ADVANCED MATERIALS
·
2022
·Vol. 34
·期 47
·2206039
·
IF 32.086
Yangyang Lai,Huixian Xie,Peng Li,Biao Li,Along Zhao,Laibing Luo,Zewen Jiang,Yongjin Fang,Shengli Chen,Xinping Ai,Dingguo Xia,Yuliang Cao
The anionic redox reaction (ARR) has attracted extensive attention due to its potential to enhance the reversible capacity of cathode materials in Li/Na-ion batteries (LIBs/SIBs). However, the understanding of its activation mechanism is still limited by the insufficient mastering of the underlying thermodynamics and kinetics. Herein, a series of Mg/Li/Zn-substituted Na x MnO 2 and Li x MnO 2 cathode materials are designed to investigate their ARR behaviors. It is found that the ARR can be activated in only Li-substituted Li x MnO 2 and not for Mg- and Zn-substituted ones, while all Mg/Li/Zn-substituted Na x MnO 2 cathode materials exhibit ARR activities. Combining theoretical calculations with experimental results, such a huge difference between Li and Na cathodes is closely related to the migration of substitution ions from the transition metal layer to the alkali metal layer in a kinetic aspect, which generates unique Li(Na)–O–□ TM and/or □ Li/ Na –O–□ TM configurations and reducing reaction activation energy to trigger the ARR. Based on these findings, an ion-migration mechanism is proposed to explain the different ARR behaviors between the Na x MnO 2 and Li x MnO 2 , which can not only reveal the origin of ARR in the kinetic aspect, but also provide a new insight for the development of high-capacity metal oxide cathode materials for LIBs/SIBs.
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ADVANCED MATERIALS
·
2025
·Vol. 37
·期 41
·e03562
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IF 26.8
Shangqing Qu,Tianhao Niu,Xianji Qiao,Yanran Shen,Guohong Cai,Xiaoge Wang,Yonggang Wang,Zhipeng Zhou,Shipeng Zhang,Zeyue Zhang,Guobao Li,Guanqun Cai,Junliang Sun
Na- β ″-Al 2 O 3 is a highly promising solid-state electrolyte (SSE) for solid-state sodium batteries (SSSBs) with a wide electrochemical stability window and excellent stability against metallic sodium. However, its practical application is hindered by the instability of β ″ phase ( R 3 ¯ $\bar 3$ m ) during sintering, low polycrystalline ionic conductivity at room temperature, and poor interfacial contact with sodium anodes. In this study, a stablized SSSB is obtained via doping Ga 3+ into Na 1.67 Mg 0.67 Al 10.33 O 17 (NMAO), which also suppresses the formation of the β ′ phase ( P 6 3 / mmc ) and decreases stacking faults. After sintering at 1550 °C for 2 h, Na 1.67 Mg 0.67 Al 9.33 GaO 17 (NMA9.33GO) exhibits an ionic conductivity of 9.2 × 10 −4 S cm −1 at 30 °C, ≈1.7 times greater than NMAO. Furthermore, Ga 3+ doping enhances the wettability with sodium, achieving superior contact stability and the formation of Na-Ga alloys at the interface significantly improves electrode-electrolyte contact stability, achieving a high critical current density (CCD) of 0.8 mA cm −2 and a low interfacial impedance of 16 Ω cm 2 . A quasi-solid-state battery assembled with Na 3 V 2 (PO 4 ) 3 (NVP) as the cathode demonstrates excellent cycling stability and rate performance, retaining a high discharge capacity of 91 mAh g −1 at 5 C, and maintaining 87% capacity retention after 1000 cycles at 1 C. This work provides new insights into improving electrolyte performance and interfacial engineering through doping strategies, thereby promoting the development of efficient and long-term SSSBs.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Mengyao Chen,Wenjing Qin,Yanli Wang,Hanlin Zhai,Changshun Gu,Xiangchuan Zhao,Ying Bi,Yixin Xu,Zeyu Ming,Shengrong Li,Shu Hu,Xingyue Zhang,Xiaoye Ma,Shougen Yin
The synergistic optimization of high strength, strong adhesion, high conductivity, and rapid self-healing in hydrogels faces fundamental challenges arising from conflicting mechanisms. Herein, a 3D-printed, ionically conductive interpenetrating double-network hydrogel based on poly (acrylic acid) (PAAc) is developed via the innovative introduction of dynamic Na⁺ bridges. This molecular design enables a unique dual mechanism: the Na⁺ ions not only form reversible ionic bonds that accelerate chain diffusion through bond rupture-recombination but also create an electrostatic shielding effect in the covalent network, which promotes chain extension to improve mechanical strength without sacrificing dynamic properties. Furthermore, Na⁺ ions regulate bound/free water states and reduces energy dissipation during topological rearrangement. These synergistic mechanisms collectively enable the hydrogel to overcome conventional performance trade-offs. The resulting material concurrently enhances mechanical properties (300 kPa tensile, 1.2 MPa compressive strength), adhesion (160 kPa), and self-healing (>90% recovery in 1 h). Biomimetic devices such as an underwater octopus-tentacle gripper, biomimetic crawling suckers, and pressure sensors are fabricated. By integrating hydrogels with 1D convolutional neural network algorithms, a real-time motion behavior recognition system is further developed. The multi-property cooperative design strategy offers a new pathway for the application of intelligent hydrogel materials in soft robotics and flexible electronics.
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Energy Storage Materials
·
2021
·
IF 17.789
Yuansheng Shi,Zhizhen Zhang,Pengfeng Jiang,Ang Gao,Kangwan Li,Qinghua Zhang,Yang Sun,Xueyi Lu,Dapeng Cao,Xia Lu
Layered sodium transition metal oxides (NaTMO 2 ) have garned considerate attention as candidates for cathode materials in practical Na-ion batteries because of their potentially high energy density and operating voltage. Among the several categories (P2, P3, O3) of layered NaTMO 2 materials, P3 type cathodes are least studied due to the fast capacity/voltage fading induced by P3-O3 phase transition, as shown by the very few compositions visited in previous reports. It is highly desirable to stabilize the P3 phase throughout the sodium extraction/insertion process as P polytype allows facile migration of Na + -ions between two adjacent prismatic sites. In this work, we synthesized a phase pure P3-Na 0.75 Mg 0.08 Co 0.10 Ni 0.2 Mn 0.60 O 2 (P3-MNCM) via the incorporation of Mg, while successfully maintains the P3 structure during the charging/discharging process. This together with good ionic conductivity , endows good structural reversibility, and consequently leads to superior cycling performance and rate performance than undoped composition. In situ X-ray diffraction (XRD) further verifies that P3-MNCM cathode demonstrates a near zero strain feature. Of special importance is that the P3-O3 phase transition is effectively suppressed with the incoporation of Mg into the transition metal layer. These findings demonstrate the potential of P3 structure as a promising choice for Na ion cathode materials, which open a feritile avenue and will hopefully inspire more endeavors in the exploration of high performance sodium ion batteries.
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ENERGY & FUELS
·
2024
·
IF 5.2
Tianxu Su,Bin Guan,Chunzheng Zheng,Jiefei Zhou,Zhen Huang
Developing low-temperature, high-efficiency ammonia decomposition catalysts for hydrogen production is essential for the broad application of hydrogen. This study conducted a systematic investigation of Ru/MgO catalysts modified with different alkali metals (Na, K, Cs), unveiling the impact of these modifications on catalyst performance and developing a highly efficient low-temperature ammonia decomposition catalyst. The addition of all alkali metals enhances the catalytic performance of Ru/MgO for ammonia decomposition, especially the addition of K, which results in the optimal enhancement of the catalyst, achieving a 75% ammonia decomposition efficiency at 350 °C (GHSV= 2,000 mL/h·gcat), more than doubling the performance of the unmodified Ru/MgO catalyst. The study revealed that the addition of potassium (K) altered the rate-determining step of the ammonia decomposition reaction from nitrogen recombination to the dissociation of the first hydrogen atom, and reduced the overall energy barrier required for the reaction. This facilitated the desorption of nitrogen from the Ru surface and the conversion of NH3, thereby accelerating the rate of the ammonia decomposition reaction.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zikang Hou,Wen Zhang,Xiangze Kong,Qingjuan Ren,Zhiheng Wang,Yufei Qin,Zhiqiang Shi
Sodium-ion batteries (SIBs) offer compelling advantages for grid-scale energy storage, owing to their safety and cost competitiveness. However, the implementation of economically competitive cellulose separators in SIBs is hindered by oversized pore structures and insufficient electrochemical stability. Here, we develop a high-performance cellulose separator through in situ polymerization of a Bis[(3-methyldimethoxysilyl)propyl]-polypropylene oxide (BSPPO) coating on commercial substrates. The BSPPO modification synergistically optimizes pore architecture for homogeneous Na + deposition while expanding the electrochemical stability window to 4.87 V through functional group engineering. Crucially, the polymer coating enables a dual-pathway Na + transport mechanism, integrating high-rate ion conduction through pore channels with polymer chain-mediated transport, resulting in superior ionic conductivity (1.33 mS cm −1 ) and Na + transference number (0.69). Hard carbon||Na cells incorporating the 20 % BSPPO-modified separator demonstrate exceptional cycling stability, maintaining 99.5 % coulombic efficiency and 90.7 % capacity retention over 100 cycles at 2C. This work introduces a dual-pathway ion transport strategy, advancing cellulose separators toward practical high-performance SIB applications.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2025
·
IF 4.6
Wei Gao,Hao Hu,Jinkun Xue,Yongrun Dong,Wen Li,Xia Zhao,Xiang Mao,Zequan Li
Carbon dots (CDs) have attracted considerable interest as fluorescent nanomaterials; however, their long-afterglow emission properties remain underexplored. In this study, we synthesized dual-mode afterglow CDs exhibiting room-temperature phosphorescence (RTP) and thermally activated delayed fluorescence (TADF) via fluorine-sodium (F, Na) co-doping, achieving an extended afterglow lifetime of 574 ms. Under 365 nm UV excitation, the afterglow emission persists for 14 s (naked-eye observation) and 40 s (instrumentally quantified), demonstrating exceptional temporal resolution. Na doping enhances afterglow intensity by 11.3 %, while fluorine doping reduces the singlet–triplet energy gap (ΔE ST ) to 0.036 eV, facilitating efficient Reverse Intersystem Crossing and enabling TADF behavior. These synergistic effects position the developed CDs as promising candidates for anti-counterfeiting systems, multilevel data encryption, and high-security optical tagging.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
YuKai Hua,MingPei Tan,Ming Liu,Xiao Yu,Donghai Wang,Yong Liu
P2-type layered metal oxides are promising cathode materials for Na-ion batteries (NIBs), but they suffer from Na + /vacancy ordering and P2-O2 phase transitions during charge–discharge processes, resulting in rapid capacity decay and poor rate performance. In this study, a non-equimolar five-component medium-entropy strategy was employed to design a Na 0.67 Ni 0.19 Cu 0.07 Zn 0.07 Mn 0.60 Ti 0.07 O 2 (NNCZMT) material. Unlike equimolar high-entropy designs, Ni and Mn remain as the main components, with Ni providing high capacity through the Ni 2+ /Ni 4+ redox couple and Mn stabilizing the P2 structure. The introduction of Cu 2+ , Zn 2+ , and Ti 4+ , which have slightly larger ionic radii and the same valence states as Ni 2+ and Mn 4+ , respectively, allows for mutual substitution, synergistically promoting a solid-solution reaction and excellent Na + diffusion kinetics. The NNCZMT electrode delivers a high reversible capacity of 110 mAh g −1 at 10 mA g −1 , an initial Coulombic efficiency of 96.8 %, remarkable cycling stability (94.7 % capacity retention after 100 cycles at 200 mA g −1 ), and excellent rate performance (57.2mAh g −1 at 2000 mA g −1 ).
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Biomaterials Advances
·
2025
·
IF 6
Chen Wang,Yin Li,Xiaoxue Shen,Shiwei Xiao,Huiying Du,Qianye Zhao,Ying Wang,Qiangtao Zhang,Shuxin Wen
Background Patients with locally advanced head and neck squamous cell carcinoma (HNSCC) exhibit poor survival due to tumor microenvironment (TME) barriers and systemic toxicity of chemo-immunotherapy associated with chemo-immunotherapy. Methods An injectable thermoresponsive hydrogel was engineered by crosslinking D-α-tocopheryl polyethylene glycol succinate (TPGS) with Na₂CO₃ (15 % w/v TPGS: 9 % w/v Na₂CO₃). This platform co-encapsulated doxorubicin-loaded nanoparticles (DOX NP) synthesized via PEI-cis-aconitic acid conjugation and CpG-loaded adjuvant nanoparticles (CpG NP) prepared through genipin-mediated PEI crosslinking. The hydrogel exhibited rapid temperature-triggered gelation, shear-thinning injectability, and a macroporous architecture that enabled dual drug retention and immune cell infiltration. Results In vitro , the hydrogel provided the sustained release of DOX NP with pH-responsive acceleration in acidic TME. In vivo , localized delivery of Gel-DOX NP-CpG NP significantly suppressed tumor growth ( p < 0.05) and enhanced cytotoxic CD8 + T-cell infiltration in TME (3.1-fold) and spleens (2.4-fold). RNA sequencing revealed 88 immune-related differentially expressed genes, including downregulated immunosuppressors and enriched cytokine pathways. Conclusion This TPGS/Na₂CO₃ hydrogel platform coordinates chemotherapy-induced immunogenic cell death (DOX NP) with CpG-driven innate immunity, overcoming TME barriers to enhance localized and systemic anti-tumor responses in HNSCC.
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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Weichen Xu,Xiaomeng Li,Hong Wang,Fuliang Wang,Shouqiang Han,Jing Guo
Microwave dielectric ceramics are critical components in wireless communications. However, it is still a challenge to develop microwave dielectric ceramics with reduced sintering temperatures, high thermal stabilities and good dielectric properties at the same time. Herein, the entropy value, which is able to modulate the grain boundary energy and adjust the inherent sintering temperature, is engineered to develop high-performance microwave dielectric ceramics with low sintering temperatures. The structure-property relationships of AWO 4 ceramics, including (NaCaBi) 1/3 WO 4 , (NaCaSrBi) 1/4 WO 4 , (NaLiCaBiSm) 1/5 WO 4 and (NaLiCaSrBiSm) 1/6 WO 4 with increased entropy values are investigated systematically. X-ray diffraction and high-resolution TEM analyses confirm the formation of single-phase solid solutions with the tetragonal scheelite structure in AWO 4 ceramics. As the number of elements in the A-site varies, the relative permittivities, Q × f values and TCF values shift in the range of 12.2–16.5, 8,000–25,000 GHz and −32.3–31.6 ppm/°C, respectively. Simultaneously, the high-entropy samples demonstrate the lowest sintering temperature of 750 °C among the four formulations. Phillips-Van Vechten-Levine (PVL) complex chemical bond theory reveals that the covalency, lattice energy and bond energy affect the relative permittivity, Q × f value and TCF value, respectively. Raman spectra suggest that high entropy value leads to increased disorder, and infrared reflectivity spectra illustrate that the dielectric response is dominated by polarized optical phonons of [WO 4 ] tetrahedron. It is anticipated that entropy design will facilitate the development of microwave dielectric ceramics in low temperature co-fired ceramic applications.
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Journal of Water Process Engineering
·
2025
·
IF 6.7
Junguo He,Yuanyi Zhao,Heliang Pang,Yili Wang,Lin Li,Yunlong Liu,Xinxin Cui,Tong Wei,Shengye Duan,Suiyin Yu
Sulfaquinoxaline sodium (SQ-Na), a veterinary sulfonamide antibiotic, poses potential risks to anaerobic digestion (AD) systems due to its antimicrobial properties, yet its impacts on methanogenic efficiency and microbial dynamics remain poorly understood. This study systematically evaluated the effects of SQ-Na (0–50 mg/L) on AD of simulated wastewater through batch experiments, integrating methane yield analysis, enzyme activity assays, 16S rRNA sequencing and metagenomic insights. Results demonstrated a dose-dependent inhibition of cumulative methane production, with 1 and 5 mg/L SQ-Na reducing yields to 41.21 % and 8.12 % of the control, respectively, while 20–50 mg/L caused near-complete stagnation. The modified Gompertz equation revealed prolonged lag phases (up to 53.52 % extension) and suppressed maximum methane production rates (Rmax). Function enzyme analyses indicated SQ-Na-induced adenosine triphosphatase (ATPase) inhibition (0.26–0.63–fold reduction) alongside accumulated Acetyl-CoA (A-CoA, 0.23–2.32 folds) and Coenzyme F 420 (F 420 , 0.48–2.52 folds), suggesting metabolic imbalance. Microbial shifts highlighted SQ-Na-driven suppression of acetoclastic methanogens (e.g., Methanosaeta ). Metagenomic evidence further pinpointed decreases in the abundance of methanogenesis-associated genes (e.g., EC 7.2.1.4, EC 2.8.4.1) and folate biosynthesis pathways, revealing an inhibition mechanism where SQ-Na competitively inhibits dihydropteroate synthase (EC 2.5.1.15), impairing the metabolic chain of energy, enzymes and function substances. This study offering critical data for optimizing SQ-Na-wastewater treatment and sustainable bioenergy recovery.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2025
·
IF 2.1
Jing Li,Linglin Fu,Zongde Ma,Jinniu Chen,Changhao Wu,Nan Zhang,Xudong Yu
To understand the interrelationships within the multi-ion coexisting sulfate system during the solid–liquid transformation of polyhalite in the Bieletan area, phase equilibria of ternary systems M, Ca2+//SO42–-H2O (M = Na+, K+, Mg2+) at 288.2 K were studied by the isothermal dissolution equilibrium method. The solubility and density of the equilibrium liquid phases of the system were measured experimentally, and the composition of the equilibrium solid phase at the ternary invariant point was determined by X-ray powder diffractometry. It is found that the ternary system K+, Ca2+//SO42–-H2O at 288.2 K forms the double salt syngenite (K2SO4·CaSO4·H2O), while the systems Na+, Ca2+//SO42–-H2O and Mg2+, Ca2+//SO42–-H2O at 288.2 K only form with the formation of CaSO4·2H2O and Na2SO4·10H2O (MgSO4·7H2O). Multitemperature comparison of the M, Ca2+//SO42–-H2O (M = Na+, K+, Mg2+) systems shows that the phase diagrams of Mg2+, Ca2+//SO42–-H2O are consistent at the selected temperature, only containing CaSO4·2H2O and MgSO4·nH2O (n = 1, 6, 7). While K+, Ca2+//SO42–-H2O and Na+, Ca2+//SO42–-H2O change from 288.2 and 298.2 to 348.2 K, the phase diagram forms double salt(s) K2SO4·5CaSO4·H2O (Na2SO4·5CaSO4·3H2O and Na2SO4·CaSO4).
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