ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Ze Li,Yidan Fu,Lina Han,Pengfei Zheng,Xiaoyuan Zeng,Peng Dong,Jing Feng,Yingjie Zhang
The insufficient d-electron density in V metal atoms limits O2 dissociation, constraining the kinetics and activity of the oxygen reduction reaction and the oxygen evolution reaction in VN-based catalysts. Herein, Co dopant was employed to modulate the electronic characteristics of the d-orbitals and associated free energy of VN, thereby further enhancing its catalytic activity. XPS and XANES spectra revealed that Co atoms replaced V and strongly bonded with neighboring N atoms, effectively regulating the local electronic structure. DFT analysis show that the Co doping strategy effectively regulates the adsorption/desorption equilibrium of oxygen reduction reaction intermediates through d-electron transfer to V atoms, while significantly lowering the activation energy barrier of the rate-determining step. Electrochemically, V0.95Co0.05N/NC/C achieved a low bifunctional index (ΔE = 0.78 V), with a half-wave potential for the ORR of 0.83 V and an OER overpotential of 380 mV at 10 mA cm–2. In Zn-air batteries, it achieved a high specific capacity (708.98 mAh gZn–1) and retained 88% initial voltage after 280 h cycling, demonstrating robust stability for practical applications. This study presents a doping strategy to modulate d-band centers in transition metal nitrides for energy conversion devices.
研究领域:
电化学
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材料科学
·
能量转换
·
催化
·
纳米技术
·
电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2025
·
IF 26.8
Shuhong Yi,Chenlong Gao,Qingfeng Fu,Shiru Wu,Jian-Fang Wu,Yan Duan,Menghao Yang,Jilei Liu
Solid-state potassium-ion batteries are promising options for large-scale energy storage due to their high safety and abundance of potassium resources. However, solid-state potassium-ion batteries are still in their infancy and the reported electrolyte materials are very limited, making the exploration of solid electrolytes with high ionic conductivity and physical/electrochemical stability a major challenge. Here novel triclinic K 3 LnSi 3 O 9 (Ln = Y and Gd) potassium-ion solid electrolyte is reported with low activation energy and high stability. A rational vacancy design strategy is adopted to synthesize K 3−x GdP x Si 3−x O 9 and the result of DFT calculation shows that the diffusion pathways of potassium ions on the ac plane exhibit a fish scale-like network structure. Specifically, the K 2.8 GdP 0.2 Si 2.8 O 9 delivers a high ionic conductivity of 2.9 × 10 −5 S cm −1 at 25 °C, accompanied by a stable potassium stripping/plating (a long-life cycle over 2000 h). As a result, the assembled quasi-solid-state KC/K 2.8 GdP 0.2 Si 2.8 O 9 /PB cell achieves a remarkable cycling performance at a high current density of 1 C (500 cycles, 95.9% capacity retention). These results would no doubt boost research for high-safety and high-energy-density solid-state potassium-ion batteries.
研究领域:
材料科学
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电化学
·
能源存储
·
固体离子学
·
无机非金属材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Xin Zhang,Li-Hua Wang,Yu-Wei Xiang,Zhi-Yong Tang,Bao-Ju Wang,Hai-Kui Zou,Yong Luo,Jian-Feng Chen
As the most common type of synthetic dyes, azo dyes are widely used for coloring fibers, paints, plastics, rubber, etc. However, due to the high local concentration in azolation, the decomposition and hydrolysis of diazo salts lead to the decline in the quality of azo dyes. In this work, the azolation of p -aminobenzene diazo sulfate ( p -ADS) and N -cyanoethyl- N -benzyl aniline ( N -CBA) as the model reaction to analyze the potential of rotating packed bed (RPB) reactor in improving the quality of azo dyes. Firstly, the intrinsic kinetic models of main reaction and side reactions were proposed and verified, revealing that the high local concentrations could accelerate the side reactions. After that, the DFT calculation indicates that the azolation process needs to be completed in two steps, and the process of generating the complex has a higher reaction energy barrier (19.88 kcal/mol). Under optimal process conditions, the purity and yield of product were 92.80 % and 98.37 % in the RPB reactor, while 89.90 % and 96.09 % in the stirred tank reactor (STR). Moreover, the strength and average particle size of DO-288 synthesized in the RPB reactor were 728 and 0.6 μm respectively, which were significantly better than 715 and 0.78 μm in STR. These results indicate that the RPB reactor has obvious advantages in the synthesis of high-quality, highly dispersed and highly strength azo dyes.
研究领域:
化学工程
·
染料合成
·
反应动力学
·
工艺优化
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2019
·Vol. 10
·期 1
·1-7
·
IF 11.878
Tan Zhibing,Zhang Dan,Tian Han-Rui,Wu Qingqing,Hou Songjun,Pi Jiuchan,Sadeghi Hatef,Tang Zheng,Yang Yang,Liu Junyang,Tan Yuan-Zhi,Chen Zhao-Bin,Shi Jia,Xiao Zongyuan,Lambert Colin,Xie Su-Yuan,Hong Wenjing
Full-carbon electronics at the scale of several angstroms is an expeimental challenge, which could be overcome by exploiting the versatility of carbon allotropes. Here, we investigate charge transport through graphene/single-fullerene/graphene hybrid junctions using a single-molecule manipulation technique. Such sub-nanoscale electronic junctions can be tuned by band gap engineering as exemplified by various pristine fullerenes such as C 60 , C 70 , C 76 and C 90 . In addition, we demonstrate further control of charge transport by breaking the conjugation of their π systems which lowers their conductance, and via heteroatom doping of fullerene, which introduces transport resonances and increase their conductance. Supported by our combined density functional theory (DFT) calculations, a promising future of tunable full-carbon electronics based on numerous sub-nanoscale fullerenes in the large family of carbon allotropes is anticipated.
研究领域:
纳米技术
·
材料科学
·
电子学
·
化学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Long Zhang,Dongsheng Yang,Lilei Miao,Chunmeng Zhang,Jiexiang Li,Jiawei Wen,Chunxia Wang,Tiantian Cao,Guoyong Huang,Shengming Xu
The nickel-rich layered cathode material LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) has high energy density , lower cost and is a promising cathode material currently under development. However, its electrochemical and structural stability is poor during cycling. Among the many modification methods, cation doping has been consistently proven to be an effective strategy for enhancing electrochemical performance . Herein, the NCM811 cathode material was modified by solid-phase reactions with Mg and Al doped. In addition, the corresponding mechanism of NCM811 cathode material-doped modification is explored by density functional theory (DFT) calculations, and we have extended this approach to other ternary cathode materials with different ratios and obtained universal laws. Combined with DFT calculations, the results show that Mg 2+ occupies the Li + site and reduces the degree of Li + /Ni 2+ mixture; Al 3+ acts as a structural support during charging and discharging to prevent structural collapse. The electrochemical properties were tested by an electrochemical workstation and the LAND system, and the results showed that the capacity retention rate increased to varying degrees from 63.66% to 69.87% and 89.05% for NCM811-Mg and NCM811-Al at room temperature after 300 cycles, respectively. This study provides a theoretical basis and design strategy for commercializing cationic-doped modification of nickel-rich cathode materials.
研究领域:
材料科学
·
电化学
·
能源存储
·
计算材料学
·
无机固体化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yanan Yu,Yao Shen,Ke Wang,Jingkai Zhao,Jiexu Ye,Lidong Wang,Shihan Zhang
Amine-based technology is promising for CO 2 capture from the flue gas . However, it encounters high energy penalty and thus hampers its industrial application. Currently, the catalytic solvent regeneration is developing to lower down regeneration temperature, accelerate regeneration rate, and cut down energy consumption for monoethanolamine (MEA)-based process. However, the information on catalytic regeneration of biphasic solvent is seldom available. This work develops a facile synthesized robust catalyst, α-Fe 2 O 3, to promote the biphasic solvent regeneration such as triethylenetetramine (TETA) and 2-(diethylamino) ethanol (DEEA) blend. Experimental results revealed that, with the aid of α-Fe 2 O 3 , the efficient regeneration of TETA-DEEA occurred at 94 °C, which is far below the conventional MEA-based process (110–120 °C). The corresponding CO 2 stripping rate increased by 2.4 times compared with uncatalytic scenario. Furthermore, the relative energy consumption was furtherly decreased by 41.6%. Different from MEA regeneration, the biphasic solvent regeneration with α-Fe 2 O 3 depended on the enhancement of water molecules proton donation rather than the abundant Brønsted acid and Lewis acid of the catalyst. Based on DFT calculation and 13 C NMR spectra analysis, the water molecules on α-Fe 2 O 3 surface and the protonated DEEA were parallel served as proton donors for carbamate decomposition. Consequently, a novel proton transfer mechanism was proposed for the biphasic solvent TETA-DEEA regeneration. The water molecules adsorbed on α-Fe 2 O 3 surface generated oxyhydrogen groups and thus donate protons for the carbamate decomposition. This work proposes a novel proton transfer mechanism for solvent regeneration and advances its industrial application with a low energy penalty.
研究领域:
环境科学
·
化学工程
·
催化
·
能源技术
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 12
·期 3
·737-749
·
IF 6.119
Zhicheng Xu,Yuran Li,Yuting Lin,Bin Wang,Panting Gao,Tingyu Zhu
The reduction of NO by CO was proposed to be applied for regeneration gas to remove NOx from industrial flue gas with activated carbon purification technology. To improve the activity and sulfur resistance for the reduction of NO by CO in regeneration gas, Cu and Fe modifications on activated carbon were investigated. And various samples were characterized by XRD, XPS, TPD, H2-TPR, in situ DRIFTS and DFT calculations to explain the reaction mechanism and poisoning mechanism. The synergistic effects of oxygen-containing functional groups and metal sites show that –COOH acts as an anchor site for metals and that C–O–C acts as a protective site for Fe3+ under a SO2 atmosphere. Cu2+ sites have a high activity at low temperatures due to the large amount of adsorbed NO and the intermediate NOx− participating in the reaction with the NOx− pathway. Fe3+ sites have a high activity at high temperatures due to the high N–O dissociation activity with the *N pathway and –NCO pathway. DFT calculations proved that the binding Cu2+ and Fe3+ sites have higher activity than free Cu2+ and Fe3+ sites. A high content of SO2 exhibits various poisoning effects, mainly including the sulfation of metal sites, deposition of S, and consumption of CO. AC-Fe-H exhibits excellent resistance and stability against SO2 and H2O due to less S deposition caused by consumption through the S–CO reaction, slight sulfation caused by the protective effect of Fe2+ and C–O–C on Fe3+ sites and better hydrophobicity.
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
TETRAHEDRON
·
2014
·Vol. 70
·期 47
·9033-9040
·
IF 2.817
Tao Liu,Meng-Meng Liu,Xiao-Wen Zheng,Chong-Yang Du,Xiang-Yang Cui,Lu Wang,Ling-Li Han,Zhang-Yu Yu
The redox reactions of p -hydroquinone and pyrocatechol undergo a two-proton-two-electron process in aqueous solution. We calculated their redox potentials at the B3LYP/6-311+G(d,p) level, and verified the values by employing cyclic voltammetry experiments. Then we selected seven substituent groups (–F, –Cl, –OH, –COOH, –CN, –NH 2 , and –NO 2 groups) to systematically investigate the substituent effect , including the sort, position, and number of the substituent, on the redox potentials of p -hydroquinone and pyrocatechol. The calculated results show that –NH 2 and –OH groups can decrease the redox potentials, while –F, –Cl, –COOH, –CN, and –NO 2 groups increase the potential values of p -hydroquinone and pyrocatechol. The calculations can accurately predict the substituent effects on the redox potentials of pyrocatechol and p -hydroquinone. We would expect that the accurate calculation results for the model systems could be applied in the prediction of electrode potentials of other molecules.
研究领域:
物理有机化学
·
电化学
·
计算化学
·
分子设计
·
生物电化学
✓ 已验证
DOI
高影响因子
Journal of Physical Chemistry C
·
2023
·
IF 3.7
Ming Feng,Xiao-li Xi,Li-wen Zhang,Zuo-ren Nie
Understanding the reduction mechanism and coordination of tungsten ions in molten salt is one of the key factors to improve the electrolysis efficiency of tungsten carbide. In situ spectroscopy combined with simulation calculation is a strong analytical technique for characterizing chemical species and their behaviors in molten salts. The tungsten ion group was investigated by in situ high-temperature and room-temperature spectroscopy combined with density functional theory (DFT) calculations. For the described in situ spectroscopic studies, a new setup was used, which allowed the registration of UV–vis spectra of tungsten ions in cationic and anionic molten salt systems. The DFT calculation results proved useful for estimating the trend of experimental spectra. Through experimental and theoretical studies, the tungsten ion groups in various molten salt systems were identified, and the effect of cations and anions in molten salt systems onto tungsten ion group formation could be elucidated.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Yuzhao Hou,Binyan Yang,Simon Sani Ocholi,Fengchao Wang,Zhifei Fu,Liming Wang,Lifeng Han,Pengli Du,Jia Zhao,Ping He,Zixin Zhang,Erwei Liu
Estrogen compounds in food exhibit bioaccumulation and endocrine-disrupting effects, posing serious risks to ecosystems and human health. Here, a novel core–shell magnetic covalent organic framework (COFs @ Fe 3 O 4 @C NPs) was developed for efficient enrichment and sensitive detection of estrogens in meat samples. The adsorption feasibility and mechanism of TAPB-DVA-COF were investigated using density functional theory (DFT) and molecular dynamics simulation (MDS). DFT calculations confirmed that hydrogen bonding and π–π stacking drive spontaneous adsorption, with adsorption energies ranging from −21.26 to −11.59 kcal mol −1 . MDS further revealed the formation of stable estrogen-COF complexes through close interfacial contact and persistent hydrogen bonding, confirming the existence of low-energy conformations. Based on these insights, COFs were anchored onto polydopamine-modified carbon-coated Fe 3 O 4 nanoparticles at room temperature to fabricate a magnetic adsorbent, which was then employed as a magnetic solid-phase extraction (MSPE) material. The adsorbent exhibited high surface area, strong magnetic responsiveness, and excellent stability. Coupled with high-performance liquid chromatography (HPLC), the established MSPE–HPLC method achieved a wide linear range ( R ≥ 0.9996) and low detection limits (0.21–12.79 μg L −1 ). In pork and chicken samples, recoveries ranged from 91.7 % to 113.5 % with relative standard deviations of 1.0–6.1 %. This study demonstrates the superior performance of COFs @ Fe 3 O 4 @C NPs for estrogen detection and highlights MDS as an efficient and economical tool for predicting adsorption behavior, offering valuable guidance for material design.
研究领域:
分析化学
·
食品安全
·
纳米材料
·
计算化学
·
环境毒理学
·
药物代谢
·
分离科学
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2025
·
IF 4.6
Ahsan Nazir,Ameena Tur Rasool,Chuntao Chen,Otabek Mukhitdinov,Doniyor Jumanazarov,Dongping Sun
In this study, novel Z-scheme AgI@PbBiO 2 Br heterojunctions were prepared using a simple in situ precipitation approach to effectively degrade organic pollutants and inactivate gram-negative Escherichia coli (E. coli) and gram-positive Staphylococcus aureus (S. aureus) bacteria when exposed to visible light. The prepared materials were comprehensively evaluated using several analytical procedures. The 20 %-AgI@PbBiO 2 Br presented the best photocatalytic performance of all the catalysts prepared. The rhodamine B (RhB) molecules were significantly reduced within 70 min (98.72 %), showing a much higher degradation efficiency than bare AgI (73.58 %) and PbBiO 2 Br (46.77 %) under the same conditions. The degradation of methyl orange (MO), neutral red (NR), and tetracycline (TC) by 20 %-AgI@PbBiO 2 Br was also examined, resulting in nearly total elimination of MO, NR, and TC pollutants, respectively. In addition, the antibacterial efficacy of 20 %-AgI@PbBiO 2 Br against E. coli and S. aureus reaches about 99.99 %. The improved photodegradation efficacy of AgI@PbBiO 2 Br is owing to the construction of a heterojunction between AgI and PbBiO 2 Br, which increases effective charge separation and visible light absorption, thus enabling the decomposition of pollutants. Cycling experiments confirmed the stability and reusability of the material, demonstrating exceptional photocatalytic durability. The photocatalytic mechanism was thoroughly examined by reactive species capture assays and ESR analysis, confirming that holes and superoxide radicals are crucial in the photodegradation system. Additionally, the density functional theory (DFT) simulations and liquid chromatography-mass spectrometry (LC-MS) helped to clarify the susceptible active sites and possible degradation pathways of RhB. Overall, this work underlines the considerable ability of AgI@PbBiO 2 Br heterojunctions to effectively remove persistent pollutants from wastewater.
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120938
·
IF 7.2
Jinmei He,Mengge Cao,Jiehui Li,Dachuan He,Yuhang Gao,Menglin Zhu,Jin Zhang,Lei Zhu,Mengnan Qu
In recent years, the increasing discharge of microplastics (MPs) and oil pollutants into aquatic environments has posed serious ecological and health concerns, driving the urgent need for efficient and sustainable removal technologies. In response to this challenge, this study successfully prepared a multifunctional superhydrophobic sponge (HFNA) with photothermal conversion capability and magnetic responsiveness via a simple dip-coating method, which can be used for the adsorption of microplastic particles (MPs) and oil pollutants in aquatic environments. By introducing polydopamine (PDA) onto the melamine sponge (MF) skeleton, incorporating high specific surface area Ni-MOF, and adding Fe 3 O 4 with magnetic driving capability, the material’s adsorption capacity toward MPs was enhanced. The HFNA achieved a maximum removal efficiency of 99.3 % for MPs and exhibited excellent removal performance for various oil pollutants, while its photothermal effect effectively reduced crude oil viscosity, improving adsorption efficiency. Subsequently, the adsorption mechanism of the material was further revealed through density functional theory (DFT) calculations. The analysis showed that Ni-MOF and MPs exhibit excellent HOMO-LUMO energy level matching, with a small energy gap (ΔE gap ), facilitating electron transfer from MPs to Ni-MOF. At the same time, electrostatic potential and charge distribution maps indicated the presence of multiple high electron affinity sites on the surfaces of Fe 3 O 4 and Ni-MOF, which help in the enrichment of MPs. Theoretical results were highly consistent with experimental data, establishing a complete correlation mechanism from electronic structure to adsorption performance and material construction, thus providing important theoretical support for the rational design of MOF-based adsorbent materials.
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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）