FUEL
·
2023
·
IF 7.4
Xianbin Huang,Zhiwen Dai,Chao Zhang,Kaihe Lv,Xu Meng,Ren Wang,Shaine Muhammadali Lalji,Muhammad Arqam Khan
Wellbore instability in complex shale formations is a major technical problem that threatens drilling safety and efficiency. In this paper, a hydrophobic cationic polyamine shale inhibitor (HCPA) was prepared by introducing a hydrophobic group in the molecular structure of an amine-based shale inhibitor having a branched structure. The shale inhibition performance of HCPA and the amine-based shale inhibitor without the hydrophobic group (CPA) was investigated. The hydration inhibition mechanism of HCPA was studied by experiments of zeta potential, particle size, contact angle, thermogravimetric analysis (TGA), X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), etc. The evaluation results show that HCPA had a better performance than CPA in terms of inhibition of hydration swelling, hydration dispersion and mud making, which indicates that the hydrophobic group is beneficial to improve the inhibition ability of the amine-based shale inhibitor. The mechanism study shows that there is no hydrogen bond between HCPA and clay. The adsorption on the clay surface is mainly driven by electrostatic interaction, which reduces the repulsion of the electric double layer and thus inhibits the osmotic swelling of clay. HCPA could increase the water contact angle of the rock from 36.6° to 133° at a concentration 0.5%, beneficial to reduce surface free energy. The bentonite modified by HCPA had a lower weight loss of at 200 °C than bentonite modified by CPA according to TGA test, and the interlayer spacing of HCPA-modified bentonite was reduced compared with that of the unmodified bentonite, indicating that the ability of bentonite to adsorb water molecules is reduced after the introduction of hydrophobic groups, beneficial to inhibit the crystalline swelling of clays. In addition, HCPA can reduce the imbibition capacity of rocks by reducing the surface tension of water. Therefore, the concept of introducing hydrophobic groups in the molecular structure proposed herein could provide an avenue to develop high-performance shale inhibitors.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Haiqing Chang,Naiming Liu,Fangshu Qu,Xiaoxiang Cheng,Zhiwei Zhou,Ying Liang,Ying Yu,Heng Liang
Membrane fouling is the Achilles heel of membrane-based technologies. Severe membrane fouling occurs when a single microfiltration (MF) membrane is used to treat shale gas produced water (SGPW). Activated by Fe(II), sodium percarbonate (SPC) oxidation combined with aluminum sulfate coagulation was used in this study to evaluate the alleviation of MF fouling for the treatment of two typical SGPW samples with different water quality characteristics from Sichuan Basin. Results showed that pre-treated by oxidation and coagulation, more than 88% of turbidity, 11%–23% of UV 254 , and 11%-36% of DOC were removed. With the increase in SPC dosage, there was a decrease in fluorescent organics, primarily reducing soluble microbial by-product-like components by up to 37.0% for sample 1 and aromatic protein and soluble microbial by-product-like components by up to 66.7% and 71.2% for sample 2, respectively. Compared to low normalized fluxes (2%-6%) for the raw SGPW, 61%-79% of normalized fluxes were obtained using the combination of 10 mmol/L SPC and 0.9 mmol/L Al 2 (SO 4 ) 3 ·18H 2 O. There was a general evolution of complete blocking to intermediate blocking or cake layer filtration for membrane fouling mechanism. Scanning electron microscopy observation, deposited foulants on membrane surface and Fourier transform infrared analysis further confirmed the superior performance of the combination of SPC oxidation and coagulation. Correlation analysis showed that UV 254 ( R 2 = 0.79–0.95) played the most significant role in membrane fouling. Overall, this combined pretreatment process showed a great potential in MF membrane fouling control during the treatment of SGPW.
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高影响因子
FUEL
·
2023
·
IF 7.4
Jiale Gu,Huan Li,Wencai Peng,Di Zhu,Jiajia Chen,Shengjie Luo,Siming Liu,Wenxiang Zhao,Youqing Wu,Sheng Huang,Shiyong Wu
The hydrogenation properties of dibenzyl ether (an oxygenated model compound of lignite) via the water–gas shift reaction (WGSR) were studied in a subcritical CO-H 2 O system. The result showed during the hydrogenation process, the C-O bond was broken, and the fragments of dibenzyl ether were stabilized by the hydrogen generated by WGSR, generating benzene, toluene, benzyl alcohol and benzaldehyde. The presence of excess water inhibited the hydrogen transfer, largely reducing the conversion of dibenzyl ether. However, the inhibition effect was substantially reduced when the reaction environment reached the critical temperature and subcritical pressure of water. The hydrogen and deuterium generated by H 2 O and D 2 O via WGSR were utilized to label and analyze the hydrogenation position of the product, respectively. The results showed that the hydrogen generated by WGSR was added to the methylene after the break of dibenzyl ether, and this hydrogen appeared on the benzene ring structure via hydrogen transfer. The bond dissociation energy and energy required for the hydrogenation process of dibenzyl ether under aqueous condition were calculated by utilizing density functional theory (DFT). First, hydrides (H − ) are formed by the WGSR under alkaline conditions. Then, the formation energy (140.81 kJ/mol) of hydrides and the energy (15.54 kJ/mol) of hydrides attacking the dibenzyl ether to form the transition state were lower than the bond dissociation energy (259.26 kJ/mol) of the dibenzyl ether. That is, the hydrogenation of dibenzyl ether via WGSR prefers to be a nucleophilic reaction rather than a pyrolysis reaction. In the coal liquefaction process, the hydrides produced by WGSR under the catalysis of alkali is conducive to the hydrocracking of oxygen containing functional groups.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xinxin Li,Linchuan Cong,Yupeng Wu,Nan Lin,Fangbing Liu,Deyuan Xin,Fuyu Han,Jin Yang,Weitong Chen,Haibo Lin
Electrochemical methods for catalytic furfural conversion have drawn significant interest in both academic and industrial research communities. Paired electrocatalytic conversion has been identified as a promising strategy for reducing energy consumption and promoting carbon neutrality. To optimize product distribution and conversion efficiency, we have developed a divergent paired electrochemical upgrading approach for furfural in acidic environments, with a focus on prioritizing strong gas evolution reactions and product transformations. The high electrocatalytic activity of CuSn/CuF@Cu prepared by electrodeposition can effectively inhibit the hydrogen evolution. The performance of the electrocatalysts and the pathways of electrocatalytic hydrogenation (ECH) of furfural to 2-methylfuran (MF) were investigated by combination of experiments and the density functional theory (DFT) calculations. A stable Ti/PbO 2 electrode with high oxygen evolution overpotential was prepared for anodic electrocatalytic oxidation (ECO) and the product transformation route was described. The conversion of furfural to maleic acid (MA) and MF in acidic environment was successfully achieved. In the paired electrosynthesis system, the electrons generated from anodic ECO of furfural are utilized in valuable and controllable cathodic ECH. It significantly and continuously reduces the power cost associated with renewable energy sources and further promotes the development of biomass electrochemical conversion.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Yingshu Liu,Haiyang Tao,Xiong Yang,Xiaoyong Wu,Jinjuan Li,Chuanzhao Zhang,Ralph T. Yang,Ziyi Li
Adsorption is a promising technology for capturing nitrogen oxides (NO x ) from humid flue gases , for which as the preferred NO x adsorbent, zeolite with an appropriate silica to alumina (Si/Al) ratio provides the key step for success in practical applications. In this work, the effects of Si/Al ratio, temperature, relative humidity (RH), and feed gas (NO x -H 2 O(g)–CO 2 –O 2 -N 2 ) compositions on NO x sorption behavior on HZSM-5 zeolites were systematically investigated, based on a series of characterizations, fixed-bed adsorption and temperature programmed desorption (TPD) tests. The low-silica HZSM-5(25) showed the best performance (326.6 μmol/g and 39.2 μmol/g at dry and 90%RH) as compared to others with higher Si/Al ratios at each RH, in which the roll-up effect was positively correlated with the Si/Al ratios and humidity. O 2 enhanced NO x adsorption and reached an optimal adsorption capacity at the concentration of 14%, while CO 2 had little effect on NO x adsorption. The decrease in temperature increased NO x adsorption capacity on HZSM-5(25), benefitting from NO 2 physisorption as well as satisfactory NO oxidation within the active adsorbent structure. The facile thermal desorption of NO x and significant NO–NO 2 conversion on HZSM-5(25) was exhibited by bimodal TPD peaks at 343–353K and 533–543K respective for NO and NO 2 , in contrast to those on Silicalite-1. A potential “water-resistant” strategy via the enhancement of NO x adsorption competitiveness was revealed, providing a theoretical guideline for NO x adsorbent screening in industrial applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Shanshan Shang,Chao Yang,Mingzhe Sun,Zeyu Tao,Aamir Hanif,Qinfen Gu,Jin Shang
CO 2 capture from large point sources is indispensable for achieving 1.5 degree target as long as fossil fuels are still in use. Selective adsorption of CO 2 from flue gas constitutes a promising CO 2 capture technology, thanks to the development of numerous fascinating solid adsorbents in the past three decades. However, very few adsorbents can retain their required performance in the presence of moisture which is unfortunately always the case in reality. In this study, we elevated the CO 2 adsorption and separation performance of a water-stable aluminum-based porphyrin metal-organic frameworks (Al-PMOF) by inserting transition metals as adsorption sites. Compared with the pristine Al-PMOF and other four transition metals (TMs) incorporated PMOFs (Al-PMOF(M)), the Co-inserted Al-PMOF (Al-PMOF(Co)) exhibited the highest CO 2 adsorption capacity (3.32 mmol/g) and highest CO 2 /N 2 and CO 2 /CH 4 selectivity (87 and 20, respectively) at 273 K and 1.0 bar. After three consecutive cyclic moisture treatments, the CO 2 adsorption capacity of Al-PMOF(Co) remained almost unchanged. More importantly, the dynamic binary CO 2 /N 2 breakthrough adsorption of Al-PMOF(Co) exhibited negligible differences in CO 2 adsorption capacities between dry and wet flue gas conditions, suggesting that TMs incorporated Al-PMOF possess excellent moisture-resistant properties. Mechanistic studies using the combined in situ synchrotron infrared spectroscopic and powder X-ray diffraction together with density functional theory calculations unambiguously revealed the inserted metals are the dominant CO 2 adsorption sites. This study materializes the rational design of efficient adsorbents for CO 2 capture and contributes to mitigating climate change.
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高影响因子
Polymers
·
2022
·Vol. 14
·期 18
·3888
·
IF 4.967
Yingying Zhong,Qibei Bao,Lifeng Yuan,Jiawen Liu,Yan Cai,Xianfeng Chen
Microplastics are harmful to both marine life and humans. Herein, a pyrolysis–gas chromatography–mass spectrometry (Py-GC/MS) technique for the detection of microplastics in aquatic shellfish is demonstrated. The organic matter in aquatic shellfish was removed by alkali digestion. Subsequently, using hexafluoroisopropanol as the extraction solvent, the extraction method was optimized. The influence of the digestion process on the nature of microplastics was investigated by analyzing the samples before and after the alkali treatment via infrared spectrometry, laser particle sizing, and scanning electron microscopy. Spiked recovery experiments and an analysis of actual samples were performed using PA6 and PA66 as analytes. A quantitative analysis of the characteristic ion fragment produced by high-temperature cracking was performed after chromatographic separation and mass spectrometry identification. The linear range of this method for PA6 and PA66 was 2–64 μg. The limits of detection of PA6 and PA66 were 0.2 and 0.6 μg, while the limits of quantitation were 0.6 and 2.0 μg, respectively. Recovery ranged from 74.4 to 101.62%, with a precision of 4.53–7.56%. The results suggest that the Py-GC/MS technique is suitable for the analysis and detection of trace microplastics in aquatic shellfish.Keywords:microplastics;alkali digestion;pyrolysis–gas chromatography–mass spectrometry;aquatic shellfish;nylon
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PubMed
高影响因子
Materials Chemistry Frontiers
·
2022
·Vol. 6
·期 21
·3205-3212
·
IF 8.683
Jiangting Zhao,Zhuo Xiong,Junyi Wang,Yaqin Qiu,Yongchun Zhao,Pengfei Liu,Junying Zhang
In this study, a 1D/2D ZnO nanofiber/graphdiyne oxide heterojunction was designed for photocatalytic CO2 reduction, and the difference between graphdiyne and graphdiyne oxide was investigated as co-catalysts. The ZGDO heterostructure has strong reactant adsorption capacity due to the enlarged specific surface area and abundant hydrophilic oxygen-containing functional groups. DFT calculations, EPR, and in situ XPS further verified the S-scheme charge transfer mechanism in ZGDO. In contrast, the abilities of GD to adsorb CO2 and enhance light absorption are not as good as those of GDO, and the band structure of GD is not conducive to the formation of a favorable electric field drive at the interface with ZnO. The CO yield of ZGDO with only 3% GDO was up to 34.9 μmol h−1 g−1 in the gas–phase photocatalytic reduction of CO2, which was 4.4, 24, and 1.5 times that of ZnO, GDO, and ZnO/GD, respectively. This work opens new possibilities for the application of new non-metallic photocatalysts in the photoreduction of CO2.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Tao Yan,Jianhua Yang,Jinming Lu,Liang Zhou,Yan Zhang,Gaohong He
Due to the poor heterogeneous nucleation properties of MOFs crystal on ceramic substrates resulting from the absence of interaction of MOFs with support substrate surface, it is usually difficult to prepare well-intergrown MOF membranes on substrate by simple in situ growth. In this work, a novel synthesis strategy was used to prepare defect-free ZIF-8 membranes on α-Al 2 O 3 supports by depositing gold particles modified with 2-mercaptoimidazole which creates pseudo-surfaces to bridge the metal centers with support. The end groups of the 2-mercaptoimidazole guides the heterogeneous nuclei to the support surface as homologous-like ligands. Furthermore, investigation of the metal sources revealed that the ZIF-8 membranes prepared with Zn(OAc) 2 as the zinc source possessed more continuous and well-intergrown ZIF-8 membranes with a thickness of about 1 μm compared to other zinc sources. The results of gas separation performance show that the optimized ZIF-8 membranes possess high hydrogen permeance and thermal stability. The gas separation selectivity for binary H 2 /CH 4 mixture reached 20.8 at 150 °C and 1 bar, with a high H 2 permeance of about 6.15 × 10 −7 mol m −2 s −1 Pa −1 , which is promising for hydrogen separation and purification. Moreover, free-organic solvents and room temperature growth by our strategy dramatically reduces the difficulty of preparation and environmental destruction, thus offering a new avenue to prepare MOFs membrane with good separation performance.
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高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 48
·25453-25462
·
IF 14.511
Shaoyuan Yu,Jingshi Dong,He Wang,Sirui Li,Hang Zhu,Tianye Yang
In this study, we have successfully fabricated high-performance trimethylamine (TMA) sensors. Defect-engineering (DE) strategy in which two organic ligands, i.e., dicarboxylate and tricarboxylate coordinated with Zn2+ ions, simultaneously, was adopted to obtain MOF-derived ZnO nanoclusters with tunable surface oxygen vacancies after the annealing process. The coordinate competition is expected to introduce more coordinate unsaturated metal sites (CUSs) in MOF materials and thus introduce more oxygen vacancies in MOF-derived materials. Results of gas sensing tests indicate that the dual ligand sensor (DL4) exhibits optimal TMA sensing performance including a high response value of 270.1, excellent selectivity, and good stability to 20 ppm TMA at a low operating temperature of 140 °C. Results of comprehensive characterization experiments including XPS, UV-vis spectra, PL spectra, and EPR indicate that the extraordinary TMA-sensing performance of the sensor can be attributed to abundant doubly positive oxygen vacancies on the ZnO nanocluster surface. The first-principles calculations including the TMA adsorption energy of the ZnO surface and the corresponding differential charge density were calculated using the software VASP (Vienna Ab initio Simulation Package), which further proved that the surface oxygen vacancy is beneficial to TMA sensing performance improvement. Furthermore, the TMA sensing mechanism is also discussed. The DE MOF-derived preparation strategy is a facile and effective method for designing high-performance metal oxide semiconductor gas sensing materials with tunable surface oxygen vacancies.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Youzhi Yang,Shuang Li,Di Liu,Siyuan Guo,Zhijun Liang,Kaikai Ba,Yanhong Lin,Tengfeng Xie
So far, for photoelectric metal oxide semiconductor gas sensors, it is a huge bottleneck to achieve high response performance and low detection limit of formaldehyde at room temperature. This work introduced the synthesis of cauliflower-like graphene-modified In-doped ZnO (GR/In-ZnO) composites via a facile one-pot method with a large comparative surface area for low-concentration formaldehyde sensing at room temperature. GR/In-ZnO-300 showed the highest response to 10 ppm formaldehyde, up to 1891%, which was 12 times that of In-ZnO-300. In addition, the theoretical detection limit of GR/In-ZnO-300 was as low as 13 ppb, and the response at this concentration was 137%. Through the characterization of Surface Photovoltage (SPV), Transient Photovoltage (TPV), Surface Photocurrent (SPC), X-ray Photoelectron Spectroscopy (XPS), and nitrogen gas adsorption isotherms , good formaldehyde sensing performance of GR/In-ZnO-300 was attributed to the excellent separation and transmission capacity of photogenerated carriers, the high specific surface area (109.2 m 2 /g), and abundant oxygen defects on the surface. This work provides a feasible strategy for the design of low-concentration formaldehyde sensing materials with a rapid response at room temperature.
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高影响因子
Materials Today Chemistry
·
2022
·
IF 7.613
X. Liu,J. Song,B. Yin,T. Jiang,H. Pang,L. Yang,S. Wu
Ascorbic acid (AA) is a critical nutrition and chemical for humans, due to its crucial role in metabolic processes and medical treatments. It is necessary to develop a simple and rapid method for real-time tracking AA level in the body. In this work, we fabricated a powerless, gas-permeable, flexible and transparent AA biosensor based on carbon micromesh electrode (CME). The AA biosensor worked without an external power supply and exhibited excellent performances, including high transmittance (>95%), wide detection range (1 μM–1 mM), low limit of detection (10 nM), good selectivity and long-term storage stability (30 days). In addition, we integrated a pH-sensing electrode to correct the AA analysis. A layer of polyaniline (PANI) film was electrodeposited on the carbon micromesh as pH-sensing electrode that had an average sensitivity of 58.1 mV/pH with a high correlation coefficient ( R 2 = 0.997) within the physiological range of human body fluids (pH 4.0–8.7). To verify the availability of the CME in practical application, the Ag/C electrode was used as reference electrode to fabricate the integrated dual-functional biosensors for artificial tears detection. The CME-based biosensors showed good sensitivity, selectivity and correlation coefficient, indicating its excellent practicability towards wearable electronics.
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