AICHE JOURNAL
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2026
·
IF 4.4
Yirong Wang,Qin Sun,Junbo Li,Tiantian Liu,Xiaohua Li,Liangzhi Yu,Sen Wang,Prasert Reubroycharoen,Lizhi Wu,Yu Tang,Li Tan
Propylene is a key chemical. Propane dehydrogenation (PDH) over non-noble cobalt catalysts suffers rapid deactivation from sintering and coking. Herein, we report a core–shell catalyst (1.0Co/BEA@ x Si) with a mesoporous silica shell on Co-impregnated dealuminated Beta zeolite. The silica shell enhances Co dispersion and modulates Co reduction: it promotes the formation of active tetrahedral Co 2+ sites from Co 3 O 4 while suppressing over-reduction to metallic Co 0 . The optimized 1.0Co/BEA@1.0Si maintains ~99% propylene selectivity and achieves a formation rate of 71.0 gC 3 H 6 ·g Co −1 ·h −1 after 980 min, far surpassing uncoated 1.0Co/BEA and most reported Co-based PDH catalysts. In situ and post-reaction analyses show the shell strengthens propane adsorption/activation and reduces coke formation. Core–shell engineering thus stabilizes active metal states via local redox microenvironment modulation, offering new design principles for robust alkane dehydrogenation catalysts.
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Science Advances
·
2026
·Vol. 12
·期 35
·
IF 13.9
Lei Li,Ming Zheng,Chunhua Cui
The origin of abiotic methane in Earth’s shallow crust remains unresolved, as existing theories require extreme conditions or catalytic surfaces. Here we show that hydrogen bond reorganization in pressurized bicarbonate aqueous solution (3 MPa, 25°C) activates radical chemistry for CO 2 -to-methane conversion (0.6 μM for 14 days). Through electron paramagnetic resonance (EPR) and in situ Raman spectroscopy, we demonstrate that pressure-induced restructuring of water’s hydrogen bond (HB) network generates hydrated electrons (e − aq ) and hydrogen radicals ( • H), which drive CO 2 reduction via a solution-chemistry mechanism independent of mineral catalysts. This water-mediated radical process provides experimental evidence for abiotic methanogenesis under geologically relevant conditions, fundamentally redefining water’s role from solvent to redox-active participant in subsurface carbon cycling. The findings open alternative avenues for understanding natural hydrocarbon reservoirs and engineered carbon sequestration.
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
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2026
·
IF 2.2
Kaili Liao,Bowen Wu,Minglu Shao,Haiqun Chen,Lipei Fu,Ailian Chang,Daigang Wang,Lifeng Chen,Yingrui Bai,Xingtao Wang,Bing Feng,Zhiguo Yang
Emulsification flooding is a key mechanism for enhanced oil recovery. However, while strong emulsification significantly improves displacement efficiency, it concurrently poses substantial challenges to the subsequent oil–water separation of produced fluids. Therefore, developing smart surfactants that integrate robust emulsifying capacity with facile and efficient demulsification functionality is of considerable importance. In this study, a novel CO2-responsive surfactant (DFD-DA) featuring a dynamic imine bond was synthesized via a Schiff base reaction between disodium 4-formylbenzene-1,3-disulfonate (DFD) and dodecylamine. Its interfacial activity, emulsification performance, and oil displacement efficiency were systematically evaluated. The CO2-responsive demulsification behavior was examined, and the underlying emulsification mechanism was further elucidated through molecular dynamics simulations, complemented by experimental evidence. Results demonstrate that blending DFD-DA with lauroamidopropyl hydroxysulfobetaine (LHSB) at a 1:2 molar ratio significantly reduces interfacial tension to an order of 10−1 mN/m. This blended system exhibits exceptional emulsification performance, achieving an emulsified oil rate (E0) of 91.67% ± 1.05% and an emulsification index (EI) of 1.48 ± 0.03, along with remarkable CO2 responsiveness. Microscopic oil displacement experiments confirmed that the system effectively mobilizes crude oil and enhances the recovery of residual oil. Molecular simulation results provided supplementary insights into the emulsification process and the stabilization mechanism at the molecular level. This work presents a promising CO2-responsive surfactant system for both enhanced oil recovery and controllable demulsification in high water-cut oilfields.
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AICHE JOURNAL
·
2026
·
IF 4.4
Peixin Zhang,Chaoming Hu,Zhenglong Zhu,Zhenwei Zhou,Hao Wang,Jingwen Chen,Shixia Chen,Zhenyu Zhou,Shuguang Deng,Jun Wang
The practical application of metal–organic frameworks (MOFs) for CO 2 capture requires balancing high efficiency, cyclability, and scalable production. Herein, we report a novel MOF adsorbent, Cu 3 (ntrz) 2 (ox) 2 , which allows for low-cost and scalable synthesis in aqueous solutions under ambient conditions. Its tailored large pocket-like cavities interconnected by narrow pore apertures provide exceptional CO 2 adsorption capacities of 6.80 and 3.48 mmol g −1 at 1.0 bar and 0.15 bar (298 K), achieving a record-high VPSA working capacity of 5.03 mmol g −1 within 0.05–1.0 bar. Shaped pellets retain 95% CO 2 adsorption capacity and good mechanical strength, fulfilling industrial requirements. Experimental VPSA analysis demonstrates that a 15% CO 2 gas-stream can be enriched to 91.37% and 95.06% with productivities of 0.402 and 1.86 m 3 t −1 h −1 within 0.08–1.0 bar and 0.08–6.0 bar, outperforming zeolite 13X. The adsorption behaviors and mechanisms are elucidated via Grand Canonical Monte Carlo and dispersion-corrected density functional theory simulations.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2020
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IF 4.551
Junjie Zhou,Hao Liu,Yichao Lin,Chen Zhou,Aisheng Huang
A well-shaped Ce (IV)-based metal organic framework (Ce-BDC) is prepared under solvothermal method. The influence of synthesis time, temperature and the amount of acetic acid (HAc) as a modulator is studied to develop a new strategy for the synthesis of well-shaped Ce-based MOF. The relationship between the synthesis parameters and morphology as well as crystallinity of Ce-BDC is investigated by XRD and SEM. Furthermore, the obtained well-shaped Ce-BDC shows a CO 2 uptake capacity of 2.28 mmol g −1 at 0 °C and 1.0 bar. Meanwhile, the breakthrough curve behaviors of Ce-BDC are investigated for a CO 2 /CH 4 and CO 2 /N 2 mixture gas . It is found that the Ce-based MOF adsorbs CO 2 under ambient temperature and pressure, but completely excludes CH 4 and N 2 , suggesting that it is a promising adsorbent for efficient separation of CO 2 from natural gas.
研究领域:
材料科学
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无机化学
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多孔材料
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气体分离
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环境催化
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FUEL
·
2018
·
IF 4.908
Yan Zhang,Mingwei Gao,Qing You,Hongfu Fan,Wenhui Li,Yifei Liu,Jichao Fang,Guang Zhao,Zhehui Jin,Caili Dai
The development of natural/artificial fractures leads to significant differences of the physical properties between the matrix and the fractures, which usually causes serious channeling and low sweep efficiency during CO 2 flooding in ultra-low permeability reservoirs , the use of a CO 2 -responsive smart mobility control system to generate bulk gel by wormlike micelles (WLMs) to mitigate gas channeling has great potentials for enhanced oil recovery (EOR) in ultra-low permeability reservoirs. In this study, five kinds of chemicals with CO 2 -sensitive groups are screened to measure the apparent viscosity using a rheometer . The experimental results show that the optimum system consists of 4.4 wt% N, N-dimethyl octylamide-propyl tertiary amine (DOAPA) and 2.0 wt% sodium p-toluenesulfonate (SPTS). Subsequently, the plugging capacity and EOR performance of the system are systematically evaluated using core flooding experiments. The optimized system (DOAPA/SPTS) exhibits outstanding plugging capacity for gas channeling with a plugging efficiency of 99.2%. The oil recovery of the CO 2 flooding increases by 20.0%. In addition, the thickening mechanism of the CO 2 -responsive system is studied using rheological experiments and a cryogenic transmission electron microscopy (Cryo-TEM). The shear-thinning behavior demonstrates that the thickening effect of the high-viscosity WLMs is strong in the DOAPA/SPTS-CO 2 solution, and the Cryo-TEM results indicate a transition from spherical micelles to the WLMs. The protonation contributes to the formation of the WLMs in the solution during phase transformation process. The results of this study are expected to provide benchmark to select the mobility control agent for CO 2 flooding in ultra-low permeability reservoirs.
研究领域:
石油工程
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提高采收率
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胶体与界面科学
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油藏工程
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智能材料
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·123805
·
IF 7.5
Jianxin Zhang,Liu Yang,Hongwei Yang,Zhenhuan Li,Shanghan Han,Xiaoyao Tan
In gas separation processes, magnetic induction heating (MIH) offers a promising alternative to conventional heating by avoiding its poor energy efficiency. In this paper, we report a CO 2 sorbent comprised of magnetic nanoparticles (MNPs), hollow fiber, and solid amine for efficient direct air capture (DAC) of CO 2 . The MNPs have the nature of temperature controlling, which making the composite hollow fibers have self-regulating temperature properties. Furthermore, the maximum temperature of composite hollow fiber can be tuned by varying the MNPs content. The heating rate and cooling rate of the composite hollow fibers were compared with those of conventional heating method. The results showed that the magnetic nanoparticles composited hollow fibers exhibited higher heating rate and cooling rate. For the self-regulating temperature solid amine hollow fibers, the magnetic nanoparticle content has effects on CO 2 adsorption capacity, desorption rate and cooling rate. Increasing the magnetic nanoparticles content led to a trade-off effect between heating rate and CO 2 adsorption capacity. The CO 2 adsorption capacity decreased whereas the heating rate increased. The advantage of induction heating over conventional heating for regenerating the CO 2 sorbent were demonstrated. Specifically, the PEI-ECH-MNP20%-PAN HFs achieved heating rate, cooling rate, and desorption rates of 6.7 ℃ min −1 , 3.8 ℃ min −1 , and 0.11 mmol CO 2 g −1 min −1 , respectively. The induction heating method yielded a higher heating rate, cooling rate and desorption rate than conventional heating, which is expected to significantly shorten the cycle time, and thus improve the overall efficiency of the CO 2 capture system. For direct air capture, PEI-ECH-MNP20%-PAN HFs exhibit a CO 2 adsorption capacity of 2.59 mmol g −1 , and saturated PEI-ECH-MNP20%-PAN HFs can be efficiently regenerated via a magnetic induction heating-vacuum swing (MIH-VS) desorption process.
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CATALYSIS TODAY
·
2023
·
IF 5.3
Wensheng Wei,Yuxin Wang,Zizhen Yan,Jiaxiang Hou,Guangwen Xu,Lei Shi
Three quaternary ammonium ionic liquids with strong nucleophilicity and distinctive structures were synthesized with high yield and purity based on the 1,2-propylene glycol anion (CH 3 CH 2 OHCH 2 O - ) derived from transesterification products. Dimethyl carbonate (DMC) was in turn produced via a one-step reaction among propylene oxide (PO), CO 2 , and methanol (MeOH) by using the synthesized ionic liquids. The involved two-stage catalytic reaction of PO-CO 2 cycloaddition and PC-MeOH transesterification was implemented without catalyst separation. Under mild conditions, the PO conversion reached 99.0%, with a PC yield of 99.0%, and a TON value of 119.5. Following the cycloaddition, MeOH was immediately introduced to achieve a PC conversion of 71.2%, a selectivity to DMC above 99%, and a TON value of 57.4 for the transesterification reaction. The influences of temperature as well as time for cycloaddition and transesterification were investigated. Cycloaddition of CO 2 with various epoxides was also examined and all showed good performance. By taking advantage of the decomposability of as-prepared ionic liquids and the recyclability of decomposition products, a new catalyst circulation process was designed to complete the full cycle without introduction of any impurities into the product system.
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CHEMICAL PAPERS
·
2023
·Vol. 77
·期 6
·3347-3359
·
IF 2.2
Wang Chaozhi,Li Hualin,Huang Zhenhong,Ding Zhu,He Zonglin,Liu Baohua,Ai Jiaoyan,Song Lina
The subject of this study was the application of a novel CO 2 -based low-molecular weight poly (propylene carbonate) diol (PPCD) in the field of adhesive. Two-component polyurethane adhesive (PPCD-PU) was prepared with PPCD and polymethylene polyphenyl polyisocyanate (PAPI) as raw materials, propylene carbonate diol (PCD-EDA) as extender. The effects of the molecular weight, carbonate linkage content of PPCD and content of PCD-EDA on the properties of PPCD-PU were also investigated. The results showed that the novel CO 2 -based low-molecular weight poly (propylene carbonate) diol had higher carbonate linkage content (35%). The PPCD-PU synthesized by the PPCD had good adhesion performance, and the lap shear strength reached to 15 MPa. The addition of PCD-EDA not only improved the bonding properties of the adhesive, but also made PPCD-PU adhesive achieved higher lap shear strength in a shorter curing time. When the amount of PCD-EDA was 20 wt.%, the lap shear strength increased to 17 MPa, and the lap shear strength increased significantly from 3.7 to 10.6 MPa after curing at 80 °C for 30 min. Water absorption rate of PPCD-PU film was about 1.7%, and the lap shear strength was almost unchanged after 24 h of immersion in water. The temperature of 5%-weight loss of PPCD-PU was 284 °C, and the glass transition temperature was 79.3 °C. All the polyurethane adhesives obtained performed good heat and water resistance.
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FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Jie Xu,Xiaowei Liu,Rui Li,Boxiong Shen,Zijian Zhou,Lidan Deng,Lei Liu,Xinbo Zhu
Converting CO 2 into renewable fuel via photocatalysis is of significance to solving the energy crisis and climate change. However, the limited electron transfer in single catalysts always limits the reduction reaction. In this work, a p-n heterojunction was constructed between Cr doped MgAl–LDH (abbreviated as LDH) and Co 3 O 4 for visible-light-driven fuel production. Since LDH and Co 3 O 4 both have the sufficient potentials to drive CO 2 photoreduction, the constructed type-II heterojunction is more favorable for electron utilization efficiency. The optimal Co 3 O 4 /LDH heterojunction exhibited the highest CO evolution rate of 7.42 μmol•g −1 •h −1 and a CO selectivity of 90.5% with TEOA as sacrificial agent . The further characterizations highlight that the addition of Co 3 O 4 greatly improves the light absorption and the heterojunction effectively promotes the reverse migration of electrons and holes. This work investigates and verifies the designed type-II heterojunction based on MgAl–LDH, which has the guidance for the design of heterojunction catalysts and promotes the practical application of MgAl–LDH in photocatalytic region.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Longyun Zheng,Bo Zhang,Yi Luo,Kai Guo,Zhengchao Wang,Kun Liu,Xutao Mei,Chunjiang Liu
Carbon dioxide (CO 2 ) absorption into amine-based absorbents is a widely used method for carbon emission reduction to deal with global warming problems. The intensification of the absorption process relies on an in-depth understanding of the mass transfer mechanisms between CO 2 gas and the reaction media. However, the influence of products of a chemical reaction on mass transfer dynamics is usually underestimated. In this study, we perform research studies on the absorption process of single CO 2 bubbles rising in monoethanolamine (MEA) solutions. Firstly, we perform an experimental study to visualize and measure the spatial position and the diameter of the bubbles using the high-speed camera. We observe a special phenomenon that the CO 2 bubble diameter rapidly decreases to a nearly constant value in MEA solutions, and the terminal bubble diameter increases with the MEA concentration. Based on the phenomenon, we divide the absorption process into two stages. One is the mass transfer enhancement stage, where the bubble diameter decreases rapidly. The other is the mass transfer deterioration stage, where the bubble diameter remains almost constant. Furthermore, we propose an elaborate mass transfer dynamics model considering the combined effect of chemical reaction kinetics and reaction-induced bubble surface contamination. Finally, a well-predictive performance by the mass transfer dynamics model is validated by experiment. The findings of this study are of theoretical and practical significance for the mass transfer in gas–liquid reactive flow and multiphase reactor design.
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MOLECULES
·
2023
·Vol. 28
·期 6
·2435
·
IF 4.6
Fulin Wang,Zhenzhen Yu,Kaiyang Shi,Xiangwei Li,Kangqiang Lu,Weiya Huang,Changlin Yu,Kai Yang
The green and clean sunlight-driven catalytic conversion of CO2into high-value-added chemicals can simultaneously solve the greenhouse effect and energy problems. The controllable preparation of semiconductor catalyst materials and the study of refined structures are of great significance for the in-depth understanding of solar-energy-conversion technology. In this study, we prepared nitrogen-doped NiO semiconductors using a one-pot molten-salt method. The research shows that the molten-salt system made NiO change from p-type to n-type. In addition, nitrogen doping enhanced the adsorption of CO2on NiO and increased the separation of photogenerated carriers on the NiO. It synergistically optimized the CO2-reduction system and achieved highly active and selective CO2photoreduction. The CO yield on the optimal nitrogen-doped photocatalyst was 235 μmol·g−1·h−1(selectivity 98%), which was 16.8 times that of the p-type NiO and 2.4 times that of the n-type NiO. This can be attributed to the fact that the nitrogen doping enhanced the oxygen vacancies of the NiOs and their ability to adsorb and activate CO2molecules. Photoelectrochemical characterization also confirmed that the nitrogen-doped NiO had excellent electron -transfer and separation properties. This study provides a reference for improving NiO-based semiconductors for photocatalytic CO2reduction.Keywords:NiO;nitrogen doping;photocatalysis;reduction of CO2
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