Advanced Science
·
2026
·
IF 14.1
Ruihua Li,Haiwei Wu,Hairu Wei,Wenhao Jia,Frederik Bettels,Leon Schenk,Zhihua Lin,Hanbin Liu,Guodong Liu,Zhijian Li,Lin Zhang
Lithium–sulfur (Li–S) batteries face low sulfur utilization and limited rate capability. Although electrolyte engineering is a key strategy for improving the conversion kinetics of lithium polysulfides (LiPS), achieving a balance between high energy density and high power density remains challenging. This study combines an ultra-low concentration electrolyte with a dual-functional hybrid organic selenium/organic tellurium additive (DPDSe/DPDTe). The system exhibits higher ionic conductivity and enhanced LiPS conversion kinetics. This is attributed to the high solubility of LiPS at low concentrations, which enhances the accessibility of active materials. By adjusting the mixing ratio of DPDSe/DPDTe, the formed DPDSe-Te exhibits unique solvation structure regulation and synergistic catalytic effects. This Li–S battery delivers an initial specific capacity of 1103 mAh g −1 (65.9% sulfur utilization) at 0.5 C and retains 89.3% of its capacity after 100 cycles. Even at 2 C, a capacity of 783 mAh g −1 is achieved. The pouch cell exhibits a high energy density of 340 Wh kg −1 at 0.5 C with stable cycling. This low-concentration, dual-functional additive strategy synergistically addresses LiPS solubility limitations and kinetic bottlenecks, offering an effective route toward Li–S batteries with both high energy density and high-power density.
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Science China-Chemistry
·
2026
·
IF 9.8
Wang Nan,An Tinghui,Li Jiaqi,Wang Yuhao,Xiang Dong,Cai Kedi
Cu-based electrocatalysts are promising for the electrocatalytic CO 2 reduction reaction (eCO 2 RR) to realize valuable chemicals production. Here, a Mg-doped Cu based electrocatalysts via transient CO 2 pulsed laser (L 4 -Mg/Cu x O) was synthesized for highly selective eCO 2 RR to ethanol (C 2 H 5 OH). The synergistic effect of Mg-doping and transient CO 2 pulsed laser irradiation enables excellent eCO 2 RR performance, realizing Faradaic efficiencies (FE) of 52.2% and 74.1% for C 2 H 5 OH and C 2 products under a high current density of 298.9 mA cm −2 , respectively. Operando Raman spectroscopy and DFT simulations results confirm that Mg-doping strategy suppresses the hydrogen evolution reaction (HER), enhances CO adsorption, elevates local pH and accelerates H 2 O dissociation, which could be beneficial for promoting OC–CO coupling and proton supply in eCO 2 RR. Furthermore, Mg incorporation induces electron delocalization in which electron accumulation on the C atom of *CHCOH intermediate and its enhanced p-d orbital coupling with Cu interface, which stabilizes the C–O bond from breakage and selectively favours the C 2 H 5 OH pathway, thus decoupling the selectivity between C 2 H 5 OH and ethylene. When employed in Li-CO 2 batteries, L 4 -Mg/Cu x O delivers 20480 mAh g −1 discharge capacity and cycling stability over 187 cycles. This work presents a universal strategy for regulating eCO 2 RR selectivity through precise laser energy delivery, demonstrating significant potential for renewable energy conversion and storage.
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Journal of Energy Storage
·
2026
·
IF 10.7
Xu Zhang,Qifan Gu,Jiabao Bai,Guoting Long,Yana Liu,Yunfeng Zhu,Jiguang Zhang,Jun Wang,Rui Shi,Xiaohui Hu
VS 2 has attracted extensive attention as potential host material for Mg 2+ /Li + hybrid-ion batteries (MLHBs) because of its considerable capacity and large interlayer spacing. However, the relatively weak adsorption ability and huge volume variations lead to slow reaction kinetics and poor cycle lifespan, which greatly restricts their further application in MLHBs. Herein, we have proposed a synergistic engineering of morphology regulation and sulfur vacancy for the construction of hierarchical VS 2 microflower via two pivotal procedures, which is demonstrated as a high-energy density cathode for MLHBs. Specifically, such special microflower morphology with sufficient interspace and abundant sulfur vacancies can release the inner stress to maintain structural integrity, thus leading to enhanced cycling stability. Meanwhile, the synergistic effect of flower-like structure and abundant sulfur vacancies contributes to providing sufficient redox-active sites, facilitating charge transfer, improving Li + adsorption capacity, and accelerating ion diffusion, as verified by kinetic analysis and theoretical calculations. Consequently, the hierarchical VS 2 microflower exhibits a high reversible capacity of 488.8 mAh g −1 at 100 mA g −1 , an excellent energy density of 406.6 Wh kg −1 , and an ultralong cycling stability with a capacity retention of 72.8% at 4000 mA g −1 after 2000 cycles. Besides, surface-controlled capacitive contribution analysis coupled with in-situ electrochemical impedance spectra (EIS) measurements confirm the excellent reaction kinetics. Therefore, this work presents a synergistic engineering strategy that combines morphology regulation and vacancy introduction in the fabrication of VS 2 -based cathodes for advanced MLHBs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Lu Yu,Xiaomeng Liu,Rongping Yun,Min Wang,Xu Xiang
Oilfield brine, a by-product of oil and gas extraction, contains valuable resources such as Li + , K + and Ca 2+ , offering potential utilisation benefits but also presenting separation challenges. We developed a reaction-coupled separation strategy to separate Ca 2+ and Li + while simultaneously synthesising a calcium-based layered double hydroxide (Ca-based LDH) from the brine. This technology enables the recovery of over 90 % of Ca 2+ into the solid product, with 98.5 % of Li + retained in the liquid phase, achieving highly efficient separation of Ca 2+ and Li + . The resulting Ca-based LDH demonstrated excellent capacity for removing heavy metals, such as Cu 2+ , Ni 2+ and Zn 2+ , from electroplating wastewater. The removal capacities reached up to 384.2 mg/g for Cu 2+ , 319.3 mg/g for Ni 2+ and 367.9 mg/g for Zn 2+ . In both single-cation and mixed-cation wastewaters, metal concentrations were dramatically reduced to parts-per-billion (ppb) levels. Kinetic studies indicated rapid adsorption behaviour of Cu 2+ , Ni 2+ and Zn 2+ by the Ca-based LDH. Mechanistic analysis revealed that Ca 2+ ions in the LDH layers are isomorphously substituted by Cu 2+ , Ni 2+ and Zn 2+ from the solution, forming Cu-, Ni- and Zn-containing LDHs with enhanced structural stability. Additionally, the released Ca 2+ ions precipitate with CO₃ 2− , derived either from intercalated anions or carbonate in the water. Such conditions promote further substitution of Ca 2+ in the LDH layers by Cu 2+ , Ni 2+ and Zn 2+ , resulting in robust metal removal and ultralow residue concentrations in the treated wastewater. This work presents an efficient, economical and sustainable approach for the simultaneous separation and utilisation of oilfield brine resources and treatment of electroplating wastewater.
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GREEN CHEMISTRY
·
2025
·
IF 9.2
Fengyin Zhou,Beilei Zhang,Hongya Wang,Danfeng Wang,Xin Qu,Shiyu Wang,Mengyi Tang,Ling Peng,Xiang Chen,Dihua Wang,Lawrence Yoon Suk Lee,Huayi Yin
Pyrolysis, thermal reduction, and mechanochemical force are commonly used for biomass utilization, materials synthesis, and spent Li-ion batteries recycling. However, the effect of mechanical treatment on pyrolysis gas generation and thermal reduction remains unclear. Herein, we study the effect of mechanical treatment on the biomass pyrolysis reduction of LiCoO2. The mechanical milling generates oxygen vacancies in the LiCoO2 lattice. In addition, the mechanical treatment can regulate the pyrolysis gas of sawdust in terms of increasing the content of H2, CH4, and CO while decreasing the CO2 content. The oxygen vacancies and pyrolysis gas are beneficial for the thermal collapse of the LiCoO2 structure, leading to the rapid and complete separation of Li and Co, thereby increasing the recovery efficiency to above 98%. The understanding of the interplay of mechanical force, oxide structure, and pyrolysis gas composition helps design green approaches to enabling metal and organic resource recovery and utilization.
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ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Yuxin Gong,Mengyu Fu,Yingmin Jin,Yumeng Li,Ruifan Lin,Yong Zhang,Lei Lei,Ying Zhang,Changsong Dai,Yueping Xiong
Halide solid-state electrolytes (HSSEs), exemplified by low-cost Li 2 ZrCl 6 , exhibit high ionic conductivity and a wide electrochemical stability window, making them promising for all-solid-state batteries (ASSBs). Yet, optimizing HSSEs by elemental doping is either inefficient or costly, necessitating alternative approaches. Inspired by the filler-modified LiI-Al 2 O 3 system with fast-conductive interfacial percolation layer (IPL) and with regard to the underlying insufficient interfacial filler/electrolyte contact with Li 2 ZrCl 6 matrix, which hinders the IPL formation, the use of transition metal oxide Fe 2 O 3 is pioneered as a filler to generate oxygen vacancies and foster benign filler/electrolyte interfaces. At the Fe 2 O 3 /electrolyte interface, synchrotron X-ray adsorption spectra and electron energy loss spectra mapping reveal a distinctive O-Cl exchange reaction and improved interfacial contact. Density function theory, bond-valence site energy calculations, and finite-element simulations validate improved Li + migration via mitigated electrostatic confinement, reduced migration energy barriers, and spatially confined electric-field-accelerated IPLs. Benefiting from these merits, the ionic conductivity of the composite electrolyte surges from 0.4 to 2.15 mS cm −1 , with Li + migration activation energy reduced to 0.28 eV. Paired with the NCM811 cathode, the ASSB delivers 90% capacity retention over 1000 cycles at 0.5 C. This work offers a novel, cost-effective strategy for high-performance halide-oxide composite electrolytes from the counterintuitive perspective of nanofiller integration.
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Hui Wang,Minyao Liu,Guangzhao Zhang,Yukun Chen,Yonggang Min,Jin Li
The propagation of lithium dendrites and the “shuttle effect” of polysulfide represent two critical challenges hindering the practical application of lithium sulfur batteries (LSBs). Herein, a dual-functional integrated Janus separator is proposed, which simultaneously inhibits the shuttle effect of polysulfide and lithium dendrites to enhance the electrochemical performance of LSBs. On the lithium metal anode interface, directional denaturation treatment was first applied to increase the α-helix content in soy protein isolate (SPI), yielding α-SPI with enhanced Li+ affinity. Phytic acid (PA) served simultaneously as cross-linker and acidity regulator, anchoring α-SPI nanoparticle onto carboxylated cellulose nanofibers (C–CNF). The resulting composite was uniformly sprayed onto the separator to construct a lithiophilic α-SPI@C–CNF framework, which homogenizes Li+ flux and suppresses lithium dendrite. At the cathode interface, the made-to-measure three-dimensional carbon (M-3DC) physically entraps lithium polysulfides and thus prevent the shuttle effect. Finally, the LSB using the Janus separator delivers a high initial capacity of 938 mAh g–1 and exhibits an excellent operation stability by retaining 537.8 mAh g–1 after 1000 cycles (with a capacity degradation rate of only 0.043% per cycle). This study presents a versatile approach to simultaneously mitigate the intrinsic limitations of both the lithium metal anode and the sulfur cathode in LSBs.
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Batteries-Basel
·
2023
·Vol. 9
·期 5
·
IF 4
Ningning Feng,Chaoqiang Wang,Jing Wang,Yang Lin,Gang Yang
Lithium–oxygen (Li-O2) batteries have captured worldwide attention owing to their highest theoretical specific energy density. However, this promising system still suffers from huge discharge/charge overpotentials and poor cycling stability, which are related to the leakage/volatilization of organic liquid electrolytes and the inefficiency of solid catalysts. A mixing ionic liquid-based gel polymer electrolyte (IL-GPE)-based Li-O2battery, consisting of a 20 mM 2,5-di-tert-butyl-1,4-benzoquinone (DBBQ) 40 mM N-methylphenothiazine (MPT)-containing IL-GPE and a single-walled carbon nanotube cathode, is designed for the first time here. This unique dual redox mediators-based GPE, which contains a polymer matrix immersed with mixed ionic liquid electrolyte, provides a proper ionic conductivity (0.48 mS cm−1) and effective protection for lithium anode. In addition, DBBQ, as the catalyst for an oxygen reduction reaction, can support the growth of discharge products through the solution–phase pathway. Simultaneously, MPT, as the catalyst for an oxygen evolution reaction, can decompose Li2O2at low charge overpotentials. Hence, the DBBQ-MPT-IL-GPE-based Li-O2battery can operate for 100 cycles with lower charge/discharge overpotentials. This investigation may offer a promising method to realize high-efficiency Li-O2/air batteries.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Xiaowei Yang,Yanfei Zou,Chen Hu,Shikun Su,Zhenghang Wang,Houhe Dong,Wenying Teng,Bing Teng,Bingtao Zhang,Degao Zhong
Cr4+-activated phosphors are important candidate materials for NIR-II light sources, but providing a suitable lattice coordination environment for Cr4+ and achieving long wavelength broadband emission remains a challenge. In this work, a series of Cr4+-activated ABO2 (A = Li, Na; B = Al, Ga) phosphors were successfully prepared. Due to the presence of only tetrahedral coordination structures available for Cr4+ to occupy in the matrix crystal ABO2, the valence state and luminescence stability of Cr4+ are effectively guaranteed. Through the cation substitution design of A-site (Na → Li) and B-site (Ga → Al), the [BO4] tetrahedron is distorted and expanded, which degrades the symmetry of the Cr4+ coordination crystal field. Consequently, the central wavelength of the Cr4+ emission peak is tuned from 1280 to 1430 nm, and the fwhm is significantly extended from 257 to 355 nm. Thebroadband NIR-II light sources constructed with LiAlO2: 0.03Cr4+ and NaGaO2: 0.03Cr4+ phosphors verify their important potential applications in nondestructive testing and biological imaging.
研究领域:
材料科学
·
光学材料
·
固态化学
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光子学
·
近红外光源
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NANOTECHNOLOGY
·
2022
·Vol. 34
·期 8
·085401
·
IF 3.953
Hongna Jia,Yao Wang,Shuya Zhao,Haipeng Wang,Na Ju,Xinyue Zhang,Hong Li,Zejun Sun,Hong-bin Sun
Carbon materials derived from metal-organic frameworks have attracted increasing attention as anodes for energy storage. In this study, Fe, Ni-doped ZIF-8 is carbonized at high temperature to obtain bimetallic Fe and Ni modified tension -relaxed carbon (FeNi@trC). Fe and Ni have opposite structural modification effects when the metal ions are doped into the ZIF-8 dodecahedron. The obtained carbon material maintains the regular dodecahedron morphology, which means the relaxation of tension and strong thermal stability during annealing. Moreover, the presence of nickel enhances the carbonization degree and electrochemical stability of FeNi@trC, while the calcination of the tensive ZIF-8 precursor offers more defect sites. The discharge capacities of FeNi@trC materials are stable at 182.9 mAh·g−1 and 567.9 mAh·g−1 for sodium-ion batterie (SIB) and lithium-ion batterie (LIB) at 0.05 A·g−1. Compared with the current density of 0.05 A·g−1, the discharge capacity of SIB and LIB attenuates by 29.4% and 55.9% at 1 A·g−1, respectively, and the FeNi@trC shows good performance stability in the following cycles.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Xiangxiang Fu,Huanhuan Duan,Shiwei Zhang,Ran Bi,Yuanfu Deng,Guohua Chen
Lithium (Li) metal is considered as one of the attractive anodes for next-generation high-energy-density batteries due to its ultrahigh theoretical specific capacity and low potential. However, many great challenges including uncontrolled dendrite growth and undesired side reactions during repeated cycling still seriously hinder its practical application in Li metal secondary batteries. Herein, we report the hexachloro-1,3-butadiene (HCBD) molecule as a functional additive to stabilize the Li anode by forming a stable solid electrolyte interface (SEI) layer with high Li ion conductivity via in situ surface and electrochemical reactions. Density functional theory calculations demonstrate that HCBD can preferentially react with the Li anode, which generates an ionic conducting species (LiCl) into an SEI layer. The LiCl-rich SEI layer effectively regulates Li+ deposition/stripping kinetics and then induces uniform nucleation of Li+ and reduces the side reactions between the Li anode and electrolyte. With an optimal amount of HCBD in an ether-based electrolyte, an excellent cycling lifespan (7000 h) was achieved with a low hysteresis voltage of ∼10 mV at 1.0 mA cm–2 in a Li||Li symmetrical cell. Furthermore, the LiFePO4-based cell with the additive-functionalized Li anode displays obviously improved cycling stability (with a high specific capacity of 141.1 mAh g–1 after 350 cycles at 1 C).
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IONICS
·
2022
·Vol. 29
·期 1
·183-191
·
IF 2.961
Wang Yang,Liang Xin,Wu Xiaolong,Wang Lulu,Xu Kun,Sun Yi,Wang Jiazhao,Xiang Hongfa
Li–S batteries have been
considered as the most desirable candidate for next-generation batteries because of their high energy density and low cost, although the problems of the insulating nature of S and Li 2 S and the “shuttle effect” of polysulfides in Li–S batteries have to be addressed. In this work, we propose NaCl templates and a solid–liquid coexistence strategy to synthesize an N-doped carbon matrix with interconnected micro-mesoporous structure. Benefiting from the critical state of solid–liquid coexistence at the melting point of NaCl and a pretreatment by pressure, a unique porous structure with an interconnected network of micropores and mesopores is obtained. The micropores can prevent the dissolution of polysulfides, the mesopores can increase the S loading, and the interconnected pore network can significantly improve the usage of active materials. As a result, the cathode with the N-doped carbon matrix shows improved electrochemical performances.
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