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学者姓名：刘福建
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Abstract ：
Selective adsorption of sulfur dioxide (SO2) is an important clean technology for purification of exhaust gas from fossil fuel combustion. The widely applied zeolite-based adsorbents interact with SO2 through weakly physical adsorption, resulting in low adsorption capacity and selectivity for SO2. Herein, a facile strategy that combines improving the textural property of zeolite and optimizing adsorption sites is developed for efficient and stable SO2 adsorption. The micro-mesoporous silica sphere (MS) with high specific surface area and well-defined pore structure is obtained through a micelle expander assisted soft-template method, which can facilitate the dispersion and exposure of designed adsorption sites- methylated polyethyleneimine (mPEI). Since the Lewis basic sites of N in mPEI can strongly interact with the pi-receptor SO2, and the tertiary amine groups exhibit a weak attraction for CO2, the optimized MS supported mPEI adsorbent exhibits remarkable SO2 adsorption performance (7.5 mmol/g), exceptionally high SO2/N2 selectivity (16673) and SO2/CO2 selectivity (551). Moreover, it presents an outstanding stability in the adsorption-regeneration test. This work sheds light on the design of high-performance organic-solid composite adsorbent for selective capture of SO2.
Keyword ：
Adsorption Adsorption Micro-mesoporous silica sphere Micro-mesoporous silica sphere Polytertiary amine Polytertiary amine Selective desulfurization Selective desulfurization SO 2 capture SO 2 capture
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| GB/T 7714 | Zhang, Qiongdan , Wei, Jixiang , Gao, Changbo et al. Highly selective capture of SO2 with supported micro-mesoporous silica sphere from CO2-rich environment [J]. | JOURNAL OF CLEANER PRODUCTION , 2024 , 436 . |
| MLA | Zhang, Qiongdan et al. "Highly selective capture of SO2 with supported micro-mesoporous silica sphere from CO2-rich environment" . | JOURNAL OF CLEANER PRODUCTION 436 (2024) . |
| APA | Zhang, Qiongdan , Wei, Jixiang , Gao, Changbo , Zheng, Yong , Xiao, Yihong , Liu, Fujian et al. Highly selective capture of SO2 with supported micro-mesoporous silica sphere from CO2-rich environment . | JOURNAL OF CLEANER PRODUCTION , 2024 , 436 . |
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gamma-ray radiation-induced grafting strategy was first employed to immobilize 4-aminobenzo-15-crown-5 onto a covalent organic framework (COF). This endeavor culminated in the successful synthesis of a class of two-dimensional crown ether-modified COFs (named [15C5]n%-(TzDa-G-x%)), marking the maiden utilization of COFs in the realm of 6Li/7Li isotope separation. These COFs exhibited swifter adsorption kinetics than alternative adsorbents. Among them, [15C5]57%-(TzDa-G-50%) with its excellent crystallinity, porosity, and stability exhibited the best performance in Li+ adsorption and 6Li/7Li isotope separation. The Li+ adsorption in acetonitrile achieved a capacity of 3.6 mg center dot g-1 within 30 min and a saturation capacity of 7.3 mg center dot g-1. The single -stage separation factor of 6Li/7Li isotopes was 1.014 +/- 0.001. The results of dynamic adsorption column experiments showed that the packed column made of [15C5]57%-(TzDa-G-50%) maintained stable performance during four cycles of Li+ adsorptionelution, with over 99% Li+ removal rate in acetonitrile. This crown ether-modified COF has potential application in 6Li/7Li isotope separation, and this radiation-assisted synthesis strategy is expected to become universal in the modification of COFs for diverse applications.
Keyword ：
6Li/7Li isotope separation 6Li/7Li isotope separation adsorption column adsorption column covalent organic framework covalent organic framework crown ether crown ether gamma ra- diation modification gamma ra- diation modification
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| GB/T 7714 | Zhong, Shouchao , Wang, Yue , Lan, Jianhui et al. Radiation-Assisted Synthesis of Crown Ether-Modified Covalent Organic Frameworks for Lithium Isotope Separation [J]. | CCS CHEMISTRY , 2024 , 6 (10) : 2594-2606 . |
| MLA | Zhong, Shouchao et al. "Radiation-Assisted Synthesis of Crown Ether-Modified Covalent Organic Frameworks for Lithium Isotope Separation" . | CCS CHEMISTRY 6 . 10 (2024) : 2594-2606 . |
| APA | Zhong, Shouchao , Wang, Yue , Lan, Jianhui , Xie, Mingshu , Wu, Yiqian , Li, Jiuqiang et al. Radiation-Assisted Synthesis of Crown Ether-Modified Covalent Organic Frameworks for Lithium Isotope Separation . | CCS CHEMISTRY , 2024 , 6 (10) , 2594-2606 . |
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A solid ionic liquid adsorbent, obtained by grafting [C3N][SO4H] onto porous carbon was reported. Characterizations including IR, XPS and TEM provided the structural information of the sulfonic acid groups on the porous carbon matrix, affirming the feasibility of this synthesis method. The results elucidated the synergy between the sulfonic acid groups and the pore structure of porous carbon, resulting in substantial enhancements in both ammonia adsorption capacity and adsorption selectivity. Moreover, this absorbent exhibited the ability to capture minute concentrations of ammonia below 0.1 ppm with great efficacy and excellent regeneration property within 8 cycles. This simple grafting and acid activation technique proffers a valuable tool for designing adsorbent of trace ammonia within ammonia-hydrogen fuel cells.
Keyword ：
Ammonia fuel cells Ammonia fuel cells Porous carbon Porous carbon Solid ionic liquids Solid ionic liquids Trace ammonia capture Trace ammonia capture
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| GB/T 7714 | Zhu, Qiliang , Zhang, Wentao , Zhong, Shouchao et al. Precisely capture trace ammonia from fuel cell system over ionic liquid grafted hierarchically porous carbons [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 483 . |
| MLA | Zhu, Qiliang et al. "Precisely capture trace ammonia from fuel cell system over ionic liquid grafted hierarchically porous carbons" . | CHEMICAL ENGINEERING JOURNAL 483 (2024) . |
| APA | Zhu, Qiliang , Zhang, Wentao , Zhong, Shouchao , Xiao, Yao , Qian, Hao , Zheng, Anmin et al. Precisely capture trace ammonia from fuel cell system over ionic liquid grafted hierarchically porous carbons . | CHEMICAL ENGINEERING JOURNAL , 2024 , 483 . |
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The introduction of enlarged and interconnected nanochannels into metal-organic frameworks (MOFs) overcome their micropore size restriction, enhances mass transportation, and improves the accessibility of anchored metal clusters. Herein, foamed Ce-MOF single crystals (F-Ce-MOF-SC-x) designed from a multiscale co-assembly is reported in the presence of a copolymer template and 1,3,5-trimethylbenzene as a structural regulator. The resultant F-Ce-MOF-SC-x possessed well-defined microporous tandem-ordered meso-macroporous foams with superior connectivity and versatile Ce-defective unsaturated sites (Ce-DUS). F-Ce-MOF-SC-x is applied as a stable carrier for anchoring polytertiary amines (PA) via coordination interactions with Ce-DUS. Owing to the superior ability of PA to recognize SO2, the resultant F-Ce-MOF-SC-x@yPA delivers exceptional performance in terms of the high-temperature reversible adsorption and separation of SO2, including a remarkable capacity for SO2, spectacular selectivity for SO2/CO2/N-2, an ultrafast adsorption equilibrium rate, and stability for 50 cycles. These characteristics are outstanding among those of MOFs and superior to those of many reported SO2 adsorbents.
Keyword ：
foam nanostructure foam nanostructure macromolecule immobilization macromolecule immobilization metal-organic framework metal-organic framework multiscale assembly multiscale assembly separation separation SO2 adsorption SO2 adsorption
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| GB/T 7714 | Kan, Xun , Zhang, Guanqing , Ma, Jun et al. Multiscale Co-Assembly to Meso-Macroporous Foamed Single-Crystal Metal-Organic Frameworks for the Supported Capture of Sulfur Dioxide [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (19) . |
| MLA | Kan, Xun et al. "Multiscale Co-Assembly to Meso-Macroporous Foamed Single-Crystal Metal-Organic Frameworks for the Supported Capture of Sulfur Dioxide" . | ADVANCED FUNCTIONAL MATERIALS 34 . 19 (2024) . |
| APA | Kan, Xun , Zhang, Guanqing , Ma, Jun , Liu, Fengqing , Tang, Yu , Liu, Fujian et al. Multiscale Co-Assembly to Meso-Macroporous Foamed Single-Crystal Metal-Organic Frameworks for the Supported Capture of Sulfur Dioxide . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (19) . |
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Ordered mesoporous carbon@silica hybrid frameworks with high nitrogen content and good stabilities show great significance to improve their functionalities. Herein, we report novel nitrogen-doped (3.51 - 4.62 wt%) and ordered mesoporous carbon@silica frameworks (N-OMC@SiO2) with reinforced nitrogen stability. The NOMC@SiO2 were designed from tricomponent direct co-assembly between block copolymer template and mixed precursors containing urea and tetramethoxysilane without using additional solvent. The N-OMC@SiO2 have large BET surface areas (444.3 - 674.9 m2/g), uniform mesoporous channels (5.8 - 10.9 nm) with well-defined hexagonal symmetry, and stable carbon@silica "reinforced concrete" framework that can be transformed into carbon@silicon by controllable reduction. The nitrogen sites were firmly embedded into their frameworks via the formation of Si-N bonding. Thus, the resulted N-OMC@SiO2 exhibit multi-functionalities and enhanced recyclability in acid waste gas capture and gaseous sulfides catalytic utilization, better than many reported porous adsorbents and catalysts. This study may help develop stable and efficient N-OMCs nanocomposites for acidic gas selective removal.
Keyword ：
Acid gas selective capture Acid gas selective capture Carbon@silica composites Carbon@silica composites Gaseous sulfides elimination Gaseous sulfides elimination Nitrogen -doping Nitrogen -doping Ordered mesoporosity Ordered mesoporosity Solvent -free synthesis Solvent -free synthesis
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| GB/T 7714 | Kan, Xun , Liu, Zihao , Sun, Yafei et al. Tricomponent direct co-assembly to nitrogen-doped, ordered mesoporous carbon@silica frameworks with enhanced nitrogen stability and multi-functionalities [J]. | CHEMICAL ENGINEERING SCIENCE , 2024 , 292 . |
| MLA | Kan, Xun et al. "Tricomponent direct co-assembly to nitrogen-doped, ordered mesoporous carbon@silica frameworks with enhanced nitrogen stability and multi-functionalities" . | CHEMICAL ENGINEERING SCIENCE 292 (2024) . |
| APA | Kan, Xun , Liu, Zihao , Sun, Yafei , Zhong, Shouchao , Zheng, Yong , Liang, Shijing et al. Tricomponent direct co-assembly to nitrogen-doped, ordered mesoporous carbon@silica frameworks with enhanced nitrogen stability and multi-functionalities . | CHEMICAL ENGINEERING SCIENCE , 2024 , 292 . |
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The efficient deoxygenation of renewable biolipids into liquid alkanes within the diesel range is a key protocol for producing high-quality biofuels. In this work, the conversion of methyl palmitate and raw palm oil were accomplished utilizing a bifunctional catalyst of Ni catalysts supported on B2O3-ZrO2 under solvent-free conditions. Among various Ni loading ratios investigated, the catalyst featuring a 10 % Ni loading achieved 100 % conversion of methyl palmitate and 84.4 % of liquid yield, with approximately 65 % being C15 alkanes. Additionally, more than 91 % of hydrocarbons were also generated from raw palm oil. These results can be attributed to the synergistic interplay between the acid sites, following B2O3 modification, and the presence of Ni species. Furthermore, the analysis of product distribution, gas product detection and the kinetics calculation strongly supports that the deoxygenation process of methyl palmitate primarily follows the hydrodecarbonylation route, leading to the predominant formation of C15 alkane. © 2024
Keyword ：
Bifunctional catalyst Bifunctional catalyst Biodiesel Biodiesel Deoxygenation Deoxygenation Liquid alkanes Liquid alkanes Methyl palmitate Methyl palmitate
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| GB/T 7714 | Yu, P. , Xu, J. , Liang, R. et al. Solvent-free deoxygenation of biolipid into liquid alkanes over bifunctional Ni/B2O3-ZrO2 catalyst [J]. | Fuel , 2024 , 375 . |
| MLA | Yu, P. et al. "Solvent-free deoxygenation of biolipid into liquid alkanes over bifunctional Ni/B2O3-ZrO2 catalyst" . | Fuel 375 (2024) . |
| APA | Yu, P. , Xu, J. , Liang, R. , Cai, Z. , Ma, Y. , Zhang, H. et al. Solvent-free deoxygenation of biolipid into liquid alkanes over bifunctional Ni/B2O3-ZrO2 catalyst . | Fuel , 2024 , 375 . |
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The amine -based materials pose high potential for the adsorption of sulfur dioxide (SO 2 ). This work is aimed at modulating the morphologies of SBA -15 adsorbents by controlling the precursor self -assembly processes, for the sake of optimizing the utilization efficiency of amine species in the polytertiary amine (PTA)-functionalized SBA15. It results that worm -like SBA -15 (WLS) material shows a better particle aspect ratio and well-defined pore structure, which helps to optimize the adsorption sites invoked by the preferable dispersion and exposure of PTA, thus amplifying the chemisorption of SO 2 on the adsorbent. Consequently, the functionalized WLS-PTA adsorbent exhibits remarkable SO 2 adsorption performance (15.43 mmol/g), exceptionally high selectivities of SO 2 /N 2 (27522) and SO 2 /CO 2 (652). Surprisingly, the desulfurization capacity can be further enhanced by the positive effect of the water vapor co -fed. It is unveiled that the whole SO 2 adsorption process mainly follows the dual site Langmuir-Freundlich isotherm model and Bangham model. This work sheds light on the design of polymer -solid composite adsorbents for selective capture of SO 2 .
Keyword ：
Mesoporous SBA-15 Mesoporous SBA-15 Polytertiary amine Polytertiary amine Selective desulfurization Selective desulfurization SO2 adsorption SO2 adsorption Solid amine adsorbent Solid amine adsorbent
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| GB/T 7714 | Zhang, Qiongdan , Lei, Yuanyi , Ye, Ming et al. Facilely tuning the morphologies of tertiary amine-functionalized SBA-15 for optimizing selective SO 2 capture [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 487 . |
| MLA | Zhang, Qiongdan et al. "Facilely tuning the morphologies of tertiary amine-functionalized SBA-15 for optimizing selective SO 2 capture" . | CHEMICAL ENGINEERING JOURNAL 487 (2024) . |
| APA | Zhang, Qiongdan , Lei, Yuanyi , Ye, Ming , Wang, Heng , Zheng, Yong , Xiao, Yihong et al. Facilely tuning the morphologies of tertiary amine-functionalized SBA-15 for optimizing selective SO 2 capture . | CHEMICAL ENGINEERING JOURNAL , 2024 , 487 . |
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NH3 adsorption and separation are pivotal for its safety and efficient utilization, but most solid adsorbents show either low capacity or unsatisfied separation performance. Herein, we report sulfonated and ordered mesoporous polymers (SOMPs) synthesized from solvent-free manual-grinding of resorcinol and 1,4-phthalaldehyde with copolymer template, curing at 140 -220 C, simultaneous sulfonation and template removal by treating with H2SO4. The prepared SOMPs possess ordered mesopores with abundant microporosity, large surface areas (-697 m(2)/g), and extremely-high -SO3H densities (-4.48 mmol/g). Their NH3 adsorption capacities are as high as 15.09 mmol/g (25 C, 1.0 bar), exhibiting NH3 breakthrough time and saturated capacity up to 138 min/g and 6.16 mmol/g, respectively (5.0v%NH3/23.75v%N2/71.25v%H-2). Versatile characterizations together with mo-lecular dynamics simulations demonstrate the superior NH3 adsorption performance originates from strong affinity of -SO3H group with NH3 in sequential pore-space of SOMPs, which not only enhances the molecular recognition ability, but also effectively promotes NH3 fast diffusion inside SOMPs.
Keyword ：
NH3 adsorption and separation NH3 adsorption and separation Ordered mesopores Ordered mesopores porous organic polymers porous organic polymers solid acids solid acids solvent-free synthesis solvent-free synthesis
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| GB/T 7714 | Kan, Xun , Liu, Zhiqiang , Liu, Fujian et al. Sulfonated and ordered mesoporous polymers for reversible adsorption of ammonia: Elucidation of sequential pore-space diffusion [J]. | CHEMICAL ENGINEERING JOURNAL , 2023 , 451 . |
| MLA | Kan, Xun et al. "Sulfonated and ordered mesoporous polymers for reversible adsorption of ammonia: Elucidation of sequential pore-space diffusion" . | CHEMICAL ENGINEERING JOURNAL 451 (2023) . |
| APA | Kan, Xun , Liu, Zhiqiang , Liu, Fujian , Li, Fangyao , Chen, Wei , Yi, Xianfeng et al. Sulfonated and ordered mesoporous polymers for reversible adsorption of ammonia: Elucidation of sequential pore-space diffusion . | CHEMICAL ENGINEERING JOURNAL , 2023 , 451 . |
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NH3 reversible adsorption and separation show great significance during its production and utilization, tradi-tional adsorbents show either complex synthetic procedures or unsatisfied separation precision. We report here a class of sulfonic group functionalized and ordered mesoporous silica superacids (OMS-SO3H-xs) via enhanced host-guest assembly between copolymer templates and silica precursors without additional solvent. The OMS-SO3H-xs have large surface areas (463.7-910.5 m2/g), abundant micropores tandem well-ordered mesopores, high concentration of -SO3H (2.5 mmol/g) with extremely-high acid strength. Consequently, the OMS-SO3H-xs exhibit ultra-high precision for NH3 reversible adsorption and separation, giving high NH3 capacity (9.0 & 7.6 mmol/g at 25 & 50 degrees C and 1.0 bar) with extraordinary NH3/N2 (0.1/0.9) Ideal Adsorption Solution Theory (IAST) selectivities (1200 & 2235). The room temperature saturated breakthrough NH3 capacities of OMS-SO3H-xs were up to 3.38 mmol/g (3.0v%NH3/24.75v%N2/72.25v%H2), which can be well-maintained after 8th cycling without attenuation. The above features found in the OMS-SO3H-xs were resulted from their high density of -SO3H superacid sites those were homogeneously anchored into the ordered mesoporosity, which not only enhances their interaction with NH3, but also achieves the controllable NH3 interaction and transportation inside the mesochannels.
Keyword ：
Enahnced host-guest assembly Enahnced host-guest assembly NH 3 controllable transportation NH 3 controllable transportation Ordered mesopores Ordered mesopores Reversible adsorption and separation Reversible adsorption and separation Solid superacids Solid superacids
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| GB/T 7714 | Zhang, Wentao , Liu, Fengqing , Kan, Xun et al. Developing ordered mesoporous silica superacids for high-precision adsorption and separation of ammonia [J]. | CHEMICAL ENGINEERING JOURNAL , 2023 , 457 . |
| MLA | Zhang, Wentao et al. "Developing ordered mesoporous silica superacids for high-precision adsorption and separation of ammonia" . | CHEMICAL ENGINEERING JOURNAL 457 (2023) . |
| APA | Zhang, Wentao , Liu, Fengqing , Kan, Xun , Zheng, Yong , Zheng, Anmin , Liu, Fujian et al. Developing ordered mesoporous silica superacids for high-precision adsorption and separation of ammonia . | CHEMICAL ENGINEERING JOURNAL , 2023 , 457 . |
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Selective catalytic oxidation of H2S into elemental sulfur has been recognized as the optimal route for H2S reutilization, but traditional metal catalysts show poor sulfur resistance. Herein, we report a solvent-free route for designing nitrogen and defects co-doped, ordered mesoporous carbons (ND-OMCs) from co-assembly of block copolymer template with nitrogen-containing oligomers and silica defects directing agent. Through thermal curing, carbonization and etching of silica, the microporosity tandem ordered mesopores, abundant nitrogen sites (6.13 wt%) and structural defects were introduced into ND-OMCs. The ND-OMCs were successfully applied as efficient and long-lived metal-free catalysts for H2S selective oxidation to sulfur, giving nearly 100 % H2S conversion and sulfur selectivity at only 150 degrees C. Their remark-able activities of ND-OMCs can be well-maintained over 157 h of continuous reaction, exhibiting the sul-fur capacity as high as 3295 mg/g, which were much better than mostly desulfurizes such as commercial Fe2O3, g-C3N4, and nitrogen-containing, ordered mesoporous carbons.(c) 2023 Elsevier Ltd. All rights reserved.
Keyword ：
H2S catalytic reutilization H2S catalytic reutilization Nitrogen-doped porous carbon Nitrogen-doped porous carbon Ordered mesoporosity Ordered mesoporosity Structural defects Structural defects Sustainable design Sustainable design
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| GB/T 7714 | Kan, Xun , Song, Feiyu , Zhang, Guanqing et al. Sustainable design of co-doped ordered mesoporous carbons as efficient and long-lived catalysts for H2S reutilization [J]. | CHEMICAL ENGINEERING SCIENCE , 2023 , 269 . |
| MLA | Kan, Xun et al. "Sustainable design of co-doped ordered mesoporous carbons as efficient and long-lived catalysts for H2S reutilization" . | CHEMICAL ENGINEERING SCIENCE 269 (2023) . |
| APA | Kan, Xun , Song, Feiyu , Zhang, Guanqing , Zheng, Yong , Zhu, Qiliang , Liu, Fujian et al. Sustainable design of co-doped ordered mesoporous carbons as efficient and long-lived catalysts for H2S reutilization . | CHEMICAL ENGINEERING SCIENCE , 2023 , 269 . |
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