Crystals
·
2018
·Vol. 8
·期 10
·367
·
IF 2.144
Fang Fu,Bin Zheng,Lin-Hua Xie,Huiling Du,Shuangming Du,Zhenhua Dong
Composite materials that combine the unique properties of zeolitic imidazolate frameworks (ZIFs) and carbon nanotubes (CNTs) can give rise to novel applications. Here, ZIF-8/CNT composites were successfully prepared with and without the addition of an agent template. The size of the ZIF-8 crystals in the composite materials was controlled by varying the template, feeding order, and concentration of reactants. Thus, ZIF-8 crystals with a wide variety of sizes (from nano- to micrometer size, which is range that differs by a factor of 10) were obtained, depending on the conditions. This size-controllable synthesis of ZIF-8 was achieved by modifying the number of nucleation sites on the CNTs, as revealed by density functional theory (DFT) calculations. This work provides an efficient method for preparing ZIF-8/CNT composites with controllable size and can pave the way for the synthesis of other metal-organic framework (MOF)/CNT composite materials.Keywords:crystal growth;ZIF-8;carbon nanotube;DFT calculation
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2019
·
IF 12.221
Yunrui Zhang,Yongjun Gao,Siyu Yao,Siwei Li,Hiroyuki Asakura,Kentaro Teramura,Haijun Wang,Ding Ma
MoS2 catalysts with abundant S and Mo defects have been developed for the one-pot reductive amination of nitro compounds with aldehydes to synthesize secondary amines. The combination of multiple structural characterizations demonstrates that the density of S vacancies can be tuned by changing the thermal sublimation temperature. The experimental results and DFT calculations demonstrate that S vacancies on the surface of MoS2 are the active sites for the hydrogenation of the intermediate imines to the final products secondary amines.
研究领域:
催化化学
·
材料科学
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
Polymers
·
2021
·Vol. 13
·期 24
·4317
·
IF 4.329
Xinxin Wang,Yanan Zhao,Ting Wang,Yan Liang,Xiangzhong Zhao,Ke Tang,Yutong Guan,Hua Wang
As lactoferrin (LF) plays an essential role in physiological processes, the detection of LF has attracted increasing attention in the field of disease diagnosis. However, most current methods require expensive equipment, laborious pretreatment, and long processing time. In this work, carboxyl-rich carbon dots (COOH-CDs) were facilely prepared through a one-step, low-cost hydrothermal process with tartaric acid as the precursor. The COOH-CDs had abundant carboxyl on the surface and showed strong blue emission. Moreover, COOH-CDs were used as a fluorescent sensor toward Fe3+and showed high selectivity for Fe3+with the limit of detection (LoD) of 3.18 nM. Density functional theory (DFT) calculations were performed to reveal the mechanism of excellent performance for Fe3+detection. Meanwhile, COOH-CDs showed no obvious effect on lactobacillus plantarum growth, which means that COOH-CDs have good biocompatibility. Due to the nontoxicity and excellent detection performance for Fe3+, COOH-CDs were employed as a fluorescent sensor toward LF and showed satisfying performance with an LoD of 0.776 µg/mL, which was better than those of the other methods.Keywords:carbon dots;DFT calculations;Fe3+;lactoferrin;fluorescent sensor
研究领域:
分析化学
·
生物医学工程
✓ 已验证
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Yunlong Xu,Linlin Yang,Chunying Si,Shuoqi Zhang,Quanxing Zhang,Guixiang Zeng,Wei Jiang
Sn-beta zeolite is a promising catalyst for the direct synthesis of lactide from lactic acid; here, we clarify the relationship between its local structure and activity through the interplay of experiments and DFT calculations. The open sites (HO-Sn-(OSi)3 with adjacent Si–OH) play a key role in the high activity of Sn-beta zeolite, where the reaction rate significantly decreases from 0.2258 mmol min–1 gcat–1 to 0.0724 mmol min–1 gcat–1 if the open sites were masked with Na+. Density functional theory (DFT) calculations show that the decrease in reaction rate comes from the weaker interaction between substrate and the open Sn site by Na+ exchange, which leads to the significant increase in the Gibbs energy barrier from 34.0 kcal/mol to 57.2 kcal/mol (rate-determining step). Other activities of heteroatom M-beta zeolites (where M = Ti, Zr, Hf) were also investigated, where the open sites were found to be crucial for the high activity in the direct synthesis of lactide as well. The information provided by this work is valuable for precise design of efficient catalysts for the one-step synthesis of lactide.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Energy
·
2022
·
IF 9.257
Xinlong Zheng,Daoxiong Wu,Yuhao Liu,Jing Li,Yingjie Yang,Wei Huang,Weifeng Liu,Yijun Shen,Xinlong Tian
The photocatalyst is a key component of efficient photocatalytic hydrogen evolution (PHE) via water splitting. Bournonite CuPbSbS 3 has a great application potential in solar-to-energy due to its tremendous semiconductor properties and earth-abundant components. Although CuPbSbS 3 has achieved the highest power conversion efficiency (PCE) of 2.65% in thin-film photovoltaics , its application in PHE via water splitting has been rarely studied. In this work, CuPbSbS 3 nanoflakes with dominate (002) facet is fabricated by a facile butyldithiocarbamate acid (BDCA) solution process, which exhibits a PHE rate of 250.8 μmol g −1 /h without any co-catalyst under simulated solar irradiation. Density functional theory calculations show that plentiful catalytic sites with low ΔG H∗ are responsible for the high hydrogen evolution reaction performance of CuPbSbS 3 . This study represents an effective approach to realize photovoltaic-to-photocatalyst hydrogen evolution of Cu-based quaternary chalcogenides .
研究领域:
材料科学
·
能源化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Kunjie Wang,Yanan Li,Dongxu Yang,Yunsi Wang,Fuan Wei,Bingxin Liu,Peng Zhang,Benhua Xu,Yongcheng Li
Coupling noble metals on molybdenum disulfide (MoS 2 ) has emerged as a promising strategy for triggering inert basal plane and boosting hydrogen evolution reaction (HER) performances. Herein, ultrafine Ru nanoparticles (NPs) are decorated on vertical 2H MoS 2 nanosheets via a facile hydrothermal method. Benefiting from new active site centers triggered by ultrafine Ru NPs and vertically grown 2H MoS 2 nanosheets on carbon cloth (CC), Ru 0.15 @2H MoS 2 exhibits impressive HER performances in dual pH media, with low overpotentials of 20 and 111 mV and small Tafel slope of 67.6 and 76.3 mV dec ‑1 in alkaline and acid solutions to drive a current density of 10 mA cm -2 . DFT calculation results prove that ultrafine Ru NPs decorated on 2H MoS 2 nanosheets endow Ru 0.15 @2H MoS 2 with low hydrogen adsorption free energy and fast charge transfer kinetics. This work provides an effective and simple method for designing MoS 2 -based catalysts with high catalytic activity to decorate precious metal in a wide pH medium.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2020
·Vol. 28
·期 10
·12909-12917
·
IF 3.056
Ren Jingyu,Li Jie,Lv Lei,Wang Jian
Ionic liquids (ILs) are a kind of promising extractants for removing undesirable organics from industrial wastewater and crude oil, etc. Herein, IL regeneration by ozonation was proposed for its recycling. 1-Butyl-3-methylimidazolium tetrafluoroborate ([Bmim]BF 4 ) and phenol were used as the representative IL and organic matter, respectively. The regeneration performance, stability of [Bmim]BF 4 , and roles of hydrogen bonds between O 3 and [Bmim]BF 4 in the phenol removal were studied. The experimental results showed that 90.2% of phenol was degraded in [Bmim]BF 4 after ozonation treatment for 30 min with the O 3 concentration of 1.2 mg/L. The nonvolatility of [Bmim]BF 4 -made phenol was adequately degraded, while the concentration of phenol increased during ozone treatment in the conventional extractants (ethanol, ethyl acetate, and dichloromethane) due to their high volatility. The reuse experiments, spectra of Fourier transform infrared spectroscopy and 1 H nuclear magnetic resonance spectroscopy indicated that [Bmim]BF 4 was steady under the ozonation process. Density functional theory simulation confirmed that hydrogen bonds between [Bmim] + and O 3 could be formed, and calculational results of Hirshfeld charges indicated that the nucleophilicity of O 3 was enhanced by the hydrogen bonds. The enhanced nucleophilicity resulted in the increase of phenol degradation efficiency by ozonation, and the synergistic effect between O 3 and ILs was proportional to the hydrogen bond donor ability of ILs.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 45
·27969-27977
·
IF 3.361
Yaoyang Liu,Sheng Liu,Zhibin Liu,Chuang Zhao,Chunhui Li,Yu Zhou,Caishan Jiao,Yang Gao,Hui He,Shaowen Zhang
A novel asymmetric diglycolamide N,N-dimethyl-N′,N′-dioctyl diglycolamide (LII) was synthesized. The Nd(III) extraction behavior from HNO3 and loading capability of the solution of LII in 40/60 (v/v)% n-octanol/kerosene were studied. Analyses by the slope method, ESI-MS, and FT-IR indicated that, similar to the previously studied isomer ligand N,N′-dimethyl-N,N′-dioctyl diglycolamide (LI), 1 : 3 Nd(III)/LII complexes formed. Under the same experimental conditions, the distribution ratio and limiting organic concentration of LII towards Nd(III) were smaller than those of LI, but the critical aqueous concentration of LII was larger, which implies that LII exhibited poorer extraction and loading capabilities towards Nd(III) than LI, and LII has a tendency to be less likely to form the third phase. The quasi-relativistic density functional theory (DFT) calculation was performed to provide some explanations for the differences in their extraction behaviors. The electrostatic potential of the ligands indicated that the electron-donating ability of the amide O atoms in LII displayed certain differences compared with LI. This inhomogeneity in LII affected the interaction between LII and Nd(III), as supported by QTAIM and bonding nature analysis, and it seemed to reflect in the extraction performance towards Nd(III).
研究领域:
化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
CHEMISTRY OF MATERIALS
·
2019
·
IF 10.159
Jiang-Zhen Qiu,Jibo Hu,Jinggang Lan,Long-Fei Wang,Guangying Fu,Rujian Xiao,Binghui Ge,Jiuxing Jiang
As the most active new frontier, a single-atom catalyst (SAC) combining the merits of heterogeneous and homogeneous catalysts would have a significant effect on the 100 year history of ammonia synthesis research. Here, the Ru SAC has been demonstrated to be active and efficient for ammonia synthesis. To this end, an ideal model catalyst, pure siliceous zeolite-supported Ru SAC (Ru SAs/S-1), which shows surprising catalytic ammonia synthesis activity compared to that of a conventional Ru catalyst, was designed. Both atomic-resolution scanning transmission electron microscopy, X-ray absorption spectrometric analysis, and in situ diffuse reflectance infrared Fourier transform spectroscopy identify the single-Ru-atom nature of Ru SAs/S-1 before and after the reaction. Further DFT calculations reveal that the reaction mechanism is different from traditional mechanisms. Therefore, this paper provides an alternative SAC strategy to design high-performance Ru catalysts for ammonia synthesis.
研究领域:
催化化学
·
材料科学
·
物理化学
✓ 已验证
DOI
高影响因子
WATER AIR AND SOIL POLLUTION
·
2024
·Vol. 235
·期 1
·1-20
·
IF 3.8
Liu Bangwei,Zhou Yan,Zhang Yiwei,Chen Dandan,Liu Wenhui,Lu Ping,Su Xiaoyu,Xia Tian
A zero-valent iron-loaded corn straw char (ZVI-CSC) was synthesized in this study for the remediation of As(V) and Cd(II) contamination. The impact of ZVI-CSC on the adsorption performance of As(V) and Cd(II) in solution, as well as their migration properties in soil, was investigated through adsorption kinetics and soil column leaching experiments, respectively. The results showed that the adsorption capacity of As(V) by ZVI-CSC was significantly improved to 14.42 g·kg −1 at pH = 3, compared with unmodified corn straw char (CSC). However, the adsorption capacity of Cd(II) was not improved. In the leaching experiments, the addition of ZVI-CSC to As(V)-contaminated soil resulted in a significant reduction of cumulative As(V) release rate from 32.26 to 3.11%, compared with corn straw char (CSC). Moreover, the role of ZVI in As(V)/Cd(II) remediation was analyzed. nZVI forms ≡Fe-OH and ≡Fe-OOH due to oxidation, which can form monodentate and bidentate complexes with As(V) via ligand exchange, thus promoting As immobilization. Furthermore, to further improve the adsorption performance of Cd(II), the electrostatic potential (ESP) of biochars with different surface functional groups (C = O, C–O–C, –OH, and –COOH) and their bond dissociation enthalpy (BDE) with As(V) and Cd(II) were calculated based on density functional theory (DFT). The results showed that –OH was the most effective for As(V) adsorption, and C–O–C was the most effective for Cd(II) adsorption. C = O and –COOH can be used to the simultaneous adsorption of As(V) and Cd(II). Therefore, the surface functional groups of ZVI-CSC can be selectively modified to improve its adsorption performance of As(V) and Cd(II). Graphical
研究领域:
环境科学
·
材料科学
·
化学工程
·
土壤修复
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2021
·Vol. 33
·期 11
·2005587
·
IF 30.849
Ke Wang,Hongfang Du,Song He,Lei Liu,Kai Yang,Jinmeng Sun,Yuhang Liu,Zhuzhu Du,Linghai Xie,Wei Ai,Wei Huang
Layered γ-type iron oxyhydroxide (γ-FeOOH) is a promising material for various applications; however, its sheet-shaped structure often suffers from instability that results in aggregation and leads to inferior performance. Herein, a kinetically controlled hydrolysis strategy is proposed for the scalable synthesis of γ-FeOOH nanosheets arrays (NAs) with enhanced structural stability on diverse substrates at ambient conditions. The underlying mechanisms for the growth of γ-FeOOH NAs associated with their structural evolution are systematically elucidated by alkalinity-controlled synthesis and time-dependent experiments. As a proof-of-concept application, γ-FeOOH NAs are developed as electrocatalysts for the oxygen evolution reaction (OER), where the sample grown on nickel foam (NF) exhibits superior performance of high catalytic current density, small Tafel slope, and exceptional durability, which is among the top level of FeOOH-based electrocatalysts. Density functional theory calculations suggest that γ-NiOOH in situ generated from the electrooxidation of NF would induce charge accumulation on the Fe sites of γ-FeOOH NAs, leading to enhanced OER intermediates adsorption for water splitting. This work affords a new technique to rationally design and synthesize γ-FeOOH NAs for various applications.
研究领域:
材料科学
·
电化学
·
理论计算
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120851
·
IF 7.2
Zhifeng Zhang,Junhao Fu,Jianhua Kang,Wei Sun,Haisheng Han
The core of mineral flotation resides in specific matching between collectors and mineral surfaces. Amid new energy-driven fluorite demand, efficiently separating it from similarly interfaced calcite remains challenging due to non-selective fatty acid collectors. Herein, a novel "crab"-shaped dicarboxylic collector, N-Benzyloxycarbonyl-glutamic acid (ZGA), was synthesized and its flotation performance was evaluated. Single-mineral flotation showed that at a concentration of 2 × 10 −5 mol/L and pH 9, the recovery difference between fluorite and calcite reaches 56.96 %, while the synergistic enhancement of terpineol further boosts fluorite recovery to over 90 %. Surface characterizations confirmed that ZGA undergoes selective adsorption via chemical and electrostatic interactions, which effectively modifies the surface roughness of fluorite and significantly enhances its hydrophobicity. DFT calculations demonstrated the dicarboxylic distance matches alternating Ca 2+ on fluorite (111), enabling stable adsorption with an adsorption energy of −325.256 kJ/mol. Flotation practice yielded improved metrics, with the CaF 2 concentrate grade reaching 96.45 % and recovery increasing by 2.76 %. These findings offer valuable insights for the design of collector selective to fluorite, while facilitating the efficient and clean separation of strategic calcium-containing minerals.
✓ 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）