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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Highly selective and reversible adsorption of trace gaseous ammonia by a stable nanoporous carboxylic acid-functionalized silica aerogel

Zai-Dong Shao,Ting-Ting Hu,J. Paul Chen,Qi-Jun Zhang,Peng Wu,Rui-Sang Liu,Jiang Lu,Xiao-Meng Ren,Yu-Ming Zheng

Gaseous ammonia (NH 3 ), a highly corrosive and toxic pollutant, poses significant risks to human health and the environment. This study addresses the challenge of trace NH 3 removal by synthesizing carboxylic acid-functionalized silica aerogels (CMSA-X) through a simple, cost-effective two-step grafting approach. The fabricated CMSA-4 aerogel exhibited a high -COOH group content (4.13 mmol·g −1 ) and a stable nanoporous structure, enabling reversible and highly selective adsorption for trace gaseous ammonia. It demonstrated exceptional adsorption capacity (3.90 mmol·g - 1 at 0.1 bar and 7.30 mmol·g -1 at 1.0 bar) and outstanding adsorption selectivity (selectivity coefficients of ∼43031 for NH 3 /N 2 and ∼2200 for NH 3 /CO 2 , respectively). The NH 3 -saturated CMSA-4 can be easily regenerated by low temperature treatment (393 K), and maintained 94% adsorption capacity after ten adsorption-desorption cycles. The superior dynamic adsorption capacities of 3.36 mmol·g - 1 under dry condition and 3.28 mmol·g - 1 under humid condition outperformed previously reported adsorbents. Field tests further confirmed its efficacy in removing trace NH 3 (2 ppm), achieving removal rates 1.6-3.8 times higher than commercial alternatives. In-situ diffusion infrared spectroscopy revealed that proton transfer caused OCO - NH 4 + formation is the key adsorption mechanism. This study provides a promising method to develop high-performance adsorbent for efficient trace NH 3 removal in environmental and industrial applications.

CAS / MDL: 4422-95-1 919-30-2
研究领域: 环境科学 · 材料科学
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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 38 ·19984-19990 · IF 11.301

Switchable molecular sieving of a capped metal organic framework membrane

Shuai Zhang,Bo Gui,Teng Ben,Shilun Qiu

Crystalline microporous membranes are promising materials as they have confined functional channels for molecular sieving and adsorption–diffusion. To date, a convenient method to control the permselectivity of a microporous membrane has remained a challenge. Herein, a functional MOF with an azobenzene side group was fabricated into a continuous, defect-free membrane and the surface could be conveniently covered using β-cyclodextrin through adjusting the configuration of azobenzene via vis light. Thus, the resulting β-CD@UiO-68-azo membrane exhibits enhanced ultra-high H2/CO2 permselectivity and the performance can be controlled by reversible adsorption/desorption of capped β-CD.

研究领域: 材料科学 · 化学工程
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2024 · IF 10.8

Electrochemically Switchable Sulfurized Polyacrylonitrile for Controllable Recovery of Copper in Wastewater Based on Reversible Adsorption/Desorption Regulation

Shengli Wang,Chi Ding,Jinna Zhang,Nanqi Ren,Yanbiao Liu,Shijie You

Within the context of circular economy and industrial ecology, adsorption offers an effective manner for recycling resources from wastewater, but controllable desorption remains a challenge. Inspired by metal–thiol binding and reversible thiol–disulfide redox transformation in biological systems, this study reports the development of a reversible adsorption/desorption (RAD) system for controllable recovery of copper based on electrochemically switchable sulfurized polyacrylonitrile (SPAN). Density functional theory calculations offered theoretical prediction for the formation of S–Cu bonds and reversible weak interaction between S–S bonds and Cu2+. The SPAN anchored onto titanium suboxide ceramic foam (SPAN@TiSO) could regulate Cu2+ adsorption/desorption stimulated by the electrode potential, indicated by the adsorption capacity of 243.3 mg g–1 (30 min) at 0.2 V vs SHE and a desorption efficiency of 98.4% (5 min) at 0.8 V vs SHE. Electrochemical analysis revealed that the reversible redox transformation of S–S/–S– groups in SPAN was responsible for selective adsorption and rapid desorption in response to the electrode potential. This study provides a proof-of-concept demonstration of an electrochemically switchable polymer to build up a reversible RAD system for controllable recovery of heavy metals in wastewater, making value-added resource recovery more efficient, more intelligent, and more sustainable.

研究领域: 环境科学 · 材料科学 · 电化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Efficient selection and reversible adsorption of sulfur dioxide by methylated polyethylenimide supported by porous carbon microspheres

Shaohe Wang,Jiansong Ma,Yingrong Ye,Sen Chen,Jianwen Tian,Huiping Chen,Hailong Peng,Jun Du

Solid-supported materials are extensively utilized for SO 2 capture. Polytertiary amine compounds, which are abundant in tertiary amine groups, efficiently capture SO 2 . In this study, we propose the loading of methylated polyethylenimide (mPEI), which is rich in tertiary amine groups, into chitin-derived carbon microspheres (NCMs), which have a robust pore structure and large surface area. The produced adsorbent (mPEI@NCMs) showed good performance for capturing SO 2 . Further, the adsorption capacity of mPEI@NCMs for SO 2 at 25 °C and 1 bar was 12.23–18.12 mmol/g, whereas at 25 °C and 0.01 bar, it was 4.58–6.96 mmol/g. The mPEI@NCMs sample showed good selectivity for adsorbing SO 2 from mixtures containing N 2 and CO 2 . Furthermore, mPEI@NCMs showed a good reversible adsorption capacity for SO 2 .

CAS / MDL: 9005-70-3
研究领域: 环境科学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

Construction of hydrophobic interface on natural biomaterials for higher efficient and reversible radioactive iodine adsorption in water

Baozhan Zheng,Xiaoxia Liu,Jing Hu,Fengyi Wang,Xuan Hu,Yue Zhu,Xu Lv,Juan Du,Dan Xiao

For the pollution of radioactive materials, it is of great importance to develop efficient adsorbents for radioactive iodine adsorption in aqueous solution. In this work, a simple and green strategy was developed to construct hydrophobic surface on natural cotton fibers (n-CF) based on organic-soluble carbon dots (OCDs) for the first time. The results demonstrated the successful constructed hydrophobic n-CF@OCDs expressed excellent stability and selectivity for iodine (I 2 ) adsorption in water. The maximum adsorption capacity for I 2 on n-CF@OCDs is calculated to be 190.1 mg g −1 , which is about 6.8 times higher than that of n-CF (28.1 mg g −1 ), this highly I 2 adsorption efficiency should be attributed to the hydrophobic properties of adsorbent. The adsorption mechanism was also discussed in this work. In addition, the adsorbed I 2 could be desorbed easily with a simple reductive process at ambient conditions, which can lead to not only the restore of I 2 but also the recycling of adsorbent, illustrating their good practicability. Furthermore, this universal strategy can also be used for construction of hydrophobic surface on various natural biomaterials, demonstrating its potential application in constructing of hydrophobic surface and used for the adsorption and removal of nonpolar pollutions or radioactive waste in aqueous solutions.

研究领域: 环境科学 · 材料科学
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Separations · 2023 ·Vol. 10 ·期 10 ·523 · IF 2.6

Adsorption of Phenols from Aqueous Solution with A pH-Sensitive Surfactant-Modified Bentonite

Xiangfen Cui,Jingmei Liao,Huaying Liu,Wei Tang,Cheng Tie,Senlin Tian,Yingjie Li

The presence of organic pollutants in wastewater remains a prominent environmental concern due to the related ecological and health hazards. In response, this study employs an adsorptive methodology to address the removal of phenol and catechol, utilizing an organo-bentonite material modified with a pH-responsive switchable surfactant, dodecyldimethylamine oxide (C12DAO). The synthesized organo-bentonite (C12DAO-Bt) manifests commendable thermostability resulting from thermogravimetric analyses. The adsorption capacities of C12DAO-Bt concerning phenol and catechol intensify with the augmentation of the C12DAO/bentonite mass ratio. The utmost adsorption capacities of 150C12DAO-Bt, deduced through a pseudo-second-order kinetic model, stand at 5.72 mg·g−1for phenol and 5.55 mg·g−1for catechol, respectively. Subject to modification by a pH-responsive surfactant, conditions leaning towards weakly acidic and neutral conditions (pH = 6~7) are conducive to the adsorption of phenolic compounds. Conversely, alkaline conditions (pH = 8~9) facilitate the dissociation of adsorbates from adsorbents. The augmentation of cationic strength within the examined scope incites the adsorption procedure while impeding the desorption efficacy. In the case of cationic species with comparable ionic strengths, Na+exhibited a superior effect on the adsorption–desorption dynamics of phenol, while Ca2+exerts a more pronounced effect on those of catechol. Moreover, even following five consecutive acid–base regulation cycles, C12DAO-Bt retains a relatively high adsorption capacity and desorption efficacy, which underscores its exceptional regenerative capacity for removing phenolic compounds from wastewater.Keywords:pH-responsive surfactants;organic bentonite;reversible adsorption;phenolic pollutants;wastewater

研究领域: 环境科学 · 化学工程
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ADVANCED MATERIALS · 2017 ·Vol. 30 ·期 4 ·1700104 · IF 19.791

Enhanced Capacity and Rate Capability of Nitrogen/Oxygen Dual-Doped Hard Carbon in Capacitive Potassium-Ion Storage

Jinlin Yang,Zhicheng Ju,Yong Jiang,Zheng Xing,Baojuan Xi,Jinkui Feng,Shenglin Xiong

The intercalation of potassium ions into graphite is demonstrated to be feasible, while the electrochemical performance of potassium-ion batteries (KIBs) remains unsatisfying. More effort is needed to improve the specific capacity while maintaining a superior rate capability. As an attempt, nitrogen/oxygen dual-doped hierarchical porous hard carbon (NOHPHC) is introduced as the anode in KIBs by carbonizing and acidizing the NH 2 -MIL-101(Al) precursor. Specifically, the NOHPHC electrode delivers high reversible capacities of 365 and 118 mA h g −1 at 25 and 3000 mA g −1 , respectively. The capacity retention reaches 69.5% at 1050 mA g −1 for 1100 cycles. The reasons for the enhanced electrochemical performance, such as the high capacity, good cycling stability, and superior rate capability, are analyzed qualitatively and quantitatively. Quantitative analysis reveals that mixed mechanisms, including capacitance and diffusion, account for the K-ion storage, in which the capacitance plays a more important role. Specifically, the enhanced interlayer spacing (0.39 nm) enables the intercalation of large K ions, while the high specific surface area of ≈1030 m 2 g −1 and the dual-heteroatom doping (N and O) are conducive to the reversible adsorption of K ions.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 固态化学 · 电极材料
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JOURNAL OF HAZARDOUS MATERIALS · 2022 · IF 14.224

Efficient adsorption removal of NO2 by covalent triazine frameworks with fine-tuned binding sites

Yuanmeng Tian,Ming Kong,Zeyu Tao,Chen Yang,Shanshan Shang,Qinfen Gu,Daniel C.W. Tsang,Liangchun Li,Jin Shang

One promising method for mitigating low-temperature and low-concentration NO 2 pollution is selective adsorption using porous solid materials. However, the corrosive nature of NO 2 renders the development of an adsorbent with high and cyclable NO 2 uptake a formidable challenge. Herein, we attempted to address this challenge by developing a microporous covalent triazine framework (CTF) as effective adsorbents for NO 2 capture, achieving unprecedented high cyclable capacity enabled by simultaneous high adsorbent stability and moderate adsorption affinity via tuning specific binding sites. Using dynamic column breakthrough experiments, we demonstrated that the pristine CTF exhibited a high NO 2 adsorption capacity (dry: 3.83 mmol/g; wet: 5.26 mmol/g) overtaking most reported solid adsorbents, thanks to abundant active sites (e.g., nitrogen/carbon/triazine rings). Post-synthesis converted the surface nitrogen to protonated nitrogen site and further to transition metal site affording more effective binding sites that allows for moderately strong adsorption, resulting in elevated NO 2 adsorption capacity (dry: 6.11 mmol/g; wet: 8.97 mmol/g) and a highest reversible NO 2 adsorption (retaining 91 % and 64 % at dry and wet conditions after five cycles, respectively), as illustrated by our mechanistic study using in situ DRIFTS and DFT calculations. This work affords not only promising adsorbents for real-world applications in mitigating NO 2 pollution, but also a strategy of developing robust adsorbents with desired affinity generally applicable to adsorptive capture of corrosive and toxic gases.

CAS / MDL: 7791-13-1
研究领域: 环境科学 · 材料科学
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ELECTROCHIMICA ACTA · 2017 · IF 4.798

Reduced Polysulfide Shuttle Effect by Using Polyimide Separators with Ionic Liquid-based Electrolytes in Lithium-Sulfur Battery

Yanqing Wang,Zengqi Zhang,Masaki Haibara,Deye Sun,Xiaodi Ma,Yongcheng Jin,Hirokazu Munakata,Kiyoshi Kanamura

In this research, we demonstrate a new method for reducing the shuttle effect by confining polysulfide in separator area through the use of polyimide (PI) separator with reversible adsorption functions in lithium-sulfur batteries. As a comparison, the cells with polypropylene (PP) separators which have no function to adsorb dissoluble polysulfide show a result that the content of sulfur on lithium anode surface is increased up to 63.94% after 100th cycles with the content of N-methyl-N-butylpiperidinium bis-(trifluoromethylsulfonyl) imide (PP 14 TFSI) in the mixture electrolyte increasing. This result illustrates that the migration and reaction between dissolved polysulfide in PP 14 TFSI and lithium cannot be neglected although the solubility of polysulfide is slight in PP 14 TFSI solvent. However, when PI separators are introduced, besides improving the wettability with PP 14 TFSI-based electrolytes, experimental results also show that the PI separator has a reversible adsorption function to dissoluble polysulfide which is used to confining polysulfide in separator area to a certain extent due to the abundant nitrogen-, oxygen-containing functional groups in PI skeleton. What’s more, PI separator can decreases the sulfur content on lithium surface after cycling to 17.92% which decreases greatly than that with PP separator and improves its electrochemical performance.

研究领域: 材料科学 · 电化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

The immobilization of Sr(ll) and Co(ll) via magnetic easy-separation organophosphonate-hydroxyapatite hybrid nanoparticles

Keren Lu,Zhiren Zhao,Jin Cui,Cuiyun Bai,Hongling Zhang,Xuetao Zhao,Fengyun Wang,Mingzhu Xia,Yanru Zhang

The magnetic Hexamethylene diamine tetramethylene phosphonic acid (HDTMP)-hydroxyapatite nanoparticles (HD-MHAP) were firstly prepared and applied for the immobilization of radioactive Sr 2+ (Strontium ion) and Co 2+ (Cobalt ion). The molar ratio of organic phosphine in HDTMP to total phosphorus was 10% (10HD-MHAP) and can also be easily separated from aqueous solution. At the equilibrium concentration of Sr 2+ and Co 2+ (200 mg/L), the adsorption capacity of MHAP and 10HD-MHAP on Co 2+ was 28.4 mg/g and 172.3 mg/g, respectively and for Sr 2+ , the adsorption capacity was 54.9 mg/g and 320.7 mg/g. Additionally, the desorption percentage of Sr 2+ (%) and Co 2+ (%) was very low, which was 0.66 and 1.61, respectively. This is significant because the irreversible adsorption of HDTMP/Fe 3 O 4 /HAP composite for Sr 2+ and Co 2+ ensures the captured radionuclides will not be released back into the aquatic systems. Moreover, the affinity between HDTMP and HAP and the coordination of HDTMP and Sr 2+ or Co 2+ was probed by Multiwfn wavefunction analysis. The results indicated that the formation of a ternary surface complex of MHAP-HDTMP-M (Sr 2+ or Co 2+ ) was the key to the excellent immobilization performance of HD-MHAP composite for Sr 2+ or Co 2+ .

研究领域: 环境科学 · 材料科学 · 放射化学
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JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY · 2013 ·Vol. 67 ·期 3 ·442-450 · IF 1.66

The preparation and characterization of photo-responsive sol–gel materials for 2,4-dichlorophenoxyacetic acid by surface imprinting

Gong Cheng-Bin,Yang Yu-Zhu,Gao Chao,Tang Qian,Chow Cheuk-Fai,Peng Jing-Dong,Lam Michael Hon-Wah

Abstract The primary objective of this work is to develop a photo - responsive surface molecularly imprinted polymer (SMIP) for 2,4 - dichlorophenoxyacetic acid (2,4 - D) to overcome the shortcomings of conventional molecularly imprinted polymers. A photo - responsive functional monomer was firstly prepared by covalent connecting azobenzene and 2,4 - D. The photo - responsive SMIP was then prepared on SiO 2 nanoparticles via sol–gel process, and 2,4 - D was removed via hydrolysis in acid. The SMIP shows specific affinity to 2,4 - D and reversible uptake and release of 2,4 - D upon alternate irradiation at 365 and 440 nm, respectively. The favorable binding strength of the imprinted receptor sites in the SMIP for 2,4 - D is found to be 2.51 × 10 4  M −1 . Density of receptor sites in the SMIP material is 10.59 μmol/g SMIP. The SMIP requires a shorter time to reach equilibrium than does the conventional molecularly imprinted polymer. The well - defined core - shell structure was clearly visualized by high resolution transmission electron microscopy. Graphical Abstract

研究领域: 材料科学 · 环境科学
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NEW JOURNAL OF CHEMISTRY · 2024 · IF 2.7

Underlying molecular mechanism of topical fluid foam with microsphere assistance

Chunbao Du,Zichun Feng,Changji Yin,Xingang Jia,Yameng Zhao,Yuan Cheng

Topical fluid foam has a considerable application value in the field of topical medicine due to benefits such as simple uniform distribution on the skin’s surface, ease of use, and good patient compliance. The longevity of topical fluid foam is crucial in assessing its therapeutic success, particularly in complicated heat and salt settings. Nanoparticles could improve the stability of topical fluid foam, but their density, size, homogeneity, and surface characteristics are difficult to be taken into consideration simultaneously, resulting in the unclear underlying molecular mechanism. In this work, the raspberry-like microspheres (RM) with a high cross-linked structure were synthesized using a simple one-step dispersion polymerization. The stabilizing foam function of RM in fluid foam was connected to their size, surface chemical characteristics, and foaming temperature. The effect of gravity on foam stability induced by liquid flow acceleration of RM competed fiercely with their size and surface chemical characteristics, and this competitive connection was highly influenced by temperature. The unique surface properties of RM1 (polymerization time of 1h) allowed for their irreversible adsorption at the gas-liquid interface following sodium dodecyl sulfate (SDS) adsorption. RM1 could counteract the harmful effect of gravity on foam stability at a high temperature of 60 oC, enhancing the surface elasticity of the liquid film and improving foam stability. This work is a fantastic starting point for the development of novel nanomaterials to improve the stability of topical fluid foam for pharmaceutical and medical applications.

CAS / MDL: 78-67-1 7647-14-5
研究领域: 药学 · 材料科学 · 胶体与表面化学
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