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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY · 2024 · IF 5.9

Nitrogen-Doped High-Surface-Area activated carbon: Innovative adsorbent for enhanced SO2 and benzene removal

Hongliang Sheng,Xiaoben Zhao,Shuainan Wang,Tao He,Jinfeng Zhang,Song He,Yajun Huang

In this paper, we investigated the properties of nitrogen-doped activated carbon produced via the co-activation of KSCN and KOH, using hydrothermal lignin as a precursor. The resulting activated carbon exhibited a high specific surface area of 3504 m 2 /g and contained 3.37 % nitrogen from KSCN, which enhanced its adsorption efficiency. The adsorption capacities for SO 2 and benzene at 273 K were measured at 2260.68 mg/g and 1668.90 mg/g, respectively. Competitive adsorption experiments at 298 K showed that in the presence of SO 2 , the activated carbon maintained a high adsorption capacity for benzene at 1008.81 mg/g, while the adsorption capacity for SO 2 decreased to only 12.31 mg/g, indicating a higher affinity for benzene. The selectivity coefficient, calculated using the Ideal Adsorbed Solution Theory (IAST), reached 44.76 at a benzene-to-SO 2 ratio of 2:1. To gain deeper insights into the selective adsorption mechanism, Density Functional Theory (DFT) simulations were conducted. These simulations confirmed the experimental findings, indicating that benzene can be selectively adsorbed and effectively separated from SO 2 flue gas.

CAS / MDL: 9005-53-2 333-20-0
研究领域: 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Experimental study on adsorption removal of SO2 in flue gas by defective UiO-66

Yuling Ma,Airong Li,Cheng Wang

Metal-organic frameworks (MOFs) with a high specific surface area, an adjustable pore structure, and functionalized pore environment have a broad application prospect in gas adsorption and separation. In this work, a series of defective UiO-66 (UiO-66-monocarboxylic acid) samples were prepared by adding different monocarboxylic acids during the synthesis of UiO-66. UiO-66-monocarboxylic acid samples (UiO-66-formic acid, UiO-66-acetic acid, UiO-66-benzoic acid, UiO-66-acrylic acid, and UiO-66-cyanoacetic acid) had a high specific surface area (1200–1400 m 2 /g) and a good thermal stability (560 °C). In the desulfurization experiment of simulated flue gas (SO 2 /CO 2 /O 2 /N 2 , 0.3/10.0/5.5/84.2 vol%), the breakthrough time of UiO-66-cyanoacetic acid for SO 2 was higher (194 min/g), and the selectivity of SO 2 /CO 2 reached 33.8. Through optimizing the moles of cyanoacetic acid added, the breakthrough time of SO 2 on 18-UiO-66-cyanoacetic acid increased to 251 min/g. At a pressure of 1.0 bar and a temperature of 298 K, the adsorption capacity of SO 2 by 18-UiO-66-cyanoacetic acid reached 762.1 mg/g. In addition, the adsorption behavior of 18-UiO-66-cyanoacetic acid for SO 2 was considered as a combination of chemical and physical adsorption, and fractional chemisorption sites was provided by cyanoacetic acid.

研究领域: 材料科学 · 环境科学
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FUEL · 2018 · IF 4.908

Enhance SO2 adsorption performance of biochar modified by CO2 activation and amine impregnation

Jingai Shao,Junjie Zhang,Xiong Zhang,Ye Feng,Han Zhang,Shihong Zhang,Hanping Chen

To enhance the SO 2 adsorption of biochar, CO 2 activation and impregnation with methyldiethanolamine (MDEA) was simultaneously employed to improve its physicochemical characteristics. Furthermore, the effects of the pore structure and nitrogen functionality on SO 2 adsorption were also explored. The results show that after CO 2 activation, the specific surface area of biochar increased from 56.91 m 2 /g to 755.35 m 2 /g, while this figure dropped to 25.54 m 2 /g or even lower after impregnation with MDEA. Although the pore structure of activated biochar was destroyed, the surface nitrogen content of the nitrogen-enriched biochar (with 10% MDEA impregnation) increased from 1.46% to its highest level (7.20%); moreover, as indicated by Fourier Transform Infrared (FTIR) spectroscopy, the nitrogen functional groups introduced on the surface of the nitrogen-enriched biochar were mainly C-N. After 10% MDEA impregnation, the maximum SO 2 adsorption capacity increased from 57.8 mg/g to 156.2 mg/g. Changes to physical and chemical properties in the nitrogen-enriched biochar indicate that the nitrogen functional groups on the surface are more important than the pore structure for SO 2 adsorption at 393 K, and that the dominant nitrogen species are quaternary nitrogen.

CAS / MDL: 105-59-9
研究领域: 环境科学 · 材料科学
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ACS Applied Nano Materials · 2022 · IF 6.14

Self-Assembled Zeolitic Imidazolate Framework/Polyimide Nanofibers for Efficient Air Pollution Control

Zhimin Hao,Juntao Wu

A complex air pollution environment requires filters to be multifunctional. Nanofibrous materials with surface-loaded metal–organic frameworks (MOF-fibers) are reasonable structures for multifunctional air filtration. These materials can not only utilize the network structure of fibers to intercept particulate matter (PM) but also retain the porous structure of the MOFs to adsorb toxic gas. Epitaxial growth methods are commonly utilized to prepare MOF-fibers but are uneconomical and time-consuming. Herein, a facile self-assembly strategy is developed to prepare zeolitic imidazolate framework-polyimide (ZIF-PI) nanofibers with an interconnected network structure and high porosity for air filtration applications. Due to their unique structure, the ZIF-PI nanofibrous membrane exhibited high PM2.5 filtration efficiency and enhanced SO2 adsorption capacity. Moreover, by exploring the morphology evolution of the ZIF-PI nanofibrous membrane, a possible “synergistic effect of hydrophobic and electrostatic force” self-assembly mechanism was demonstrated.

研究领域: 材料科学 · 环境科学
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2019 ·Vol. 21 ·期 18 ·9181-9188 · IF 3.567

A new insight into the SO2 adsorption behavior of oxidized carbon materials using model adsorbents and DFT calculations

Xinxin Pi,Fei Sun,Jihui Gao,Zhibin Qu,Ani Wang,Zhipeng Qie,Lijie Wang,Hui Liu

Heteroatom-doped carbon materials have been proven to be very effective for gas adsorption. Herein, edge-carboxylated graphene nanoplatelets with gradient oxygen contents and consistent pore structures were used as model adsorbents to independently determine the effects of the oxygen functionalization of carbon materials on the SO2 adsorption. The OGnPs were obtained by employing a simple ball milling method using dry ice by which an oxygen content as high as 14.06 wt% could be achieved, resulting in a 20 times increase in SO2 adsorption capacity as compared to that of oxygen-free graphene nanoplatelets. Both the experiments and density functional theory calculations demonstrated that the enhanced SO2 adsorption on the oxygenated carbon surface had a physisorption nature, which provided new insights into the development of advanced carbon materials with heteroatom doping for gas molecule adsorption.

CAS / MDL: 7782-42-5
研究领域: 材料科学 · 环境科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2019 · IF 3.375

Facile Preparation of Biomass-Derived Mesoporous Carbons for Highly Efficient and Selective SO2 Capture

Jinghan Zhang,Peixin Zhang,Minyu Li,Ziwei Shan,Jun Wang,Qiang Deng,Zheling Zeng,Shuguang Deng

The efficient elimination of SO2 from flue gases and natural gases is critical for energy utilization and environmental protection. However, selecting or preparing an efficient adsorbent with a high SO2 capacity, good selectivity, and excellent recyclability is very challenging, and the adsorption mechanism at an atomic level is still controversial. We report a facile one-step method for the synthesis of biomass-derived porous carbons with high specific surface areas (1195–1449 m2 g–1), mesoporous pore size (4–6 nm), and good SO2 adsorption properties. Our carbon adsorbents exhibited an outstanding SO2 adsorption capacity of 10.7 mmol g–1 at 298 K and 1.0 bar, which is more than twice the SO2 capacity of benchmark carbon material cs1000a (approximately 5.0 mmol g–1) and commercial ordered mesoporous carbon CKM-3 (5.1 mmol g–1). The new carbon adsorbents also showed unprecedented SO2/CO2, SO2/CH4, and SO2/N2 separation selectivities of 32, 127, and 2349, respectively, which are comparable with the best performance MOF adsorbents. Dynamic breakthrough experiments confirmed the feasibility of efficient removal of SO2 from flue gas in an adsorbent column. Even with the presence of water vapor, clear and efficient separation of SO2 could also be achieved with excellent recycling stability. In addition, a density function theory simulation further illustrates that −NOx and −OH groups in the carbon frameworks provide strong interactions with SO2 molecules. The carbon adsorbents synthesized in this work are promising for flue gas desulfurization and natural gas purification applications.

CAS / MDL: 7646-85-7
研究领域: 环境科学 · 材料科学
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APPLIED SURFACE SCIENCE · 2025 · IF 6.9

Plasma-assisted coating mitigates degradation of (Sr,Ca)AlSiN3:Eu2+ phosphors under thermal‐moisture‐sulfur condition: from synergistic aging mechanisms to protective strategies

Changran Zheng,Zhoudong Yang,Baotong Guo,Hanqing Dai,Tianhe Lu,Xi Zhu,Huimin Xu,Bobo Yang,Jun Zou,Sergey Lishik,Jiajie Fan

(Sr, Ca)AlSiN 3 :Eu 2+ (SCASN) phosphors are widely used in white LEDs due to their excellent red spectral performance. However, exposure to high temperature, high humidity, and sulfur-containing environments significantly degrades their performance and long-term stability. Herein, a rapid plasma-assisted deposition technique is employed to apply an ultrathin Si-based nanolayer onto SCASN (SCASN-Coated), enhancing its durability under such harsh conditions. Accelerated aging tests conducted at 100 °C, 100 % relative humidity (RH), and in a sulfur-containing atmosphere reveal that unmodified SCASN retains only 24.1 % of its initial luminous intensity after 1008 h, whereas the SCASN-Coated preserves approximately 41.2 % of their original brightness without compromising intrinsic luminescent properties. First-principles calculations and molecular dynamics simulations further elucidate that SCASN has a strong chemical adsorption effect on SO 2 (−3.056  eV). And the combined presence of SO 2 and H 2 O promotes the displacement of Ca 2+ ions, accelerating degradation. The protective SiO 2 nanolayer drastically reduces the SO 2 adsorption energy (−0.124  eV) and inhibits Ca 2+ ion migration. This surface protection strategy not only augments the resilience of SCASN phosphors under extreme conditions but also provides research paradigm into the degradation mechanisms, thereby offering new avenues for extending the service life of LED devices in challenging environments.

CAS / MDL: 107-46-0
研究领域: 材料科学 · 光电子学 · 表面工程 · 固态照明 · 计算化学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Structural control for inhibiting SO2 adsorption in porous MnCe nanowire aerogel catalysts for low-temperature NH3-SCR

Chengzhi Wang,Fengyu Gao,Songjin Ko,Hengheng Liu,Honghong Yi,Xiaolong Tang

The presence of SO 2 in industrial flue gases will cause permanent deactivation of the catalyst active centre. Therefore, an effective method to improve the SO 2 resistance of manganese-based catalysts at low temperatures is urgently needed. In this work, a hierarchical porous nanowire structure catalyst was designed by the in situ self-assembly method to inhibit SO 2 adsorption. This hierarchical porous nanowire aerogel catalyst with great BET surface area and surface acidity exhibited NOx conversion above 90% at 100–400 °C. Notably, the NOx conversion of the MnCe-N catalyst was almost not inhibited by SO 2 (250 ppm) compared to the 33% decrease of the MnCe-P catalyst. On the MnCe-P catalyst, SO 2 has strong competitive adsorption with NH 3 and NO, and the stronger adsorption capacity of SO 2 inhibits the adsorption activation of the reaction gas and hinders the reaction proceeding through the L-H mechanism. Meanwhile, a large quantity of sulfate is formed on the catalyst surface, which prevents the active centre to participate in the redox reaction. The structure of nanowires enhances the number of acid sites, facilitates the adsorption and activation of NH 3 , and effectively inhibits the adsorption of SO 2 on the MnCe-N catalyst. Fewer sulfate species are generated and difficult to deposit and aggregate on the catalyst surface, as a result, the active centre is less affected by sulfate species. The stable adsorption of NH 3 -related species ensures reliable reaction on MnCe-N through the E-R mechanism. This work emphasizes the importance of hierarchically porous structures in improving the NH 3 -SCR performance and SO 2 resistance of monolithic catalysts, and provides new insights into the design of highly efficient and stable catalytic materials.

CAS / MDL: 7783-20-2
研究领域: 催化 · 环境科学 · 材料科学
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CHEMICAL ENGINEERING SCIENCE · 2025 · IF 4.3

Mesoporous carbon spheres loading with ionic liquids for adsorption of low-concentration SO2

Ying Zeng,Xinlu Li

Biomass-activated carbon is generally used in ultra-clean rooms to remove sulfur dioxide (SO 2 ) molecular impurities. However, its high air resistance and excessive chemical residues needs resolution. In this study, we have developed millimeter-sized mesoporous carbon beads (MCBs) using a silica sol and reverse-phase suspension polymerization. The microstructure of MCBs was characterized by various techniques, including X-ray diffraction, Raman spectroscopy and scanning electron microscopy. The MCBs were categorized into three distinct groups based on particle size and were loaded with tetramethyl guanidine lactate (TMGL) or 1-ethyl-3-methylimidazolium acetate   ([EMIM][OAc]), respectively. It was found that the MCBs exhibit a perfect spherical shape, smooth surface, high strength, and effectively reduce air resistance. Notably, the MCBs loaded with [EMIM][OAc] demonstrated a remarkable SO 2 adsorption capacity of up to 36.7 mg/ml, and the feasibility to remove SO 2 as a new absorption material for ultra-clean room.

CAS / MDL: 143314-17-4
研究领域: 环境科学 · 材料科学 · 化学工程 · 吸附技术
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Small · 2024 · IF 13

Triple Templates Directed Synthesis of Nitrogen-Doped Hierarchically Porous Carbons from Pyridine Rich Monomer as Efficient and Reversible SO2 Adsorbents

Guanqing Zhang,Fengqing Liu,Qiliang Zhu,Hao Qian,Shouchao Zhong,Jingze Tan,Anmin Zheng,Fujian Liu,Lilong Jiang

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-SiO 2 -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(NO 3 ) 2 and tetramethoxysilane. In the pyrolysis process, P123 and SiO 2 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 (≈956–1126 m 2 g −1 ), hierarchical porosity with micro-supermicro-mesoporous feature and high nitrogen contents (≈10.44–5.99 at%) with tunable density of pyridine-based nitrogen sites (≈5.99–3.32 at%), exhibiting good accessibility and reinforced interaction with SO 2 . Consequently, the DAP-NHPC-T show high SO 2 capacity (14.7 mmol g −1 , 25 °C and 1.0 bar) and SO 2 /CO 2 /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 SO 2 adsorption via the unique charge transfer, the adsorption mechanism and reaction model have been finally clarified.

研究领域: 材料科学 · 化学工程 · 环境科学
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