Small
·
2023
·Vol. 19
·期 49
·2304644
·
IF 13.3
Ping Lu,Zhaoyang Qi,Jie Chen,Changshen Ye,Ting Qiu
High-efficiency adsorption of aromatic sulfur-containing compounds from liquid hydrocarbon fuels over metal-organic frameworks (MOFs) is challenging because of inert metal sites. A new method, the Ce-enhanced modulation of MOFs’ microenvironment, is proposed to modulate the –COO···Cu(II)– coordination microenvironment of Hong Kong University of Science and Technology (HKUST-1) using Ce(III) as a molecular scalpel for fabricating abundant high-efficiency Cu(I) and Cu-coordination-unsaturated sites and improving the pore structures around adsorptive sites. The optimal CH-250 thus exhibits adsorptive capacities for 20.2, 28.0, and 58.3 mg S g –1 of thiophene, benzo-thiophene, and dibenzothiophene, respectively, which are superior to most reported MOFs, zeolites, and nanoporous carbons. The constructed Cu(I) sites show stronger affinity for dibenzothiophene (−0.86 eV) than the initial Cu(II) (−0.74 eV) for out-of-plane adsorption. Further, they are far stronger in-plane adsorption interactions in DBT/CH-250 (−0.90 eV) than those in DBT/HKUST-1 (−0.37 eV). Thus, molecular engineering for modulating the coordination microenvironment of MOFs shows great potential for adsorption desulfurization.
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Small
·
2023
·Vol. 19
·期 47
·2303885
·
IF 13.3
Yuhao Li,Minchao Qin,Yunfan Wang,Shiang Li,Zhaotong Qin,Sai-Wing Tsang,Chun-Jen Su,Yubin Ke,Xinhui Lu
The black-to-yellow phase transition in perovskite quantum dots (QDs) is more complex than in bulk perovskites, regarding the role of surface energy. Here, with the assistance of in situ grazing-incidence wide-angle and small-angle X-ray scattering (GIWAXS/GISAXS), distinct phase behaviors of cesium lead iodide (CsPbI 3 ) QD films under two different temperature profiles–instant heating-up (IHU) and slow heating-up (SHU) is investigated. The IHU process can cause the phase transition from black phase to yellow phase, while under the SHU process, the majority remains in black phase. Detailed studies and structural refinement analysis reveal that the phase transition is triggered by the removal of surface ligands, which switches the energy landscape. The lattice symmetry determines the transition rate and the coexistence black-to-yellow phase ratio. The SHU process allows longer relaxation time for a more ordered QD packing, which helps sustain the lattice symmetry and stabilizes the black phase. Therefore, one can use the lattice symmetry as a general index to monitor the CsPbI 3 QD phase transition and finetune the coexistence black-to-yellow phase ratio for niche applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Ping Lu,Zhenhua Sun,Zhaoyang Qi,Jie Chen,Changshen Ye,Ting Qiu
Aromatic sulfur-containing compounds are main constraints for liquid hydrocarbon fuels upgrading furtherly. Efficient adsorption of the sulfur-containing compounds by metal–organic frameworks (MOFs) is still a challenging because of single and inert adsorptive sites. We herein represent a new strategy, constructing dinuclear-crossed secondary building units (SBUs) in MOFs, for generating Cu(I) and Cu-coordination-unsaturated sites (Cu-CUS). The high-performance Cu(I) and Cu-CUS sites are controllable by modulating the organic ligands molar ratio of 1,3,5-benzenetricarboxylic acid / 4-pyrazolecarboxylic acid (BTC/PyC). The optimal Cu-BTC/PyC-1/1 with abundant Cu(I), Cu-CUS, and large surface areas thus exhibits dibenzothiophene adsorption capacity of 51.11 mg S/g. The result shows 100.3% and 47.8% increased adsorption capacity comparison with that of sole Cu-PyC (25.52 mg S/g) and Cu-BTC (34.57 mg S/g) respectively. The high adsorption capacity originates from electron-transfer mechanism between empty-electron-orbital Cu(I)/Cu-CUS and electron-enriched aromatic sulfur-containing compounds. The molecular engineering for building multiple adsorptive sites by dinuclear-crossed SBUs strategy exhibits great promising for MOFs-based adsorbents design.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Yong Liu,Xinghua Zhang,Lungang Chen,Jianguo Liu,Qi Zhang,Longlong Ma
This study explores the efficacy of a cost-effective Cu-ZnO-Al 2 O 3 catalyst for one-pot hydrodeoxygenation of guaiacol into hydrocarbons. Notably, complete conversion of guaiacol was achieved, yielding a 99.6% hydrocarbon over the robust Cu(6)Zn(3)Al(1) catalyst under the conditions of 4 MPa H 2 , 300 °C, and 8 h with a catalyst/guaiacol ratio of 0.5 g/1.0 g. In-depth catalyst characterizations unveiled the presence of oxygen vacancies within the ZnO surface layer, acting as pivotal active sites that facilitated the hydrodeoxygenation of guaiacol. Furthermore, Density Functional Theory (DFT) calculations were employed to evaluate several potential active sites, revealing that the oxygen vacancy of ZnO on the Cu surface played a crucial role. This vacancy enhanced the adsorption of intermediate cyclohexanol and markedly reduced the energy barrier for the rate-limiting step. This comprehensive investigation sheds light on the catalytic pathway and offers insights into designing efficient and sustainable biofuel production processes.
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Journal of Physical Chemistry C
·
2023
·
IF 3.7
Shifeng Ke,Boyu Peng,Ruihan Wu,Jie Ren,Yujie Zhao,Qiuyue Sheng,Hanying Li
Surface tension is a crucial factor in the crystallization of organic semiconductors from solutions. However, the current conclusions based on experimental results have been primarily empirical and qualitative, making it hard to distinguish the role of surface tension from other solvent properties. In this study, we employed both molecular dynamics simulations and experiments to investigate crystal nuclei behavior at the liquid-air interface. Through equilibrium simulations and free energy calculations, we quantitatively described the moving behavior of nuclei in various solvents, relating it to an interfacial transition, in terms of interfacial tension. Nuclei tend to remain at the liquid-air interface if the surface tension of solvents is higher than the surface free energy of nuclei but sink into the bulk liquid otherwise. Furthermore, aside from governing the nuclei behavior, surface tension also determines the crystallization location, as confirmed through growing crystals on substrates with Ag nanowires as impediments. By clarifying the role of surface tension, our research contributes to the knowledge of solution crystallization of organic semiconductors and the establishment of a framework for tuning processing conditions and crystal morphology for future studies.
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FUEL
·
2023
·
IF 7.4
Qipeng Ma,Weiyao Zhu,Zhiyong Song,Jie Zhang,Bingbing Li,Wengang Bu,Bin Pan
Interfacial tension (IFT) and wettability are two key parameters determining pore-scale oil/water distributions and reservoir-scale hydrocarbon production performances. However, how ionic liquid (IL, a green, stable, and efficient chemical) will manipulate IFT and wettability for EOR in sandstone reservoirs has not been sufficiently investigated yet, and the underlying mechanisms at the micro-level are still unknown. In this study, the influences of two typical ILs at various concentrations (i.e., 0.01, 0.1, 1, and 5 mmol/L) on oil–water IFT and alpha-quartz (α-quartz) wettability were investigated. This study shows that low concentrations of ILs can greatly reduce alkane-water IFT, and gemini IL has higher interfacial activity than mono-cationic IL, which is due to the fact that gemini IL with longer alkyl chains is more likely to form conglomerates at lower concentrations. Both the advancing and receding contact angles increase continuously with concentration in ILs solution, which can be given responsibility for the decrease in IFT and the solid–liquid interaction resulting in an increased capacity of alkane droplets to migrate on the α-quartz surface. Additionally, the molecular dynamic simulations examined the micro-wetting process and interaction energy of the IL-alkane-quartz system, and revealed that ILs can effectively reduce interaction energy between octane droplets and α-quartz surface. These insights have promising applications to enhanced oil recovery and oil contamination removal at subsurface.
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Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 29
·9996-10003
·
IF 6.4
Xudong Jin,Yanqin Miao,Jianhua Dong,Jingkun Wang,Qiqing Lu,Min Zhao,Bingshe Xu,Junjie Guo
The room-temperature triple-ligand surface engineering strategy demonstrates the advantages of low-cost and high-yield in the preparation of perovskite nanocrystals (PeNCs). However, conventional octanoic acid (OTAc) with short-chain length shows weak binding energy with Pb2+, resulting in higher trap states density and inferior stability of PeNCs. Here, we prepare CsPbBr3 PeNCs capped with 4-dodecylbenzene sulfonic acid (DBSA) to maintain lower trap states density, a higher photoluminescence quantum yield of 91%, larger yield production and better stability compared to OTAc-PeNCs. Consequently, DBSA-PeNCs based PeLEDs with a peak external quantum efficiency (EQE) of 8.95% and a maximum luminance of 4452 cd m−2 are achieved, which constitute about 3-fold and 2-fold enhancement compared to OTAc-PeNCs based PeLEDs, respectively. These results demonstrate that introducing DBSA as the surface ligand is an effective way to realize highly efficient PeLEDs.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Yue Liu,Dianlong Ge,Jijuan Zhou,Yajing Chu,Xiangxue Zheng,Li Ke,Pan Li,Yan Lu,Xue Zou,Lei Xia,Yawei Liu,Chaoqun Huang,Chengyin Shen,Yannan Chu
The investigation of volatile organic compounds (VOCs) in human metabolites has been a topic of interest as it holds the potential for the development of non-invasive technologies to screen for organ lesions in vivo. However, it remains unclear whether VOCs differ among healthy organs. Consequently, a study was conducted to analyze VOCs in ex vivo organ tissues obtained from 16 Wistar rats, comprising 12 different organs. The VOCs released from each organ tissue were detected by the headspace-solid phase microextraction-gas chromatography-mass spectrometry technique. In the untargeted analysis of 147 chromatographic peaks, the differential volatiles of rat organs were explored based on the Mann–Whitney U test and fold change (FC > 2.0) compared with other organs. It was found that there were differential VOCs in seven organs. A discussion on the possible metabolic pathways and related biomarkers of organ differential VOCs was conducted. Based on the orthogonal partial least squares discriminant analysis and receiver operating characteristic curve, we found that differential VOCs in the liver, cecum, spleen, and kidney can be used as the unique identification of the corresponding organ. In this study, differential VOCs of organs in rats were systematically reported for the first time. Profiles of VOCs produced by healthy organs can serve as a reference or baseline that may indicate the presence of disease or abnormalities in the organ’s function. Differential VOCs can be used as the fingerprint of organs, and future integration with metabolic research may contribute to the development of healthcare.
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ChemistrySelect
·
2023
·Vol. 8
·期 29
·e202300694
·
IF 2.1
Haitao Meng,Xuecong Pan,Xuemei Li,Haijun Meng,Shouzhu Li
Graphical An efficient and durable hydrophilic SiO 2 fiber membrane was designed by a template-free strategy combined with electrostatic spinning technology. The material can perform separation of oily wastewater under gravity-only conditions and has demonstrated high separation performance for effective separation of oil-water mixtures and oil-in-water (O/W) emulsions. The discharge of oily wastewater seriously affects human health and the sustainable development of the ecological environment. Therefore, developing oil-water separation materials capable of removing organic pollutants is imperative. In this study, we report the preparation of a SiO 2 nanofiber membrane based on tetraethyl orthosilicate (TEOS) using a template-free strategy combined with electrostatic spinning technology. The prepared SiO 2 nanofiber membrane was characterized using SEM, EDX, FT-IR, AFM, XRD, CA, and TG techniques. The prepared SiO 2 nanofiber membranes exhibit excellent hydrophilicity (WCA=0°) in air and oleophobicity (UWOCA=136°) underwater, with excellent anti-pollution properties for gravity-driven oil-water separation. The SiO 2 nanofiber membrane can effectively separate different kinds of oil-water mixtures with high water flux (4420 L m −2 h −1 ) and excellent separation efficiency (99.1 %), with a flux loss of 5.65 % after ten cycles, indicating excellent cycling stability. In addition, it can also be used to separate various oil-in-water emulsions stabilized by surfactants with a separation flux higher than 2079 L m −2 h −1 and a separation efficiency maintained at more than 97 %. During the separation of 150 mL lotion, the membrane was seriously scaled due to long-term pollution. Simple water washing could not restore the membrane flux, and the irreversible scaling rate was 50.74 %, which seriously affected the continuous separation. However, due to the excellent thermal stability of SiO 2 nanofiber membranes, oil contaminated membranes can be heated and regenerated, resulting in a flux recovery rate of nearly 100 %. Overall, this material has a wide range of potential applications in environmental protection, especially in the treatment of oily wastewater, due to its simple fabrication method, high flux, and superb oil resistance and recyclability.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hongyu Niu,Xing-Bao Wang,Jingjie Luo,Jiaxin Liu,Chuang Li,Wen-Ying Li,Changhai Liang
Desulfurization plays a critical role in refining crude oil to produce fuel and the manufacture of fine chemicals. However, its low efficiency becomes a great challenge for the present desulfurization if only the C-S cleavage is considered a promising approach to reducing hydrogen consumption under atmospheric pressure. Accordingly, we investigate the critical factors necessary to achieve high C-S cleavage of dibenzothiophenes under mild conditions of 0.1 MPa and H 2 /oil = 100. The mechanism of reactive adsorption desulfurization of dibenzothiophenes with or without steric hindrance at atmospheric pressure on Pt/ZnO is proposed by studying the adsorption model of active metal sites, the Pt efficiency in C-S cleavage influenced by the steric hindrance and the structural evolution of Pt active centers in the presence of sulfur adsorption/deposition. Based on both experimental and DFT results, we report C-S cleavage of dibenzothiophenes with (TOF = 15 h −1 ) or without steric hindrance (TOF = 128 h −1 ) that can be highly efficiently fractured (99.9%) by the interface between PtS x and ZnO . This work has great practical significance for developing atmospheric industrial adsorbents for ultra-deep reactive adsorption desulfurization.
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Crystals
·
2022
·Vol. 12
·期 9
·1286
·
IF 2.67
Yu Yan,Qi Zhang,Zhijian Wang,Qifeng Du,Ruitao Tang,Xiaoyu Wang
The performance of monochromatic perovskite light-emitting diodes (PeLEDs) has undergone rapid development in recent years, while white PeLEDs are still in their infancy. The tandem devices prepared by connecting light-emitting units of different colors with intermediate connectors comprise one of the promising approaches for realizing white light emission. The intermediate connector plays a crucial role in determining the effectiveness of the light-emitting units. In this work, all-perovskite-based white LEDs are assembled by employing sky-blue (490 nm) and red (690 nm) perovskite emitters as active layers. With mixed p-type and n-type organic charge transport materials as the intermediate connector, the highest external quantum efficiency (EQE) of the device was 1.4%, the electroluminescence (EL) peak position of the blue light part was shifted to 512 nm, and the red light part was shifted to 673 nm. In contrast, with organic and inorganic charge transport materials as the intermediate connector, the devices exhibited better charge generation/injection capabilities and a record EQE of 8.5%. The EL peak position of the device prepared from the stored film was not shifted, implying that the organic/inorganic layer effectively suppresses halide migration. Our work paves the way for highly efficient tandem white PeLEDs.Keywords:tandem;white perovskite light-emitting diodes;organic/inorganic intermediate connector
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JOURNAL OF CHROMATOGRAPHY A
·
2022
·
IF 4.601
Ziqi Sun,Meiling Qi
This work presents the investigation of a novel CO 2 -based poly(ether-carbonate) copolymer, namely poly(propylene ether-carbonate)diol (PPCD), for gas chromatographic (GC) analyses. The PPCD column exhibited column efficiency of 4000 plates/m determined by naphthalene at 120 ℃ with the retention factor 6.23. Its separation performance was investigated by adopting a wide variety of analytes and isomers, including the isomer mixtures of alkanes, substituted benzene isomers with diverse groups, phenols and anilines, and the mixtures of organic solvents of high volatility, aliphatic amines and N-heterocycles. As a result, the PPCD column displayed distinctly higher resolving capability than the commercial columns described herein and achieved high column inertness towards acidic/basic analytes without involving any deactivation procedure. Additionally, it displayed excellent separation repeatability and reproducibility with the relative standard deviation (RSD) values less than 0.01% for within-day and in the range of 0.26% – 0.36% for between-day and 3.0% – 4.1% for between-column ( n = 4). Further, the PPCD column (30 m) was used to GC–MS analysis of the lemongrass essential oil and resolved more components well than the indicated commercial columns, evidencing its outstanding separation performance for analyses of complex samples. Up to date, the CO 2 -based poly(ether-carbonate) copolymers are not reported in the field of chromatography. This work demonstrates their promising future as a new type of selective and inert stationary phases for practical GC analyses.
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