enhancements, including a high reversible capacity of 350.3 mA h g-1 after 50 cycles at 50 mA g-1, a high-capacity retention rate of 95.3% after 1000 cycles, and excellent rate performance (108.4 mA h g-1 at 2 A g-1). This work sheds light on valuable insight into the structural adjustment of high-rate HCs, facilitating the widespread utilization of SIBs.

5.
Adv Mater ; 36(7): e2310270, 2024 Feb.
Article in English | MEDLINE | ID: mdl-38014758

ABSTRACT

While cost-effective sodium-ion batteries (SIBs) with crystalline silicon anodes promise high theoretical capacities, they perform poorly because silicon stores sodium ineffectively (capacity <40 mAh g-1 ). To address this issue, herein an atomic-order structural-design tactic is adopted for obtaining unique multilevel gradient-ordered silicon (MGO-Si) by simple electrochemical reconstruction. In situ-formed short-range-, medium-range-, and long-range-ordered structures construct a stable MGO-Si, which contributes to favorable Na-Si interaction and fast ion diffusion channels. These characteristics afford a high reversible capacity (352.7 mAh g-1 at 50 mA g-1 ) and stable cycling performance (95.2% capacity retention after 4000 cycles), exhibiting record values among those reported for pure silicon electrodes. Sodium storage of MGO-Si involves an adsorption-intercalation mechanism, and a stepwise construction strategy of gradient-ordered structure further improves the specific capacity (339.5 mAh g-1 at 100 mA g-1 ). Reconstructed Si/C composites show a high reversible capacity of 449.5 mAh g-1 , significantly better than most carbonaceous anodes. The universality of this design principle is demonstrated for other inert or low-capacity materials (micro-Si, SiO2 , SiC, graphite, and TiO2 ), boosting their capacities by 1.5-6 times that of pristine materials, thereby providing new solutions to facilitate sodium storage capability for better-performing battery designs.

6.
J Cancer ; 14(8): 1350-1361, 2023.
Article in English | MEDLINE | ID: mdl-37283803

ABSTRACT

Chemotherapeutic agents remain the first-line treatment for solid tumors, including lung cancer, but chemotherapy resistance is hampering global efforts to treat this disease. CC-115 is a novel antitumoral compound used in phase I clinical trials. However, it is unclear whether CC-115 is effective against lung adenocarcinoma (LUAD). In the present study, we found that CC-115 induced lytic cell death in A549 and H1650 tumor cells via swelling of cells and formation of large bubbles on the plasma membrane that closely resembled those typical of pyroptosis, a type of programmed cell death linked to chemotherapy. We demonstrated that CC-115 exerts antitumor effects in LUAD through gasdermin E (GSDME)-mediated pyroptosis by acting as a dual inhibitor of DNA-PK and mTOR. CC-115 can inhibit Akt phosphorylation, impairing its inhibitory effect on Bax, thereby inducing pyroptosis via the Bax-mitochondrial intrinsic pathway. CC-115-induced pyroptosis was abrogated by treatment with the Akt activator SC79 or by depletion of Bax. Importantly, CC-115 significantly upregulated the expression of Bax and GSDME-N in a xenograft mouse model, with a reduction in tumor size. Our results revealed that CC-115 suppresses tumor growth by inducing GSDME-mediated pyroptosis through the Akt/Bax-mitochondrial intrinsic pathway, indicating CC-115 as a promising therapeutic agent for LUAD.

7.
Small ; 19(33): e2301230, 2023 Aug.
Article in English | MEDLINE | ID: mdl-37081280

ABSTRACT

In this work, an efficient screening method to select appropriate sintering aids for a wide range of oxide material systems is developed. Consequently, Na2 B4 O7 , NaF, and CuO are selected as sintering aids for sodium super ionic conductor (NASICON)-type Na3 Zr2 Si2 PO12 ceramic to verify the feasibility of the as-proposed method. As evidenced by the results, the sinterability and densification of ceramic matrix are apparently improved. Specifically, Na3 Zr2 Si2 PO12 -7%Na2 B4 O7 , Na3 Zr2 Si2 PO12 -3%NaF, and Na3 Zr2 Si2 PO12 -3%CuO endow much higher room temperature ionic conductivity of 1.03 × 10-3 , 1.61 × 10-3 , and 1.63 × 10-3  S cm-1 , respectively, in comparison with the pristine (7.23 × 10-4  S cm-1 ). The underlying mechanism for the enhanced performance is also discussed. The symmetric sodium cells assembled with sintering aids modified Na3 Zr2 Si2 PO12 ceramic electrolyte exhibit ultra-stable metallic Na plating/stripping at room temperature. Moreover, solid-state sodium batteries paired with Na3 V1.5 Cr0.5 (PO4 )3 cathode active material and modified Na3 Zr2 Si2 PO12 ceramic electrolyte demonstrate superior cycling stability and excellent rate capability. Furthermore, an as-developed strategy can be universally extended to synthesize high-performance oxide ceramics.

8.
Adv Mater ; 35(29): e2300002, 2023 Jul.
Article in English | MEDLINE | ID: mdl-37018163

ABSTRACT

Constructing a homogenous and inorganic-rich solid electrolyte interface (SEI) can efficiently improve the overall sodium-storage performance of hard carbon (HC) anodes. However, the thick and heterogenous SEI derived from conventional ester electrolytes fails to meet the above requirements. Herein, an innovative interfacial catalysis mechanism is proposed to design a favorable SEI in ester electrolytes by reconstructing the surface functionality of HC, of which abundant CO (carbonyl) bonds are accurately and homogenously implanted. The CO (carbonyl) bonds act as active centers that controllably catalyze the preferential reduction of salts and directionally guide SEI growth to form a homogenous, layered, and inorganic-rich SEI. Therefore, excessive solvent decomposition is suppressed, and the interfacial Na+ transfer and structural stability of SEI on HC anodes are greatly promoted, contributing to a comprehensive enhancement in sodium-storage performance. The optimal anodes exhibit an outstanding reversible capacity (379.6 mAh g-1 ), an ultrahigh initial Coulombic efficiency (93.2%), a largely improved rate capability, and an extremely stable cycling performance with a capacity decay rate of 0.0018% for 10 000 cycles at 5 A g-1 . This work provides novel insights into smart regulation of interface chemistry to realize high-performance HC anodes for sodium storage.

9.
Small ; 19(4): e2206194, 2023 Jan.
Article in English | MEDLINE | ID: mdl-36437114

ABSTRACT

The powerful and rapid development of lithium-ion batteries (LIBs) in secondary batteries field makes lithium resources in short supply, leading to rising battery costs. Under the circumstances, sodium-ion batteries (SIBs) with low cost, inexhaustible sodium reserves, and analogous work principle to LIBs, have evolved as one of the most anticipated candidates for large-scale energy storage devices. Thereinto, the applicable electrode is a core element for the smooth development of SIBs. Among various anode materials, metal selenides (MSex ) with relatively high theoretical capacity and unique structures have aroused extensive interest. Regrettably, MSex suffers from large volume expansion and unwished side reactions, which result in poor electrochemistry performance. Thus, strategies such as carbon modification, structural design, voltage control as well as electrolyte and binder optimization are adopted to alleviate these issues. In this review, the synthesis methods and main reaction mechanisms of MSex are systematically summarized. Meanwhile, the major challenges of MSex and the corresponding available strategies are proposed. Furthermore, the recent research progress on layered and nonlayered MSex for application in SIBs is presented and discussed in detail. Finally, the future development focuses of MSex in the field of rechargeable ion batteries are highlighted.

10.
Front Pharmacol ; 13: 956402, 2022.
Article in English | MEDLINE | ID: mdl-36452219

ABSTRACT

Multiple sclerosis (MS) is a chronic inflammatory autoimmune disease characterized by demyelination and neurodegeneration, for which traditional treatment offers limited relief. Microglial/macrophage modulation plays a critical role in the pathogenesis of MS. Oxygen free radical accumulation can induce axonal and nerve cell damage, and further promote MS development. We created a new recombinant protein based on flagellin from Legionella pneumophila named flagellin A with linked C- and N-terminal ends (FLaAN/C), which is an independent intellectual property of our team. We previously showed that FLaAN/C might mitigate radiation-induced damage by inhibiting inflammatory responses and oxidative stress. However, whether FLaAN/C protects against MS remains unknown. Here, we investigated the anti-inflammatory effects of FLaAN/C on mice with experimental autoimmune encephalomyelitis (EAE) induced by oligodendrocyte glycoprotein peptide 35-55 (MOG35-55). The mice were injected intraperitoneally with FLaAN/C after the onset of clinical symptoms, then clinical behavior scores and changes in body weight were recorded daily. The spinal lumbar spine in model mice was enlarged and accompanied by inflammatory cell infiltration and demyelination that were reversed by FLaAN/C. FLaAN/C also induced microglia/macrophages to generate less pro-inflammatory (CD86, iNOS, and TNF-α), and more anti-inflammatory (CD206, IL-10, and Arginase-1) cytokines. These findings suggesting that FLaAN/C promoted microglial/macrophages polarization from the inflammatory M1 to the anti-inflammatory M2 phenotype. Moreover, FLaAN/C inhibited release of the inflammatory cytokines, TNF-α, IL-8, IL-6, IL-17, and IFN-γ. These results indicated that the anti-inflammatory effect of FLaAN/C was associated with the inhibited generation of reactive oxygen species. FLaAN/C downregulated the expression of phosphorylated NF-κB-p65 and prevented downstream NLRP3 inflammasome-mediated pyroptosis. Collectively, these results indicated that FLaAN/C prevents pyroptosis by inhibiting the ROS/NF-κB/NLRP3 signaling pathway, and promotes the microglial/macrophage M1/M2 polarization that significantly alleviated inflammation in mouse models of EAE. Our findings suggested that FLaAN/C could be a promising candidate for MS therapy.

11.
BMC Microbiol ; 22(1): 284, 2022 11 29.
Article in English | MEDLINE | ID: mdl-36443681

ABSTRACT

BACKGROUND: Enterobacter cloacae complex (ECC) is a common opportunistic pathogen and is responsible for causing various infections in humans. Owing to its inducible chromosomal AmpC ß-lactamase (AmpC), ECC is inherently resistant to the 1st- and 2nd- generation cephalosporins. However, whether ß-lactams antibiotics enhance ECC resistance remains unclear. RESULTS: In this study, we found that subinhibitory concentrations (SICs) of cefazolin (CFZ) and imipenem (IMP) can advance the expression of AmpC and enhance its resistance towards ß-lactams through NagZ in Enterobacter cloacae (EC). Further, AmpC manifested a substantial upregulation in EC in response to SICs of CFZ and IMP. In nagZ knockout EC (ΔnagZ), the resistance to ß-lactam antibiotics was rather weakened and the effect of CFZ and IMP on AmpC induction was completely abrogated. NagZ ectopic expression can rescue the induction effects of CFZ and IMP on AmpC and increase ΔnagZ resistance. More importantly, CFZ and IMP have the potential to induce the expression of AmpR's target genes in a NagZ-dependent manner. CONCLUSIONS: Our findings suggest that NagZ is a critical determinant for CFZ and IMP to promote AmpC expression and resistance and that CFZ and IMP should be used with caution since they may aggravate ECC resistance. At the same time, this study further improves our understanding of resistance mechanisms in ECC.


Subject(s)
Cefazolin , Imipenem , Humans , Anti-Bacterial Agents/pharmacology , Cefazolin/pharmacology , Enterobacter cloacae/genetics , Imipenem/pharmacology , Monobactams
12.
ACS Appl Mater Interfaces ; 14(45): 50992-51000, 2022 Nov 16.
Article in English | MEDLINE | ID: mdl-36331897

ABSTRACT

MOF-based materials are a class of efficient precursors for the preparation of heteroatom-doped porous carbon materials that have been widely applied as anode materials for Na-ion batteries. Thereinto, sulfur is often introduced to increase defects and act as an active species to directly react with sodium ions. Although the sulfur introduction and high surface area can synergistically improve capacity and rate capability, the initial Coulombic efficiency (ICE) and electrical conductivity of carbon material are inevitably reduced. Therefore, balancing sodium storage capacity and ICE is still the bottleneck faced by adsorbent carbon materials. Here, sulfur-encapsulated microporous carbon material with nitrogen, sulfur dual-doping (NSPC) is synthesized by postprocessing, achieving the reduced specific surface area by encapsulating sulfur in micropores, and the increased active sites by edge sulfur doping. The synergy between encapsulation and sulfur doping effectively balances specific capacity, rate capability, and ICE. The NSPC material exhibits capacities of 591.5 and 244.2 mAh g-1 at 0.5 and at 10 A g-1, respectively, and the ICE is as high as 72.3%. Moreover, the effect of nitrogen and sulfur on the improvement of electron/ion diffusion kinetics is resonantly demonstrated by density functional theory calculations. This synergistic preparation method may reveal a feasible thought for fabricating excellent-performance adsorption-type carbon materials for Na-ion batteries.

13.
Infect Drug Resist ; 15: 5879-5886, 2022.
Article in English | MEDLINE | ID: mdl-36247739

ABSTRACT

Background: Candidemia caused by Candida tropicalis has more serious adverse consequences and an even higher mortality. Time to positivity (TTP) has been widely used to identify microbial species, resistant microorganisms and distinguish real pathogens and pollutants. However, few studies have demonstrated TTP as a presumptive diagnosis of C. tropicalis in patients with candidemia. Patients and Methods: A retrospective study of 136 episodes of candidemia and simulated blood cultures with 314 episodes of confirmed Candida strains were applied to explore the role of TTPs in diagnosing C. tropicalis. TTPs were recorded as the shorter one if both aerobic and anaerobic vials were positive. Lastly, relationships were tested between TTPs and resistance and initial inocula concentration. Results: For the retrospective study, the mean of TTPs for C. tropicalis from 136 patients with candidemia was significantly shorter than other Candida species. The area under the receiver operating characteristics (ROC) curve was 0.8896 ± 0.030 with a sensitivity of 92.86% and a specificity of 77.87%, respectively, indicating TTPs with a cut-off value of <25.50 h had a strong diagnostic power for C. tropicalis in patients with candidemia. Moreover, TTPs from 314 simulated blood cultures showed similar results as the retrospective study, demonstrating TTP is a powerful diagnostic tool in early diagnosing C. tropicalis in patients with candidemia. Additionally, our results showed no statistical significance between TTPs and initial inocula concentration and resistance of Candida species, suggesting initial inocula concentration does not impact TTPs, and TTPs may not be promising in predicting the resistance of all Candida species. Conclusion: TTP can be employed to early distinguish C. tropicalis from other Candida species in patients with candidemia, which is extremely helpful to initiate empiric antifungal treatments to improve clinical outcomes.

14.
ACS Appl Mater Interfaces ; 14(27): 30786-30795, 2022 Jul 13.
Article in English | MEDLINE | ID: mdl-35776855

ABSTRACT

Solid electrolytes with both interface compatibility and efficient ion transport have been an urgent technical requirement for the practical application of solid-state lithium batteries. Herein, a multifuctional poly(1,3-dioxolane) (PDOL) electrolyte combining the gradient structure from the solid state to the gel state with the Li6.4La3Zr1.4Ta0.6O12 (LLZTO) interfacial modification layer was designed, in which the "solid-to-gel" gradient structure greatly improved the electrode/electrolyte interface compatibility and ion transport, while the solid PDOL and LLZTO layers effectively improved the interface stability of the electrolyte/lithium anode and the inhibition of the lithium dendrites via their high mechanical strength and forming a stable interfacial SEI composite film. This gradient PDOL/LLZTO composite electrolyte possesses a high ionic conductivity of 2.9 × 10-4 S/cm with a wide electrochemical window up to 4.9 V vs Li/Li+. Compared with the pristine PDOL electrolyte and PDOL solid electrolyte membrane coated with a layer of LLZTO, the gradient PDOL/LLZTO composite electrolyte shows better electrode/electrolyte interfacial compatibility, lower interface impedance, and smaller polarization, resulting in enhanced rate and cycle performances. The NCM622/PDOL-LLZTO/Li battery can be stably cycled 200 times at 0.3C and 25 °C. This multifunctional gradient structure design will promote the development of high-performance solid electrolytes and is expected to be widely used in solid-state lithium batteries.

15.
Chem Soc Rev ; 51(11): 4484-4536, 2022 Jun 06.
Article in English | MEDLINE | ID: mdl-35543354

ABSTRACT

Sodium-ion batteries (SIBs) are considered to be strong candidates for large-scale energy storage with the benefits of cost-effectiveness and sodium abundance. Reliable electrolytes, as ionic conductors that regulate the electrochemical reaction behavior and the nature of the interface and electrode, are indispensable in the development of advanced SIBs with high Coulombic efficiency, stable cycling performance and high rate capability. Conventional carbonate-based electrolytes encounter numerous obstacles for their wide application in SIBs due to the formation of a dissolvable, continuous-thickening solid electrolyte interface (SEI) layer and inferior stability with electrodes. Comparatively, ether-based electrolytes (EBEs) are emerging in the secondary battery field with fascinating properties to improve the performance of batteries, especially SIBs. Their stable solvation structure enables highly reversible solvent-co-intercalation reactions and the formation of a thin and stable SEI. However, although EBEs can provide more stable cycling and rapid sodiation kinetics in electrodes, benefitting from their favorable electrolyte/electrode interactions such as chemical compatibility and good wettability, their special chemistry is still being investigated and puzzling. In this review, we provide a thorough and comprehensive overview on the developmental history, fundamental characteristics, superiorities and mechanisms of EBEs, together with their advances in other battery systems. Notably, the relation among electrolyte science, interfacial chemistry and electrochemical performance is highlighted, which is of great significance for the in-depth understanding of battery chemistry. Finally, future perspectives and potential directions are proposed to navigate the design and optimization of electrolytes and electrolyte/electrode interfaces for advanced batteries.

16.
J Colloid Interface Sci ; 620: 199-208, 2022 Aug 15.
Article in English | MEDLINE | ID: mdl-35428002

ABSTRACT

High interface impedance, slow ion transmission, and easy growth of lithium dendrites in solid-state lithium battery are main obstacles to its development and application. Good interface combination and compatibility between electrolyte and electrodes is an important way to solve these problems. In this work, we successfully combined a high ionic conductive polymerized 1,3-dioxolane (PDOL) solid-state electrolyte and a PDOL gel-state electrolyte to form a rigid-flexible composite structural electrolyte and realized the gelation modification of solid electrolyte/electrode interface. This "PDOL SE + PDOL Gel" composite structure not only improves the electrode/electrolyte interfacial contact, reduces the interfacial impedance, but also inhibits the growth of lithium dendrites in the interface between lithium anode and electrolyte by forming an uniform Li-Zr-O and LiF composite protection layer. This composite electrolyte has high ionic conductivity of 5.96 × 10-4 S/cm and wide electrochemical stability window of 5.0 V. The Li/PDOL SE + PDOL Gel/Li cells can be cycled stably for nearly 400 h at a current density of 1.0 mA/cm2. The assembled LiCoO2/PDOL SE + PDOL Gel/Li cells can be cycled for 250 cycles at 0.5 C with a capacity retention of 80%. This PDOL solid/gel composite electrolyte shows high promising commercial application prospect due to its high security performance, excellent interfacial properties and dendrite inhibition ability.

17.
J Colloid Interface Sci ; 608(Pt 2): 1432-1440, 2022 Feb 15.
Article in English | MEDLINE | ID: mdl-34749136

ABSTRACT

Hetero-atoms doping or morphology controlling of carbon nitride (g-C3N4) can availably regulate its electronic band structure and optimize photocatalytic performance under visible light. Herein, sulful (S), phosphorus (P) co-doped porous carbon nitride microtubes (SPCN) was synthesized by using ammonium dihydrogen phosphate and melamine as precursors, in which ammonium dihydrogen phosphate can not only control the morphology of carbon nitride from nanorods to porous microtubes, but also provide a potential P source for P-doped CN. The prepared SPCN0.1 with the content of 0.1 g ammonium dihydrogen phosphate displayed the highest photocatalytic hydrogen generation rate of 4200.3 µmol g-1h-1, which was approximately 25 and 1.6 folds by bulk g-C3N4 (CN) and sulphur doped g-C3N4 microrods (SCN), respectively. Moreover, the apparent quantum efficiency of HER reached up to 10.3 % at 420 nm. The enhanced photocatalytic performance may be attributed to the synergistic effect of S, P doping and morphology structure of carbon nitride, which effectively accelerated the separation and transfer of photogenerated electron-hole pairs, proved by photoluminescence spectra, time-resolved PL spectra, electrochemical impedance spectrum and transient photocurrent responses. The novel synthetic method described in this paper is an effective approach to regulate the morphology of g-C3N4via non-metal doping with superior photocatalytic performance.

18.
ACS Appl Mater Interfaces ; 13(47): 56285-56295, 2021 Dec 01.
Article in English | MEDLINE | ID: mdl-34784164

ABSTRACT

Nitrogen doping carbon materials are considered to be promising candidates for Na+ storage anodes. However, hitherto, the effects and mechanism of specific single N configuration (among pyrrolic N, quaternary N, and pyridinic N), on the sodium storage behaviors of carbon materials, are still puzzling, owing to the difficulties in accurately synthesizing a certain type of single N configuration dominated carbon materials (NCDCMs). Here, various NCDCMs have been successfully controlled and synthesized by small molecule polymerization methods, and their synthesis process has been also verified by NMR, MOLDI-TOF, TG-MS, etc. When serving as sodium ion battery anodes, the NCDCMs dominated by a high concentration of pyrrolic N (>80.3%) exhibits a satisfactory reversible capacity (434.5 mA h g-1 at 50 mA g-1 and 146.7 mA h g-1 at 2000 mA g-1, respectively). It is revealed that pyrrolic N has more suitable adsorption energy and larger interlayer spacing, by density functional theory calculations and electron orbital theory, respectively, which synergistically makes the material obtain excellent electrochemical performance. This research exhibits a more efficient way to reveal the differences in the sodium ions storage behavior of different nitrogen configurations doped carbon, and provides new insight for the precise design and synthesis of a certain type of heteroatom doping to achieve satisfactory electrochemical performance.

19.
ACS Appl Mater Interfaces ; 13(40): 47671-47683, 2021 Oct 13.
Article in English | MEDLINE | ID: mdl-34597033

ABSTRACT

Hard carbon (HC) displays great potential for high-performance sodium-ion batteries (SIBs) due to its cost-effective, simple fabrication and most likely to be commercialized. However, the complicated microstructures of HC lead to difficulties in deeply understanding the structure-performance correlation. Particularly, evaluation of influence of pore structure on Na storage performances is still causing disputes and rational strategies of designing pore architecture of HC are still necessary. In this work, the skillful and controllable phase-inversion method is applied to construct porous HC with abundantly interconnected and permeable tunnel-like pores, which can promote ionic diffusion and improve electrode-electrolyte interfacial affinity. Structure-performance investigation reveals that porous HC with cross-coupled macropore architecture can boost Na storage performances comprehensively. Compared to pristine HC with negligible pores, well-regulated porous HC anodes show an obvious enhancement on initial Coulombic efficiency (ICE) of 68.3% (only 51.5% for pristine HC), reversible capacity of 332.7 mAh g-1 at 0.05 A g-1, rate performance with 67.4% capacity retention at 2 A g-1 (46.5% for pristine HC), and cycling stability with 95% capacity maintained for 90 cycles (86.4% for pristine HC). Additionally, the ICE can be optimized up to 76% by using sodium carboxymethyl cellulose as a binder. This work provides an important view of optimizing Na storage performances of HC anodes by pore engineering, which can be broadened into other electrode materials.

20.
ACS Appl Mater Interfaces ; 13(19): 22549-22558, 2021 May 19.
Article in English | MEDLINE | ID: mdl-33945253

ABSTRACT

The rational design and synthesis of capable cathode materials with low cost that can exhibit good electrochemical performance are key to the development of rechargeable aluminum batteries (RABs). In this article, we have developed low-cost expanded graphite as typical cathode materials for high-performance RABs in pouch cells. Remarkably, the commercial expanded graphite can show high-rate performance, long-term cyclic life, and high energy density (64 Wh kg-1 based on a whole pouch cell). In particular, it delivers a high capacity of 111 mAh g-1 at a current density of 2 A g-1 after 300 cycles and 61.1 mAh g-1 at a high current density of 50 A g-1 after 10 000 cycles. The high-rate performance is derived from the rapid kinetic enhancement caused by the chemisorption-involved-intercalation pseudocapacitance effect. Further, a series of facile electrochemical means are used to confirm the intercalation (1.5-2.4 V)-adsorption mechanism (0.5-1.5 V) of expanded graphite. This work can provide significant support for further understanding the Al-storage behaviors of graphite materials in RABs.

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