JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Ao Li,Binfang He,Guangchao Jin,Dongmei Liu,Jingbo Chen
Li-rich manganese-based cathode material is expected to be extremely promising for next-generation lithium-ion batteries due to its high specific capacity derived from additional anion redox behavior and low cost of the main element manganese. However, the irreversible release of lattice oxygen results in poor structural stability and inferior electrochemical performances , such as low initial Coulomb efficiency, irreversible capacity decay and serious voltage decay, which limits its commercialization. Herein, a simple strategy to improve the structural stability and electrochemical performances by one-step treatment with triethylamine (TEA) at moderate temperature is reported. TEA was used as a surface treatment reagent to prepare the modified Li-rich manganese-based cathode materials with oxygen vacancies and local structural distortion on the surface. The presence of surface distortion layer and oxygen vacancies inhibits irreversible oxygen release. The result exhibits that initial Coulomb efficiency, rate performance and initial discharge specific capacities are improved. After 100 cycles at a current density of 1 C, the specific capacity of the surface-treated material is 204.3 mAh g -1 (172.6 mAh g -1 for the pristine material), with a capacity retention of 81.26%. Even at a high current density of 10 C, the discharge specific capacity of 139.4 mAh g -1 is still achieved, demonstrating the excellent electrochemical performance. This study provides a simple and effective strategy for constructing special surface structures on Li-rich manganese-based materials to achieve high performance.
研究领域:
材料科学
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电化学
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能源存储
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锂离子电池
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固态化学
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yu Liu,Heng Zhang,Kaiyan Xiang,Chenghao Zeng
Toll-like receptor agonists have been extensively applied as immunostimulatory adjuvants because of their well-defined pharmacological mechanisms, while systemic administration of Toll-like receptor agonists have shown limited efficacy due to their unfavorable pharmacokinetic properties. Here we constructed an albumin-binding Toll-like receptor 7 agonist (Ab1V209) by conjugating the Toll-like receptor 7 agonist 1V209 with truncated Evans Blue for binding to endogenous albumin. The resulting Ab1V209 has the ability to hijack albumin and is retained in tumor tissues for a higher accumulation than 1V209. As monotherapy, the systemic administration of Ab1V209 alters the function of tumor-associated macrophages towards anti-tumor phenotype, and increases the infiltration of CD8 + T cells, leading to controlled tumor growth with minimal systemic toxicity. When used in combination with an mRNA cancer vaccine, the combination therapy activated dendritic cells to provide antigen presentation molecule and co-stimulatory molecule, resulting in a strong T cell activation and expansion. This study presents a strategy for the rational engineering of albumin-binding adjuvants to enhance cancer immunotherapy.
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ADVANCED FUNCTIONAL MATERIALS
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2026
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IF 19.9
Yilin Liu,Jingming Wang,Weizhen Li,Zhenlin Jiang,Piming Ma,Honghao Hou,Shiqiang Song
Stretchable ionic conductors are essential for wearable electronics and iontronic systems. However, their electrical stability is fundamentally limited by strain-induced resistance changes. Most reported systems exhibit strain-insensitive behavior only within limited deformation ranges, while maintaining stable ionic conductivity under large strains remains challenging because mechanical deformation simultaneously alters macroscopic conduction pathways and local ion coordination environments. Here, we report a microphase-engineered ion-conductive elastomer fiber that spatially decouples mechanical deformation from ionic transport through orthogonal dynamic interactions. This strategy overcomes key fabrication challenges in ion-conductive fibers, where conventional melt or wet spinning suffers from salt aggregation, thermal degradation, or ion loss. The resulting dual-continuous architecture selectively integrates hydrogen-bonded soft domains with lithium-coordinated rigid conductive domains. The fiber exhibits high stretchability (∼834%), toughness (8.1 MJ m −3 ), and self-healing efficiency (>80%). Notably, it achieves strain-insensitive ionic conduction over the full deformation range (0%–834%) with nearly constant resistance (ΔR/R 0 <0.1), outperforming previously reported systems that only work under partial strains. Multiscale characterizations reveal that strain-induced alignment of rigid conductive domains reduces transport tortuosity while preserving local Li + coordination. The fiber further enables stable signal transmission and reliable operation as a stretchable triboelectric nanogenerator electrode, demonstrating its potential for wearable electronics and iontronic devices.
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APPLIED SURFACE SCIENCE
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2026
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IF 6.6
Fei Yan,Luao Wu,Guangle Zhou,Lina Wei,Jialei Wang,Chaoran Song,Wenhui You,Ping Li,Lidong Wang
Rough spherical O v -rich Fenton-like catalysts were fabricated by hard-template method and chemical reduction. • Dimethylamine could be mineralized to non-toxic carbon dioxide, water and NO 3 − . • Rich oxygen vacancies and bimetallic synergism promoted the activation of PMS. • The catalyst could adsorb DMA and PMS, thus shortening the distance between DMA and ROS. As a widely used volatile organic solvent, dimethylamine (DMA) easily escapes into atmosphere, causing great threat to the environment. In this study, a novel heterogeneous Fenton-like catalyst, spherical CoFe 2 O x with rich oxygen vacancies and rough surface (S-CoFe 2 O x -O v ) is fabricated with the hard-template method to effectively activate PMS for removing DMA. Compared with CoFe 2 O x prepared by traditional coprecipitation method, the DMA degradation rate is enhanced by 13 times over S-CoFe 2 O x -O v . Quenching experiments, EPR analysis, and electrochemical tests confirmed that SO 4 •− , O 2 •− , 1 O 2 , and electron transfer pathway are responsible for the degradation of DMA. XPS analysis proves that O v and the Co 2+ –Co 3+ redox cycle are responsible for the production of ROS from PMS, and the presence of Fe 2+ facilitated the redox cycle of Co 2+ –Co 3+ . DFT calculations prove that the adsorption and activation of PMS on the surface of catalyst is thermodynamically favorable. In addition, DMA could also be adsorbed on the catalyst surface, which can shorten the migration distance between DMA and ROS. The degradation mechanism of DMA is proposed and verified using the detected intermediates. The catalyst also exhibits effective degradation of other organic amines, demonstrating the broad applicability. Therefore, this study provides a feasible hard-template method for fabricating efficient Fenton-like catalyst. Download: Download high-res image (153KB) Download: Download full-size image
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Nature Communications
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2026
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IF 18.1
Xia Shuai,Tan Hao,Zhang Jianfang,Han Miao,Xu Chang,Yu Cuiping,Chen Kui,Zhang Yong,Wu Yucheng,Wang Yan
The electrocatalytic synthesis of amides from abundant small molecules offers a sustainable route for green chemical production, yet faces fundamental challenges due to kinetic competition between C–C and C–N bond formation. Here we show an atomically engineered dual-site catalyst featuring nickel single atoms adjacent to copper nanoclusters (Ni-SA/Cu-NCs) on a nitrogen-doped carbon matrix for efficient CO 2 and NO 3 − co-reduction to acetamide. This architecture enables complementary functions, with Ni sites selectively converting CO 2 to CO and neighboring Cu nanoclusters promoting C–C coupling to form the *CCO intermediate while concurrently reducing NO 3 − to form the *NH 2 intermediate. The resulting synergy facilitates rapid intermediate transfer and C–N coupling, delivering an acetamide yield rate of 257.3 mmol h −1 g cat . −1 at an industrial current density of 215.7 mA cm −2 , with stable operation over 160 h. In situ spectroscopic studies and theoretical calculations suggest that strong Ni–Cu electronic coupling promotes reactant adsorption and reduces the activation barriers for critical steps, including *CO dimerization and *CCO–*NH 2 coupling. This work provides an atomic-level design strategy for multi-site catalysts to steer complex electrocatalytic reactions toward value-added products.
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MICROCHEMICAL JOURNAL
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2026
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IF 5.1
Li Zhang,Shanxia Jin,Xiaofeng Guo,Yi Yu,Ping Zhou
Lipids are structural components of biomembrane and also have multiple cellular functions. Lipids are difficult to be studied due to their great diversity. Matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) has played an important role in lipid analysis. However, the detection of specific lipids still suffers from challenges such as low selectivity and signal interference from other lipids, especially in complex biological samples. In this study, we have synthesized a series of N-alkyl-9-aminoacridines (N-alkyl-9AAs) with different alkyl chain lengths as the matrices for MALDI-MS analysis of phospholipids and created a unique strategy to distinguish phosphatidylethanolamine (PE) from other membrane phospholipids. A laser-induced ultrafast photochemical click reaction between N-alkyl-9AA and the amino group enabled to selectively tag PE species in source with an apparent yield up to 97%. Meanwhile the interference from phosphatidylcholine, most frequently encountered in MS analysis, was avoided. Among the N-alkyl-9AAs, C6-9AA exhibited the best performances and offered higher detection sensitivity for PEs in comparison to 9AA. This approach was successfully applied to the identification of PEs in Gram-positive and Gram-negative bacteria. This work not only provides a novel matrix for selective analysis of PE but also demonstrates a new way for fast screening of target biomolecules based on photochemical click reaction, avoiding tedious procedures for derivatization. In addition, it makes a valuable contribution to the understanding on the mechanism of MALDI.
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Journal of Inorganic and Organometallic Polymers and Materials
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2023
·Vol. 33
·期 7
·2000-2012
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IF 4
Gao Die,Zhu Qingqing,Liu Peng,Zhou Qing,Cheng Xiujie,Liu Li,Xu Junli,Lu Xingmei
Proton-type ionic liquids have been proved to be promising for the pretreatment of lignocellulosic biomass, because they can provide high yield cellulase hydrolysis and high lignin removal rate. In this work, three proton-type ionic liquids, ethyl methanesulfonamide (EAM), ethyl amine nitrate (EAN) and ethyl amine acetate (EAN[OAc]), were successfully synthesized to pretreat corn straw, and five sugar platform organic solvents were selected as co-solvents for biomass pretreatment. The experimental results showed that under the optimal pretreatment conditions (10 wt% EAM, 130 °C, 2 h, 7 wt% straw loading in PDO solvent), the delignification rate of corn straw could reach 96 wt%, the sugar yield of cellulose-rich substrate could reach 95 wt% in 96 h, the regeneration rate of lignin dissolved in the solvent was 86 wt%, and the remainder of the solvent was small molecular compound, the hemicellulose dissolved in the solvent is degraded to monomolecular sugars (xylose and arabinose). The XRD, SEM characterization data and spectrograms of cellulosic substrate also fully proved that the lignin was successfully dissolved and separated from corn straw by pretreatment of composite system, and in the remaining straw the content and crystallinity of cellulose was improved. In this paper, density functional theory (DFT) is used to explore the pretreatment principle. From the optimized structure, it can be seen that the interaction energy between the ionic liquid cosolvent system and lignin is higher than that in the pure ionic liquid system. The simulation results, experimental analysis and characterization can effectively explain the essence of the system for efficient straw pretreatment, and the system can provide new ideas for the development of biomass pretreatment.
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ACS Nano
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2023
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IF 17.1
Chuansheng He,Linlin Yang,Xiaohui Peng,Shangheng Liu,Jia Wang,Chengyuan Dong,Delin Du,Leigang Li,Lingzheng Bu,Xiaoqing Huang
Thickness regulation of transition metal hydroxides/oxides nanosheets with superior catalytic properties represents a promising strategy to enhance catalytic performance, but it remains an enormous challenge to achieve precise control, especially when it comes to the ultrathin limit (several atomic layers). In this work, a facile strategy of alkylamine-confined growth is proposed for the synthesis of thickness-tunable metal hydroxide/oxide nanosheets. Specifically, ultrathin cobalt hydroxide and cobaltous oxide hybrid (Co(OH)2-CoO) nanosheets (Co–O NSs) with a thickness in the range of 2–6 nm (5–13 atomic layers) are synthesized by using alkylamines with different carbon chain lengths as the ligand to modulate vertical coordination ability. Co–O NSs with a thickness of 2 nm (Co–O NSs-2 nm) exhibit excellent oxygen evolution reaction (OER) performance with an overpotential of 278 mV at 10 mA/cm2. The maximized number of active sites including oxygen vacancies, optimal adsorption strength, and the highest electrical conductivity are considered as the potential factors contributing to the excellent OER performance of Co–O NSs-2 nm. This work holds great significance for the precise thickness-tunable synthesis of transition metal layered hydroxide nanosheets with modulated and improved catalytic performance.
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PubMed
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
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IF 16.6
Chen Zhe,Li Jili,Meng Lingshen,Li Jianan,Hao Yaming,Jiang Tao,Yang Xuejing,Li Yefei,Liu Zhi-Pan,Gong Ming
Simultaneously achieving abundant and well-defined active sites with high selectivity has been one of the ultimate goals for heterogeneous catalysis. Herein, we construct a class of Ni hydroxychloride-based inorganic-organic hybrid electrocatalysts with the inorganic Ni hydroxychloride chains pillared by the bidentate N-N ligands. The precise evacuation of N-N ligands under ultrahigh-vacuum forms ligand vacancies while partially retaining some ligands as structural pillars. The high density of ligand vacancies forms the active vacancy channel with abundant and highly-accessible undercoordinated Ni sites, exhibiting 5-25 fold and 20-400 fold activity enhancement compared to the hybrid pre-catalyst and standard β-Ni(OH) 2 for the electrochemical oxidation of 25 different organic substrates, respectively. The tunable N-N ligand can also tailor the sizes of the vacancy channels to significantly impact the substrate configuration leading to unprecedented substrate-dependent reactivities on hydroxide/oxide catalysts. This approach bridges heterogenous and homogeneous catalysis for creating efficient and functional catalysis with enzyme-like properties.
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CHEMISTRY OF MATERIALS
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2023
·
IF 8.6
Dongying Fu,Wenjuan Jia,Shichao Wu,Junli Chang,Zhuo Chen,Junhua Luo
Two-dimensional (2D) Dion–Jacobson (DJ) hybrid perovskites (HPs) are widely used in the photodetection field due to their high stability and excellent carrier transport performance. However, current photodetectors based on DJ HPs can work only in the ultraviolet and visible wavebands, which limits their application in near-infrared (NIR) photodetection. Herein, for the first time, ultraviolet–visible–NIR photodetection is realized in the bulk single crystal of 2D bilayered DJ HP (3AMPY)(EA)Pb2Br7 (3AMPY = 3-(aminomethyl)pyridinium, EA = ethylamine). Structurally, the introduction of aromatic diammonium makes (3AMPY)(EA)Pb2Br7 have a shorter layer spacing (3.561 Å) and a more rigid structure. In addition, benefiting from the strong quantum and dielectric confinements of 2D HPs, (3AMPY)(EA)Pb2Br7 shows an excellent two-photon absorption (TPA) coefficient of up to 61.1 cm/MW under the excitation of an 800 nm femtosecond laser. Notably, (3AMPY)(EA)Pb2Br7 exhibits efficient photodetection from ultraviolet (377 nm) and visible (405 nm) to NIR (800 nm) wavebands, with on/off ratios of current higher than 103.
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ACS Catalysis
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2023
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IF 12.9
Yaming Hao,Jili Li,Xueting Cao,Lingshen Meng,Jianxiang Wu,Xuejing Yang,Yefei Li,Zhipan Liu,Ming Gong
The paired electrolysis via anodic organic oxidation and cathodic hydrogen evolution has been an emerging hydrogen production technology with high efficiency and high values. Nickel oxyhydroxide is a special electrocatalyst that is capable of selectively oxidizing various alcohols, aldehydes, and amines to the corresponding carboxylates and nitriles at more favorable potentials compared to the oxygen evolution reaction. However, its detailed molecular-level mechanism is still in debate, especially for the potential-dependent behavior of some organic substrates. In this study, we revealed that the nickel oxyhydroxide can be dissected into two functional regions with a more facilely oxidized surface for facilitated substrate adsorption and a relatively inert bulk phase for accelerated electron transfer via probe-assisted kinetics and in situ surface-enhanced Raman spectroscopy. The prerequisite of the two regions conceals a universal potential-dependent oxidation behavior for almost all organic substrates. Further combining with the computational investigation unravels the origin of this potential dependence from the exothermic O/N-centered adsorption process on the surface and the rate-limiting proton-coupled electron-transfer (PCET) steps for the C–H bond breaking that demands bulk electron conductivity. This provides a rationale for designing more conductive underlayers to break the intrinsic limitations of nickel oxyhydroxide toward more efficient organic electrooxidation processes.
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ACS Applied Materials & Interfaces
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2023
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IF 9.5
Tingyue Zhang,Liwei Guo,Ruolan Li,Jiang Shao,Lei Lu,Ping Yang,Ansha Zhao,Yanqiu Liu
Hydrogel dressings not only have basic functions such as swelling, water retention, gas permeability, and good biocompatibility but also can be endowed with advanced functions such as antibacterial, antioxidant, adhesion, hemostasis, and anti-inflammation, which make hydrogels have great application potential in clinical trauma. However, the complexity of the wound healing process makes the development of multifunctional wound dressings a great challenge. In this work, based on the thiol–ene photoclickable PEG hydrogel, the inclusion complex of the hydrophobic drug ellagic acid (EA) with mono-(6-mercapto-6-deoxy)-β-cyclodextrin (SH-β-CD) participated in the formation of a hydrogel as a crosslinker. The drug EA with antioxidant, antibacterial, and anti-inflammatory activities was introduced into the hydrogel. This strategy increases the loading capacity of the hydrogel for EA and endows the hydrogel with multifunctional properties. Then, dithiothreitol was added to adjust the mechanical stiffness of the hydrogel to meet the requirements of the wound dressing. Our results demonstrated that this wound dressing has excellent cytocompatibility, antioxidant, antibacterial, and anti-inflammatory activities. Furthermore, the results of the infected wound healing model experiment in rats confirmed that the hydrogel has the ability to rapidly shrink the wound area, prevent wound infection, and promote angiogenesis and collagen deposition. All these results suggest that this hydrogel could be a candidate for the treatment of infected wounds and shed new light on the development of multifunctional wound dressings.
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