Nature Communications
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2024
·Vol. 15
·期 1
·1-13
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IF 14.7
Li Yifan,Huang Aijian,Zhou Lingxi,Li Bohan,Zheng Muyun,Zhuang Zewen,Chen Chang,Chen Chen,Kang Feiyu,Lv Ruitao
Developing highly active and durable air cathode catalysts is crucial yet challenging for rechargeable zinc-air batteries. Herein, a size-adjustable, flexible, and self-standing carbon membrane catalyst encapsulating adjacent Cu/Na dual-atom sites is prepared using a solution blow spinning technique combined with a pyrolysis strategy. The intrinsic activity of the Cu-N 4 site is boosted by the neighboring Na-containing functional group, which enhances O 2 adsorption and optimizes the rate-determining step of O 2 activation (*O 2 → *OOH) during the oxygen reduction reaction process. Meanwhile, the Cu-N 4 sites are encapsulated within carbon nanofibers and anchored by the carbon matrix to form a C 2 -Cu-N 4 configuration, thereby reinforcing the stability of the Cu centers. Moreover, the introduction of Na-containing functional groups on the carbon atoms significantly reduces the positive charge on their outer shell C atoms, rendering the carbon skeletons less susceptible to corrosion by oxygen species and further preventing the dissolution of Cu centers. Under these multi-type regulations, the zinc-air battery with Cu/Na-carbon membrane catalyst as the air cathode demonstrates long-term discharge/charge cycle stability of over 5000 h. This considerable stability improvement represents a critical step towards developing Cu-N 4 active sites modified with the neighboring main-group metal-containing functional groups to overcome the durability barriers of zinc-air batteries for future practical applications.
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Nanomaterials
·
2024
·Vol. 14
·期 20
·1629
·
IF 4.4
Penghui Lei,Qing Chang,Mingkun Xiao,Chao Ye,Pan Qi,Fangjie Shi,Yuhua Hang,Qianwu Li,Qing Peng
A new type of SiCf/TiC-Ti3SiC2composite was prepared by the Spark Plasma Sintering (SPS) method in this work. The phase transformation and interface cracking of this composite under ion irradiation (single Xe, Xe + He, and Xe + He + H ions) and subsequent annealing were analyzed using transmission electron microscopy (TEM), mainly focusing on the interface regions. Xe ion irradiation resulted in the formation of high-density stacking faults in the TiC coatings and the complete amorphization of SiC fibers. The implanted H ions exacerbated interface coarsening. After annealing at 900 °C for 2 h, the interface in the Xe + He + H ion-irradiated samples was seriously damaged, resulting in the formation of large bubbles and cracks. This damage occurred because the H atoms reduced the surface free energy, thereby promoting the nucleation and growth of bubbles. Due to the absorption effect of the SiCf/TiC interface on defects, the SiC fiber areas near the interface recovered back to the initial nano-polycrystalline structure after annealing.
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Food & Function
·
2024
·
IF 5.1
Qingqing Lv,Aolin Yang,Ziyu Han,Ruirui Yu,Junying Zhu,Zhan Shi,Chenggang Yang,Shimiao Dai,Mengru Hao,Yuqing Chen,Ji-Chang Zhou
Low selenium levels are closely associated with reduced cognitive performance and lipid dysregulation, yet the mechanism of action remains unclear. The physiological function of selenium is primarily mediated by selenoproteins. Selenoprotein H (SELENOH), as one of the selenium-containing proteins, has an unelucidated role in regulating cognitive status and lipid metabolism. In this study, we established a Selenoh gene knockout (HKO) mouse model to investigate whether Selenoh mediates the impact of selenium on cognitive function. We found that HKO mice showed a significant decline in cognition compared with the wild-type (HWT) littermates, and were not affected by deficient or excessive selenium, while no differences in anxiety and depression behavior were observed. HKO mice showed reduced myelin basic protein expression in hippocampal oligodendrocytes, with decreased glycolipid levels and increased phospholipid and sphingolipid levels in the hippocampus. Furthermore, the high-fat diet (HFD) exerted no effect on cognition and limited impact on the gene profile in the hippocampus of HKO mice. Compared with those of HWT mice, the myelination pathways in the hippocampus of HKO mice were downregulated as revealed by RNA-seq, which was further confirmed by the reduced expression levels of myelin-related proteins. Finally, HKO increased the expression of hippocampal fatty acid transporter (FATP) 4, and HFD increased the FATP4 expression in HWT mice but not in HKO mice. In summary, our study demonstrated that HKO induced cognitive decline by impairing myelination in oligodendrocytes with disrupted hippocampal lipid metabolism, which provided a novel viewpoint on the selenoprotein-mediated neurodegenerative diseases of selenium.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
·
IF 4.9
Hongxin Yan,Guoqing Xiao,Chunlin Chen,Mingtan Wang,Rui Zou,Yinke Lan,Jing Gou,Junjie Cao,Xiyi Ma
Hexagonal boron nitride (h-BN) has excellent lamellar structure and electrical insulation properties, and excels in improving the corrosion resistance of coatings. By utilizing the abundant hydroxyl and amino functional groups on the polydopamine surface, h-BN is endowed with excellent hydrophilicity. Simultaneously, the polysaccharide polymer MD-GT-CS (MGC), formed by cross-linking maltodextrin (MD), gelatin (GT), and chitosan (CS), was combined with the active sites on the surface of BN@PDA, which conferred pH-responsive functionality to the BN@PDA@MGC hybrid material. In addition, cerium ions were introduced into the carboxyl and amino sites on the MGC surface, resulting in the synthesis of BN@PDA@MGC(Ce) (BPMGC), a hybrid material that combines the layered barrier properties, pH responsiveness, and self-repairing functions. The BPMGC/EP composite coating was prepared by doping the hybrid material with EP. The EIS test results showed that the |Z| 0.01 Hz value of the composite coating reached 1.45 × 10 9 Ω cm 2 after 40 d, which is an improvement of four orders of magnitude compared to EP (6.85 × 10 5 Ω cm 2 ). The results of EIS tests at different pH conditions showed that after 40 d of immersion at pH = 3 and 5, the |Z| 0.01 Hz value decreased by two orders of magnitude, but was still two orders of magnitude higher than that of EP at pH = 7. Meanwhile, the strong self-healing ability of BPMGC/EP was determined by EIS analysis of the scratched coating, salt spray test, SEM and EDS analysis of the corroded area. The experimental results show that the incorporation of BPMGC provides a new method to improve the barrier and self-healing properties of epoxy resins.
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CONSTRUCTION AND BUILDING MATERIALS
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2024
·
IF 7.4
Kaifeng Wang,Yuxun Kan,Yunsheng Zhu,Kaihong Zhong,Jiabing Hu
Calcium silicate hydrate (C-S-H) is considered a novel early strength agent, showing immense potential in enhancing the early strength of cement-based materials. Polycarboxylate (PCE) is widely used as a dispersant in the synthesis of nano-C-S-H to prevent agglomeration during synthesis. However, a comprehensive investigation is still required to establish a stable method for preparing stable C-S-H/PCE nanocomposites using chemical co-precipitation. This study employed orthogonal experiments, range analysis, variance analysis, and multi-index matrix analysis to explore the effect of the chemical co-precipitation synthesis process on the stability of C-S-H/PCE nanocomposites. It conclusively identified the calcium-to-silicon (C/S) ratio as the sole significant influencing factor, establishing optimal synthesis parameters: a C/S ratio of 1.6, stirring at 8000 r/min, a 2-hour reaction time, and a reaction temperature of 30 °C. Additionally, X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) were utilized to investigate the impact of the C/S ratio on the structure and morphology of C-S-H/PCE nanocomposites. Results indicated that under the optimal synthesis parameters, the average particle size and precipitation rate of the synthesized C-S-H/PCE nanocomposites were 0.122 µm and 0.44%, respectively, exhibiting a 4.7% and 47.6% improvement over the best samples in the orthogonal test. Increasing the C/S ratio decreased the crystallinity of the C-S-H/PCE nanocomposites, resulting in the emergence of multiple crystal structures, compact and ordered morphology, and reduced sedimentation. These findings collectively underscore that C-S-H/PCE nanocomposites with higher C/S ratios exhibit enhanced dispersion and stability, validating the rationality of the optimal synthesis parameters identified in this study.
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ACS Nano
·
2024
·
IF 15.8
Xu Li,Wenlong Tan,Jinsong Fan,Kun Li
Although the past decade has witnessed a rapid development of oxidoreductase-mimicking nanozymes, the mimicry of cofactors that play key roles in mediating electron and proton transfer remains limited. This study explores how surface Au–H species conjugated to Au nanoparticles (NPs) that imitate formate dehydrogenase (FDH) can serve as cofactors, analogous to NADH in natural enzymes, offering diverse possibilities for FDH-mimicking Au nanozymes to mimic various enzymes. Once O2 is present, Au–H species assist Au NPs to complete the on-demand H2O2 generation for cascade reactions. Alternatively, when oxidizing organic molecules are introduced as substrates, Au–H species confer nitro reductase- and aldehyde reductase-like activities on Au NPs under anaerobic conditions. Furthermore, similar to the dehydrogenase–NADH complex, Au NPs possessing Au–H species are gifted with esterase-like activity for ester hydrolysis. By revealing that Au–H species are prosthetic groups for FDH-mimicking Au nanozymes, this work may inspire explorations into future self-generated cofactor mimics for nanozymes, thereby circumventing the need for exogenous cofactors.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Xiao-Jian Li,Xinli Lu,Yunxia Wang,Zhanquan Zhang,Yongfa Zhang
This study successfully developed a highly sensitive electrochemiluminescence (ECL) sensor based on the ECL resonance energy transfer mechanism for detecting the key biomarker of acute myocardial infarction, heart–type fatty acid binding protein (h–FABP). Through the meticulous design of the Ag/Cu2O/Ti3C2 ternary nanocomposite material, this material demonstrated significant catalase–like catalytic activity, enabling the efficient decomposition of H2O2 to generate more superoxide radicals (O₂•⁻), thereby significantly enhancing the ECL signal of the luminol–H2O2 system. Notably, AgS quantum dots (AgS QDs), due to broad–spectrum ultraviolet absorption overlapping with the ECL emission spectrum of luminol, triggered an efficient energy resonance transfer effect, resulting in the decrease of ECL intensity. NH2–MIL–101(Fe) was utilized to couple with AgS QDs (AgS QDs@NH2–MIL–101(Fe)), which can further enhance the quenching efficiency. Based on this signal–off strategy, an ultrasensitive detection platform for h–FABP was successfully constructed. Experimental results indicated that the immunosensor exhibited an excellent response relationship within a wide linear range from 1.00 fg mL–1 to 100 ng mL–1, and a low detection limit reached 0.36 fg mL–1 (S/N = 3). This study provides an innovative methodological approach for ultra–trace detection of myocardial injury markers and demonstrates significant application potential in early clinical diagnosis.
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Advanced Science
·
2025
·
IF 14.1
Jingting Jin,Wenzhi Li,Liqun Wang,Lulu Zhang,Xia Zhang
Direct and efficient methane oxidation to methanol is an appealing route for upgrading abundant methane resources while acquiring building blocks of clean fuels and chemicals. However, owing to its highly symmetrical nature imparted chemical stability and steric hindrance, the design of multi-ångstrom (<3.0 Å) spaced active species capable of activating its first C−H bond remains a fundamental challenge. Herein, Cu−Ni dual-atom Pair is constructed using defect engineering and a stepwise deposition method over indium oxide to precisely modulate the C−H polarization with the Cu atom showing affinity to H end and Ni anchoring the C side. The optimal CuNi/InNT achieves an oxygenates (CH 3 OH and CH 3 OOH) productivity of 106 mmol g cat h −1 , surpassing reported systems. Theoretical calculations validate the dominating role of interatomic distance for methane activation. Specifically, the dual-atom orbital coupling effect in the minimally spaced Cu−Ni pair up-shifts the overall d-band center, significantly enhancing its hybridization with C/O 2p. Further modification through macroscopic reactor design boosts CH 3 OH yield to 36818.84 µmol g cat h −1 with 79.37% selectivity in a 1000 mL semi-industrial prototype. This work provides a comprehensive explanation of the Cu−Ni synergy, bridging atomic-scale catalysis with reactor design, and establishes a common design principle for binary catalysts at the electron and orbital level.
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Advanced Membranes
·
2025
·
IF 9.5
Yixin Wang,Yingda Huang,Kang Geng,Bin Hu,Ruofei Gao,Erqiang Yang,Junfen Li,Jiandang Xue,Nanwen Li
Anion exchange membrane (AEM) is a core component of potentially more efficient and cost-effective anion exchange membrane water electrolyzers (AEMWEs), which combine the advantages of traditional alkaline water electrolyzers (AWEs) and proton exchange membrane water electrolyzers (PEMWEs). Despite extensive research efforts in recent years, AEMs still face significant challenges, particularly insufficient alkaline stability and limited dimensional/mechanical stability. In this work, we enhanced the mechanical and alkaline stability of AEMs by incorporating the thermoplastic elastomer polystyrene-block-polybutadiene-block-polystyrene (SBS) into the poly (terphenyl piperidinium) (PTP) matrix. The optimal PTP-SBS-2.5% membrane exhibits outstanding dimensional stability (9.4% swelling at 20 °C), robust mechanical properties (tensile strength of 51.5 MPa and elongation of 63.1% at break in wet state), low alkali absorption (0.875%) and exceptional alkaline stability (92.4% conductivity retention after 1500 h). Notably, the membrane demonstrates stable operation in AEMWE for over 3000 h with a low voltage decay rate of 41.1 μV h –1 . These results highlight the significance of SBS in enhancing both the alkaline stability and mechanical performance of PTP-based AEMs.
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Molecular Catalysis
·
2024
·
IF 3.9
XiaoNing Gao,YanXiao Zhang,Wei Fu,Hong Zhou,Lu Feng
Conventional hydrolysis of total saponins for the extraction of diosgenin, an essential ingredient in the production of steroid hormones, has caused significant ecological pollution, making efficient and clean extraction methods necessary. Here, UiO-66-NH 2 with defect sites containing Zr-coordinated hydroxide and water groups was synthesized using concentrated HCl as a crystal modulator, which was further treated with trimethylsilyl trifluoromethanesulfonate (Me 3 SiOTf) to afford UiO-66-NH 2 OTf using the oxygen affinity of the Me 3 Si group. The strong Lewis acid UiO-66-NH 2 OTf was used to extract diosgenin from the total saponin, and the extraction temperature, extraction time and amount of addition were optimized using single-factor experiments and the response surface method. In addition, high-resolution mass spectrometry has been used to analyze the resulting compounds, thus suggesting an alcoholysis pathway and an alcoholysis mechanism for the total saponins.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Yu Bai,Haiping Zhou,Jia-Lin Yang,Qingqing Pan,Jiawei Wang,Yunpeng Wu,Xing-Long Wu
Aqueous zinc-ion batteries (AZIBs) have great potential for large-scale energy storage applications. However, the parasitic reactions, such as continuous hydrogen evolution reaction (HER), seriously hamper the reversibility and cycling stability of the zinc metal anode (ZMA), limiting its practical application. In this paper, a pre-growth interfacial layer strategy is adopted to grow the enol/ketone conversion interfacial layer on the surface of ZMA (denoted as Zn@AA). H + can be reversible “lock/unlock” during reversible enol/ketone conversion reaction. It not only broadens the capacity of AZIBs (Zn 2+ /H + co-insertion), but also inhibits the HER reaction (the amounts of H 2 evolution decreased obviously in both Zn@AA||Zn@AA and Zn@AA||VO 2 ·H 2 O@Ppy (Ppy denote as polypyrrole) cells by on-line differential electrochemical mass spectrometry analysis), thereby improving its stability performance. The cycle life of the assembled Zn@AA||Zn@AA cell exceeded 3200 h at 1 mA cm −2 and 1 mA h cm −2 . Furtherly, the Zn@AA||VO 2 ·H 2 O@Ppy full cell also exhibited excellent cycling stability and capacity retention. This work provides new ideas for modifying the ZMA interfacial layer to inhibit the HER, which guides the development of AZIBs.
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JOURNAL OF MOLECULAR LIQUIDS
·
2024
·
IF 5.3
Qihui Ding,Qian Shan,Qi Zhang,Mengda Chen,Ding Cai,Wei Wu
Hexagonal boron nitride (h-BN) with a large specific surface area and unique optoelectronic properties has good application prospects in many fields. The liquid phase exfoliation method is considered the most promising method for achieving controllable preparation of boron nitride nanosheets (BNNSs), but the low-cost, relatively environmentally friendly and efficient liquid phase exfoliation is still difficult to achieve. Choosing a suitable solvent system is the key to achieving efficient exfoliation. Deep eutectic solvents (DESs) have the advantages of simple synthesis, low cost, high thermal and chemical stability and strong biocompatibility and are expected to be green solvents for preparation of BNNSs . In this paper, it was found that the properties of DESs and its interaction with h-BN had a significant impact on the electrochemical exfoliation of h-BN. The intercalation effect of DES and the compatibility between DES and h-BN were the main factors affecting the yield, while the quality of BNNSs mainly depended on the decomposition and expansion effect of DES. This rule also can be applied to prepare highly conductive and hydrophilic two-dimensional material Ti-MXene. This research explores the structure–activity relationship between two-dimensional materials and DESs, and provides a theoretical basis for the environmentally friendly and efficient preparation of two-dimensional materials using DESs as exfoliation solvents.
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