INORGANICA CHIMICA ACTA
·
2017
·
IF 2.002
Xiujuan Jiang,Hailong Wang,Yonggang Feng,Erxing Gu,Xiaoming Liu
Three diiron carbonyl complexes with different carbonyl ligands have been synthesized. Pentacarbonyl and tetracarbonyl complexes 2 and 3 were prepared by the substitution of the bound CO of complex 1 by PPh 3 . The photo-induced CO-releasing behaviours of these complexes correlate linearly to their reduction potentials and further to the energy level of their LUMOs. The more negative the reduction potentials, the more reactive the complexes. The photo-induced CO-release can be further promoted when a nucleophile is presented such as thiopronin.
研究领域:
化学
·
生物无机化学
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产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2021
·
IF 4.126
Kaiqiang Wei,Fan Liao,Hui Huang,Mingwang Shao,Haiping Lin,Yang Liu,Zhenhui Kang
Carbon dots (C-Dots) have many unique properties, which endow them with a promising platform from catalysis to biology applications. However, quantitative understanding of those properties of C-Dots is still a tremendous challenge, and thus an urgent task is to develop a simple theoretical prediction method to quantitatively determine the energy levels of highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) by a simple equation. Here, we determine the energy levels of LUMO and HOMO of C-Dots using the tight-binding method as well as the adjustment from the surface functional groups. A quantitative linear relationship between HOMO and HOMO–LUMO gap of C-Dots was obtained, which allows us to deeply understand the optical and photoelectrochemical properties.
研究领域:
材料科学
·
理论化学
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DOI
高影响因子
Energy Storage Materials
·
2023
·
IF 20.4
Cong Kang,Jiaming Zhu,Yijie Wang,Shanshan Ye,Yueping Xiong,Fanpeng Kong,Geping Yin
Nitrile electrolytes have attracted extensive attention for achieving high-voltage lithium metal batteries. However, the poor compatibility of nitrile electrolyte with Li anode remains a huge challenge owing to severe side reactions. Herein, changing concentration of LiTFSI in succinonitrile (SN) is proposed to improve interface compatibility by regulating the solvation structure. The higher coordination number (1.3) of TFSI − in high concentration electrolytes results in a LiF-rich SEI film, accounting for the superior performance of LiNi 0.8 Co 0.1 Mn 0.1 O 2 |Li cell with negligible capacity fade after 100 cycles at 0.5 C. Density functional theory (DFT) suggests that the solvation structure with a high coordination number of TFSI − towards Li + leads to a reduced Lowest Unoccupied Molecular Orbital (LUMO) energy level, which promotes the decomposition of TFSI − to form LiF-rich film. Also, a reduced decomposition energy barrier of anion is demonstrated. This work provides an encouraging way to enhance interface stability via modulating the solvation structure achieved by regulating concentration.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 47
·16623-16630
·
IF 6.4
Zhicheng Li,Yu Zhang,Zhongbin Pan,Xu Fan,Hao Wang,Peng Li,Haiming Huang,Weiliang Wang,Jinjun Liu,Jiwei Zhai
Flexible dielectric and electronic materials are widely employed in emerging fields. Dielectric energy storage technologies and materials are needed to simultaneously cope with stringent requirements, such as high-stability and compact-size energy storage. Nonetheless, many mainstream polymer dielectrics prematurely fail under the coupling of rising electric field strength and space charge accumulation. Herein, we constructed a one-dimensional core–shell heterogeneous filler (BiFeO3@Al2O3) and added it to wide HOMO–LUMO gap cyanoethyl cellulose, achieving ultrahigh breakdown strength (∼801 MV m−1) and dielectric constant (∼17.3), thus obtaining a substantial discharged energy density of ∼31.3 J cm−3, accompanied by stabilized cyclic charge/discharge of 105. The superior energy storage performance is ascribed to the shell (Al2O3) having a higher work function, forming built-in electric fields with core (BiFeO3), simultaneously decreasing the density of state and increasing the bandgap of nanofibers. This research provides an optimization technique for crafting advanced polymer dielectrics, catering to the evolving demands of modern energy storage applications.
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DOI
高影响因子
RUSSIAN JOURNAL OF GENERAL CHEMISTRY
·
2016
·Vol. 86
·期 7
·1747-1752
·
IF 0.481
Lin Meijuan,Tang Qiang,Zeng Huijuan,Xing Guang,Ling Qidan
Several new Ir(III) complexes with 2-(4-bromophenyl)-1 H -benzo[d]imidazole or 2-(4-bromophenyl)- 1-methyl-benzo[ d ]imidazole ligands as cylcometalated ligand and acetylacetonate or picolinate as the ancillary ligand were synthesized and their structures and photophysical properties were characterized. HOMO and LUMO energy levels and the molecular structures of Ir(III) complexes were scrutinized by DFT calculations. The complexes exhibited green luminescence at the maximum emission peaks at ca 495–522 nm. The methyl group substituent and replacing of acetylacetonate with picolinate complex can enhance the complex thermal stability. HOMO energy levels of the complexes vary from –4.99 to –5.44 eV, the LUMO energy levels are between –1.52 and –1.97 eV.
研究领域:
材料科学
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化学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Jiangtao Xu,Cheng Cheng,Songmin Shang,Wei Gao,Ping Zeng,Shouxiang Jiang
Conventionally, surface-enhanced Raman spectroscopy (SERS)-active materials mainly include nanosized noble metals, semiconductors, or the complex of both, most of which are limited in practical applications because of their symbiotic materials, complex and difficult to control fabrication processes, and reuse and sampling challenges. To address these issues, novel SERS substrates have been developed in this study by anchoring zeolitic imidazolate framework-67 (ZIF-67) and derivatives of ZIF-67 to cotton fabric. The designed SERS substrates show extraordinary flexibility, an excellent enhancement factor, and reusable performance. By adjusting the lowest unoccupied molecular orbital and highest occupied molecular orbital of ZIF-67 through a doping process with different metal ions, the substrates exhibit a high enhancement factor of 6.07 × 106 and a low limit of detection of 10–8 M, as well as reusability resulting from photocatalysis. The enhancement process is studied based on charge transfer resonance, interband transition resonance, ground state charge transfer, and the light coupling effect. The results contribute to the approaches in designing SERS substrates by using ZIFs as unique SERS-active materials, and provide new insights into the development of novel SERS-active materials, along with promoting the use of SERS detection in the real world by improving the flexibility of substrates.
研究领域:
材料科学
·
光谱学
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 47
·22335-22343
·
IF 3.591
Siqi Wei,Haoyi Li,Xinghang Yin,Qiang Yang,Anli Chen,Renjie Li,Jing Wang,Rui Yang
Synthesizing high-efficiency red carbon dots (R-CDs) and exploring their photoluminescence mechanism remain challenges as well as critical issues hindering the development of red room-temperature phosphorescence (RTP) materials of CDs. Herein, a series of highly efficient R-CDs are prepared from citric acid and formamide by solvothermal method on account of the protective and destructive effects of solvents. The larger sp2 conjugated domains of the carbon core and the high content of graphitic N are identified as the key factors for R-CDs to exhibit red fluorescence. Surface groups also contribute to red emission by means of the formation of the N, O-related defect state. By establishing N-doping models and using DFT calculation, it is further demonstrated that the strong p–π conjugation effect caused by the non-bonding electrons of graphitic N would facilitate HOMO–LUMO splitting of the carbon core, thus leading to a significant decrease in the HOMO–LUMO gap. Energy level splitting could lead to a certain degree of energy level crossing, which could contribute to effective intersystem crossing and produce red RTP. From this, the potential applications of R-CDs in the information encryption field are proposed and demonstrated.
研究领域:
材料科学
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光电技术
·
纳米技术
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化学
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产品关联
DOI
高影响因子
RARE METALS
·
2022
·Vol. 42
·期 1
·122-133
·
IF 6.318
Dong Wu-Jie,Le Jia-Bo,Jin Yan,Zhang Guo-Qing,Ye Bin,Qin Peng,Huang Fu-Qiang
Organic cathodes for alkali-metal-ion batteries attract great attentions in recent years, but the ion storage sites are limited to some finite functional groups. This is because an organic cathode must have proper lowest unoccupied molecular orbitals (LUMO) to accept electrons at high potential. Herein, a novel type of organophosphate-based cathode has successfully been explored by tuning the LUMO energy level of organophosphates through metal ions with an inert electron pair. For the first time, the P=O of phytate (PA), N,N,N′,N′-ethylenediaminetetrakis(methylene phytate) (EDTMP), and diethylenetriaminepentakis(methyl phytate) (DTPMP) is activated by lead/bismuth (with 6s 2 electron pair) to storage Li/Na/K ions reversibly. Typically, density functional theory calculations indicate that the LUMO energy of Bi-PA is greatly reduced from − 0.99 (PA) to − 4.61 eV, which shows the first discharge capacity of 173, 182 and 206 mAh·g −1 and the reversibly capacity of 102, 102 and 101 mAh·g −1 with the discharge platform of 2.4, 2.1 and 2.4 V for Li/Na/K-ion battery cathodes, respectively. Similarly, with proper LUMO energy level, Pb-PA (− 4.63 eV), Pb-EDTMP (− 3.71 eV), and Pb-DTPMP (− 4.45 eV) all exhibit admirable performance. This unique strategy of organic materials to alkali-metal-ion battery cathodes offers a new avenue for future energy storage systems. Graphical abstract
研究领域:
材料科学
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化学
·
能源科学
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产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2025
·
IF 26.8
Xiang Gao,Ao-Qi Yang,Wen-Bei Yu,Jia-Cong Zhou,Mao-Jun Pei,Jia-Cheng Chen,Wei Yan,Guo-Qiang Luo,Yao Liu,Jian-Hua Xiao,Jiujun Zhang
Traditional trial-and-error methods are inefficient and costly in discovering novel solvents for next-generation magnesium (Mg) metal-based batteries. Therefore, this work establishes a simple yet efficient screening criterion for solvents by integrating artificial intelligence techniques with a virtual molecular database, potentially revolutionizing the traditional solvent design pathway. A total of 823 solvents are generated using a self-developed algorithm, and LUMO, ΔLUMO, ESP min , ESP max , and E b are identified to establish the screening criterion through the analysis with machine learning (ML) models. Eighteen candidate solvents are successfully identified, and two of which are subsequently selected and experimentally validated, i.e., C1COCOC1 and COCC(C)OC (abbreviated as “DOX” and “DMP”). Notably, neither of these solvents has been previously reported for use in Mg batteries. Experimental results indicate that the DOX solvent, when paired with the Mg boron-based salt, i.e., Mg[B(hfip) 4 ] 2 , can significantly enhance the electrochemical performance. At a current density of 1.0 mAcm −2 , the average coulombic efficiency for Mg plating/stripping reaches 99.54 % after 5200 cycles. Furthermore, the Mg//Cu cell achieves a cumulative capacity exceeding 2000 mAhcm −2 , surpassing previously reported results. In summary, this work establishes a virtual molecular database and develops a streamlined screening methodology for Mg battery solvents based on their physicochemical properties, reducing the candidate pool from 823 to 18 and improving efficiency by nearly 50-fold. This research paradigm is not limited to the development of Mg batteries and can be readily extended to the exploration of other battery systems.
研究领域:
电化学
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材料科学
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能源存储
·
计算化学
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人工智能应用
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电池技术
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产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Huanhuan Sun,Hongyan Yu,Boyang Han,Junjie Ma,Rensheng Wang,Yanping Song
Pressure-induced surface-enhanced Raman spectroscopy (PI-SERS) is among the foremost achievements of high-pressure fields, benefiting from the advantage that pressure-modulated interactions between substrates and molecules overcome the weakness of individual substrates or molecules. However, the pressure corresponding to PI-SERS enhancement is currently still at a low-pressure stage within 8 GPa. Therefore, how to realize PI-SERS enhancement under higher or ultrahigh pressure remains a huge challenge. Here, we applied few-layer WS2 (FL-WS2) nanosheets as PI-SERS substrates and selected 4-mercaptobenzoic acid (4-MBA) molecules with a big energy gap as probes to explore PI-SERS enhancement in more depth. The experimental results indicate that the PI-SERS signals increase gradually as pressure increases and reaches a maximum at 18 GPa, which has set a pressure record for the PI-SERS field so far. Different from the C exciton resonance-induced SERS intensities at ambient conditions, the charge-transfer transition between FL-WS2 and 4-MBA is strengthened via the pressure-induced increase in the band gap of FL-WS2 and decrease in the highest-occupied molecular orbital–lowest unoccupied molecular orbital (HOMO–LUMO) energy gap of 4-MBA, thus enhancing PI-SERS signals accordingly. Therefore, this strategy will be beneficial for practical applications in the field of optoelectronics and for the design of other PI-SERS sensors for trace detection in complex and extreme environments.
研究领域:
材料科学
·
纳米技术
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光电子学
·
光谱学
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产品关联
DOI
高影响因子
Energy Storage Materials
·
2023
·
IF 20.4
Xin Ren,Donggang Tao,Shuai Cui,Ting Li,Yuliang Cao,Fei Xu
Rechargeable Mg batteries are advantageous substitutes for lithium-ion batteries in large-scale energy storage with low cost and high safety, but the lack of cathode materials is blocking the development. Organic polymers are promising Mg-storage materials, and the construction of suitable Mg-storage active sites is of great significance for the performance. In the present study, a double-chain conjugated carbonyl polymer is designed and investigated as cathode material of rechargeable Mg batteries. The double-chain structure builds favorable active sites for reversible storage of bivalent Mg 2+ cation by means of immobilization of the two adjacent carbonyls. This double-chain polymer shows a higher Mg-storage capacity (194 mAg –1 ) than the corresponding single-chain polymer (116 mAg –1 ). The Mg-storage capacity of this double-chain polymer also exceeds the Li-storage capacity (106 mAg –1 ) significantly. A mechanism study demonstrates the reversible carbonyl enolization in Mg-storage reactions. A theoretical computation demonstrates the magnesiation structure has a higher HOMO and a lower LUMO energy level, as well as a smaller HOMO–LUMO gap. This is favorable for the Mg-storage reaction reversibility and stability of the magnesiation structure, thus improving the capacities and cycling stabilities. The principle revealed in the present study provides an important insight to design organic conjugated polymers with favorable Mg-storage active sites, which would assist the development of high-performance Mg-storage materials.
研究领域:
材料科学
·
储能
·
电化学
·
聚合物化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Youhua Xiao,Ruifeng Hu,Jiahao Li,Jingwen Ni,Xiao Yu,Xiaodong Lu,Xingyu Shang,Jie Mao,Shengxiang Yang
Dielectric elastomer (DE) materials hold promise as artificial muscles due to their ability to deform under external electric field stimulation. To enhance their actuation performance, we have improved the dielectric breakdown strength of polyurethane (PU) based DE materials by incorporating voltage stabilizers into their hard segment through copolymerization. Voltage stabilizers with a lower HOMO-LUMO energy gap can effectively capture high-energy electrons, thereby mitigating the degradation of polymer molecular chains and increasing the dielectric breakdown strength. Specifically, when 50 % of the hard segments in PU contain a kind of voltage stabilizer (4,4′-dihydroxybenzophenone, DHBP), the PU exhibits the optimized dielectric breakdown strength, increasing from an initial value of 32 V /μm to 58 V/μm. Notably, the modified PU retains a low initial modulus (0.24 MPa) without experiencing the stiffening problem, as the rigid structure of the DHBP is incorporated into the hard segments of PU. Without pre-stretching, the 50 % DHBP-PU achieves an improved maximum actuation strain of 57 % and a theoretical energy density of 14.4 J/m 3 at 83 V /μm, outperforming most PU-DE materials. The DHBP-PU, characterized by its enhanced dielectric breakdown strength and improved electroactuation performance, holds great potential for applications in flexible actuators and soft robotics.
研究领域:
材料科学
·
高分子科学
·
机电系统
·
软体机器人
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）