JOURNAL OF MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Guangxin Tian,Ying Luo,Boxuan Lou,Jingjiao Sui,Xiaolan Qin,Yuhui Shen,Xueyan Zhu,Jie Lu
Resmetirom (MGL-3196) can form masses of solvates with a variety of solvents. In this study, a series of solvates, including those reported in patents and newly discovered solvates, were prepared by experimental screening. Hansen solubility parameters (HSPs) were used to investigate the formation rules of MGL-3196 solvates, and the results showed that the formation of MGL-3196 solvates was most related to the parameter Δ δ t . When the Δ δ t value between MGL-3196 and solvent was less than 14.23 MP0.5 a, MGL-3196 tended to form solvate with an accuracy of 84.09%. The precise crystal structures of six solvates and one solvent-free form (form A) were acquired by single crystal X-ray diffraction (SCXRD). After analyzing the structures of obtained solvates in-depth from the aspects of conformation, dimeric synthon, molecular packing, porosity and isostructuralism, the six solvates were classified into alcohol solvates (group 2), ester solvates (group 3) and other types of solvates (group 1). Generally, these three groups of solvates had completely different crystal structures. The solvates in group 1 and group 3 were channelized and isostructural in which solvents could be substituted without great influence on the structure, while in the alcohol solvates (group 2) solvents were fixed by strong hydrogen bonds to be a part of the crystal structure. Moreover, when solvates were desolvated, two metastable solvent-free forms (i.e., B and C) were crystallized and then transformed to form A through a structural rearrangement. The possible mechanisms for the phase transformation during different desolvation processes were finally proposed. All results shall provide an understanding and inspiration on the screening and production of polymorphic and pseudopolymorphic forms of MGL-3196 for the pharmaceutical industry.
研究领域:
药学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yiran Miao,Pengyun Yu,Fan Yang,Yueting Zhao,Haiyan Xu,Jianping Wang
In sodium-ion batteries (SIBs), the performance of a single solvent often does not meet actual requirements and a cosolvent or nonsolvating solvent is needed. However, the effect of these electrolyte additives on the solvation structure and dynamics of Na+ in SIBs is yet to be fully understood. Herein, electrolyte structural dynamics are examined for NaPF6 in dimethyl carbonate (DMC) with 1,1,2,2-tetrafluoro-2,2,2-trifluoroethoxy ethane (HFE) as the nonsolvating solvent or propylene carbonate (PC) as the cosolvent using steady-state and time-resolved infrared (IR) spectroscopies. Molecular dynamics simulations show that the solvation size of Na+ decreases with a loosened structure upon adding the nonsolvating solvent, whereas its first solvation shell becomes denser and the second one becomes softened with decreased participation of the PF6– anion upon adding the cosolvent. While a decreased participation of DMC in the solvation layer of Na+ is suggested by linear IR results, an increased structural inhomogeneity (and hence overall more dynamical fluctuations) is found for Na+-coordinated DMC upon adding both additives by two-dimensional (2D) IR spectroscopy where the carbonyl stretch is used as a probe. The Na+/DMC/PC complex is found to structurally evolve slower than both Na+/DMC and Na+/DMC/HFE complexes on the picosecond time scales by spectral diffusion dynamics extracted from 2D IR diagonal signals. Frontier orbital theory calculations also indicate that both solvent additives are beneficial to increasing the stability of PF6–. The results obtained in this work provide important insights into the roles played by the solvent additives in influencing the solvation structures and dynamics of Na+, which are critical for understanding the Na+ transfer mechanism in SIBs.
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2024
·Vol. 121
·期 5
·e2316914121
·
IF 9.4
Xunzhu Zhou,Yaohui Huang,Bo Wen,Zhuo Yang,Zhiqiang Hao,Lin Li,Shu-Lei Chou,Fujun Li
High-performance sodium storage at low temperature is urgent with the increasingly stringent demand for energy storage systems. However, the aggravated capacity loss is induced by the sluggish interfacial kinetics, which originates from the interfacial Na+ desolvation. Herein, all-fluorinated anions with ultrahigh electron donicity, trifluoroacetate (TFA−), are introduced into the diglyme (G2)-based electrolyte for the anion-reinforced solvates in a wide temperature range. The unique solvation structure with TFA− anions and decreased G2 molecules occupying the inner sheath accelerates desolvation of Na+ to exhibit decreased desolvation energy from 4.16 to 3.49 kJ mol−1 and 24.74 to 16.55 kJ mol−1 beyond and below −20 °C, respectively, compared with that in 1.0 M NaPF6-G2. These enable the cell of Na||Na3V2(PO4)3 to deliver 60.2% of its room-temperature capacity and high capacity retention of 99.2% after 100 cycles at −40 °C. This work highlights regulation of solvation chemistry for highly stable sodium-ion batteries at low temperature.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
Small
·
2024
·Vol. 20
·期 49
·2407484
·
IF 13
Lin Xie,Yihong Liang,Jialin Wang,Wanbao Wu,Jichuan Zhang,Jiaheng Zhang
Proper design of the solvation structure is crucial for the development of lithium metal batteries (LMBs). In this paper, the use of 1,2-Dimethoxyethane (DME) as a non-solvating cosolvent in amide-based eutectic electrolytes is proposed to address challenges related to high viscosity, high polarization, and low conductivity, thus enhancing the compatibility with lithium metal anodes. Through physical characterization combined with simulation calculations the existence of a weak interaction between DME and anions is confirmed, which promotes the dissociation of lithium salts and increases the Li + transference number and diffusion coefficient, thus improving the fast charging performance of eutectic electrolytes. In addition, stable SEI layer enriched with inorganic components is formed during the cycling process, resulting in uniform and dense lithium deposition. The fast charging performance of the cell can be effectively improved by utilizing the interaction between anions and solvents. The LiFePO 4 (LFP)||Li cell has a capacity retention of 97% after 1200 cycles at 5 C and also performs well at high temperature of 50 °C. Overall, the use of a non-solvating cosolvent in eutectic electrolytes presents a promising and innovative approach for enhancing electrolyte performance in LMBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
He Liu,Ke-Feng Ren,Yun-Fei Du,Jia-Xin Guo,Zhong-Yu Li,Zhen-Hui Luo,Xin Sun,Cong Guo,Weizhai Bao,Feng Yu,Xin Shen,Xin-Bing Cheng,Jingfa Li
The concept of high entropy is applied to various rechargeable batteries to improve the thermodynamic and kinetic behavior of electrolytes. However, the quantization and functionality of entropy are still ambiguous in liquid electrolytes. Herein, the regulation of entropy in non-aqueous electrolytes is quantitatively understood to construct robust Li metal batteries. Electrolyte entropy is first quantified through combining the Boltzmann statistical mechanics with the statistics of solvation structure configurations in the non-aqueous electrolyte. Entropy values do not necessarily increase with the increasing electrolyte components. Electrolytes with higher entropy dissociate ion aggregation to form homogeneous solvation structures, which effectively balance strong/weak solvation effects. This induces smaller cluster size, accelerating diffusion kinetics and desolvation process of Li + . An average Coulombic efficiency of 99.1% is obtained in Li||Cu batteries. Li||LiNi 0.5 Co 0.2 Mn 0.3 O 2 cells with a high cathode loading (19.7 mg cm −2 , 3.0 mAh cm −2 ) can maintain a capacity retention of 87.1% after 200 cycles. This finding offers novel understandings in the role of high-entropy effect, which is of great importance for the development of high-energy-density Li metal batteries.
研究领域:
电化学
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储能
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材料科学
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物理化学
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电池技术
✓ 已验证
产品关联
DOI
高影响因子
CRYSTENGCOMM
·
2021
·Vol. 23
·期 22
·3995-4004
·
IF 3.545
Pingping Cui,Qiuxiang Yin,Shihao Zhang,Wenchao Yang,Lihong Jia,Jiayu Dai,Ling Zhou,Zhao Wang
Amoxicillin sodium heterosolvates, including SM–M (methanol–methyl acetate solvate), SE–M (ethanol–methyl acetate solvate), and SM–E (methanol–ethyl acetate solvate), were obtained for the first time in this work. The single crystal of non-solvated crystal form (form I) was successful obtained via the phase transformation of amoxicillin sodium heterosolvate. The crystallographic data of amoxicillin sodium form I and heterosolvate were obtained via single crystal X-ray diffraction. Amoxicillin sodium molecules in form I and SM–M exhibited a similar conformation. In comparison with SM–M, the relative positions of the benzene ring and Na+ ion in form I was changed, thus facilitating the formation of a new coordinate bond between Na+ ion and phenolic hydroxyl group during the desolvation of SM–M. Methanol and methyl acetate molecules played different roles in the formation of SM–M. Methanol molecules formed strong coordinate bonds with amoxicillin sodium molecules, while methyl acetate molecules helped in improving the packing efficiency. The phase transformation behavior was explored via thermal analyses. The two-step desolvation mechanism of the heterosolvates was proposed and further verified via density functional theory computational analysis. Finally, the accelerated stability tests showed high relative humidity break the desolvation of heterosolvates and form I exhibited higher physical stability than the three heterosolvates.
研究领域:
药物化学
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晶体学
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材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xinming Xu,Long Su,Xiao Zhang,Rui Xu,Fei Lu,Liqiang Zheng,Hansen Wang,Chuying Ouyang,Xinpei Gao
The inherent issues of aqueous Zn-ion batteries, including side reactions and dendrite growth, can be effectively addressed through designing solvation structures enriched with anions to facilitate the formation of an anion-derived solid electrolyte interphase (SEI) layer. Here, the weakly solvating effect is utilized to modulate Zn 2+ solvation structure for constructing an anion-derived SEI layer. Trifluoroacetamide (TFACE), with a specific weak solvating ability, serves as an ideal ligand for preparing hydrated eutectic electrolytes (HEEs) combining the anion-containing solvation structures and high ionic conductivity. The results demonstrate that coordinated anions preferentially decompose and generate an inorganic/organic hybrid SEI layer on the Zn anode, which efficiently suppresses both side reactions and dendritic growth. Such an electrolyte enables assembled Zn//polyaniline (PANI) full cells to process an impressive capacity retention, maintaining 80 % after 3000 cycles at 0.5 A g −1 . This work provides a fundamental insight into building the anion-derived SEI by the weakly solvating effect and gives a viable route for designing advanced aqueous electrolytes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING & TECHNOLOGY
·
2022
·Vol. 45
·期 4
·678-686
·
IF 2.215
Guijun Zhu,Jianxin Chen,Jian Han,Jihui Li,Yupeng Li,Kaili Liu
5-Sulfoisophthalic acid sodium salt (5-SSIPA) is a crucial intermediate for pharmaceuticals, pesticides, and polyesters. Several acidic groups lead to an unstable crystal structure. Two new polymorphs and three novel solvates were identified during the solvent screening. These crystals were characterized by powder X-ray diffraction, Fourier transform infrared, and scanning electron microscopy. The desolvation temperature of solvates was found to be higher than the boiling point of pure solvents, which tentatively indicated the existence of an interaction between solvents and 5-SSIPA molecules. The phenomenon that the three solvates gradually darkened with desolvation in the hot-stage microscopic images proved the occurrence of crystal desolvation. The non-isothermal desolvation kinetics of the 5-SSIPA solvates was analyzed and discussed.
研究领域:
材料化学
·
药物化学
✓ 已验证
DOI
高影响因子
ACS Nano
·
2024
·
IF 15.8
Weijie Chen,Dianwei Zhang,Hongwei Fu,Jinfan Li,Xinzhi Yu,Jiang Zhou,Bingan Lu
Ether-based electrolytes are among the most important electrolytes for potassium-ion batteries (PIBs) due to their low polarization voltage and notable compatibility with potassium metal. However, their development is hindered by the strong binding between K+ and ether solvents, leading to [K+–solvent] cointercalation on graphite anodes. Herein, we propose a partially and weakly solvating electrolyte (PWSE) wherein the local solvation environment of the conventional 1,2-dimethoxyethane (DME)-based electrolyte is efficiently reconfigured by a partially and weakly solvating diethoxy methane (DEM) cosolvent. For the PWSE in particular, DEM partially participates in the solvation shell and weakens the chelation between K+ and DME, facilitating desolvation and suppressing cointercalation behavior. Notably, the solvation structure of the DME-based electrolyte is transformed into a more cation–anion–cluster-dominated structure, consequently promoting thin and stable solid–electrolyte interphase (SEI) generation. Benefiting from optimized solvation and SEI generation, the PWSE enables a graphite electrode with reversible K+ (de)intercalation (for over 1000 cycles) and K with reversible plating/stripping (the K||Cu cell with an average Coulombic efficiency of 98.72% over 400 cycles) and dendrite-free properties (the K||K cell operates over 1800 h). We demonstrate that rational PWSE design provides an approach to tailoring electrolytes toward stable PIBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2025
·
IF 26.8
Rui Pan,Yucheng Xie,Bowen Jiang,Tong Liu,YingYu Han,Zhipeng Shao,Andreu Cabot,Shulin Jiao,Litao Sun,Kuibo Yin,Qichong Zhang
Aqueous zinc-ion batteries are promising candidates beyond lithium-ion technologies, but the intrinsic hydrogen-down orientation of interfacial water under negative bias, together with ion depletion at the electrode surface, promotes inhomogeneous Zn plating and substantial hydrogen evolution. Here, a high-entropy flexible electrolyte (HEFE) is demonstrated that leverages the fast water-exchange kinetics of Li⁺, K⁺, and Cs⁺. By deliberately inducing cation-hydration disequilibrium, the HEFE forms flexible Zn(H 2 O) m 2+ ( m ≤ 6) solvation structures embedded in a disordered water network, enhancing ionic conductivity and alleviating ion-transport limitations. Under cathodic bias, a progressive desolvation from Zn(H 2 O) 6 2+ to Zn(H 2 O) x 2+ ( x ≤ 5) proceeds while retaining aqueous disorder, thereby suppressing hydrogen evolution and enabling 3500 h of deep cycling at 1 mA cm −2 /3 mAh cm −2 . For iodine cathodes, the HEFE induces a pathway shift from the conventional I − →I 2 route to a solid–solid (CsI→I 2 ) conversion, fundamentally inhibiting iodide shuttling and extending full-cell life to 3600 cycles at 1 A g −1 . Beyond Zn, the solvation-heterogeneity strategy opens avenues for reversible multivalent electrochemistry and advancing next-generation energy-storage systems.
研究领域:
电化学储能
·
材料科学
·
能源化学
·
界面科学
·
电池技术
·
多价离子电化学
✓ 已验证
DOI
PubMed
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2018
·Vol. 20
·期 10
·7351-7360
·
IF 3.906
Shan Jin,Yongjun Hu,Pengchao Wang,Huaqi Zhan,Qiao Lu,Fuyi Liu,Liusi Sheng
Water molecules, which serve as both hydrogen bond donors and acceptors, have been found to influence the conformational landscape of gas-phase phenyl-β-D-glucopyranoside. Herein, tetrahydrofurfuryl alcohol (THFA), a sugar-like molecule without chromophores (e.g. phenyl-substitution), was used as the model sugar molecule for exploring the behaviour of water molecules on the conformational landscape of a pentose sugar such as deoxyribose. We used mass selected infrared-vacuum ultraviolet (IR-VUV) (118 nm) spectroscopy to investigate the hydrated neutral THFA and its complex cation in a supersonic jet. High level density functional theory (DFT) calculations were performed to ascertain the experimental results. The results revealed that the water molecule tends to insert into the twisted conformer at a position where two stronger intermolecular hydrogen bonds were formed by breaking the weak intramolecular interactions. We found that the twisted conformer of the hydrated neutral THFA complex is more stable than the envelope conformation, while the latter is more stable for the THFA molecule. However, the conformational landscape of the hydrated THFA complex cation did not significantly change on microsolvation with water molecules. These results indicated that the dominant structural landscape of the hydrated cationic complex is the twisted configuration with a trans-hydroxymethyl group. This finding provides valuable insight into the microsolvation of gas-phase sugar molecules.
研究领域:
化学
·
分子生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Enmin Li,Xin Tang,Juncheng Zhou,Haomiao Zhao,Jinhan Teng,Junjie Huang,Binghan Dai,Tianming Lu,Qingdong Tao,Kaibo Zhang,Weifeng Deng,Jing Li
Sodium-ion batteries are a promising energy storage system due to their rich sodium resources and many other advantages. However, its development is severely hampered by the electrolyte's low compatibility with the electrode contact. Herein, we propose a solvation control strategy with ethoxy (pentafluoro) cyclotriphosphazene (PFPN) and NaClO 4 double additives to reconstruct the solvation structure of sodium ions in electrolytes. This enables the electrolyte to form a dense and stable solid electrolyte interlayer (SEI) and double-layer cathode electrolyte interphase (CEI) on the surface of the electrode material to achieve long-cycle and high-capacity sodium-ion batteries. PFPN can form a stable SEI rich in inorganic components at the anode interface. ClO 4 - can first reach the cathode surface to create a NaCl and polymer-like chain CEI with sodium ions and solvents, and then the PFPN derivatives are migrated to the cathode surface to open the ring and decompose, thus forming a double-layer stable CEI. Therefore, the PEDN electrolyte can simultaneously improve the interface stability of the battery's cathode and anode solid electrolyte. Hence, the capacity retention rate of the 4.5 Ah Na 3 Fe 2 (PO 4 )P 2 O 7 (NFP)||hard carbon (HC) pouch cell after 2500 cycles at 1C is 88.26%.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）