Reaction Chemistry & Engineering
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2026
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IF 2.9
mengting li,Yongrui Wang,Yibin Luo,Xingtian Shu
Carbonyl compounds were transformed to oximes by transoximation reaction with HY zeolite under solvent-free condition through reaction-distillation coupling process. First, single factor experiments were conducted to investigate the effects of temperature, feed molar ratio, catalyst loading and vacuum degree on the yield of cyclododecanone oxime (CDOX); Secondly, the Plackett-Burman screening and Box-Behnken response surface methodology were further utilized to deeply optimize the process parameters, and the optimal conditions were obtained, temperature of 90 °C, cyclododecanone (CDON)/ cyclohexanone oxime (CHO) molar ratio of 1.4:1, catalyst loading of 1.6 g, and vacuum degree of 240 mbar. Under these conditions, the yield of CDOX can reach 99.45%, which is similar to the predicted value of 99.76% by response surface methodology. Also, the zeolite with large pore size and Brønsted acidity are essential for good catalytic performance, and the HY-5 show the highest yield of CDOX under reaction-distillation process. The catalyst can be recovered and reused several times. The mechanism was proposed.
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JOURNAL OF MEMBRANE SCIENCE
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2026
·
IF 8.8
Jianfa Liu,Yang Liu,Haonan Luo,Hui-Fang Wang,Zhenggong Wang,Jian Jin,Zheng Niu,J. Liu,Y. Liu,H. Luo,H. Wang,Z. Wang,J. Jin,Z. Niu
Hybrid membranes combine the excellent processability of polymer with the superior permeability and selectivity of porous fillers, demonstrating exceptional separation performance. However, interfacial incompatibility remains a fundamental challenge in such systems. Herein, we report a strategy incluced by molecular adsorption sites to mitigate interfacial incompatibility issues. MOF has been proved as a efficient ethyne adsorbents and applied in the separation of C 2 H 2 /C 2 H 4 . Its inorganic adsorption units, which exhibit a high affinity for ethyne, were uniformly high-quality dispersed within a polymer matrix to enable efficient C 2 H 2 /C 2 H 4 separation. The optimized hybrid membrane exhibits a 249% enhancement in C 2 H 2 /C 2 H 4 perm-selectivity compared to the pristine polymer membrane, while maintaining competitive C 2 H 2 permeability. This performance surpasses that of most reported hybrid membranes incorporating conventional fillers. Remarkably, the membranes maintain stable operation under varying pressures and prolonged testing durations. This study presents a facile yet effective strategy for fabricating high-performance gas separation membranes through the dispersion of molecular adsorption sites, opening new avenues for advanced alkyne/olefin separation.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Jiayan Liang,Hongyu Zhang,Jian Zhang,Xuwen Wang,Yangming Wang,Hao Bai,Yi Rong,Kaifeng Lin,Debin Xia,Yulin Yang
Pomegranate-like B@(NH 4 ) 2 SiF 6 @LiClO 4 enables ordered boron combustion. • Sequential fluorination–oxidation suppresses oxide re-passivation. • The optimized composite shows faster ignition and stronger flames. Boron suffers from severely limited combustion efficiency due to the kinetic barrier imposed by its native oxide layer. In this work, a pomegranate-inspired B@(NH 4 ) 2 SiF 6 @LiClO 4 composite was fabricated via a two-step solvent evaporation-induced self-assembly strategy, enabling highly dispersed reactive domains and intimate interfacial contact. The distinctive pomegranate-inspired architecture establishes particle-level spatial organization of the reactive components, while their distinct thermal activation windows provide the temporal basis for a proposed spatiotemporally coordinated reaction pathway. TG-DSC and TG-FTIR analyses reveal that fluorine-containing species derived from (NH 4 ) 2 SiF 6 evolve prior to LiClO 4 melting and major oxidizer release, supporting a proposed sequential fluorination-oxidation pathway involving early fluorine-mediated interfacial modification followed by oxidizer-driven boron oxidation. At an optimal (NH 4 ) 2 SiF 6 content of 10 wt%, the ignition delay and combustion duration are reduced by 15.47% and 68.22%, respectively, compared with B@LiClO 4 , demonstrating substantially improved ignition and combustion kinetics. Combined structural, thermal, and combustion analyses support the proposed spatiotemporally coordinated fluorination-oxidation pathway arising from the coupling of particle-level organization and temporally separated thermal events. This work provides a particle-level interfacial engineering strategy for coordinating fluorination and oxidation in high-performance boron-based energetic systems. A pomegranate-inspired B@(NH₄)₂SiF₆@LiClO₄ enables spatiotemporally ordered boron combustion by coupling fluorination and oxidation reactions within confined nanoscale domains. Sequential interfacial activation and molten-salt-mediated oxygen transport promote continuous reaction propagation and suppress oxide re-passivation, resulting in faster ignition, intensified flame propagation, and more efficient energy release compared with conventional physically mixed systems. Download: Download high-res image (176KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
·
2026
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IF 13.2
Bo Xue,Chuanruo Yang,Ruihan Wang,Ting Wang,Pengtao Guo,Gan Li,Dahuan Liu
The development of high-performance porous adsorbents for the efficient recovery of C 2 H 2 from C 2 H 2 /CO 2 mixtures holds significant industrial value. However, the separation of C 2 H 2 /CO 2 remains highly challenging due to their similarities in physicochemical properties. To tackle this key obstacle, we utilize a feasible fluorinated anion modulation strategy to optimize the negative electrostatic microenvironment of ultra-microporous MOFs for the preferential recognition of C 2 H 2 . Notably, compared to SIFSIX-dpds-Cu, TIFSIX-dpds-Cu exhibits higher C 2 H 2 uptake (81.0 cm 3 g −1 ) and C 2 H 2 /CO 2 selectivity (43.2). Furthermore, the C 2 H 2 packing density of TIFSIX-dpds-Cu can reach 522 g L −1 , outperforming most previously reported materials. Density functional theory calculations and in situ FT-IR spectra collaboratively demonstrate that the multiple C−H···F and C−H···C interactions are formed between TIFSIX-dpds-Cu and C 2 H 2 molecules. With the synergistic drive of multiple hydrogen bonds and van der Waals forces within the confined pores, ultimately achieving efficient C 2 H 2 purification. Breakthrough experiments reveal that TIFSIX-dpds-Cu achieves complete separation of C 2 H 2 /CO 2 mixtures, yielding the high-purity C 2 H 2 productivity (≥99.5 %) of 58.42 cm 3 g −1 in a single adsorption−desorption cycle.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Hui Zhang,Qiang Fu,Hongyun Qin,Xia Chen,Qicheng Zhang,Zixu Dong,Haoyuan Li,Shoudong Wang,Ming Wang
Hydrogen recovery from ammonia purge gas is a desirable method to relieve the pressure of increasing demand for hydrogen. Metal-organic frameworks (MOFs) are promising adsorbents for the separation of the H 2 –N 2 mixture. However, the separation of the H 2 –N 2 mixture using MOFs remains challenging due to the lack of adsorptive mechanism. Herein, the adsorption mechanism of the H 2 –N 2 mixture in SIFSIX-2-Cu-i has been systematically investigated with the method of a combination of excess adsorption experiments, molecular simulations , and DFT calculations. In the Grand Canonical Monte Carlo (GCMC) simulations, the polarizable force field was first applied to the adsorption of pure H 2 or N 2 and H 2 –N 2 mixture in SIFSIX-2-Cu-i. Ab Initio Molecular Dynamics (AIMD) was performed to investigate the distribution of the guest molecules in the pores of SIFSIX-2-Cu-i. Finally, Density functional theory (DFT) calculations were performed to predict the transfer of charge between MOF and guest molecules. Results revealed two binding sites of H 2 or N 2 in SIFSIX-2-Cu-i. A relatively high thermodynamic adsorption selectivity for N 2 over H 2 has been observed in SIFSIX-2-Cu-i. Furthermore, SIFSIX-2-Cu-i also exhibits a greater affinity with N 2 than with H 2 , which is probably because of the stronger induction interactions between F2 atoms and N 2 molecules. These findings are of significance to guide the design of the new highly selective adsorbents for the separation of H 2 /N 2 .
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AICHE JOURNAL
·
2023
·Vol. 69
·期 7
·e18091
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IF 3.7
Siheng Qian,Jing Hu,Xiaobing Wang,Lifeng Yang,Xian Suo,Zhengbao Wang,Xili Cui,Huabin Xing
Separation and purification of light hydrocarbons have been the critical processes for producing basic chemicals and polymers in petrochemical industry. Adsorbents with high performance are highly demanded for the separation of light hydrocarbons. However, the adsorbents filling in the packed bed when evaluated will inevitably induce reduced performance and increased pressure drop that considerably impede their application. Herein, mixed-matrix fiber adsorbents with anion-pillared hybrid microporous materials (SIFSIX-2-Cu-i) embedded within poly (ether sulfone) (PES) are constructed to enable an energy-efficient propylene/propyne separation. Owing to the sufficient binding sites and abundant channels for selective gas transfer, the fiber adsorbents achieve high C 3 H 4 uptake capacity of 0.963 mmol g −1 in the propylene/propyne (99/1) mixture breakthrough experiments. Moreover, fiber adsorbents exhibit good tolerance toward high gas velocity and show distinctively low pressure drop, which will be advantageous in industrial applications. This work provides a strategy for fabricating high-performance mixed-matrix fiber adsorbents.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Jun Ma,Jiahe Zhang,Ye Yuan,Yunqi Zhou,Shenzhen Cong,Guangyu Xing,Jixiao Wang,Zhi Wang
N 2 /CH 4 separation membranes based on N 2 preferential permeation can effectively reduce the recompression cost of CH 4 gas and show promising application prospects in the field of natural gas purification. However, the performance of N 2 /CH 4 separation membranes still needs to be improved. Here, we report a kind of mixed matrix membranes (MMMs) for N 2 /CH 4 separation via using HOF-21 as nanofiller and 6FDA-DAM polyimide as polymer matrix . In this work, the effects of HOF-21 loading, feed side pressure and temperature based on membrane performance were explored, and finally performance variation of the MMMs with operation time was tested. The incorporated HOF-21 nanoparticles with the most probable pore size of about 3.6 Å can significantly increase the diffusion rate of smaller N 2 molecules and enhance the N 2 /CH 4 diffusivity selectivity of the membrane. In addition, compared with polyimide, HOF-21 exhibits almost the same dynamic adsorption of N 2 and CH 4 , which can weaken the solubility of CH 4 and enhance the N 2 /CH 4 solubility selectivity of the membrane. When feed gas pressure was 0.2 MPa, the optimum membrane performance was achieved at the HOF-21 loading of 7 wt%, with N 2 permeance of 5.13 GPU and N 2 /CH 4 (50/50, vol%) selectivity of 20.52 at 298.15 K. Compared with N 2 permeation and N 2 /CH 4 selectivity of the 6FDA-DAM/PAN membrane, the MMMs increased by 67% and 54%, respectively, possessing potential applications in the field of N 2 removal in CH 4 purification.
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FUEL
·
2022
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IF 8.035
Jianguo Zhuang,Siyan Yan,Peng Zhang,Xinhui Liu,Yitao Zhao,Yijun Yu,Yuchen Wang,Qichao Zhao,Haidan Wu,Xuedong Zhu,Fan Yang
Nickel (Ni) supported on MCM-41 zeolite as hydrogenation catalysts have been widely applied in various reactions, however, the synergism between Ni and the support remains obscure. To prepare more efficient catalysts and reveal the metal-support interaction, MCM-41 zeolite was modified with ammonium hexafluorosilicate (AHFS) before Ni loading. Results show that fluoride ions could selectively convert the vicinal silanols into isolated silanols on MCM-41 surface, which weakens the interactions between Ni precursors and the SiO 2 supports. Over the modified MCM-41 zeolites, the attenuated interaction results in the agglomeration of NiO particles that is more easily to be reduced, rather than the formation of nickel phyllosilicate which is extraordinarily difficult towards reduction. The easily-reduced Ni particles provided more adsorption sites for C C bond instead of C O bond, and the adsorption strength was also regulated. Therefore, the AHFS modified catalyst demonstrated a notable enhancement in hydrogenation of maleic anhydride (MA) into succinic anhydride (SA), presenting 98.4 % MA conversion and 99.8 % SA selectivity at 90 °C under 3.0 MPa H 2 . Moreover, the optimum catalyst was recycled for 5 runs to analyze the deactivation mechanism, it was found out that the loss of activities stems from the leaching of large Ni particles. Overall, our work shed light on the metal-support interactions for Ni/MCM-41 catalyst, determining the vicinal hydroxyl groups were responsible for the state of Ni species, which is helpful for the rational design of other hydrogenation catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Yifei Song,Tian Ke,Jin Shen,Jinjian Li,Xiaoqian Zhu,Liu Yang,Zhiguo Zhang,Zongbi Bao,Qilong Ren,Qiwei Yang
The deep removal of trace acetylene from ethylene is crucial for producing polymer-grade ethylene. Cutting-edge powder-form porous adsorbents represented by layered two-dimensional fluorinated MOFs have shown attractive acetylene/ethylene separation ability, but few studies have landed on the shaping of MOFs essential for subsequent industrialization, especially on the layered materials lacking rigid chemical bonds. Here, we report three novel layered MOF pellets based on wet granulation via polyhydroxy binders, which not only achieved efficient acetylene/ethylene separation but also exhibited excellent mechanical properties and stability. The result of the scanning electron microscope indicated that a solid bridge was formed in ZUL-300@HPC, enhancing the adhesion between the crystal particles while minimizing the pore blockage, which affords exceptional 0.01 bar acetylene uptake of 2.60 mmol/g along with acetylene/ethylene (1/99, v/v ) selectivity of 111 at 298 K. Breakthrough experiments showed that ZUL-300@HPC achieved record 99.9999% ethylene productivity of 150.01 mmol/g for acetylene/ethylene (1/99, v/v ) and maintained excellent alkyne removal ability even for 11-component complex mixture.
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APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Guoqiang Hou,Tingjun Fu,Xin Li,Qian Ma,Zhong Li
HZSM-5 catalysts with abundant silanol nests were fabricated by removing framework Al, which effectively promoted the selective alkylation of toluene with methanol by inhibiting the deep alkylation of aromatics to heavy aromatics and the conversion of methanol to light hydrocarbons. Correspondingly, the alkylation efficiency reached 65.3% at a toluene conversion of 31.3% over dealuminated HZSM-5, higher than the 55.2% efficiency and 28.0% conversion of parent zeolites, respectively. In situ DRIFTS and single-factor experimental clarified that toluene adsorption was enhanced and methanol to hydrocarbons was inhibited with the presence of silanol nests. Additionally, by increasing the crystal size of HZSM-5 with silanol nests from 2 to 5 µm, para-xylene selectivity was increased from 36.1% to 65.5% because of the enhanced diffusion barrier . The finding of the positive effect of the silanol nests on toluene alkylation can provide a solid fundamental basis for the rational design of catalysts.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Pengyu Zhao,Zhiguang Li,Yue Zhang,Debao Cui,Qingchun Guo,Zhipeng Dong,Guodong Qi,Jun Xu,Feng Deng
One-step direct hydroxylation of aromatics is an atom-economic way for phenols production. Ti-containing MFI zeolite is considered to be one of the most potential catalysts for hydroxylation of aromatics to phenols under mild condition with aqueous H 2 O 2 as the oxidant. However, the products are often a mixture of mono- or multi-phenols. Designing TS-1 zeolite catalyst with high yield and selectivity to the target phenols remains a challenging task. Here TS-1 zeolites are prepared by direct hydrothermal and post-synthetic methods. Multiple spectroscopic characterizations show that the crystallinity and Ti-Lewis acid sites (Ti-LASs) distribution of TS-1 zeolite can be controlled by the synthetic approach. The structure-activity relationship of TS-1 zeolite is established in the catalytic hydroxylation of anisole, revealing that Ti-LASs concentration determines the conversion of anisole, while both the crystallinity and Ti-LASs distribution significantly influence the selectivity to the desired product para -hydroxyanisole.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Lifang Cui,Benlin He,Yang Ding,Jingwei Zhu,Xinpeng Yao,Junjie Ti,Haiyan Chen,Yanyan Duan,Qunwei Tang
The interfacial modification has been considered as an effective strategy to build high-efficient and stable perovskite solar cells (PSCs) by reducing the loss of charge recombination and energy at electron transport layers (ETLs)/perovskite interface. Here, a multifunctional inorganic salt of ammonium silicofluoride (ASF) is utilized as an interfacial modifier to incorporate at TiO 2 ETLs/CsPbBr 3 perovskite interface, which decreases the surface oxygen vacancy defects of TiO 2 by its bonding with silicofluoride anion and adjusts the energy level of TiO 2 by dipole effect to minimize interfacial band difference, resulting in a promotion of electrons extraction and a reduction of energy loss. Simultaneously, the ASF modification affords a more hydrophobic TiO 2 substrate for the constitution of perovskite film with larger crystal and passivates anion defects of CsPbBr 3 film via the formation of hydrogen bonds between the H atom in ammonium cations and Br atom in perovskite, which dramatically inhibits the recombination of carriers. Finally, the all-inorganic CsPbBr 3 PSCs based on the ASF-modified TiO 2 ETL achieves a remarkable higher power conversion efficiency of 10.08%, compared to 6.84% efficiency of the control device. In addition, the long-term tolerance of the device without encapsulation towards high humidity and high temperature is significantly enhanced after interface modifying with ASF.
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