SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Quan Chen,Hongjuan Feng,Jihong Dong,Yu Huang,Peng Yi,Min Wu,Bo Pan
Sorption and degradation occur simultaneously during the removal of aromatic organics by biochar. However, the unclear association between sorption and degradation limited our understanding of the underlying mechanisms of organic removal by biochars. Herein, the removal of monocyclic 2,6-dimethylphenol (DMP) and bicyclic bisphenol A (BPA) by raw and potassium hydroxide modified biochars was comparatively investigated by batch removal experiments and theoretical calculations. Under identical initial concentrations, biochar displayed lower sorption but higher degradation for DMP compared to BPA, whilst higher sorption corresponded to greater degradation for the same chemical. Sorption mechanisms revealed by molecular dynamic simulations include π-π, hydrophobic, and hydrogen bonding interactions. Density functional theory calculations identified the preferred degradation sites on biochar for adsorbed organics are graphitic nitrogen, defects, carboxyl, and hydroxyl functional groups. Analysis of free radicals and degradation intermediates concluded that the degradation pathways involve both free radical pathways and electron transfer processes for DMP, while only free radicals for BPA. Experimental and computational results indicated an increase in ring quantity can lead to higher sorption affinity but lower degradability of aromatic organics by biochar. Findings of this research provide theoretical support for the advancement of biochar based aromatic contaminant mitigation strategies.
研究领域:
环境科学
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化学
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DOI
高影响因子
DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 18
·6315-6320
·
IF 4.39
Hongbo Gao,Ruijiao Chen,Kewang Zhang,Ailijiang Abudurusuli,Kangrong Lai,Junjie Li
A new fluorine-containing chalcohalide, Ba4GaS4F3, has been synthesized by conventional high-temperature solid-state reaction. The compound crystallizes in the centrosymmetric space group I41/a with a = b = 16.628 (5) Å, c = 17.139 (10) Å, Z = 16. Experimental and theoretical results confirm that Ba4GaS4F3 is a direct band gap compound with an experimental band gap of about 3.13 eV, and the band gap is mainly determined by the Ba-5p, F-2p and S-3p orbitals. What's more, different from the many newly discovered chalcohalides in the Ba3AM4Q (A = Ga, In; M = S, Se; Q = Cl, Br, I) family, Ba4GaS4F3 is the first reported compound in the Ba4AM4D3 (A = Ga, In; M = chalcogen; D = halogen) family. The results enrich the structural diversity of metal chalcohalides.
研究领域:
材料科学
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化学
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DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2024
·
IF 5.3
Wanting Ma,Shengchao Xu,Qifeng Wei,Xiulian Ren
Hydrophobic deep eutectic solvents (HDESs) were considered as a kind of green media and were widely used for extraction, synthesis and catalytic reactions. Exploring the physicochemical property and intermolecular interaction was of great significance. In this work, we synthesized a series of HDESs using amide as hydrogen bond acceptor (HBA) and lactic acid as hydrogen bond donor (HBD). The density, acidity and intermolecular interactions of HDESs were investigated from experimental and theoretical viewpoints. Firstly, density results indicated that the increase of HBD content as well as the decrease of HBA alkyl chain could increase the density of HDESs. Secondly, acidity was found to be more accurate using milliequivalents calculation than pH measurement. The increase of HBD content as well as the decrease of HBA alkyl chain could also enhance the acidity of HDESs. In addition, the intermolecular hydrogen bond was investigated by multiple theoretical approaches, including electrostatic potential distribution map, the length of molecular bond, independent gradient model based on Hirshfeld partition and topology analysis of atoms. Ultimately, Fourier-transform infrared spectroscopy (FT-IR) was further applied to prove the existence of hydrogen bond. We believe this work would be valuable for understanding the nature of HDESs and providing guides for practical applications of HDESs.
研究领域:
化学
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材料科学
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DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Tianhao Yu,Peng Gao,Yu Wang,Maidina Muhetaer,Hong Du
In response to the limitations of slow reaction kinetics and elevated overpotentials in the OER, a novel core–shell structured electrocatalyst, termed NiCo–ZIF-67@Fe–Co–Ni-PBA or NiCo–ZIF@PBA, has been developed. This material demonstrates exceptional catalytic performance, exhibiting a minimal overpotential of approximately 188 mV at 10 mA cm–2, alongside a Tafel slope of 109 mV dec–1. Its robust stability in a 1 M KOH solution during the OER operations is noteworthy. Theoretical insights from DFT calculations reveal that a Co–O–Fe bridging configuration within NiCo–ZIF@PBA lowers the energy barrier for the reaction to 1.79 eV, a significant reduction from 2.67 eV observed with NiCo–ZIF-67. The improvement in electrochemical performance is primarily due to the emergence of Co3+ ions, which results from the efficient charge transfer occurring at the interface of the PBA and NiCo–ZIF core–shell structure. These findings suggest a promising strategy for designing advanced core–shell materials for electrocatalytic applications.
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2019
·Vol. 25
·期 33
·7826-7830
·
IF 5.16
Tingting Liu,Jianmei Wang,Changyin Zhong,Shiyu Lu,Wenrong Yang,Jian Liu,Weihua Hu,Chang Ming Li
Graphical A fair comparison : A strategy to grow nanoparticles of three Ru phosphides on graphene sheets was developed. The resulting three electrocatalysts for the hydrogen evolution reaction (HER; see figure) show similar morphology, loading density, nanoparticle size, Ru content, and electrochemical surface area, which allows a fair comparison of the effect of the phosphide phase on HER activity. Ru 2 P/graphene shows the best HER performance and highest intrinsic activity in acid solution, and all three electrocatalysts show excellent long-term HER durability. The outstanding electrocatalytic activity of ruthenium (Ru) phosphides toward the hydrogen evolution reaction (HER) has received wide attention. However, the effect of the Ru phosphide phase on the HER performance remains unclear. Herein, a two-step method was developed to synthesize nanoparticles of three types of Ru phosphides, namely, Ru 2 P, RuP, and RuP 2 , with similar morphology, dimensions, loading density, and electrochemical surface area on graphene nanosheets by simply controlling the dosage of phytic acid as P source. Electrochemical tests revealed that Ru 2 P/graphene shows the highest intrinsic HER activity, followed by RuP/graphene and RuP 2 /graphene. Ru 2 P/graphene affords a current density of 10 mA cm −2 at an overpotential of 18 mV in acid media. Theoretical calculations further showed that P-deficient Ru 2 P has a lower free energy of hydrogen adsorption on the surface than other two, P-rich Ru phosphides (RuP, RuP 2 ), which confirms the excellent intrinsic HER activity of Ru 2 P and is consistent with experiment results. The work reveals for the first time a clear trend of HER activity among three Ru phosphide phases.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2025
·
IF 16
Wen Ren,Migo Szeman Ng,Ye Zhang,Alae Eddine Lakraychi,Yanliang Liang,Dawei Feng,Michelle Lehmann,Guang Yang,Judith Jeevarajan,Wan Si Tang,Yan Yao
Magnesium batteries offer a safer alternative for next-generation battery technology due to their insusceptibility to dendrite deposition. Selective membranes tailored for magnesium-ion conduction will unlock further technological advancement. Herein, we demonstrate fluorine-free magnesiated sulfonated poly(ether ether ketone) (Mg-SPEEK) selective membranes capable of facilitating magnesium-ion conduction while effectively rejecting soluble organic species. These membranes demonstrate a reversible Mg plating and stripping Coulombic efficiency (CE) of 85.4% and an ionic conductivity of 3.3 × 10–4 S cm–1 at room temperature, surpassing those for a Mg-Nafion selective membrane. Theoretical density functional theory (DFT) calculations reveal that SPEEK possesses more localized charge centers along its backbone compared with Nafion, potentially facilitating enhanced ion conduction. Full cells assembled with Mg-SPEEK coupled with the organic cathode pyrene-4,5,9,10-tetraone (PTO) and Mg metal demonstrated significantly improved capacity retention as compared to those assembled with conventional nonselective separators.
研究领域:
材料科学
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电化学
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理论计算
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DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2024
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IF 5.5
Jiao Chen,Chao Cai,Yunfei Sun,Bai Sun,Hongyan Wang,Yongliang Tang,Yuanzheng Chen
Electrolytic water splitting (EWS), regarded as a sustainable and promising strategy for hydrogen production, has received huge attention in recent years. However, the practical application of EWS is greatly hindered by the sluggish kinetics of the oxygen evolution reaction (OER). Herein, we proposed an efficient strategy for the synthesis of hierarchical hollow nickel selenide with significant HER and OER electrocatalytic activity. The as-synthesized NiSe 2 possesses low overpotential of ∼85 mV at the current density of 10 mA/cm 2 for the HER in 0.5 M H 2 SO 4 and ∼270 mV for OER in 1 M KOH. Importantly, when employed into full water splitting on membrane electrode assembly, it merely requires an ultralow voltage of 1.73 V to achieve the current density of 1 A/cm 2 , outperforming most of the reported other Ni/Ni-Se based structures. Density Functional Theory (DFT) simulations confirm that the hierarchical hollow NiSe 2 structure facilitates the reduction of the Gibbs free energy change of H- and O-containing intermediates in the HER/OER process, which promotes the formation of intermediates and thus accelerates the catalytic kinetics. This work offers an important structure engineering route to develop high catalytic performance materials and sheds light on the promotion of electrocatalytic activity for clean energy utilization.
研究领域:
材料科学
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能源化学
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理论计算
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产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2020
·Vol. 32
·期 23
·2001082
·
IF 27.398
Ye Zhang,Pu Huang,Jia Guo,Rongchao Shi,Weichun Huang,Zhe Shi,Leiming Wu,Feng Zhang,Lingfeng Gao,Chao Li,Xiuwen Zhang,Jialiang Xu,Han Zhang
Graphdiyne (GDY), a newly emerging 2D carbon allotrope, has been widely explored in various fields owing to its outstanding electronic properties such as the intrinsic bandgap and high carrier mobility. Herein, GDY-based photoelectrochemical-type photodetection is realized by spin-coating ultrathin GDY nanosheets onto flexible poly(ethylene terephthalate) (PET) substrates. The GDY-based photodetectors (PDs) demonstrate excellent photo-responsive behaviors with high photocurrent ( P ph , 5.98 µA cm - 2 ), photoresponsivity ( R ph , 1086.96 µA W - 1 ), detectivity (7.31 × 10 10 Jones), and excellent long-term stability (more than 1 month). More importantly, the PDs maintain an excellent P ph after 1000 cycles of bending (4.45 µA cm - 2 ) and twisting (3.85 µA cm - 2 ), thanks to the great flexibility of the GDY structure that is compatible with the flexible PET substrate. Density functional theory (DFT) calculations are adopted to explore the electronic characteristics of GDY, which provides evidence for the performance enhancement of GDY in alkaline electrolyte. In this way, the GDY-based flexible PDs can enrich the fundamental study of GDY and pave the way for the exploration of GDY heterojunction-based photodetection.
研究领域:
材料科学
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电子工程
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理论计算
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
·
IF 5.816
Na Ye,Zhao Jiang,Tao Fang
The low-palladium Pd/TaN–C catalyst is synthesized by a surfactant-free solvothermal approach and exhibits high activity (2613.18 mA mg Pd −1 ), durability and CO tolerance for MOR (methanol oxidation reaction) in alkaline media , 12.4 folds that of the commercial Pd/C. XPS and electrochemical results indicate that the interfacial Pd–TaNO bond is generated. This also brings the enhancement of OH ad adsorption responsible for anti-CO poisoning ability. Density Functional Theory (DFT) calculations indicate that the reaction pathway and the rate-determining step are changed for methanol decomposition to CO on the Pd 4 /TaN(001) surface compared with Pd (111). The preferred pathway can be described as: CH 3 OH→CH 3 O→CH 2 O→CHO→CO. Furthermore, the results indicate that the adsorption of OH is enhanced and the energy barrier of COOH formation from CO + OH is reduced with the high concentration of hydroxyl on the Pd 4 /TaN(001) surface, further confirming the bi-functional effect of hydroxyl on the CO tolerance.
研究领域:
电化学
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催化材料
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理论计算
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Huiping Zhao,Guangfang Li,Fan Tian,Qintao Jia,Yunling Liu,Rong Chen
To overcome the issue of UV-light response character of Bi 2 O 2 CO 3 due to its wide band gap, we primarily attempted to understand the possibility of improving the photocatalytic activity of Bi 2 O 2 CO 3 via g-C 3 N 4 surface-decoration by the theoretical calculation. Subsequently, g-C 3 N 4 surface-decorated Bi 2 O 2 CO 3 was successfully prepared via a facile hydrothermal method. It was found that the g-C 3 N 4 surface-decorated Bi 2 O 2 CO 3 samples exhibited enhanced activities for the photodegradation of tetracycline compared with pure Bi 2 O 2 CO 3 upon simulated solar light irradiation. Among them, the 10 wt% g-C 3 N 4 surface-decorated Bi 2 O 2 CO 3 sample showed the highest photocatalytic efficiency. First principle calculation and experimental data confirmed that the charge transfer at the interface between g-C 3 N 4 and Bi 2 O 2 CO 3 could significantly suppress the recombination of photo-generated electron-holes pairs, thus improving the photocatalytic performance. The proposed mechanism for the enhanced photocatalytic activity was also discussed. Moreover, the photodegradation of antibiotics over g-C 3 N 4 surface-decorated Bi 2 O 2 CO 3 was also performed in actual water matrix.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 39
·20922-20931
·
IF 8.867
Jieyu Liu,Meng Yu,Xuewei Wang,Jie Wu,Changhong Wang,Lijun Zheng,Dachi Yang,Hui Liu,Yan Yao,Feng Lu,Weichao Wang
An alternative material SmMn2O5 mullite with regard to Pt/C is proposed to catalyze the oxygen reduction reaction (ORR) by combining density functional theory (DFT) calculations and experimental validations. Theoretical calculations are performed to investigate the bulk phase diagram, as well as the stability and electrocatalytic activity of the ORR under alkaline conditions for SmMn2O5 (001) surfaces, which are passivated by nitrogen atoms to avoid any spurious interference. The adsorptions of relevant ORR species (O*, OH*, OOH* and OO*) tend to compensate the coordination of manganese atoms to form Mn-centered octahedral or pyramidal crystal fields, and the corresponding binding energies fulfill a linear relationship. An oxygen molecule prefers to be reduced to OH−via a four-electron pathway and this prediction is verified by electrochemical measurements on the as-prepared SmMn2O5 catalyst with a nanorod structure. Volcano curves are obtained to describe the trends in theoretical ORR activity as a function of a single parameter, i.e. the oxygen binding energy. An overpotential of 0.43 V is obtained at the O* binding energy around 3.4 eV, which is close to the experimental observation (0.413 V) in this work. SmMn2O5 mullite exhibits favorable ORR activity and superior stability with only ∼5% decay in activity over 20 000 s of chronoamperometric operation in contrast to ∼15% decrease of Pt/C, making it a promising candidate for a cathode catalyst.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
Materials
·
2023
·Vol. 16
·期 20
·6712
·
IF 3.4
Zhishun Zhu,Xiulan Zhang
In this paper, zeolitic imidazolate framework-8 was modified by N-(3-aminopropyl)-imidazole to obtain a novel MOF called AMOF. Subsequently, AMOF served as a carrier for the delivery of 2-mercapto-1-methyl imidazole (MMI) to inhibit the corrosion of Cu. Scanning electron microscopy, Fourier transform infrared spectroscopy, and X-ray diffraction were applied to characterize the morphologies and structures of AMOF and AMOF@MMI. Ultraviolet-visible spectroscopy and thermogravimetric analysis were adopted to value the capacity of the load and release of the AMOF, respectively. The mass ratio of loaded MMI molecules was 18.15%. In addition, the inhibition behavior of AMOF@MMI for Cu was evaluated by polarization curves and electrochemical impedance spectroscopy. The results indicated that the AMOF loaded MMI successfully, and the released MMI could adsorb on the Cu surface and inhibit the Cu corrosion. The inhibition efficiency could reach 88.2%. The binding and interaction energies between the AMOF surface and the MMI were −16.41 kJ/mol and −20.27 kJ/mol.Keywords:corrosion inhibitor;ZIF-8;loading and delivery;AMOF;theoretical calculation
研究领域:
材料科学
·
电化学
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DOI
PubMed
高影响因子
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