PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2022
·Vol. 24
·期 28
·16973-16978
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IF 3.945
Fengyi Zhou,Ruifen Shi,Yingxiong Wang,Zhimin Xue,Baolong Zhang,Tiancheng Mu
Acidic deep eutectic solvents (ADESs) have been utilized in various applications. Clearly, it is crucial to obtain acidity information that could reveal the relationship with performance. However, appropriate methods for measuring acidity are limited. Herein, we developed two promising approaches (without additional solvents) to identify and characterize both Lewis and Brønsted acidities by applying acetonitrile as an infrared probe and trimethylphosphine oxide (TMPO) as a nuclear magnetic resonance (NMR) probe. The acetonitrile IR approach is suitable for measuring the acidity of Lewis ADESs by monitoring the peak of ν(CN) around 2300 cm−1, and the 31P-TMPO NMR approach could identify and scale both Lewis and Brønsted acidities precisely. Moreover, a perfect linear relationship between the IR shift of ν(CN) and the effective charge density of metal cations was established, which provides a better understanding of Lewis acidity. In short, this study not only offers two efficient acidity measurement methods but also provides a molecular basis for optimizing the performance of ADESs in applications.
研究领域:
化学
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材料科学
✓ 已验证
DOI
高影响因子
DALTON TRANSACTIONS
·
2024
·
IF 3.5
Zhengyan Wang,Chenhao Yuan,Dong Yang,Mifen Cui,Jihai Tang,Zhuxiu Zhang,Xu Qiao
It is of great significance to develop catalysts for the degradation of hexachlorobenzene from the industrial thermal process. In this paper, formic acid was used as a modulator to generate defect sites in Ce/Zr-UiO-66 with intrinsic Brønsted acidity. The defective formate ligands were removed through methanol–water vapor treatment to expose additional open metal sites with Lewis acidity. The intrinsic Brønsted acid sites of the resulting Ce/Zr-UiO-66-FA-P achieved a hexachlorobenzene degradation efficiency of 99.5% at 250 °C. The generated Lewis acid sites facilitated the C–C cleavage of degradation intermediates. More than 95.0% of the final products were CO2/CO, coupled with chlorinated alkanes/alkenes, which outperformed other benchmark metal oxide catalysts. The Ce/Zr-UiO-66-FA-P catalyst maintained its catalytic activity in the model industrial flue gas and humid environment. The degradation pathway of hexachlorobenzene was tracked using in situ FT-IR spectra.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Wenxia Wang,Guohe Huang,Chunjiang An,Xiaying Xin,Yan Zhang,Xia Liu
From the viewpoint of sustainability, biomass adsorbent has a high potential in pollution control and there is an emerging interest to investigate the behaviors of pollutants at the interface between biomass adsorbent and solution. This study investigated the performance of cetyltrimethylammonium bromide surfactant-modified flax shives (MFS) for removal of anionic azo dyes from aqueous solution. The equilibrium and kinetic analysis for the adsorption of Acid Orange 7 (AO-7), Acid Red 18 (AR-18) and Acid Black 1 (AB-1) on MFS were conducted. The surface of MFS was characterized by synchrotron infrared and SEM analysis. The absorbed amount of three anionic azo dyes varied with the change of adsorbent dosage, pH and ionic strength. The adsorption isotherm data well fit to the Langmuir model. The adsorption process followed the pseudo-second-order kinetics and the liquid film diffusion models. Thermodynamic studies indicated that the adsorption of three anionic azo dyes was spontaneous. The adsorption of AR-18 and AB-1 onto MFS was endothermic while the adsorption of AO-7 was exothermic. The results can help better understand the behaviors of organic pollutants at biomass adsorbent-water interface. They also present the potential of using MFS as a suitable adsorbent for the removal of anionic azo dyes from wastewater.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Zhibo Yang,Liang Zhu,Lin Chen
Core-shell structured NH 2 -functionalized UiO-66 magnetic composites (γ-Fe 2 O 3 @C@UiO-66-NH 2 ) were fabricated via a simple, facile and green approach to investigate their adsorption behaviors towards different organic dyes (methylene blue, malachite green , acid fuchsin and acid orange II). Different characterization methods containing XRD , TEM , EDXA , FTIR, BET and XPS were used to indicate that the as-prepared γ-Fe 2 O 3 @C@UiO-66-NH 2 material exhibited core-shell structure and excellent surface performance. Adsorption experiments showed that γ-Fe 2 O 3 @C@UiO-66-NH 2 could selectively adsorb anionic dyes and effectively separate the mixture, which might be mainly ascribed to the negatively-charged anionic dyes as opposite to the positively-charged Zr metal sites in γ-Fe 2 O 3 @C@UiO-66-NH 2 . The kinetics and adsorption isotherm of acid orange II and acid fuchsin adsorption in γ-Fe 2 O 3 @C@UiO-66-NH 2 were also investigated. For acid orange II and acid fuchsin, the maximum adsorption capacity obtained from the Langmuir isotherm model was 48.12 mg/g and 31.54 mg/g, respectively. Moreover, γ-Fe 2 O 3 @C@UiO-66-NH 2 exhibited good structural stability and reusability, which suggesting that γ-Fe 2 O 3 @C@ UiO-66-NH 2 as an easy-prepared adsorbent material exhibited great application potential in the selective removal of dyes from water systems.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2018
·
IF 4.521
Xuan Zhang,Rui Zhang,Xianghai Meng,Haiyan Liu,Zhichang Liu,Hao Ma,Chunming Xu,Peter A.A. Klusener
The deactivation mechanism and the activity recovery approach of composite ionic liquid (CIL), a kind of acidic chloroaluminate ionic liquids (ILs) modified with CuCl for the in 2013 successfully commercialized catalysis of isobutane alkylation are being discussed in this paper. CIL showed catalytic activity only in the presence of both Brønsted and Lewis acids. CIL deactivation was caused by the loss of Brønsted acidity and/or Lewis acidity. Brønsted acidity decreased by the loss of trace amount of formed chlorohydrocarbons with the outflowing alkylate. Lewis acidity was deactivated mainly due to the complexation of the formed acid soluble oil (ASO) with the CIL anions. Brønsted acidity was maintained by the continuous addition of hydrogen chloride (HCl) or tert -butyl chloride, and Lewis activity was recovered by AlCl 3 addition. However, Brønsted acidity could not be recovered when Lewis acidity was lost and was thus dependent on Lewis acidity. Furthermore, ASO interacted with active components of CIL, causing the loss of copper via precipitation of CuCl which is the major contributor to the high selectivity. Therefore, CuCl was added simultaneously with AlCl 3 to maintain the high selectivity of alkylate.
研究领域:
催化化学
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石油化工
✓ 已验证
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-13
·
IF 16.6
Chen Shiyi,Zhang Shishi,Guo Lei,Pan Lun,Shi Chengxiang,Zhang Xiangwen,Huang Zhen-Feng,Yang Guidong,Zou Ji-Jun
Surface reconstruction generates real active species in electrochemical conditions; rational regulating reconstruction in a targeted manner is the key for constructing highly active catalyst. Herein, we use the high-valence Mo modulated orthorhombic Pr 3 Ir 1− x Mo x O 7 as model to activate lattice oxygen and cations, achieving directional and accelerated surface reconstruction to produce self-terminated Ir‒O bri ‒Mo (O bri represents the bridge oxygen) active species that is highly active for acidic water oxidation. The doped Mo not only contributes to accelerated surface reconstruction due to optimized Ir‒O covalency and more prone dissolution of Pr, but also affords the improved durability resulted from Mo-buffered charge compensation, thereby preventing fierce Ir dissolution and excessive lattice oxygen loss. As such, Ir‒O bri ‒Mo species could be directionally generated, in which the strong Brønsted acidity of O bri induced by remaining Mo assists with the facilitated deprotonation of oxo intermediates, following bridging-oxygen-assisted deprotonation pathway. Consequently, the optimal catalyst exhibits the best activity with an overpotential of 259 mV to reach 10 mA cm geo −2 , 50 mV lower than undoped counterpart, and shows improved stability for over 200 h. This work provides a strategy of directional surface reconstruction to constructing strong Brønsted acid sites in IrO x species, demonstrating the perspective of targeted electrocatalyst fabrication under in situ realistic reaction conditions.
研究领域:
电化学
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材料科学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
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2022
·
IF 5.089
Guangbo Xia,Zhiwei Zhou,Juan Qin,Binbin He,Yangyang Liu,Peiyong Sun,Wenliang Wu
In this paper, a modified facile one-pot AcHE method was adopted to prepare the nickel nanoparticles embedded into the tungsten and niobium metal oxides with binuclear acidities. Their physical and chemical properties were characterized by XRD, liquid N 2 sorption, Py-IR, NH 3 -TPD, Raman, H 2 -TPR, XPS and SEM-EDX and TEM techniques, and their catalytic performances were investigated in the hydrogenolysis of glycerol. The characterization results showed that both nickel nanoparticles can be uniformly doped into the Ni-Nb x W 10-x samples with ordered mesoporous structures and strong interaction between tungsten and niobium species would be formed resulting in the promotion of acidity amount and intensity. The 10 Ni-Nb 3 W 7 sample by synergistic effect has higher catalytic performance in the hydrogenolysis of glycerol than other samples owing to the larger acidities with appropriate ratio of Brønsted to Lewis acidity, whose 1, 3-PDO yield of 28.3% and the molar ratio of 1, 3-PDO to 1, 2-PDO of 2.13 would be obtained. The correlations between the ratio of Brønsted to Lewis acidity and the molar ratio of 1, 3-PDO to 1, 2-PDO and Brønsted acidity and 1, 3-PDO yield can be concluded as y = 2.608x-1.502 (R 2 =0.9831) and y = 1.035x-31.579 (R 2 =0.9730), respectively. Compared to the 10 Ni/Nb 3 W 7 sample prepared by impregnation method, the 10 Ni-Nb 3 W 7 sample shows good stability with slight decrease, where the glycerol conversion of 63.2% and 1,3-PDO selectivity of 42.1% can be obtained even though after repeated use for 6 times. The catalytic performance of 10 Ni-Nb 3 W 7 sample was also higher than other previously reported nickel-based catalysts, which can further prove a valuable reference for the preparation of effective catalysts in the glycerol hydrogenolysis with high selective production for 1, 3-PDO.
研究领域:
催化
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化学工程
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材料科学
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环境化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Daqian Liu,Zuohai Liu,Min Huang,Taoyuan Xiu,Yun Wang,Zhirong Liu
A novel type of modified pyrolytic carbon (TOPO@PyC) was successfully prepared through incorporating tri-n-octyl phosphine oxide (TOPO). The adsorption behavior of TOPO@PyC for Th (IV) under strongly acidic conditions was investigated. The TOPO@PyC exhibited rapid Th(IV) adsorption rate with equilibrium time of 40 min. In 0.1–8 mol/l HNO 3 , the Th(IV) adsorption capacity reached between 43 and 50 mg/g. The adsorption kinetics and adsorption process of TOPO@PyC for Th(IV) can be well explained through the pseudo-second-order kinetic and Langmuir isothermal adsorption model. The temperature exhibited only a minor influence on Th(IV) adsorption capacity. The microstructure and adsorption mechanism of TOPO@PyC was characterized and elucidated through various techniques including SEM-EDS, BET, TGA, FT-IR, XPS and DFT calculations. By coordinating with O atom on TOPO, Th(IV) was successfully complexed on TOPO@PyC in a ratio of 1:3. Furthermore, TOPO@PyC manifested good thermal stability and acid resistance. After five times, the Th(IV) adsorption and desorption efficiency of TOPO@PyC still exceeded 95 %. Additionally, TOPO@PyC exhibited stronger selectivity towards Th(IV) from mixed solutions. Remarkably, it recovered over 90 % of thorium and uranium from the leachate of tantalum slag. Consequently, TOPO@PyC holds considerable promise in the treatment of strongly acidic wastewater containing thorium and uranium.
研究领域:
环境科学
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材料科学
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核化学
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吸附技术
✓ 已验证
产品关联
DOI
高影响因子
BIOMASS & BIOENERGY
·
2017
·
IF 3.219
Haian Xia,Hong Hu,Siquan Xu,Kehao Xiao,Songlin Zuo
A series of Fe/β zeolite catalysts with various Fe/Al ratios were prepared by liquid ion-exchanged method and were characterized by N 2 adsorption, XRD , UV–Vis DRS, EPR , NH 3 -TPD, and FTIR of pyridine adsorption techniques. The catalysts were used to catalyze the transformation of glucose into 5-hydorxymethyfural (HMF) in a biphasic reaction system under mild reaction conditions. The Fe/β catalysts with Lewis acidic Fe sites is able to effectively improve the HMF yield compared to H-β zeolite under identical reaction conditions, which is ascribed to the enhanced isomerization activity of glucose-to-fructose by Lewis acidic Fe species. Moreover, the Fe/Al ratio had a remarkable impact on the conversion of glucose and the yield of HMF, indicating that the synergetic effect of Lewis and Brønsted acid sites is critical to achieving high HMF yield. Under optimal reaction conditions, Fe/β-0.06 catalyst afforded 61% HMF yield at glucose conversion of 95% after the reaction of 90 min at 120 °C, which is one of the most effective catalysts for the conversion of glucose into HMF in a biphasic medium up to now. Furthermore, extra-framework isolated Fe species bound to the framework Al sites, are most likely the active sites for the isomerization of glucose-to-fructose in the conversion of glucose. The catalysts were very stable and could be reused at least five runs without significant loss in the catalytic activity .
研究领域:
催化化学
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生物质转化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Xile Tian,Fancheng Meng,Xianglan Zhang,Yongchao Wang,Yahui Liu,Jian Zhang,Shuai Zhao,Desheng Chen,Lina Wang,Tao Qi
The high-acidity vanadium-containing solution contains high concentrations of iron and aluminum with pH around 0.5, the ketoxime extractant with the active ingredient of 2-hydroxy-5-nonylacetophenone oxime (HNAO, HL) was proposed to extract vanadium from the solution. Under the phase ratio (O/A) of 1:2, HNAO concentration of 0.542 mol·L −1 at 25 °C for 10 min, 99.06% of vanadium was extracted after a three-stage countercurrent extraction, while the extraction of impurities was less than 1%, with the separation coefficients of vanadium from iron and aluminum were 137050 and 43197, respectively. The antioxidant properties of the extractant were studied. At 25 °C, the extractant basically did not undergo oxidative degradation. Besides, about 91.2% of the loaded vanadium was effectively stripped using 2.5 mol·L −1 Na 2 CO 3 solution. The extraction mechanism of vanadium was investigated through the slope analysis method, the spectral characterizations and density functional theory calculations. It has been observed that VO 2 + substitutes the H atom on the phenolic hydroxyl and coordinates with the N atom on the oxime and the O atom on the phenolic hydroxyl to form of a six-membered ring, and the extraction complexes were determined to be VO 2 (H 2 O)L and VO 2 L.
研究领域:
化学工程
·
冶金工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Jiaojiao Liu,Huifang Zhang,Ningyue Lu,Xiaoliang Yan,Binbin Fan,Ruifeng Li
A series of mesoporous ZSM-5-x (x = Si/Al molar ratio) supports, possessing various Si/Al ratios, were prepared without using the secondary templates, and the influences of acidity of ZSM-5-x on catalytic performance of Pt/HZSM-5-x samples prepared by the conventional wetness impregnation in naphthalene hydrogenation were investigated. The results show that decreasing Si/Al ratios of mesoporous ZSM-5 supports promotes the dispersion of the supported Pt species, and the catalytic efficiencies of Pt/HZSM-5-x samples for naphthalene hydrogenation depend on the integrated effects of the Pt dispersion, the acidity, and the mesoporous structure of ZSM-5 supports. This work provides the detailed influences of acidity of mesoporous ZSM-5 on catalytic performance of supported Pt catalysts in naphthalene hydrogenation.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
MINERALS ENGINEERING
·
2025
·
IF 5
Guosai Jiang,Ziyuan Liu,Yao Xue,Xiaoguang Zhang,Zhe Tan,Yufeng Wu,De’an Pan
Acid sludge, a hazardous waste from lead (Pb)-zinc (Zn) smelting process, typically contains selenium (Se) and mercury (Hg), both of which have high economic value. Recovering these elements contributes to resource reuse and environmental pollution reduction. However, designing an efficient recovery process for Se and Hg is a key technical challenge in the disposal of Se/Hg-containing acid sludge. In this study, we proposed a highly efficient wet recovery method for Se and Hg, which involves mechanical ball milling pretreatment of acid sludge followed by an oxidizing acid leaching process. Through single-factor experiment and response surface methodology (RSM) optimization, the leaching efficiencies of 99.69 % for Se and 99.64 % for Hg within 11 min were achieved. The thermodynamics and kinetics of the leaching process were thoroughly investigated to elucidate the conversion mechanisms of Se and Hg and the rate-controlling step from chemical reaction. Notably, the mechanical pretreatment significantly enhanced the leaching efficiencies of Se and Hg in less time compared to direct leaching process, owing to the reduced particle size, more scattered distribution and decreased crystallinity. This research offers valuable insights into the efficient leaching of Se and Hg species from acid sludge, potentially addressing the issues of resource wastage and environmental pollution from large stockpiles of acid sludge.
研究领域:
环境科学
·
冶金工程
·
资源回收
✓ 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）