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学者姓名：刘福建
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Abstract ：
Capture of acid gases holds crucial importance for addressing air pollution and climate change, where achieving a molar ratio for adsorption and separation of acid gases on an active site higher than 1.0 remains challenging. Herein, we demonstrate that three nitrogen-bonded one Zn sites within a single-crystalline-like porous carbon (Zn-N3@SC-PC) derived from controlled carbonization of ZIF-8-C equivalent to N with KCl, exhibit supra-multi-molar adsorption for CO2, COS, and H2S, even to 1:6 ratio for SO2 on the Zn-N3. This exceptional performance is attributed to the protruded structure in the Zn-N3@SC-PC for more coordination between Zn vacant orbital and acid gases evidenced by DFT calculation and in situ EXAFS. The high capacity for capturing acid gases on this adsorbent is crucial for future in carbon neutrality and environment protection.
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| GB/T 7714 | Zhang, Guanqing , Liu, Fengqing , Zhong, Shouchao et al. Surpassing stoichiometric limitation for supra-multi-molar adsorption and separation of acid gases [J]. | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
| MLA | Zhang, Guanqing et al. "Surpassing stoichiometric limitation for supra-multi-molar adsorption and separation of acid gases" . | NATURE COMMUNICATIONS 16 . 1 (2025) . |
| APA | Zhang, Guanqing , Liu, Fengqing , Zhong, Shouchao , Liu, Fujian , Zhu, Qiliang , Tang, Yu et al. Surpassing stoichiometric limitation for supra-multi-molar adsorption and separation of acid gases . | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
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Trace ammonia reversible adsorption and sieving using solid adsorbents present a critical challenge in the practical deployment of ammonia-hydrogen fuel cells. Herein, we design porous polydivinylbenzene (P-PDVB) through one-pot solvothermal polymerization without additional templates. Subsequently, solvent-induced network swelling was performed to achieve deep sulfonation of the P-PDVB using chlorosulfonic acid, resulting in P-PDVB-SO3H-x, which possess large specific surface areas, abundant micro-mesoporosity, and high acid site densities. Notably, P-PDVB-SO3H-x demonstrate superior performance for the selective capture and sieving of NH3 from an N2/H2/NH3 mixture, outperforming most previously reported NH3 adsorbents. Thus, P-PDVB-SO3H-x can serve as an efficient adsorbent for the selective removal of trace ammonia from ammonia-hydrogen fuel cell systems, significantly improving both the efficiency and longevity of the fuel cells. This work highlights the potential of P-PDVB-SO3H-x as a promising candidate for enhancing ammonia-hydrogen fuel cell performance, paving the way for further exploration of advanced adsorbent materials in energy applications.
Keyword ：
ammonia-hydrogen fuel cell ammonia-hydrogen fuel cell ammonia separation ammonia separation deep sulfonation deep sulfonation porous organic polymers porous organic polymers selective adsorption selective adsorption solvothermal synthesis solvothermal synthesis
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| GB/T 7714 | Qu, Yongfang , Zhang, Wentao , Zhong, Shouchao et al. Reversible adsorption and sieving of trace NH3 from NH3-H2 fuel cells systems using sulfonated porous polydivinylbenzene [J]. | AICHE JOURNAL , 2025 , 71 (5) . |
| MLA | Qu, Yongfang et al. "Reversible adsorption and sieving of trace NH3 from NH3-H2 fuel cells systems using sulfonated porous polydivinylbenzene" . | AICHE JOURNAL 71 . 5 (2025) . |
| APA | Qu, Yongfang , Zhang, Wentao , Zhong, Shouchao , Zhuo, Linyu , Wang, Xi , Fang, Huihuang et al. Reversible adsorption and sieving of trace NH3 from NH3-H2 fuel cells systems using sulfonated porous polydivinylbenzene . | AICHE JOURNAL , 2025 , 71 (5) . |
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A novel sp2 carbon-conjugated covalent organic framework (COF), PZ-TFPT-COF, was designed for efficient sulfur dioxide (SO2) capture, addressing the critical issue of SO2 pollution, primarily emitted from the combustion of sulfur-rich fuels. The PZ-TFPT-COF demonstrates a remarkable SO2 adsorption capacity of 9.6 mmol/g at 25 °C and 1.0 bar, with a superior SO2/CO2 (0.1/0.9) Ideal Adsorbed Solution Theory (IAST) selectivity of 36.3. Structural characterizations through powder X-ray diffraction (PXRD), N2 adsorption–desorption isotherms, scanning electron microscopy (SEM), and high-resolution transmission electron microscopy (HRTEM) confirm its excellent crystallinity, uniform bulk morphology, and abundant, uniform nanoporosity. Additionally, PZ-TFPT-COF retains 96.9 % of its initial capacity after 8 adsorption–desorption cycles, highlighting its excellent recyclability. The binding energy between SO2 and the pyrazine nitrogen sites was calculated to be −40.29 kJ/mol, indicating their strong acid-base interactions. These results demonstrate that PZ-TFPT-COF is a promising candidate for advanced flue gas desulfurization, offering significant potential for cleaner industrial processes and improved air quality. © 2025 Elsevier B.V.
Keyword ：
Adsorption isotherms Adsorption isotherms Air quality Air quality Binding sites Binding sites Desulfurization Desulfurization Gas adsorption Gas adsorption Physisorption Physisorption Sulfur dioxide Sulfur dioxide
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| GB/T 7714 | Qu, Yongfang , Liu, Fengqing , Zhuo, Linyu et al. Pyrazine-functionalized sp2 carbon-conjugated covalent organic frameworks for selective capture of sulfur dioxide [J]. | Separation and Purification Technology , 2025 , 371 . |
| MLA | Qu, Yongfang et al. "Pyrazine-functionalized sp2 carbon-conjugated covalent organic frameworks for selective capture of sulfur dioxide" . | Separation and Purification Technology 371 (2025) . |
| APA | Qu, Yongfang , Liu, Fengqing , Zhuo, Linyu , Zheng, Liping , Zhong, Shouchao , Xiao, Yihong et al. Pyrazine-functionalized sp2 carbon-conjugated covalent organic frameworks for selective capture of sulfur dioxide . | Separation and Purification Technology , 2025 , 371 . |
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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.
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, Panjie , Xu, Jing , Liang, Rengan et al. Solvent-free deoxygenation of biolipid into liquid alkanes over bifunctional Ni/B2O3-ZrO2 catalyst [J]. | FUEL , 2024 , 375 . |
| MLA | Yu, Panjie et al. "Solvent-free deoxygenation of biolipid into liquid alkanes over bifunctional Ni/B2O3-ZrO2 catalyst" . | FUEL 375 (2024) . |
| APA | Yu, Panjie , Xu, Jing , Liang, Rengan , Cai, Zhenping , Ma, Yongde , Zhang, Hongwei et al. Solvent-free deoxygenation of biolipid into liquid alkanes over bifunctional Ni/B2O3-ZrO2 catalyst . | FUEL , 2024 , 375 . |
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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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Herein, a variety of 2,6-diaminopyridine (DAP) derived nitrogen-doped hierarchically porous carbon (DAP-NHPC-T) prepared from carbonization-induced structure transformation of DAP-Zn-SiO2-P123 nanocomposites are reported, which are facilely prepared from solvent-free co-assembly of block copolymer templates P123 with pyridine-rich monomer of DAP, Zn(NO3)(2) and tetramethoxysilane. In the pyrolysis process, P123 and SiO2 templates promote the formation of mesoporous and supermicroporous structures in the DAP-NHPC-T, while high-temperature volatilization of Zn contributed to generation of micropores. The DAP-NHPC-T possess large BET surface areas (approximate to 956-1126 m(2) g(-1)), hierarchical porosity with micro-supermicro-mesoporous feature and high nitrogen contents (approximate to 10.44-5.99 at%) with tunable density of pyridine-based nitrogen sites (approximate to 5.99-3.32 at%), exhibiting good accessibility and reinforced interaction with SO2. Consequently, the DAP-NHPC-T show high SO2 capacity (14.7 mmol g(-1), 25 degrees C and 1.0 bar) and SO2/CO2/N-2 IAST selectivities, extraordinary dynamic breakthrough separation efficiency and cycling stability, far beyond any other reported nitrogen-doped metal-free carbon. As verified by in situ spectroscopy and theoretical calculations, the pyridine-based nitrogen sites of the DAP-NHPC-T boost SO2 adsorption via the unique charge transfer, the adsorption mechanism and reaction model have been finally clarified.
Keyword ：
charge transfer charge transfer hierarchical porosity hierarchical porosity pyridine-based nitrogen sites pyridine-based nitrogen sites SO2 capture SO2 capture triple template directed synthesis triple template directed synthesis
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| GB/T 7714 | Zhang, Guanqing , Liu, Fengqing , Zhu, Qiliang et al. Triple Templates Directed Synthesis of Nitrogen-Doped Hierarchically Porous Carbons from Pyridine Rich Monomer as Efficient and Reversible SO2 Adsorbents [J]. | SMALL , 2024 , 20 (46) . |
| MLA | Zhang, Guanqing et al. "Triple Templates Directed Synthesis of Nitrogen-Doped Hierarchically Porous Carbons from Pyridine Rich Monomer as Efficient and Reversible SO2 Adsorbents" . | SMALL 20 . 46 (2024) . |
| APA | Zhang, Guanqing , Liu, Fengqing , Zhu, Qiliang , Qian, Hao , Zhong, Shouchao , Tan, Jingze et al. Triple Templates Directed Synthesis of Nitrogen-Doped Hierarchically Porous Carbons from Pyridine Rich Monomer as Efficient and Reversible SO2 Adsorbents . | SMALL , 2024 , 20 (46) . |
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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 catalytic cleavage of carbon-sulfur (C & boxH;S) double bonds on the metal sites without deactivation has aroused great interest in both fundamental catalytic research and industrial chemistry. Herein, activity descriptors are developed via machine learning and density functional theory (DFT) calculations to screen transition-metal single-site catalysts, which quantify the effect of both atomic electronic properties and coordination configuration on the hydrolysis of C & boxH;S double bonds. The valence electron number and electronegativity of active sites are found to be well related to C & boxH;S activation and sulfur poisoning, where Fe demonstrates high catalytic potential among a series of metal centers. On the other hand, the isolated Fe-1 and Fe-2 sites favor carbonyl sulfide (COS) adsorption and activation, while the COS easily dissociates into *S and *CO on Fe-3 hollow site, thus resulting in the formation of robust Fe-S bonds and catalyst deactivation. As anticipated, the as-designed Fe-1-N-4 site achieves a COS conversion of ca. 96% at 100 degrees C, slightly better than the Fe-2-N-4 site, approximately 8 times higher than that of the Fe/C, which is also better than those of other monatomic catalysts (such as Co-NC, Ni-NC, Sn-NC, and Bi-NC). The combination of in situ characterizations and theoretical calculations suggests that *COS and *H2O/*OH have a competitive adsorption relationship on Fe-N-4 sites, and two Fe-N-4 sites can synergistically catalyze the COS hydrolysis through the spilled H and OH.
Keyword ：
carbon-sulfurbonds cleavage carbon-sulfurbonds cleavage hydrolysis mechanism exploration hydrolysis mechanism exploration isolated Fe-N-4 site isolated Fe-N-4 site metal activesite design metal activesite design valence electron descriptor valence electron descriptor
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| GB/T 7714 | Lei, Ganchang , Lin, Xiaoyun , Yan, Hongping et al. Valence Electron and Coordination Structure Guided Metal Active Site Design for Hydrolytic Cleavage of Carbon-Sulfide Double Bonds [J]. | ACS CATALYSIS , 2024 , 14 (22) : 17103-17112 . |
| MLA | Lei, Ganchang et al. "Valence Electron and Coordination Structure Guided Metal Active Site Design for Hydrolytic Cleavage of Carbon-Sulfide Double Bonds" . | ACS CATALYSIS 14 . 22 (2024) : 17103-17112 . |
| APA | Lei, Ganchang , Lin, Xiaoyun , Yan, Hongping , Shen, Lijuan , Wang, Shiping , Liang, Shijing et al. Valence Electron and Coordination Structure Guided Metal Active Site Design for Hydrolytic Cleavage of Carbon-Sulfide Double Bonds . | ACS CATALYSIS , 2024 , 14 (22) , 17103-17112 . |
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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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