JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xin Zhang,Rui Xu,Tao Wang,Lengyuan Niu,Yinyan Gong,Can Li
The controlled introduction of oxygen vacancies (O vac ) offers a promising strategy for enhancing the catalytic activity of materials. In this study, we effectively modulated the concentration of O vac in the zirconium-based amorphous high-entropy oxides (HEOs) by optimizing the Zr cation content. This adjustment facilitated precise tuning of the d-band center and chemical activity of Zr active sites, leading to substantial improvements in electrocatalytic performance for the oxygen evolution reaction (OER). Among the prepared zirconium-based materials, the HEO-Zr 1.0 specimen demonstrated outstanding OER electrocatalytic performance, achieving an overpotential of 257 mV at 10 mA cm −2 and 299 mV at 100 mA cm −2 , a small Tafel slope of 40.3 mV dec −1 . At the same time, the HEO-Zr 1.0 ||HEO-Zr 1.0 cell demonstrates excellent performance in complete water splitting. These findings underscore the effectiveness of moderate O vac concentrations in enhancing catalytic activity, as confirmed by both experimental data and density functional theory simulations. This approach of controlled O vac introduction provides a viable path for optimizing HEO catalytic performance, offering valuable insights for advancing electrocatalytic applications.
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
TRIBOLOGY INTERNATIONAL
·
2025
·
IF 6.9
Bin Hu,Xinhuan Niu,Jiakai Zhou,Changxin Dong,Chao He,Xinjie Li,Zheng Wu,Jiahui Li
The development of sapphire slurry follows the principles of compositional simplification, environmental sustainability, and high efficiency with low cost. This study systematically investigated the effects of polyhydroxyamine pH regulators, 2-amino-2-methyl-1-propanol (AMP), 2-amino-2-methyl-1,3-propanediol (AMPD), and tris(hydroxymethyl)aminomethane (TRIS), on the polishing performance of C-, R-, and M-plane sapphire substrates. The results demonstrated that TRIS exhibited the highest efficacy, achieving material removal rates (MRRs) of 5.512 µm/h, 3.422 µm/h, and 4.541 µm/h for C-, R-, and M-plane sapphire, respectively, while reducing surface roughness (Sq) to 0.191 nm, 0.178 nm, and 0.184 nm. Tribological analysis, SEM characterization, zeta potential measurements, particle size distribution tests, and spectroscopic techniques (UV-Vis, XPS, and FTIR) were employed to elucidate the mechanical and chemical mechanisms governing material removal. All three pH regulators can also function as complexing agents, forming complexes with Al OH 4 − , with TRIS demonstrating the strongest chelation capability. Density functional theory (DFT) calculations further verified these findings, revealing that TRIS possesses the highest number of reactive sites. The consistency between computational and experimental results established a quantitative structure-performance relationship. This work provides a green and efficient paradigm for the precision machining of hard, brittle materials.
研究领域:
材料科学
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表面工程
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半导体制造
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计算化学
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机械工程
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电子材料
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产品关联
DOI
高影响因子
WATER RESEARCH
·
2017
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IF 6.942
Mingquan Yan,Xuze Han,Chenyang Zhang
In this study, seven model compounds containing typical functional groups (phenolic and carboxylic groups) present in nature organic matter (NOM) were used to ascertain the nature of the characteristic bands in differential absorbance spectra (DAS) of NOM that are induced by metal ion binding. Some similarities were found between the DAS of the examined model compounds, caffeic acid , ferulic acid , sinapic acid , terephthalic acid , isophthalic acid , esculetin and myricetin and those of NOM. The binding of Cu(II) with carboxylic group might produce two peaks, A1 and A2, while the binding of Cu(II) with phenolic group might produce all four Gaussian peaks, from A1 to A4 displayed in the DAS of NOM. The UV–visible spectra predicted using time-dependent density functional theory (TD-DFT)-based methods met well with the experimental DAS of model compounds at different stages of Cu(II) binding. It demonstrates that the features in absorbance spectra are chiefly caused by HOMO (Highest Occupied Molecular Orbital) - LUMO (Lowest Unoccupied Molecular Orbital) transitions in the molecule and that the appearance of peaks in DAS reflects the changes of the molecular orbitals around reactive functional groups in a molecule before and after metal ion binding. The basis of the DAS features of NOM that are induced by metal ion binding could be identified primarily by the frontier molecular orbital theory .
研究领域:
环境化学
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光谱学
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计算化学
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水文地球化学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 10
·4897-4910
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IF 3.3
Daryoush Sanaei,Mohammad Hadi Dehghani,Hamidreza Sharifan,Monika Jain,Bahram Roshan,Javier A. Arcibar-Orozco,Vassilis J. Inglezakis
Mixed perovskites have vast industrial potential, but some challenges (i.e., aggregation and chemical instability) limit their applications. Herein, a novel environment-friendly carbon aerogel (CAg) synthesized from sodium alginate (SA) was used as a precursor to create a double-B-site perovskite/carbon aerogel hybrid adsorbent ((Sr0.7Mn0.3Co0.5Fe0.5O3−δ)/CAg) (DB-perovskite/CAg hybrid). The adsorbent was extensively characterized via different techniques, including X-ray photoelectron spectroscopy and Fourier transform infrared (FTIR) spectroscopy. The removal efficiency for crystal violet (CV) and acid yellow 17 (AY17) was conducted over various pH, adsorbent/adsorbate dosages, and reaction times in an aqueous system. The maximum adsorbed concentration (Qmax) recorded by 206 mg g−1 and 113 mg g−1 for CV and AY17, respectively, and compared to the performance of only DB-perovskite (114 mg g−1 and 59 mg g−1), respectively. The adsorption site energy distribution was studied by applying the density functional theory (DFT). The adsorption on the DB-perovskite/CAg hybrid was significantly regulated by pH change. The cooperative metal active/Lewis acid sites of the DB-perovskite/CAg adsorbent led to a faster and higher adsorption capacity toward CV and AY 17. The doping of Mn indicated a synergistic effect in improving the adsorption of either dye through the introduction of abundant active sites and strengthening of metal-functional groups (–C–O–C, –COOH, and C–OH/O–H)–π aromatic bonding, confirmed by DFT calculations.
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 47
·期 3
·1197-1208
·
IF 3.925
Wei-Ye Zhang,Si-Qing Ye,Xin-Tao Yang,Bao-Shi Zhu,Wei-Li Li,Hong-Xing He,Xiu-Jun Deng
A novel magnetic graphene oxide-based surface imprinted polymer (Fe3O4@GO@IIP) was synthesized using the surface imprinting technology to selectively adsorb Ni(II) from aqueous solution. The imprinted polymer was characterized by FT-IR, XRD, SEM, TEM, VSM, TGA and XPS. The results showed that the sorbent exhibited good thermal and mechanical stability, and can be quickly separated from the solution by applying an external magnetic field. The adsorption performance indicated that the prepared imprinted material had a short adsorption equilibrium time (16 min) and a high adsorption capacity (35.31 mg g−1) for Ni(II) at an optimal pH of 6.0. The selectivity coefficients of the imprinted material were 17.57, 16.27, 10.86, 14.27 and 17.65 for Ni(II)/Co(II), Ni(II)/Cu(II), Ni(II)/Pb(II) Ni(II)/Cd(II), and Ni(II)/Zn(II), respectively. Reusability studies indicated that the adsorption capacity of the prepared polymer did not decrease significantly after repeated use ten times. Moreover, the adsorption mechanism of Ni(II) by the imprinted polymer was also studied. The adsorption process was spontaneous and endothermic, and followed the pseudo-secondary kinetic model and the Langmuir model. The results of the Scatchard model indicated the presence of two Ni(II) strong binding sites on Fe3O4@GO@IIP, where the single-bond O atom of the sulfonic acid group and the N atom of the –N–CO group in AMPS played a dominant role in Ni(II) adsorption, as conformed by both DFT calculations and XPS.
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高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2022
·
IF 3.841
Rui Chen,Qiuyue Li,Kai Xu,Zhiwei Zhang,Tianhua Wang,Jinkang Ma,Yan Xi,Lifeng Cao,Bing Teng,Haitao Wu
In this present work, a chalcone derivative 1-(4-Chlorophenyl)-3-(4-ethoxyphenyl)-prop-2-en-1-one is investigated using the density functional theory. PES scan is used to find the most stable conformational structure of the title compound. The geometrical parameters, FT-IR and FT-Raman spectra are performed by the DFT method with B3LYP/6-311+G basis set, which are very comparable with the experimental results. UV-Vis spectrum, frontier molecular orbitals, global reactivity descriptors, molecular electrostatic potential surface, NLO parameters and Mulliken charge in the gas phase, various polar and non-polar solvents are performed to reveal solvents effect. Further, it is found that the electronic properties show a good correlation with the polarity of solvents. Hirshfeld Surface analysis demonstrates H···H contact is dominant in the crystal packing. By means of molecular reactivity descriptors such as natural bond orbital analysis, Fukui function and dual descriptor analysis, the chemical reactivity is theoretically estimated. ELF and LOL are used to access the energy density of electrons. Molecular docking illustrates ECC may be a potential inhibitor for 6R3K protein.
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Longde Jiang,Jingde Luan,Haowei Zhang,Yu Bai,Yu Zhang,Wengang Liu,Zheng Yan,Haiting Zhao
Photocatalytic H 2 production from seawater splitting is a promising method for sustainable energy conversion technology. The vanadium-oxygen binary doped carbon nitride (VO X -CN) is successfully prepared for H 2 production. Benefiting from the electronic structure alteration, the maximum H 2 yield on VO X -CN in artificial seawater reaches 4475.74 μmol h −1 g −1 , 10 times higher than that of CN in deionized water. The impact of ions on the photocatalytic activity of VO 2 -CN is followed by Na + > Mg 2+ > K + > Ca 2+ . The adsorption of electrolyte ions promotes the formation of delocalized electron clouds on the surface of VO 2 -CN, facilitating more electrons to participate in H + reduction. Screening based on six machine models, the decision tree regression algorithm is used to reveal the interaction between cation type, their concentration and H 2 yield. Pearson heatmap indicates that Na + , Mg 2+ , and K + ions are positively correlated with H 2 yield, whereas Ca 2+ shows a negative correlation. The interactions among Na + , Mg 2+ and K + atoms facilitate H 2 production in multi-ion system, whereas Ca 2+ ions do the opposite, especially for high concentration. This work proposes new insights into the interference on H 2 yield between the structure alteration of CN framework and the change of ion type and concentration.
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Hao Du,Rubin Huo,Aoxiang Liu,Yuxin Hui,Bo Shen,Ningyi Li,Yun Ji,Qin Jin,Baobing Zheng,Guoxiang Yang,Zhe Zhang,Qi Wang
Herein, a photo-self-Fenton system of resorcinol-formaldehyde resins/MIL-88A(Fe) (RF/88A) S-scheme heterojunction was successfully established to in-situ generate and activate H 2 O 2 toward tetracycline (TC) degradation and sterilization under visible light illumination. As a result, the 35 %-RF/88A (the mass ratio of RF to 88A was 35 %) can remove most TC and kill approximately 100 % E. coli and S. aureus . Notably, the composites presented superior repeatability and wide pH application range. Fukui index identified the reaction sites of TC molecule and quantitative structure-activity relationship (QSAR) forecasted intermediates toxicity. Density functional theory (DFT) calculations were performed to investigate electron transfer mechanism of the heterojunctions on a molecular scale. Such a S-scheme charge transfer route was also proved by in situ irradiated X-ray photoelectron and electron paramagnetic resonance measurements. In summary, this research innovatively provides deep insights into the in-situ generation and activation of H 2 O 2 and exhibited an environmentally friendly way toward pollutant degradation and sterilization.
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2020
·
IF 5.006
Renjie Deng,Kuiyi You,Wenjin Ni,Fangfang Zhao,Pingle Liu,He’an Luo
In this work, we developed a low-temperature and efficient approach for the highly selective preparation of valuable p -nitrochlorobenzene from the liquid-phase catalytic nitration of chlorobenzene with NO 2 in O 2 -Ac 2 O-Hβ composite system. The results demonstrated that the introduction of molecular oxygen remarkably enhanced the chlorobenzene conversion and the cooperation catalysis of Hβ zeolite and Ac 2 O envidently improved the selectivity to para -nitro product. Under the optimized reaction conditions, 93.6 % of the selectivity to p -nitrochlorobenzene with 84.0 % of chlorobenzene conversion was obtained, and the ratio of p -nitrochlorobenzene to o -nitrochlorobenzene could reach up to 20.3. Furthermore, the selectivity distribution of nitration products was reasonably explained by the density functional theory (DFT) calculation. Finally, the possible nitration reaction pathway of chlorobenzene with NO 2 was suggested in O 2 -Ac 2 O-Hβ composite catalytic system. The present work affords a new and mild nitration approach for highly selective preparation of valuable para -nitro products, and has potential industrial application prospects.
研究领域:
化学工程
·
催化
·
有机化学
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DOI
高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Shuhao Li,Feng Wang,Zongli Xie,Derrick Ng,Boxiong Shen
Zeolitic imidazolate framework-8 (ZIF-8) based catalysts are considered as promising candidates for the selective catalytic reduction of NO by CO (CO-SCR) reaction due to their large specific surface area. However, the structure of ZIF-8 will be damaged during the synthesis procedure of the catalyst, leading to a decrease in their physical properties, which in turn affects the catalytic performance of the catalyst. Herein, a CeO 2 -ZIF-8 core-shell structure was synthesized and doped with Fe, resulting in the formation of Fe@CeO 2 -ZIF-8, for CO-SCR reaction. Characterization results show that the Fe@CeO 2 -ZIF-8 core-shell catalyst has better morphology, thermal stability, and higher specific surface area than the FeCe co-impregnated ZIF-8 catalyst (FeCe@ZIF-8 (IM)). Moreover, the reducibility of the reactive Fe species in the Fe@CeO 2 -ZIF-8 core-shell catalyst is also enhanced. As a result, the Fe@CeO 2 -ZIF-8 core-shell catalyst exhibited higher low-temperature CO-SCR catalytic activity with its NO conversion reaching 99% at 250 °C versus the FeCe@ZIF-8 (IM) catalyst (89% at 250 °C). The experimental results were further verified by density functional theory (DFT) calculations including Electron Localization Function (ELF), Valence Charge Density Difference (VCDD), Projected Density of States (PDOS) and Bader charge analyses. The calculation results revealed that the core-shell configured Fe@CeO 2 -ZIF-8 catalyst has a stronger active metal-support charge transfer and better capacity for the adsorption of the reactants. The reaction mechanism over Fe@CeO 2 -ZIF-8 core-shell catalyst was investigated via in situ DRIFTS experiments, and results showed that the nitro compounds and formate species are critical intermediates in this reaction at a higher temperature range (300–350 °C). This work provides a new strategy for the synthesis of ZIF-8 based catalysts with better properties for CO-SCR reaction.
研究领域:
催化化学
·
环境化学
·
材料科学
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物理化学
·
能源化学
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表面科学
·
纳米材料
✓ 已验证
DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2024
·
IF 5.2
Haoyuan Zheng,Yuxiao Jia,Chen Jin,Hang Che,Chia-Tse Lee,Zhenke Chen,Guang Liu,Li Wang,Shixuan He,Xinhua Wang,Haizhen Liu,Mi Yan
The Mg(NH 2 ) 2 -2LiH composite system is a promising vehicle-mounted hydrogen storage material, but its application is limited due to serious thermodynamic and kinetic barriers. Adding additives can effectively optimize their hydrogen absorption and desorption kinetics and thermodynamic performance. In this work the comprehensive hydrogen storage performance of Mg(NH 2 ) 2 -2LiH with extremely small nano rare earth borides is improved, and a series of characterization methods and density functional theory (DFT) calculation systems was combined to study its hydrogen storage improvement mechanism. The research results show that the method of adding 5 wt% molten salt to prepare nano CeB 6 (24.5 nm) can significantly reduce the initial hydrogen absorption/release temperature of Mg(NH 2 ) 2 -2LiH from 110/130 to 45/90 °C, inhibit the generation of ammonia by-products, and improve hydrogen purity. Under low-temperature hydrogen absorption conditions at 120 °C, the improved sample can absorb 2.81 wt% hydrogen gas, with a hydrogen absorption capacity more than 3.5 times of the unmodified sample. The amount of hydrogen released at 150 °C reaches 3.35 wt%, which is more than twice that of the pristine sample, demonstrating excellent hydrogen absorption and release kinetics performance. After 10 consecutive hydrogen cycles, 4.64 wt% hydrogen can still be released, and the cycle retention rate can be increased from 85% before improvement to nearly 100%, demonstrating good reversibility. Mechanism studies show that nano CeB 6 can effectively weaken the Mg–N and N–H bonds of Mg(NH 2 ) 2 and inhibit the polycrystalline transformation of the hydrogen evolution product Li 2 MgN 2 H 2 at high temperatures. It can also provide nucleation active sites for hydrogen absorption and desorption in the material, making the system possess superior hydrogen absorption and desorption performance and cycling stability. This study provides new insights into the role of rare earth borides in Mg(NH 2 ) 2 -2LiH hydrogen storage materials, both experimentally and theoretically.
研究领域:
材料科学
·
化学工程
·
物理化学
·
理论化学
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DOI
高影响因子
ORGANOMETALLICS
·
2020
·
IF 3.804
Shuang Huang,Xi Hong,He-Zhen Cui,Bing Zhan,Zhi-Ming Li,Xiu-Feng Hou
Herein, an unprecedented bimetallic bis-NHC Cp*Ir complex 1 bearing 2-arylbenzo[d]oxazolyl and NHC ligands is reported. A significant increase in activity was observed for N-methylation of amines and reduction of aldehydes with MeOH catalyzed by 1 compared to the monometallic analogues (2–11). Under the optimal conditions, it showed to be highly effective in N-methylation of nitroarenes with MeOH as both C1 and H2 source. Substrates, including aromatic amines, ketones, and nitro compounds with various functional groups, can be well-tolerated. Mechanistic studies and DFT calculation highlight the significance of bimetallic centers cooperativity.
研究领域:
无机化学
·
催化
·
有机金属化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）