APPLIED ORGANOMETALLIC CHEMISTRY
·
2025
·Vol. 39
·期 11
·e70415
·
IF 0
Yumin Leng,Muhua Lu,Mengyang Zhang,Anyi Wang,YuChen Dong,Jinbing Cheng,Yebin Guan
Heavy metal ions pose a significant threat to the environment and human health. Developing a highly sensitive heavy metal ion detection method is desirable. In this study, the Au(I)-catenates were formed in glucoamylase (Glu) and neomycin sulfate (Ne). The polychrome metal nanoparticles (MNPs) were prepared based on the template of Au(I)-catenates. The simple and ultrasensitive visual sensor array for the determination of heavy metal ions was established based on the color information extracted from polychrome MNPs. The addition of heavy metal ions shuttled among Au(I)-catenates in the strong alkaline solution. Through the use of the microwave heating method, the spherical and cubic MNPs of various sizes and colors were synthesized. To fully utilize the polychrome MNPs, a visual sensor was constructed for the detection and discrimination of eight heavy metal ions. The fingerprint-like color response signals correspond to each heavy metal ion and can be distinguished using computer software. The detection limit (0.1 nM) of heavy metal ions discriminated by the sensor is significantly lower than the data reported. The validation of the sensor was carried out by quantitative detection of Hg 2+ compared with its content in a certified reference material. This array method shows high sensitivity, good anti-interference, and potential in complex media.
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Journal of Energy Chemistry
·
2026
·
IF 15.6
Ruijie Guo,Zhenxi Li,Yiming Guo,Shilun Gao,Chao-Peng Wang,Huabin Yang,Peng-Fei Cao
Achieving high monomer conversion of 1,3-dioxolane (DOL) enhances the electrochemical stability of PDOL-based electrolytes, while the reduced liquid contents lead to low ionic conductivity. Addition of plasticizers mitigates the conductivity decrease, yet renders decreased monomer conversion. To address this dilemma, a novel gel polymer electrolyte (In-GPE) was developed via in situ polymerization of plasticizer-rich DOL electrolyte using a highly efficient initiator, i.e., indium trifluoromethanesulphonate (In(OTf) 3 ). The In(OTf) 3 can also be reduced to metallic indium (In), which promotes the interfacial alloying with Li metal with significantly lower Li + binding energy. The incorporation of plasticizers simultaneously enhances the electrochemical window and ionic conductivity of the resulting electrolytes. The In-GPE exhibits a wide electrochemical window (∼4.5 V), high ionic conductivity of 5.14 × 10 −4 S cm −1 , and a superior stable interface. The assembled Li/In-GPE/LFP cell exhibited ultralong cycle performance over 3000 and 2000 cycles at 1 and 2 C, respectively. Meanwhile, even increasing the voltage to 4.2 V, the Li/In-GPE/LFP cell maintained the reversible capacity of 128.9 mA h g −1 at 1 C for 500 cycles. The high-voltage Li/In-GPE/NCM811 cell also delivers excellent cycling performance. The design principle of PDOL-based GPE via a highly efficient initiator in a plasticizer-rich system provides a new pathway to the large-scale application of polymer electrolyte with superior electrochemical performance.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 1
·121086
·
IF 7.2
Siyu Xiao,Leshan Yan,Changyan Lu,Nan Xiao,Yun Li,Siliang Liu,Yang Lu,Liangxing Jiang,Zongliang Zhang,Guoyu Qian,Fangyang Liu
The development of green and efficient lithium isotope separation methods is of strategic importance for sustainable nuclear energy applications. Electrodeposition represents a promising approach, yet the fundamental separation mechanisms and the role of cathode materials require further clarification. This work systematically investigates the mechanism of lithium isotope separation through electrodeposition by integrating computational simulations with experimental validation. The results indicate that the lighter isotope 6 Li exhibits weaker solvation interactions and a reduced energy barrier for electron transfer, leading to its preferential deposition. The kinetic isotope effect during the charge transfer step (Li⁺ + e⁻ → Li) is identified as the dominant factor in the separation process, contributing significantly more than the limited fractionation induced by diffusion. Two categories of cathode materials—deposition-type (Ni, Cu, stainless steel) and alloy-forming (Zn, Al, Sn)—were evaluated, revealing a strong positive correlation between charge transfer resistance and separation performance, with stainless steel achieving the highest separation factor of 1.048. Furthermore, voltage-dependent studies demonstrate that separation efficiency decreases under high overpotentials due to a transition from charge transfer control to diffusion-limited kinetics. These findings provide fundamental insights into the electrodeposition-based separation mechanism and establish practical guidelines for developing efficient lithium isotope separation systems.
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INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Bo Yang,Li Cui,Hefeng Yuan,Hualin Zhang,Yu Che,Fangqin Cheng
Efficient separation of lithium isotopes (6Li and 7Li) is critical for sustainable nuclear energy. The crown ether system exhibits outstanding lithium isotope separation performance, with the anion exerting a significant influence; however, the molecular-level mechanism of action of anions and how this affects the separation process remain unclear. This limits the design of higher performance separation systems. Through combining 6Li/7Li separation experiments, 7Li NMR spectroscopy, and quantum chemical calculations, this work makes it clear that anions control the separation factor by changing the Li+ coordination microenvironment. Through manipulation of hydration and crown ether encapsulation, charge-delocalized anions provide a coordinating environment around Li+ that balances the bond strengths inside a crown-ether container. This balance of the bonding state improves the thermodynamic driving force for the 6Li/7Li exchange between the aqueous and organic phases and substantially increases the separation coefficient. This study provides an efficient screening method for lithium isotope separation and offers theoretical guidance for designing and optimizing more efficient lithium isotope separation systems.
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Nature Sustainability
·
2026
·
IF 32.1
Zhao Chang-Xin,Li Zheng,Zhang Daoning,Zhang Nan,Zhang Qiu,Wang Zeyi,Li Yue,Chen Yawei,Wang Chunsheng
Fast charging and low-temperature operation are essential for next-generation energy storage. However, high-energy batteries struggle to meet these demands as existing electrolytes cannot simultaneously deliver fast interfacial kinetics, high ionic conductivity and favourable interphase formation. Prevailing strategies focus on weakening thermodynamic solvation, yet this approach does not directly address the kinetic bottleneck, that is, the desolvation barrier governing interfacial charge transfer. Here we reveal that the desolvation kinetics are dictated by dynamic solvent exchange rather than thermodynamic solvation energy. Guided by this mechanistic insight, we have formulated an electrolyte in which two anions carry distinct anionic potentials: high-anionic-potential anions form contact ion pairs that accelerate solvation-exchange kinetics, while low-anionic-potential anions form solvent-separated ion pairs that sustain high bulk ionic conductivity. The electrolyte enables fast charging and low-temperature operation in high-loading lithium-ion batteries. The design principle was further validated in aqueous aluminium-ion electrochemical systems, underscoring its broader relevance to sustainable, resource-abundant battery chemistries beyond the lithium ion. Together, our findings establish a new electrolyte design paradigm that decouples interfacial and bulk transport properties and expands the design space of battery electrolyte systems.
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DYES AND PIGMENTS
·
2026
·
IF 3.9
Zekuo Lv,Leipeng Zhang,Wenchao Liu,Yike Zhang,Lei Xu,Yuqiang Wang,Qiumei Jiang,Miaomiao Zhao,Rui Yang,Xingcan Han,Dongqi Liu,Jiupeng Zhao,Yao Li
Viologen-based materials are among the most promising organic electrochromic systems due to their high optical contrast, fast redox response, and molecular tunability. However, their practical deployment is fundamentally constrained by the dimerization and irreversible side reactions of viologen radical cations (V +• ), which lead to rapid performance degradation and limited cycling stability. Here, we propose an asymmetric molecular design strategy that synergistically integrates electron-withdrawing inductive effects with moderate steric hindrance to fundamentally suppress radical cation dimerization. Using site-selective functionalization of 4,4′-bipyridine, a novel asymmetric viologen derivative, 4-( p -cyanobenzyl)-4′-( p -fluorobenzyl)-4,4′-bipyridinium (FCBV), is rationally designed and synthesized.The combined effects of dual electronegative substituents and benzyl-induced steric hindrance not only inhibit V +• aggregation but also promote directional electron transfer, resulting in simultaneously enhanced stability and kinetics. Electrochromic devices based on FCBV deliver a high optical contrast exceeding 60 % in the 500–700 nm range, an exceptional coloration efficiency of 155.8 cm 2 ·C -1 , and outstanding durability, retaining 98.9 % of their initial optical modulation after 20,000 switching cycles. The devices are further demonstrated in smart windows with effective light–thermal regulation and in adaptive anti-glare rearview mirrors, confirming their practical applicability in building and automotive optoelectronic systems.
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Hanchao Liu,Yihao Huang,Yuxi Zheng,Xintong Jiang,Tong Zhang,Jinchun Li
Hydrogels based on Schiff base chemistry are widely used for in situ applications due to their rapid gelation property. However, the inherent hydrolytic instability and dynamic nature of imine bonds limit their use in scenarios requiring long-term structural stability and stress relaxation resistance, especially in non-neutral pH environments. Herein, we report an imine hydrogel with a stable cross-linked network that exhibits enhanced resistance to hydrolysis. The hydrogel forms rapidly (<3 min) through condensation between aldehyde groups from glutaraldehyde (GA) and primary amines (–NH2) generated by the deprotonation of –NH3+ groups on poly(allylamine hydrochloride) (PAH). Multipoint cross-linking between PAH and GA not only facilitates the rapid gelation process at low pH value but also imparts a robust and resilient network, enabling exceptional hydrolytic stability even under strongly acidic conditions. Based on these properties, the hydrogel can be employed as a stable acidic polyelectrolyte in the domains of signal sensing and energy storage. With moderate incorporation of LiBF4, the hydrogel can be used to fabricate antifreezing sensors for real-time monitoring of laryngeal activity or finger movements. Furthermore, the rapid gelation kinetics facilitate in situ assembly of flexible supercapacitors within 15 min, which maintain practical and stable energy storage properties after 1 h of gelation. The resulting supercapacitors demonstrate high specific capacitance (124.1 F g–1), an energy density (E) of 17.1 Wh kg–1, and stable interfacial contact during deformation, with ideal cycling stability of over 5000 charge–discharge cycles without packaging. This work provides a strategy for rapid preparation of stable hydrated imine polymers, particularly suitable for field-based in situ fabrication of polyelectrolytes for electronic and energy storage devices.
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高影响因子
Separations
·
2023
·Vol. 10
·期 2
·111
·
IF 2.6
Zexing Xie,Meiying Xie,Tingting Tang,Fan Yang,Liyan Xue,Zhengming Jiang
6Li and7Li are strategic resources. Because Li+ions have no outermost electrons and the radii of6Li and7Li differ by only one neutron, the separation of the naturally stable isotopes of Li, especially by solvent extraction, is recognized as a difficult problem worldwide. Therefore, in this paper, an advancedβ-diketone-driven deep eutectic solvent (DES) extraction system containing 2-thenoyltrifluoroacetone (HTTA) and tri-n-octyl phosphine oxide (TOPO) is introduced to the extraction and separation of6Li+and7Li+ions. Compared with those of reported HTTA extraction systems and crown ether extraction systems, the separation coefficient (β7Li/6Li) of theβ-diketone-driven DES extraction system can reach the best value of 1.068, which is now the highest knownβ-value reported in the extraction system. From the intramolecular hydrogen bond of HTTA to the intermolecular hydrogen bond of DES, the bond energy increases by 47.8%. Because the active site of the proton in DES provides a higher energy barrier for the separation of7Li, theβ7Li/6Liis significantly increased. The extractions were characterized by spectrum, using1H nuclear magnetic resonance (NMR) spectroscopy, Fourier-transform infrared (FT-IR) spectroscopy, and X-ray photoelectron spectroscopy (XPS). The mechanism was determined on the basis of the reaction kinetics and density functional theory (DFT). The DES extractant shows excellent cycle performance with regard to stripping and reusability. In conclusion, the highly efficient, economical, and stableβ-diketone-driven DES extraction system can be used for the separation of naturally stable Li isotopes, which provides good industrial application prospects.Keywords:β-diketone;Lithium-7;separation of isotopes;deep eutectic solvent (DES);solvent extraction
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Energy Storage Materials
·
2022
·
IF 20.831
Shujing Wen,Chao Luo,Qingrong Wang,Zhenyao Wei,Yanxiang Zeng,Yidong Jiang,Guangzhao Zhang,Hongli Xu,Jun Wang,Chaoyang Wang,Jian Chang,Yonghong Deng
All-solid-state lithium batteries (ASSLBs) are promising power sources for flexible and wearable electronics due to their high energy density and reliable safety. Here, we reported the novel design of an ultrathin crosslinked solid polymer electrolyte (SPE) with high ion conductivities at room temperature (RT), high mechanical strength , and fast interfacial charge transport for flexible ASSLBs. The SPE is synthesized by one-step in-situ crosslinked polymerization of 1, 3-dioxolane, and trimethylolpropane triglycidyl ether within a lithium nitrate-containing mesoporous polymer (LP) matrix. The three-dimensional crosslinked polymer network enables the composite SPE with high RT ionic conductivity of 3.0 × 10 −4 S cm −1 and improved oxidation stability. The LP matrix could promote the formation of hybrid Li 3 N/LiF interfacial layers on both sides of the SPE, resulting in uniform lithium deposition. The symmetric cell of Li/SPE/Li can be cycled with an extremely small overpotential of 45 mV for 1000 cycles. The integrated paper-type pouch cell could retain high capacities retention (>90%), negligible voltage fluctuation (<50 mV), and high operation safety during 2000 cycles of bending (bending radius: 5 mm). This work offers a feasible pathway for developing an ultrathin solid-state electrolyte with high ionic conductivities, excellent interfacial compatibility, and high mechanical robustness for flexible ASSLBs.
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Science China-Materials
·
2022
·Vol. 65
·期 9
·2585-2590
·
IF 8.64
Chen Zilong,Zeng Hao,Chu Dongdong,Zhang Fangfang,Cheng Meng,Yang Zhihua,Pan Shilie
A new deep-ultraviolet (DUV) birefringent crystal, LiB 5 O 5 F 2 (OH) 4 (LBOFH), was designed and synthesized by a high-temperature solution method. Its structure features a [B 5 O 5 F 2 (OH) 4 ] anionic group that is constructed by four π-conjugated units, i.e., two [BO 3 ] units and two [BO(OH) 2 ] units connected by the [BO 2 F 2 ] unit, which forms a near-coplanar configuration. The group exhibits large anisotropic polarizability and highest unoccupied molecular orbital-lowest unoccupied molecular orbital (HUMO-LUMO) gap, thus providing a good balance between the large birefringence (0.124 at 546 nm) and band gap (7.99 eV) in LBOFH. This work suggests new possibilities for the design and fabrication of advanced DUV birefringent crystals using the novel anionic group and the expansion of their alternative system with new hydroxyfluorooxoborates.
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Nano Energy
·
2022
·
IF 19.069
Sijing Liu,Yuewang Yang,Shusheng Chen,Jiongzhi Zheng,Dong Gyu Lee,Dan Li,Jinglei Yang,Baoling Huang
Flexible ionic thermoelectric materials with large thermopowers show great promise for ultrasensitive thermal detection in wearable devices . Here large and tunable p- and n-type thermopowers are reported in stretchable and self-healing ionogels made of a fluorocarbon elastomer poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), an ionic liquid 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMIMTFSI) and a salt acting as the thermopower regulator. Particularly, a self-healing n-type ionic thermoelectric material is developed for the first time. The thermopower of the resultant ionogels varies from + 30 mV K −1 to − 21 mV K −1 at 90% relative humidity. Meanwhile, the ionogels exhibit excellent stretchability up to 1700% and appropriate Young’s modulus of around 0.26 MPa. Both the mechanical and thermoelectric properties can self-heal spontaneously after damage. Taking advantage of the large p and n-type thermopowers, the stretchable self-healing ionogels are integrated as a flexible thermoelectric detector with 10 pairs of p- and n-type legs on copper electrodes, showing a total thermopower of 0.25 V K −1 operating with a low temperature difference of 1–2 K.
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ChemSusChem
·
2022
·Vol. 16
·期 4
·e202201218
·
IF 9.14
Yunju Wang,Shunchao Ma,Hongyu Wang
Graphical The height of intercalation : Lithium difluoro(oxalato)borate is introduced to LiBF 4 -sulfolane (SL) solutions for dual-ion batteries, and the graphite electrodes’ storage behavior of anions is studied. Each anion can intercalate into graphite with SL, and different intercalation gallery heights are formed. Intermediate height is not observed, and species inside graphite are determined. Some previous studies have found the synergistic effect of mixed anions in dual-ion batteries (DIBs). In this work, both lithium tetrafluoroborate (LiBF 4 ) and lithium difluoro(oxalato)borate (LiDFOB) were dissolved in sulfolane (SL) solvent, and the resultant solutions were applied for DIBs. The storage behavior of mixed anions in natural graphite positive electrodes was investigated. In-situ X-ray diffraction measurements revealed both anions could participate in the formation of graphite intercalation compounds. Their evolution followed with the decreasing tendency of discharge capacities as the content of LiDFOB increased in solutions. The exchange of anions was discussed.
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