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ACS Materials Letters · 2023 · IF 11.4

Resolving Molecular Size and Homologues with a Self-Assembled Metal–Organic Framework Photonic Crystal Detector

Xueying Fan,Miao Xu,Weizhe Liu,Aleksandr Kuchmizhak,Lorenzo Pattelli,Yao Li,Hongbo Xu

Traditional environmental photonic sensing based on the balanced reflection of a photonic structure can hardly be applied to distinguish molecular size and homologues, since the refractive index change introduced by these analytes can be too similar to be unambiguously distinguished. Here, a sensing method based on the pore size selectivity and organics adsorption–desorption capacity of self-assembled ZIF-8 photonics crystal is demonstrated, which can tell apart different molecular sizes, homologues, and organics with similar structures and physical properties. Specificity is improved by the inherent relationships between the pore size of ZIF-8 metal–organic frameworks and the associated molecular diffusion rates in the pores, so that the combination of the observed peak shift and recovery time are unique to each analyte. Using this method, selective detection of molecular size is also demonstrated in the case of linear vs cyclic molecules, since only the former can penetrate inside the ZIF-8 pores to induce a large wavelength shift. The reflection peak shift caused by the linear molecules was found to be about 30–40 nm, an order of magnitude larger compared to those for the cyclic molecules. A relationship between the diffusion rate of linear molecules in ZIF-8 pore and the recovery time of photonic crystal reflective peak is further established, linking the recovery time and the linear molecular diffusion coefficient. Finally, different linear molecules are identified by their associated recovery time to detect homologues or organics with similar refractive index.

研究领域: 材料科学 · 环境科学 · 化学传感
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Journal of Materials Chemistry C · 2024 ·Vol. 12 ·期 28 ·10604-10612 · IF 5.7

Tailoring the molecular size of alkylamine modifiers for fabricating efficient and stable inverted CsPbI3 perovskite solar cells

Zhongyu Liu,Hongwei Wang,Haijun Han,Hong Jiang,Ning Liu,Jianwei Wang,Jing Zhang,Tian Cui,Xiaohui Liu

An inorganic perovskite CsPbI3 with a suitable bandgap and excellent optoelectronic properties has attracted tremendous attention as a promising absorber in perovskite solar cells (PSCs). A surface modification strategy of introducing organic molecules with functional groups to treat perovskite films has been proven to be an effective route to achieve high-performance PSC devices. However, the effect of the molecular size of modifiers is almost ignored in surface passivation studies. In this work, three alkylamine modifiers with different molecular sizes were incorporated to post-treat CsPbI3 films to systematically investigate the influence of alkyl chain length on device performance. It was found that the alkylamine treatments can remarkably ameliorate film morphology and interface contact, passivate defects, and increase hydrophobicity, resulting in greatly improved device efficiency and stability. In particular, the CsPbI3 film treated with 1,5-pentanediamine (PDA) with a suitable chain length acquires optimum results owing to its most efficient passivation effect and suppressed nonradiative recombination. Consequently, the inverted PDA-based CsPbI3 PSC exhibits a champion power conversion efficiency (PCE) of 19.52%, outperforming the control device with a PCE of 13.43% and other alkylamine-treated devices. Furthermore, both the unencapsulated PDA-treated CsPbI3 films and PSC devices present considerably enhanced long-term stability. This work highlights the great significance of tailoring the molecular size of interfacial modifiers towards achieving efficient and stable inorganic PSCs.

研究领域: 材料科学 · 光电子学
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MICROPOROUS AND MESOPOROUS MATERIALS · 2015 · IF 3.453

Palladium nanoparticles supported on a two-dimensional layered zeolitic imidazolate framework-L as an efficient size-selective catalyst

Songlin Xue,Hong Jiang,Zhaoxiang Zhong,Ze-Xian Low,Rizhi Chen,Weihong Xing

A new Pd@ZIF-L hybrid catalyst having a unique crosshair-star shape with a size of about 20 μm was synthesized, in which a two-dimensional layered zeolitic imidazolate framework-L (ZIF-L) was used as a support to immobilize palladium nanoparticles via an assembly method. The hybrid catalyst with unique cushion-shaped cavities between layers with a size of 6.64 Å can be used for the diffusion of specific reactants not achievable by other ZIF systems such as ZIF-8. The crystal structure and morphology of Pd@ZIF-L are strongly dependent on the synthesis conditions. Palladium nanoparticles with an average size of 3 nm are homogeneously encapsulated in the ZIF-L crystals. The as-synthesized Pd@ZIF-L catalyst favors the conversion of alkenes with larger molecular sizes, and exhibits excellent molecule-size-selectivity and anti-leaching performance.

CAS / MDL: 100-02-7
研究领域: 材料科学 · 催化化学
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CATALYSIS LETTERS · 2022 ·Vol. 153 ·期 8 ·2504-2516 · IF 2.936

SiO2 Deposition to Regulate Surface Barriers and Its Impact on ZSM-5 Catalyzed Reactions with Distinct Molecular Sizes

Chen Jiaxuan,Hu Shen,Chen Zhuo,Sun Xincheng,Chen Minhao,Chen Tianjiao,Ye Guanghua,Zhou Xinggui

The effects of molecular size on SiO 2 deposition regulated surface barriers and zeolite catalysis are probed, taking n -pentane isomerization and benzene alkylation with ethylene as model reactions. Chemical liquid deposition of SiO 2 on the parent ZSM-5 sample only modifies its external surface slightly and passivates a small proportion of Brønsted acid sites. The apparent diffusivities increase significantly at 363–393K after SiO 2 deposition, indicating SiO 2 on ZSM-5 crystals reduces surface barriers at low temperatures. The conversion for n -pentane isomerization increases by up to 26% after SiO 2 deposition, while the conversion for benzene alkylation decreases by up to 19%. Obviously, the positive effect of SiO 2 deposition can be balanced out by the pore confinement effect at high temperatures, which is stronger for a larger molecule. This work provides a unique understanding of molecular size effects on surface barriers, which should serve to guide the design of zeolite catalysts. Graphical Abstract

CAS / MDL: 16941-12-1
研究领域: 催化化学 · 材料科学
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JOURNAL OF MOLECULAR LIQUIDS · 2018 · IF 4.513

Adsorption of two antibiotics on biochar prepared in air-containing atmosphere: Influence of biochar porosity and molecular size of antibiotics

Chunyan Li,Xiaoxiao Zhu,Hongliang He,Yunxiao Fang,Huaping Dong,Jinhong Lü,Jianfa Li,Yimin Li

The porous biochar was prepared by pyrolysis of wood at 600–800 °C in the air-containing atmosphere, so as to enhance the biochar's capacity for adsorption of antibiotics from water. The analytical results obtained from N 2 adsorption/desorption indicated that air addition in pyrolysis atmosphere improved significantly the biochar's porosity, especially the development of mesopores. The mesoporous biochars showed high adsorption of antibiotics, and the highest adsorption was observed on the A 1/5 C800 biochar prepared at the air/gas ratio of 1/5 and heat treatment temperature (HTT) of 800 °C. The adsorption isotherm data were well fitted to the Langmuir model, and the maximum adsorptions ( Q m ) of tetracycline and sulfadiazine on the A 1/5 C800 sample are 163 and 261 mg/g respectively, which are 18.8 and 52.8 folds of those on the microporous NC800 biochar prepared at the same HTT but in total nitrogen atmosphere. The outstanding performance of mesoporous biochar was linked to the utilization of more inner pore surface for adsorption, which favors the adsorption of smaller-sized sulfadiazine molecules. While the stronger interactions between tetracycline and biochar contributed to the relatively higher adsorption of tetracycline on the microporous biochar. The mesoporous biochar retained most of the adsorption capacity (>50%) in a wide pH range (3.5–10) and with the co-existence of humic acid (10 mg/L). In general, this research provides a simple and green method to enhance the biochar's efficiency as an adsorbent for remediation of water contaminated by antibiotics.

研究领域: 环境科学 · 农业科学
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FUEL · 2022 · IF 8.035

Controllable synthesis of a carbonaceous pitch from molecular dimension by a novel method of chlorination-dechlorination

Jinchang Liu,Yaping Li,Chenyang Shen,Maohong Fan,Qiang Xie,Dingcheng Liang

The carbonaceous pitch derived from coal liquefaction residue was controllably synthesized from the molecular dimension with a novel method, chlorination–dechlorination. The factors affecting the qualities of chlorination–dechlorination derived pitch, including chlorine ratios, were studied. The qualities of the pitches prepared with chlorination–dechlorination and the conventional thermal condensation method are compared. The carbons in the prepared carbonaceous pitch mainly exist in aromatic structures, which are oligomerized to transform dimers and trimers by chlorination–dechlorination. The C/H ratio, average molecular weight, and carbon aromaticity are increased by chlorination–dechlorination. According to the result of the simulation, the hydrogen atoms on the side chain of aromatic compounds are easier to be mono-substituted by chlorine atoms during chlorination, and then the substituting chlorine atoms connect with other hydrogen atoms to form to escape out of the reactor in the formation of hydrogen chloride during dechlorination , making the aromatic compounds oligomerize with each other. Thus, the conclusion that the chlorinated pitch has a more linear and cross-linking molecular structure is demonstrated, which is also confirmed by the results of 13 C NMR. The pitch precursors exhibit better thermal stability and thermochemical property even when the softening point has been raised to around 230 ℃ owing to the linear and cross-linking molecular structure. In addition, the pitches synthesized by the method of chlorination–dechlorination shows a more homogeneous state, while the pitch produced by thermal condensation contains a small number of powdery coke particles, and they also possess more excellent spinnability and appropriate viscosity for the process of melt-spinning. Chlorination–dechlorination can be used to achieve the controllable synthesis of the carbonaceous pitch from the molecular dimension. The properties of derived pitches are better as the addition of chlorine increases.

CAS / MDL: 109-99-9
研究领域: 材料科学 · 化学工程
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JOURNAL OF INCLUSION PHENOMENA AND MACROCYCLIC CHEMISTRY · 2011 ·Vol. 73 ·期 1 ·237-246 · IF 1.22

Effects of several inter-molecular interactions on the inclusion between methyl substituted β-cyclodextrin and some linear macromolecule in supercritical carbon dioxide medium

He J.

In this work, the inclusion between methyl substitute β-cyclodextrin and some linear macromolecule in supercritical carbon dioxide medium was investigated. The contributions from several factors were studied; such as the hydrogen bonding interaction between the host and guest, the hydrogen bonding interaction between the neighborhood cyclodextrin rims threaded on the polymer chain, and the matching between the host cavity and the size of the polymer axis.

研究领域: 化学 · 材料科学 · 药物传递系统
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2025 · IF 5.4

Adsorptive removal of pharmaceutical and personal care products by carbon nanotubes: Insights into the adsorbent pore size and adsorbate size

Huiming Qi,Li Zhang,Mingchao Zhang,Liya Ma,Qiang Gao,Fuzhen Jiang,Delin Qi,Shubo Deng,Wei Wang

Understanding the molecular factors that govern the adsorption of pharmaceutical and personal care products (PPCPs) on carbon nanotubes (CNTs) is essential for designing highly efficient porous adsorbents. We hypothesize that adsorbent pore and adsorbate size matching is the dominant factor controlling the adsorption process. Therefore, this study examined the effects of the molecular size of PPCPs and pore size of CNTs on the adsorption performance using the combination of experiments and molecular dynamics simulations. The results show that the adsorption capacity of unit specific surface area increased with increasing both the molecular size of PPCPs and the pore size of CNTs. In the coexisting system, adsorption capacity declined with decreasing molecular size, showing negative correlation (R²=0.842). This indicates that small PPCPs are more vulnerable to competitive inhibition, whereas larger molecules exhibit stronger resistance to competition and maintain more stable adsorption capacities in complex media. Molecular dynamics simulation revealed that the interaction between CNTs and PPCPs was mainly dominated by van der Waals forces, with larger-sized molecules showing higher binding energy and being more likely to occupy adsorption sites on CNTs. These findings not only reveal the internal relationship between the pore size of sorbents and their adsorption capacity, but also provide an important theoretical basis and practical guidance for optimizing PPCPs removal strategies.

CAS / MDL: 210169-05-4
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MICROPOROUS AND MESOPOROUS MATERIALS · 2023 · IF 5.2

Phosphorus promotion on hydrothermal stability of ZSM-5 by P precursors with different molecular sizes

Ne Ni,Xiuzhi Gao,Enhui Xing,Yuan Zhu,Jianqiang Liu,Mudi Xin,Ying Ouyang,Yibin Luo,Xingtian Shu

The promotional effects of phosphorous modification on ZSM-5 zeolites by phosphorus oxyacids (H 4 P 2 O 7 , H 3 PO 4 , H 3 PO 3 , and H 3 PO 2 ) with different molecular sizes were investigated with catalytic cracking of n -tetradecane as the probe reaction. It was verified that the diffusion of P precursor molecules into ZSM-5 channels was important to prevent aggregation of P species for better stabilization on tetra-coordinated framework aluminum . Meanwhile, the P–Al interaction was proposed based on results of 27 Al, 31 P, and 29 Si MAS NMR. With H 3 PO 2 as the P precursor, easy diffusion into ZSM-5 channels contributed to less formation of polyphosphates, homogeneous distribution of P species, better reserved crystallinity, microporous area and acidic sites for improving cracking performance of n -tetradecane.

研究领域: 化学工程 · 催化 · 材料科学
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Polymers · 2022 ·Vol. 14 ·期 21 ·4682 · IF 4.967

Development and Evaluation of a Novel Sulfonated Phenol–Formaldehyde Resin with High Dispersion Stability

Xianxing Meng,Likun Wang,Hongwei Wang,Fang Zhang,Taying Su,Kunmu Cheng

Sulfonated phenol–formaldehyde (SPF) resin used as a cross-linker for petroleum reservoir conformance control was synthesized under alkaline conditions. The reaction process of SPF resin was evaluated by measuring the solution’s viscosity with respect to phenol–formaldehyde (PF) resin. The molecular structure of SPF resin was characterized by both FTIR and HPLC–MS/MS. The influence of the formaldehyde/phenol molar ratio (F/P) and the sodium formaldehyde sulfoxylate/phenol molar ratio (S/P) on the properties of SPF were analyzed in terms of the storage time, coagulation value, molecular size, and zeta potential. The results indicate that the presence of formaldehyde sodium bisulfite could slow down condensation reaction. Phenol rings were connected by methylene bridges in the position of o–p, and sulfonated SPF resin molecules all had one sulfonate group on the oligomer structure. The storage time decreased from 87 to 6 days, and the zeta potential decreased from −3.02 to −7.70 mV with the increase in F/P (1.2–2.0). Meanwhile, the sedimentation value and the diameter increased from 3.291 × 104to 5.045 × 104mg/L and from 2.7 to 5.3 nm, respectively. Sulfonation could significantly increase the storage time and dispersion stability. With the increase in S/P (0.1–0.35), the storage time increased from 15 to 86 days, the sedimentation value increased from 1.927 × 104to 5.269 × 104mg/L, and the diameter decreased from 6.3 to 3.0 nm. This paper can present new ideas for improving the storage stability and salt tolerance of phenol–formaldehyde resin and further improving the range of its applications, which has essential reference significance.Keywords:phenol–formaldehyde resin;sulfonation;characterization;HPLC–MS/MS

CAS / MDL: 108-95-2 50-00-0
研究领域: 化学工程 · 石油工程 · 材料科学
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