ADVANCED MATERIALS
·
2024
·Vol. 36
·期 48
·2412319
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IF 27.4
Xitang Qian,Yuxiang Lyu,Siyu Zhou,Yican Qiu,Yan Sun,Yuan Yuan,Minhua Shao
Metal sulfides are increasingly favored as cathode materials in all-solid-state batteries (ASSBs) due to their high energy density, stability, affordability, and conductivity. Metal sulfides often exhibit capacities exceeding their theoretical limits, a phenomenon that remains not fully understood. In this study, it reveals that this phenomenon is primarily due to the sulfur decomposition from sulfide-based electrolyte. By employing the high-energy ball milling (HEBM) technique, the deposition of sulfide-based electrolyte onto sulfur is intentionally promoted, resulting in higher charge capacities compared to the discharge capacities and surpass theoretical limits of metal sulfides. Using chromium sulfide (Cr 2 S 3 ) as the active material, the sulfur decomposed from sulfide-based electrolyte transforms into lithium sulfide (Li 2 S) after discharge, resulting in an increased capacity by ≈439.6 mAh g −1 and improved cycling stability. Consequently, it demonstrates a specific capacity surpassing 1200 mAh g −1 with a capacity retention of over 80% after 650 cycles, maintaining cycling stability for more than 1900 cycles and achieving a Coulombic efficiency exceeding 99.9%. This versatile HEBM approach enables the fabrication of ASSBs utilizing various transition metal sulfides, such as molybdenum disulfide (MoS 2 ), niobium disulfide (NbS 2 ), and iron disulfide (FeS 2 ), all exhibiting over theoretical limited capacities and prolonged cycling capabilities.
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高影响因子
COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
·
2025
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IF 8.9
Yabin Zhang,Jiaming Wang,Xuedong Wu,Linyan Zhu,Wenguang Zhang,Lishuai Zong,Jinyan Wang,Xigao Jian
The robust operation of electromagnetic waves in communication systems with extreme temperatures relies on high-temperature resistant wave-transparent composites, with organic resin matrix being a pivotal constituent. Enhancing the heat resistance of resins while maintaining excellent processability poses a significant challenge. Herein, a novel “rigid-in-flexible” self-curing silicon-based silicon-based phthalonitrile monomer containing phenylacetylene backbone (Si-ALK-PN) was designed. The silazane component disrupts the crystallinity in Si-ALK-PN, resulting in a characteristic of low viscosity (0.3 Pa·s) and extended processing window (>3h). After curing at 450 °C, the resin, namely Si-ALK-PN-450 °C, demonstrated exceptional thermal stability ( T 5% = 631 °C) and thermo-oxidative stability ( T 5% = 560 °C). Their quartz fiber-infused composites (Si-ALK-PNs/QF) were manufactured through a straightforward melt processing approach. Upon post-curing at 450 °C, Si-ALK-PN-450 °C/QF exhibited elevated glass transition temperature, flexural strength, and consistent dielectric properties across a wide temperature ranging from 25 °C to 600 °C. Especially, it exhibited excellent flame retardancy as well, stemming from release of eco-friendlyeco-friendly inert gases (NH 3 ) and the high thermal stability of N-enriched all-aromatic PN resin. The design concept of “rigid-in-flexible”, along with the multi-functional group co-curing strategy, offers a promising solution for addressing the trade-off between processing and heat resistance in resins, extending beyond PN resins.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yuxuan Shao,Junjie Ni,Jie Yin,Xinqing Liu,Yulai Song,Yue Xu,Shuai Guo,Laima Luo
The construction of heterojunctions between non-noble-metal based compounds affords a scheme for accelerating the reaction kinetics of oxygen evolution reaction (OER) without using precious mental materials, which is extremely important but remains challenging. Herein, the heterogeneous structure between Fe 60 Co 10 Ni 10 Cr 10 Mn 10 medium-entropy alloy (MEA) and FeS 2 is developed by a mechanical alloying approach. The resulting MEA-30 wt%FeS 2 delivers a high OER activity with a low overpotential of 261.6 mV at 10 mA/cm 2 , along with Tafel slope of 52.7 mV/dec in 1.0 mol/L KOH solution, superior to the commercial RuO 2 . The combination of detailed characterization techniques and density functional theory (DFT) calculation reveals that the heterojunctions between Fe-based MEA and FeS 2 generates the synergistic effect on the activation and formation steps of OOH*, thus promoting the OER reaction kinetics. Furthermore, the abundant active sites provided by the reconstructions of MEA-30 wt%FeS 2 during OER process also contributes to the catalytic performance. This work greatly expands the application scope of medium-entropy materials and provides a new method for the fabrication of novel heterogeneous electrocatalyst of Fe-based MEA and FeS 2 .
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FUEL
·
2024
·
IF 6.7
Wenfeng Peng,Zhengxing Lv,Wenju Zhou,Bingmin Yan,Shijing Zhao,Lailei Wu,Junshuang Zhou,Huiyang Gou
Creating highly efficient bifunctional transition metal phosphide catalysts for electrochemical water splitting through cost-effective and universal methods remains an elusive challenge. Here we introduce a universal high temperature and high pressure (HTHP) technique that readily produce phase-pure TMPs, including FeNiP, CoNiP, and Fe 2/3 Co 2/3 Ni 2/3 P (CFNP), which can serve as an ideal model for investigating the relationship between electrocatalytic activity, structure, and chemical composition. The crystal structure of obtained CFNP has been carefully determined for the first time by using single-crystal X-ray diffraction (XRD) and XAS simulations. In the structure of CFNP, iron atoms form an MP4 tetrahedron with Co atoms and a 5-coordination pyramid with Ni atoms. This arrangement synergistically induces an electron-deficient state in the metals and an electron-rich state in phosphorus, enhancing CFNP/NF’s bifunctional catalytic effectiveness, achieving low overpotentials of 92 mV and 239 mV at 10 mA/cm 2 in 1 M KOH environment for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. Moreover, an integrated electrolyzer using CFNP/NF as both electrode components can achieve a current density of 10 mA cm −2 at 1.536 V, showcasing a catalytic activity for overall water splitting comparable to those of phosphide-based electrocatalysts. The HTPH technique opens new possibility for exploring pure-phase multimetallics and high-entropy phosphides as potential multifunctional materials for potential applications.
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BIORESOURCE TECHNOLOGY
·
2024
·
IF 9.7
Zongshuo Han,Ruijie Hu,Xiaoying Zheng,Zhilin Zhao,Wenfei Li,Haidong He,Tao Lin,Hang Xu
The long acclimation period and sensitivity to environmental conditions of Anammox are the bottlenecks for its promotion and application. An innovative strategy was adopted to accelerate functional microbial enhancement and improve nitrogen removal performance by inoculating cryopreserved Anammox sludge and activated sludge with intermittent dosing of nanoscale zero-valent iron (nZVI). The acclimation time was shortened by 76 days with nitrogen removal efficiency (NRE) reaching up to 91.07 %. Anammox, NDFO (nitrate/nitrite-dependent Fe(II) oxidation), Feammox (Fe(III) reduction coupled with anaerobic ammonium oxidation) and abiotic reactions were coupled in the system with nZVI, contributing to 69.79 %, 15.14 %, 9.84 % and 0.25 % of nitrogen removal, respectively. Further microbial analysis demonstrated significant enrichment of functional microorganisms, such as Candidatus Jettenia , Acidovorax and Comamonas . High-efficient nitrogen removal was attribute to the increase of functional genes involved in Anammox, electronic transfer, heme C synthesis and iron metabolism. This work provides an inspiring idea for the mainstream Anammox application.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Rui Qin,Ji Chen,Yan Bai
NdFeB waste serves not only as a crucial resource for the recovery of rare earth elements (REEs) but also as an underutilized source of gallium (Ga). In this work, to simultaneously extract REEs and Ga from NdFeB waste, an efficient and novel method was developed, which involved the process of leaching, reduction, solvent extraction, precipitation, and calcination. Initially, the Pr, Nd, and Ga were co-leached with 5 mol/L HCl and liquid-solid ratio (mL/g) of 5:1 at 90 °C for 150 min, resulting in the leaching rate of Pr, Nd, and Ga were 98 %, 99 %, and 98 %, respectively. Secondly, to mitigate the interference of Fe (III) on the extraction process, Fe (III) was reduced to Fe (II) completely using Fe powder for 10 min, given that the excess iron powder factor was 1.2. Then, the tributyl phosphate (TBP) was chosen as the extractant for Ga due to its high selectivity. Under the optimal conditions, three-stage counter-current extraction achieved an extraction efficiency of 99 % for Ga, with the addition of 10 % isodecanol to eliminate the third phase. The gallium was completely stripped by water at a phase ratio (O/A) of 2:1. Subsequently, di-2-ethylhexylphosphoric acid was selected as the Pr and Nd extractant because of its high separation ability between REEs and Fe (II). The extraction efficiency of Pr and Nd achieved more than 99 % through three-stage counter-current extraction and the entire stripping of Pr and Nd was realized by 1.8 mol/L HCl. Additionally, a significant amount of Fe (II) in the raffinate was treated via adding oxalic acid to obtain FeC 2 O 4 ⋅ 2H 2 O. Finally, the Ga 2 O 3 and Nd 2 O 3 (PrO 2 ) were prepared from the stripping solution. According to the whole process, the yield of Ga, Pr, and Nd was 93.4 %, 97 %, and 98 %, with the purity of Ga 2 O 3 and Nd 2 O 3 (PrO 2 ) being 98.6 % and 98.4 %, respectively. The results suggested that the stepwise recovery of REEs and Ga from NdFeB waste can be achieved.
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LANGMUIR
·
2024
·
IF 3.7
Xiangchi Liu,Ailing Liu,Baijun Liu,Mingyao Zhang
Sustainable development has become an inevitable trend in the world’s green chemical industry for a generation or more. In this study, a monodisperse magnetic polystyrene mesoporous composite microsphere (MPPS) composed of Fe3O4 nanoparticles loaded on polystyrene mesoporous microspheres is introduced. These microspheres serve as effective adsorbents for the swift removal of cationic dyes. The fabrication of the wastewater adsorbent, with its simple operation and economic practicality, involved a combination of dispersion polymerization, a sulfonation reaction, two-step swelling polymerization, and in situ alkaline oxidation technology. Notably, the adsorption capacity within 3 min reaches 184.0 mg/g, with an impressive adsorption efficiency of 92%. This is primarily attributed to the high specific surface area (Smax) of the MPPS providing more reaction sites for π–π interaction. Simultaneously, the attractive force between negatively charged sulfonic acid groups and cationic dyes is enhanced through surface modification of the MPPS. Furthermore, the MPPS, boasting a maximum saturation magnetization of 38.19 emu/g, ensures rapid separation from the solution for recycling within 3 s. Even after 5 cycles, the adsorption efficiency remains over 90%. The rapid separation of dyes is facilitated by the magnetic attraction of Fe3O4 nanoparticles from the MPPS under the application of a magnetic field. These composite mesoporous materials exhibit outstanding performance in both efficient selective adsorption and recyclability, presenting a novel green adsorbent with promising prospects for sustainable development. This innovation is poised to excel in fields such as sewage treatment, separation, and purification.
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SOLAR ENERGY MATERIALS AND SOLAR CELLS
·
2024
·
IF 6.3
Fei Wang,Yuliang Zhang,Mengyang Cong,Ting Shu,Ying Qin,Yanhua Lei,Miranda Liu,Xiaobo Chen,Yi Lin,Zecheng Qian
The continual optimization and advancement of solar desalination technology represent an ongoing focal point in addressing the persistent challenge of freshwater scarcity. In the solar evaporator , subjected to high concentrations of saltwater and intense solar irradiation , as well as other demanding operational conditions, the presence of salt accumulation at the photothermal interface inevitably diminishes both the evaporation efficiency and the service life of the photothermal evaporator. In this study, we have successfully coated polypyrrole with carbon nanopowder (C), iron nanopowder (Fe), boron nitride (BN), boron carbide (B 4 C), molybdenum disulphide (MoS 2 ), and molybdenum carbide (Mo 2 C) through in-situ polymerization, and have assembled these coated materials with blends of polyvinyl alcohol/poly (vinylidene fluoride), creating an innovative amphiphilic photothermal composite film . The resulting thin-film evaporator has achieved an impressive 94.7 % evaporation efficiency under 1 sun irradiation. Introducing perforations on the film evaporator's surface further improves efficiency, reaching approximately 87.0 % under prolonged exposure to high salinity (20 %) conditions. This improvement is attributed to the increased water pathway facilitated by the perforations, preventing salt particle deposition on the evaporator's surface and significantly enhancing desalination efficiency.
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Matter
·
2025
·
IF 17.5
Li Yang,Hao Wu,Fei Guo,Gaojie Zhang,Wenfeng Zhang,Haixin Chang
Electrical control of the anomalous Hall effect (AHE) provides an important gateway to reveal and regulate topological properties of spins. However, direct, immediate electrical tuning of the AHE in materials has been elusive, unfeasible, and rarely reported. Here, we demonstrate direct, immediate, nonlinear, electric current regulation of the AHE in a single, novel, van der Waals, room-temperature, ferromagnetic, ultrathin, two-dimensional (2D) crystal for intrinsic sensitivity of nodal electronic structures induced by 2D spin-orbit coupling (SOC) in a 2D quantum limit with an ultrasmall current (∼10 2 A cm −2 ). The multivalued electrical tuning of anomalous Hall resistance (R AHE ) ( R A H E 1 R A H E 2 ∗ 100 % ) is up to 584% and remains 126% at room temperature. The squared correlation between R AHE and longitudinal resistance indicates an SOC-dominated Berry curvature-induced AHE. This immediate-current AHE with distinct dependence on the dimension, crystal layer, and electronic topology provides unique quantum platforms for probing the essence of the dimension and for low-power spintronics and brain-like quantum devices.
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WATER RESEARCH
·
2025
·
IF 12.4
Qiya Sun,Dunjie Li,Yunpeng He,Qian Ping,Lin Wang,Yongmei Li
This study developed a novel strategy combining a nanoscale zero-valent iron (nZVI)/peracetic acid (PAA) pretreatment and hydrochar regulation to enhance anaerobic digestion of waste activated sludge (WAS) under ammonia-stressed conditions. The strategy significantly enhanced methane production at ammonia concentrations below 3000 mg/L, with the regulation groups (AN3000/REG) achieving a 50.1 % increase in cumulative methane yield. Metagenomic analysis demonstrated a 14.2 % enrichment of key functional microorganisms, including syntrophic fatty acid-oxidizing bacteria and hydrogenotrophic methanogens, in the AN3000/REG groups. Some of them promote the conversion of butyrate and valerate to acetate through the upregulation of key genes in the fatty acid β-oxidation pathway, thereby supplying sufficient substrates for acetoclastic methanogenesis. Beyond enhancing acetoclastic methanogenesis, the AN3000/REG groups exhibited significant upregulation of other metabolic pathways, with a 34.2 % increase in syntrophic acetate oxidation-hydrogenotrophic methanogenesis genes and a 17.1 % increase in methanol/methylotrophic methanogenesis-related genes. These findings were further validated by the metatranscriptomic and metaproteomic combination analyses. Furthermore, the AN3000/REG groups exhibited a significant enhancement in direct interspecies electron transfer, with functional microbes (e.g., Geobacter, Methanosarcina , and Methanobacterium ), pili, and cytochrome c showing significant increases of 1.38-fold, 12.7-fold, and 5.6-fold, respectively. This might be due to the synergistic effects of nZVI and hydrochar in the regulation groups. Additionally, metabolomic analyses revealed that the regulation strategy improved the microbial adaptability to ammonia stress by modulating metabolic products, such as alkaloids. Our study not only provides a promising strategy for alleviating ammonia inhibition during the anaerobic digestion of WAS but also provides a strong basis for understanding the underlying mechanism under ammonia-stressed conditions.
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ACS ES&T Engineering
·
2024
·
IF 7.4
Kai He,Yuanfang Lai,Shuchen Wang,Li Gong,Feng He
Metal doping for improving the reactivity of zerovalent iron (ZVI) has been well studied, while Mn(II)-modified microscale ZVI (Mn-mZVI) has not yet been explored. Herein, ball-milled Mn-mZVI was fabricated and used for Cr(VI) removal. Characterization analysis showed that the structure, composition, and charge of mZVI changed after the Mn(II) modification. The comparative test showed that Mn-mZVI could remove 100% of Cr(VI) within 10 min, whereas mZVI removed negligible Cr(VI) within 60 min. The zeta-potential and electrochemical evidence verified that the enhanced electrostatic attraction and electron-transfer ability contributed to the superior Cr(VI) removal performance of Mn-mZVI. Moreover, the solution pH increase caused the decline of Cr(VI) removal, and the presence of NO3– inhibited Cr(VI) removal, whereas other coexisting ions showed little influence on the Cr(VI) removal performance of Mn-mZVI. Chemical and material characterization analyses revealed that Cr(VI) reduction by Mn-mZVI was the combined action of Fe(0) and generated Fe(II). In addition, the reusability of Mn-mZVI was not ideal due to the surface passivation and loss of Mn(II), but the reactivity could be reactivated by ball-milling the reacted Mn-mZVI again with Mn(II). Overall, this work provides a new mentality for mZVI modification and is important to develop promising mZVI-based materials for Cr(VI) pollution control.
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ACS ES&T Water
·
2024
·
IF 4.8
Zhi Ye,Yunpeng Liu,Jiang Xu,Nan Xu,Juncai Dong,Haijun Chen,Dongrui Li,Lei Peng,Yuxi Gao,Jiating Zhao
The efficiency and stability of in situ remediation of Cr(VI) contamination in underground water and soil are still challenging. In this study, a green tea (GT) synthesized nano-zerovalent iron (nZVI) nanocomposite supported by diatomite (DE) (nZVI@GT/DE) via tea polyphenols was designed. The synergetic effect of DE support and tea polyphenols wrapping increased the Fe(II) component in nZVI@GT/DE and its transportability. Compared to nZVI@GT/Mont (supported by Mont with sandwich structure), nZVI@GT/DE exhibited a notably higher capacity (>100 mg g–1) for immobilizing Cr(VI) and a more pronounced ability to release iron ions in solution (corrosion parameter: K ≈ 1.046). This was attributed to the combined effect of the unwrapping process of tea polyphenols coverage and the distinctive columnar porous structure of DE, which increased the exposure of α-Fe0 core for enhanced Cr(VI) reduction during their cotransport in the water-saturated soil system. X-ray absorption fine structure and X-ray photoelectron spectroscopy analyses confirmed that nZVI@GT/DE released more Fe(II) ions to reduce Cr(VI) to bidentate binuclear Cr(OH)3 (vs FeOCr2O3) complexes. This study unraveled the molecular mechanism and highlighted the Cr speciation transformation and physiochemical property changes of nZVI@GT/DE during their cotransporting when applied in situ remediation in complex subsurface of Cr(VI)-contaminated groundwater and soil system.
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