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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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Colloid and Interface Science Communications · 2021 · IF 4.914

Preparation of porous carbon materials by polyphosphazene as precursor for sorption of U(VI)

Xiaopeng Liu,Yan Liu,Yun Wang,Dingzhong Yuan,Jinbiao Liu,Jia Wei Chew

Polyphosphazene was synthesized by ultrasonic using 4,4-diaminodiphenyl ether and hexachlorocyclotriphosphazene (HCCP) as precursors. Next, it was further carbonized and functionalized to prepare the carboxylic-acid functionalized N, P co-doped carbon materials (NPCs-COOH). The structure of NPCs-COOH was characterized by FTIR , SEM and XPS . The sorption performance of NPCs-COOH for U(VI) in solution were determined under diverse factors including pH values, initial concentration, equilibrium time and reaction temperature. The results indicated that the optimal pH value was 5.0 and the equilibrium time was 60.0 min. The maximum sorption capacity from experimental results was 425.16 mg/g. The analysis results of the sorption thermodynamics and kinetics showed that the NPCs-COOH had excellent sorption performance so that it can be utilized on removal of U(VI) effectively in aqueous solution.

研究领域: 材料科学 · 环境科学 · 化学工程
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JOURNAL OF APPLIED POLYMER SCIENCE · 2012 ·Vol. 128 ·期 6 ·3925-3932 · IF 1.289

Effects of connection mode between carboxyl groups and main chains on polycarboxylate superplasticizer properties

Shenghua Lv,Haobo Ju,Chaochao Qiu,Yujuan Ma,Qingfang Zhou

Preparation and characterization of polycarboxylate superplasticizers of IPCs ( copolymer of itaconic acid and allyl polyoxyethylene ether) and MPCs (copolymer of maleic anhydride and allyl polyoxyethylene ether) are shown. The difference between IPCs and MPCs is that half of the carboxyl groups of IPCs indirectly connect to the main chains through methylene. The effects of the carboxyl group-main chain connection mode on the properties of IPCs and MPCs were investigated by assessing the paste fluidity and the pore diameters and compressive strength. The interaction between IPCs (MPCs) and cement were revealed by zeta-potential and the adsorption amount. The results indicated that the indirect connection mode favorably improved paste fluidity, decreased pore diameters, and increased the compressive strength compared with the direct connection mode. This is likely because that when carboxyl groups are connected to the main chains indirectly, more moving space allows easier adsorption on cement particles. © 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013

研究领域: 材料科学 · 化学工程
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CATALYSIS LETTERS · 2022 ·Vol. 153 ·期 10 ·3092-3102 · IF 2.936

Rational Design of Phosphotungstate Hybrids with Dual Active Sites for Efficient Catalytic Oxidation

Li Yongwei,Pan Shiguang,Han Ronghuan,Gao Jian,Liu Dan,Gui Jianzhou

Phosphotungstate organic–inorganic hybrid materials [CH 2 COOHmim]H 2 PW 12 O 40 , [(CH 2 ) 3 COOHmim]H 2 PW 12 O 40 and [Bmim]H 2 PW 12 O 40 with dual catalytic oxidation active centers, including carboxylic acid group and phosphotungstate anion, were synthesized from bisulfate acidic ionic liquid in a one-step method, and well characterized by XRD, 1 H NMR, 13 C NMR, 31 P NMR, FT-IR, and UV–vis. Then, these obtained hybrids were employed as catalysts for the selective oxidation of N-methylmorpholine (NMM) into N-methylmorpholine-N-oxide (NMMO) using H 2 O 2 as an oxidant. As expected, the –COOH functionalized hybrids showed much better activity than the conventional hybrid [Bmim]H 2 PW 12 O 40 , and even much better than the mixture of corresponding ionic liquid and H 3 PW 12 O 40 , suggesting the existence of dual active species and synergistic effect between the cation and phosphotungstate in hybrids. The best catalyst [(CH 2 ) 3 COOHmim]H 2 PW 12 O 40 gave an NMM conversion of 98.7% and selectivity to NMMO of 98.8%. The structural characterization by 31 P NMR, UV–vis, Raman and 13 C NMR analysis of the catalyst before and after oxidation demonstrated the existence of the catalytic active species PW 12 O 40 3− and peroxy carboxylic acid. Finally, a possible catalytic mechanism has been proposed. Graphical Abstract

研究领域: 材料化学 · 催化化学
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CHEMOSPHERE · 2022 · IF 8.943

Heterogeneous compositions of oxygen-containing functional groups on biochars and their different roles in rhodamine B degradation

Danping Wu,Quan Chen,Min Wu,Peng Zhang,Liping He,Yihui Chen,Bo Pan

The reactivity of pyrogenic carbon has attracted a great deal of research attentions recently. The oxygen-containing structures are rich on the surface of biochars, and involved in accepting and donating electrons during the interactions between biochar and organic contaminants . In this work, the species and content of oxygen-containing functional groups on biochar surface were regulated through chemical modification, and batch sorption/degradation experiments were carried out for rhodamine B (RhB). Based on the comparison of surface functional groups, biochars produced below 200 °C mediated RhB degradation through phenol hydroxyl group, while semiquinone and carboxylic acid groups were the main reaction active sites for biochars produced at higher than 500 °C. Considering that various biochar properties play roles in mediating organics degradation , the strategies in manipulating biochar properties should be carefully considered.

研究领域: 环境科学 · 材料科学
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY · 2014 ·Vol. 2014 ·期 20 ·3172-3177 · IF 2.965

Synthesis of Magnetic Fe3O4@C Nanoparticles Modified with –SO3H and –COOH Groups for Fast Removal of Pb2+, Hg2+, and Cd2+ Ions

Zhiming Chen,Zhirong Geng,Zhiyang Zhang,Lianbing Ren,Tingxian Tao,Renchun Yang,Zuxiang Guo

Graphical Core–shell magnetic Fe 3 O 4 @C nanoparticles are functionalized with sulfonic and carboxylic acid groups and employed to capture heavy metal ions in aqueous media. The magnetic Fe 3 O 4 @C nanoparticles can be easily separated with an external magnet and possess rapid removal kinetics, high adsorption capacities, and removal efficiencies for Pb 2+ , Hg 2+ , and Cd 2+ ions from aqueous solution. Core–shell magnetic Fe 3 O 4 @C nanoparticles functionalized with sulfonic and carboxylic acid groups were synthesized and employed to capture heavy metal ions in aqueous media. The Fe 3 O 4 cores possess unique magnetic properties for adsorbent separation, and the –SO 3 H and –COOH groups attached to the surface of the carbon shells determine the efficiency of heavy metal ion removal. Batch adsorption experiments showed that Pb 2+ , Hg 2+ , and Cd 2+ ions can be completely and quickly removed by the Fe 3 O 4 @C nanoparticles. The equilibrium was established within 5 min, and the maximum adsorption capacities of the Fe 3 O 4 @C nanoparticles toward Pb 2+ , Hg 2+ , and Cd 2+ ions were 90.7, 83.1, and 39.7 mg/g, respectively. The removal efficiencies were 96.3, 98.1, and 93.8 % for Pb 2+ , Hg 2+ , and Cd 2+ ions, respectively. This work provides a facile and general approach to synthesize magnetic functional nanocomposites for wastewater treatment.

研究领域: 环境科学 · 材料科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2017 · IF 3.582

Preparation and properties of ion exchange membranes for PEMFC with sulfonic and carboxylic acid groups based on polynorbornenes

Chao Wang,Zhiming Feng,Yang Zhao,Xue Li,Weiwei Li,Xiaofeng Xie,Shubo Wang,Hua Hou

Bifunctional groups proton exchange membranes (PEMs) with sulfonic and carboxylic acid groups were prepared via ring-opening metathesis polymerization (ROMP) based on norbornene derivatives. The sulfonic acid groups and the carboxylic acid groups were introduced into the polymer chains in the form of sulfonyl chloride and ester separately. Because of the introduction of these two groups, not only greatly improve the proton conductivity of PEMs, but also improve their mechanical performance and thermal stability. When the highest proton conductivity of the bifunctional groups PEMs is 123.96 mS/cm, its proton conductivity is higher than that of Nafion ® 117 at 25 °C.

CAS / MDL: 77-73-6
研究领域: 化学工程 · 材料科学
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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

Active Functional Groups and Adjacent Dual-Interaction Strategies Enable Perovskite Solar Cells to Prosper: Including Unique Morphology and Enhanced Optoelectronic Performance

Yaxin Deng,Xin Li,Rui Wang

Excellent photoelectric properties entail perovskite solar cells with established position prevailing in the new-generation photovoltaic landscape. However, the traditional solution preparation inevitably yields numerous defects, which eventually bloom ion migration and lead to the gradual collapse of perovskite. Here, phthalic acid (PHA) with adjacent carboxylic acid groups (−COOH) is used to passivate defects and regulate the morphology of perovskite films. Based on density functional theory (DFT) calculations, the two adjacent −COOH of PHA construct a dual interaction with the uncoordinated Pb2+ of perovskite, thus significantly enhancing the passivation effect. Furthermore, the double-bonding interaction brought by PHA induces a unique surface-protruding morphology on perovskite films, which may act as a green channel for charge delivery, ultimately increasing the photo-generated current of perovskite solar cells (PSCs) to some extent. Under full-air preparation conditions, the PHA-optimized champion PSCs showed an efficiency of 20.02% with a boosted short-circuit current of 22.80 mA cm–2, showing one of the best performances in all-air preparation until now. Meanwhile, PHA-PSCs exhibited brilliant stability. In short, this work provides some reliable and flexible guidance for the design of small-molecule additives.

CAS / MDL: 88-99-3 100-21-0
研究领域: 材料科学 · 光伏技术 · 理论计算
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Journal of Materials Chemistry A · 2016 ·Vol. 4 ·期 7 ·2537-2549 · IF 8.262

Highly efficient macroporous adsorbents for toxic metal ions in water systems based on polyvinyl alcohol–formaldehyde sponges

Yanxiong Pan,Zhi Liu,Weicai Wang,Chao Peng,Kai Shi,Xiangling Ji

A series of macroporous adsorbents based on polyvinyl alcohol–formaldehyde (PVF) sponges was prepared using redox-initiated grafting polymerization of acrylamide (AM) followed by hydrolysis under alkaline conditions. The as-prepared sponges display average pore sizes in the range of 60–90 μm and interconnected pores with a porosity of approximately 90%. Elementary analysis confirmed that the amide groups in AM grafted PVF (PVF-g-GAM) have been rapidly converted into sodium carboxylate and the hydrolysis degree (HD) reaches approximately 65.5% within 6 h. The PVF-g-GAA (hydrolyzed PVF-g-GAM) sponges possess excellent water absorption performance with the ability to reach water absorption equilibrium within a few seconds and a saturated absorption capacity more than 300 g g−1. Importantly, the PVF-g-GAA can be used as adsorbents to remove toxic metal ions, such as Cu2+, Pb2+ and Cd2+, in wastewater efficiently due to the existence of abundant carboxylate groups in the abovementioned network. In single metal ion systems, the sponges could reach adsorption equilibrium within 10 min and the adsorption kinetics fit well with a pseudo-second order kinetic equation. The influence of pH and types of metal ions on the adsorption capacities have also been investigated extensively. PVF-g-GAA-20 displays high adsorption performances with maximum adsorption capacities for Cu2+, Pb2+ and Cd2+ up to 2.50, 3.20 and 3.15 mmol g−1 at pH 5.11, respectively. The equilibrium adsorption isotherm demonstrated that the adsorption equilibrium of the PVF-g-GAA-20 for Cu2+, Pb2+ and Cd2+ ions follows the Langmuir isotherm model very well with maximum adsorption capacities approximately 4.00, 3.97 and 3.34 mmol g−1, respectively. In the binary metal ion coexistence systems, including Cu2+/Pb2+, Cu2+/Cd2+ and Pb2+/Cd2+ mixtures, PVF-g-GAA-20 displayed excellent absorption selectivity for Cu2+ and Pb2+ and the values of and were 13.4 and 7.14, respectively. It can be noted that the adsorption capacities for the abovementioned three metal ions slightly decreased with the variation of ionic strength in the range of 0.01–0.08 M. The sample also exhibited a quick desorption procedure of less than 10 min and excellent reusability of atleast six re-cycles. The adsorption mechanism was also discussed. The PVF-g-GAA sponges are definitely ideal adsorbents for removing/separating toxic metal ions in waste/polluted water bodies.

研究领域: 环境科学 · 材料科学
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FOOD HYDROCOLLOIDS · 2021 · IF 9.147

Effect of surface charge density of bacterial cellulose nanofibrils on the rheology property of O/W Pickering emulsions

Yilan Wu,Xingzhong Zhang,Dan Qiu,Ying Pei,Yan Li,Bin Li,Shilin Liu

In this study, the effect of surface charge density of bacterial cellulose nanofibrils (BCNF) on the rheological characteristics of O/W Pickering emulsions was investigated by regulating the fibril charge density. BCNFs with different carboxylate group contents (0.66, 0.90 and 1.16 mmol/g dry cellulose, representing as TOBC-a, -b, and -c) were obtained by 2,2,6,6-tetramethylpiperidine-nitrogen-oxide (TEMPO) oxidation . These oxidized products were used as Pickering stabilizers to prepare O/W Pickering emulsions. Diffusing wave spectroscopy (DWS)-based microrheology was utilized to reflect the rheological features of emulsions. TOBC-a stabilized emulsion had a lower macroscopic viscosity, lower elasticity, and better fluidity. It was because a weaker fiber network was formed in the continuous phase during the ultrasonication emulsification . The influences of pH and ionic strength on the rheological properties of high-charged TOBC-c stabilized emulsions were also investigated. The emulsion prepared at pH 3.0 exhibited the highest viscosity. It was probably because the inter-fibrils electrostatic repulsion was weakened by the addition of HCl, and the hydrogen bonding interaction became dominant due to the protonation of carbohydrate group. At pH 11, the emulsion viscosity was lowest, which was resulted from the destruction of the intra-fibrils hydrogen bonds. With the NaCl concentration increased, the emulsion viscosity and elasticity increased. It was induced by the fact that the charge shielding effect of NaCl facilitated the formation of a tighter fibrils network in the continuous phase. These results have the potential to provide a guide for developing emulsion-based products with appropriate fluidity to broaden the practical application of emulsion.

研究领域: 食品科学 · 材料科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2020 · IF 4.939

Tetra-carboxylic acid based metal-organic framework as a high-performance bifunctional electrocatalyst for HER and OER

Qi Qiu,Tao Wang,Linhai Jing,Kun Huang,Dabin Qin

Tetra-carboxylic acid based 3D porous MOFs 1 and 2 , named {[Co 2.5 (L)]·5H 2 O} n and 0.5{[Cu(L)]·2H 2 O} n (L = 4,4′-di(ethoxy)biphenyl-3,3′,5,5′-tetra-(phenyl-4-carboxylic acid)), bearing metal clusters have been facilely constructed by hydrothermal synthesis . Structural studies indicate that 1 presents a 3-nodal (4, 4, 8)-connected topology with the point notation of {4 4 .6 2 }2{4 8 .6 7 .8 13 }, while 2 shows a uninodal (4, 4)-connected network with point symbol of {4 4 .6 2 }. The pristine MOFs are directly utilized for electrocatalysis and poor HER activities are obtained in alkaline solution, which promote the further design and fabrication of a mixed-metal Co/Cu-MOF ( 3 ). As expected, 3 shows significantly improved performances for HER with overpotential of 391 mV (10 mA cm −2 current density), low Tafel slope of 94 mV dec −1 and long-term operation stability (14 h). More importantly, the direct utilization of 3 for accelerating OER also presents a fascinating performance in overpotential at 10 mA cm −2 current and durability. The above electrocatalytic performance of pristine 3 can be ascribed to the result of hybridizing strategy for constructing MOFs under hydrothermal procedure, which may favorably produces synergistic effect and more open metal sites. This work provides in-depth understanding of hybrid pristine MOFs for electrocatalysis.

CAS / MDL: 1308-06-1
研究领域: 材料科学 · 电化学
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Molecular Catalysis · 2017 · IF 0

Aerobic oxidation of cyclohexane catalyzed by graphene oxide: Effects of surface structure and functionalization

Yepeng Xiao,Jincheng Liu,Kaihong Xie,Weibin Wang,Yanxiong Fang

Despite extensive development efforts on new catalysts for cyclohexane oxidation, current commercial processes are still desirable to further decrease the economic and environmental costs in the oxidation procedures. In this study, the catalyst properties of metal-free functionalized graphene oxide (GO) in the selective oxidation of cyclohexane is investigated to understand the effects of structure, functional groups and oxygen-containing groups. Both GO sheets and nano graphene oxide (NGO) sheets possess high cyclohexane conversions of 16.7% and 17.7% comparable to that of metal catalysts in the aerobic oxidation of cyclohexane. The higher catalytic activity of NGO sheets is caused by the smaller size and the higher content of −COOH. Within the oxygen-containing groups, the carboxylic acid groups on the surfaces of GO are supposed as the active site for the generation of O 2 − radical, which is the active oxygen species in this catalytic oxidation process.

研究领域: 催化化学 · 材料科学 · 环境化学
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