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MACROMOLECULES · 2020 · IF 5.918

Terminal Hydrophilicity-Induced Dispersion of Cationic Waterborne Polyurethane from CO2-Based Polyol

Runan Gong,Han Cao,Hongming Zhang,Lijun Qiao,Fosong Wang,Xianhong Wang

Cationic waterborne polyurethane (CWPU) was initially developed as a specific adhesive for anionic surface but now is ubiquitous in innovative material systems such as poly(ionic liquid)s, polyelectrolytes, antibacterial coatings, and drug carriers. However, state-of-the-art CWPU faces imperative challenges like easy degradation and poor water resistance, which is caused by excessive incorporation of internal emulsifiers with tertiary amines into the backbone than necessary, since emulsification performance of cationic internal emulsifier is much less efficient compared with the anionic analogue. Here, a terminal internal emulsifier-induced efficient dispersion strategy was developed. Taking oligo(carbonate ether) diol (a CO2-polyol from telomerization of CO2 and propylene oxide) as example, stable CWPU with only 1.00 wt % internal emulsifier was prepared. An emulsifying capacity parameter was introduced to quantitatively evaluate the emulsification performance of internal emulsifier according to its steric hindrance and mobility, and the terminal internal emulsifier was proven to show the highest emulsification performance. The terminal hydrophilicity-induced dispersion strategy exhibits excellent universality for a broad range of oligomer diols, effective not only for CO2-polyols but also for widely used polyether polyols and polyester polyols, affording CWPU with excellent water resistance. Therefore, the chemistry disclosed here paves a way for a vast number of water- and oxidation-resistant CWPUs which were hardly available until now.

✓ 已验证 DOI 高影响因子
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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

Molecularly Homogenized Composite Membranes Containing Solvent-Soluble Metallocavitands for CO2/CH4 Separation

Tongxin Liu,Ruili Zhang,Guang-Rui Si,Bin Liu,Yabo Xie,Lin-Hua Xie,Jian-Rong Li

The rational design of mixed matrix membranes (MMMs) combining appropriate additives and industrial processable polymers offers a new prospect for highly efficient membrane separations. However, the difficulty in their fabrication due to the lack of processability of most additives and the formation of segregated filler domains in polymer matrices hampers the development and application of MMMs. Herein, we present two new zirconocene-based metallocavitands (ZRA and ZRT) and a series of MMMs fabricated by blending ZRA, ZRT, and MOC-1-NH2 (a zirconocene-based metal–organic cage) with the polyimide (6FDA-DAM), respectively. It was found that ZRA exhibited high thermal stability and good solubility in various solvents, which can be homogeneously mixed with polymers to prepare ZRA-based MMMs without any indication of filler agglomeration. Compared to the pure 6FDA-DAM membrane, a low ZRA-loading MMM (ZRA-2.2%) exhibited better mechanical properties and 50% improved CO2 permeability for CO2/CH4 separation. ZRA-2.2% also exhibited a good performance after 6 months of aging and significantly alleviated the plasticization effect under high pressures. These results suggest the great potential of the ZRA-2.2% for CO2/CH4 separation and that the simple metallocavitands may serve as promising additives in fabricating MMMs for gas separations.

✓ 已验证 DOI 高影响因子
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LANGMUIR · 2018 · IF 3.789

Structure Design of Low-Temperature Regenerative Hyperbranched Polyamine Adsorbent for CO2 Capture

Hui He,Hanying Tang,Xingjuan Chen,Xudong Hou,Xiaochong Zhou,Hong Chen,Shanyan Wu,Shuangfei Wang

A novel low-temperature regenerative hydroxy-functionalized hyperbranched polyamine adsorbent (0.16OH-HBPA) for CO2 capture was readily prepared using glutaraldehyde to cross-link amino-terminated hyperbranched polymers (HBP) and functionalized with glycidol, followed by the reduction of the imino groups of 0.16OH-HBPA to alkyl aminos using NaBH4. Here, the HBP has been prepared through the one-pot reaction between pentaethylenehexamine and methyl acrylate. The as-prepared 0.16OH-HBPA adsorbent showed a high adsorption capacity (4.05 mmol/g) for CO2 (concentration, 10%) in the presence of water at 25 °C, and the alkyl amino utilization efficiency reached 73%. More importantly, the CO2-adsorbed 0.16OH-HBPA showed excellent regenerative performance at low temperatures (85 °C, under pure CO2 gas) due to the introduced hydroxyl that can cooperatively adsorb CO2 via the amino groups to form stable carbamic acid. This process suppressed the formation of open-chain urea and cyclic urea and could overcome the disadvantages of high regeneration temperatures (≥90 °C, under pure inert gas) of CO2-adsorbed traditional solid amine adsorbents.

✓ 已验证 DOI 高影响因子
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Nanoscale Research Letters · 2018 ·Vol. 13 ·期 1 ·1-7 · IF 3.125

New Insights into CO2 Adsorption on Layered Double Hydroxide (LDH)-Based Nanomaterials

Tang Nian,He Tingyu,Liu Jie,Li Li,Shi Han,Cen Wanglai,Ye Zhixiang

The interlamellar spacing of layered double hydroxides (LDHs) was enlarged by dodecyl sulfonate ions firstly, and then, (3-aminopropyl)triethoxysilane (APS) was chemically grafted (APS/LDHs). The structural characteristics and thermal stability of these prepared samples were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), reflectance Fourier transform infrared spectrometer (FTIR), thermogravimetric analysis (TG), and elemental analysis (EA) respectively. The CO 2 adsorption performance was investigated adopting TG and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The results presented that the CO 2 adsorption capacity on APS/LDHs was as high as 90 mg/g and showed no obvious reduction during a five cyclic adsorption-desorption test, indicating its superior performance stability. The DRIFTS results showed that both carbamates and weakly bounded CO 2 species were generated on APS/LDHs. The weakly adsorbed species was due to the different local chemical environment for CO 2 capture provided by the surface moieties of LDHs like free silanol and hydrogen bonds.

✓ 已验证 DOI 高影响因子
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JOURNAL OF MEMBRANE SCIENCE · 2011 · IF 3.673

Improvement of CO2/N2 separation characteristics of polyvinylamine by modifying with ethylenediamine

Shuangjie Yuan,Zhi Wang,Zhihua Qiao,Mingming Wang,Jixiao Wang,Shichang Wang

In this work, the idea of modifying the fixed carrier membrane for CO 2 separation by a cross-linking agent containing carriers to simultaneously improve the CO 2 -induced plasticization resistance, the CO 2 permeance and the CO 2 /N 2 selectivity of the membrane was suggested and confirmed. Polyvinylamine (PVAm), a polymer to prepare fixed carrier membrane for CO 2 separation, was synthesized by partial acidic hydrolysis of poly(N-vinylformamide) and further modified by using ethylenediamine (EDA). Elemental analysis, ATR-FTIR, XPS and XRD were employed to characterize the EDA modified PVAm. The result of ATR-FTIR and XPS showed that the EDA can effectively cross-link PVAm by the hydrogen bonds formed between amine groups of EDA and either amine or amide groups in PVAm. The composite membranes were developed by coating the PVAm–EDA mixed solutions with different mass ratio of EDA/PVAm ( m EDA / m PVAm ) on polysulfone (PS) ultrafiltration membrane. The effects of m EDA / m PVAm in coating solution and wet coating thickness on the gas performance of the PVAm–EDA/PS composite membranes were investigated. The PVAm–EDA/PS membrane prepared by using coating solution with proper m EDA / m PVAm (from 1 to 3) showed higher CO 2 permeance and much higher CO 2 /N 2 selectivity as well as better CO 2 -induced plasticization resistance than that of the PVAm/PS membrane. It is attributed to two factors: (1) the densification of polymer matrix by moderate hydrogen bond cross-linking; and (2) the increase of total carrier content in membrane. As CO 2 -induced plasticization resistance improves, the selective layer thickness of the PVAm–EDA/PS membrane can be further reduced to obtain a higher CO 2 permeance and a proper CO 2 /N 2 selectivity simultaneously. For CO 2 /N 2 gas mixture (20/80 by volume), the PVAm–EDA/PS membrane prepared by using coating solution with m EDA / m PVAm of 3 and 50   μm wet coating thickness displayed a CO 2 permeance of 607   GPU and CO 2 /N 2 selectivity of 106 at CO 2 partial pressure of 0.02   MPa. The separation performance stability of the PVAm–EDA/PS membranes was investigated for 300   h and no deterioration in membrane permselectivity was observed. Moreover, the PVAm–EDA/PS membrane had no obvious degradation after exposure to H 2 O-saturated SO 2 of 300,000   ppm   h.

✓ 已验证 DOI 高影响因子
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Research · 2018 · IF 0

Rechargeable Na-CO2 Batteries Starting from Cathode of Na2CO3 and Carbon Nanotubes

Jianchao Sun,Yong Lu,Hao Yang,Mo Han,Lianyi Shao,Jun Chen

Na-CO 2 batteries have attracted significant attentions due to their high energy density and effective utilization of greenhouse gas CO 2 . However, all reported Na-CO 2 batteries employ excessive preloaded metal Na, which will lead to safety issues such as dendrite formation and short circuit. In addition, the charging mechanism of reported Na-CO 2 batteries is not very clear. Here we report the Na-CO 2 batteries, starting from the cathode of cheap Na 2 CO 3 and multiwalled carbon nanotubes (CNTs). Due to the effective electron transfer and high reactivity, the decomposition of Na 2 CO 3 and CNTs could take place under 3.8 V. The charging mechanism of 2Na 2 CO 3 + C → 4Na + 3CO 2 without any side reactions is revealed by in/ex situ techniques such as Raman, gas chromatograph, and optical microscope. Dendrite-free Na can quantitatively deposit on the Super P/Al anode because of large specific surface area and low nucleation barrier of the anode for Na plating. The batteries could deliver an energy density of 183 Wh kg −1 (based on the whole mass of the pouch-type batteries, 4 g) with stable cycling performance. This work reveals that safe rechargeable Na-CO 2 batteries could be constructed by cheap Na 2 CO 3 and multiwalled carbon nanotubes.

✓ 已验证 DOI
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AICHE JOURNAL · 2012 ·Vol. 59 ·期 1 ·215-228 · IF 2.261

PVAm–PIP/PS Composite Membrane with High Performance for CO2/N2 Separation

Zhihua Qiao,Zhi Wang,Chenxin Zhang,Shuangjie Yuan,Yaqun Zhu,Jixiao Wang,Shichang Wang

Polyvinylamine (PVAm) was modified using a cross-linking agent containing carriers piperazine (PIP). Attenuated total reflectance fourier transform infrared, elemental analyzer, and X-ray diffraction were used to characterize the PIP-modified PVAm. The PVAm–PIP/polysulfone (PS) composite membrane was developed by coating PVAm–PIP mixed solutions with different mass ratios of PIP/PVAm (m PIP /m PVAm ) on the PS ultrafiltration membrane. The effects of m PIP /m PVAm (from 0.715 to 2.860) in the coating solutions and wet coating thickness on the gas performance of the PVAm–PIP/PS composite membrane were investigated. The PVAm–PIP/PS composite membrane prepared showed higher performance than other membranes reported in the literature due to the large increase of the introducing carrier concentration and low crystallinity. Moreover, the separation performance stability of the PVAm–PIP/PS composite membrane was investigated and no deterioration in the membrane permselectivity was observed. Finally, the economic evaluation of the membrane with the highest performance prepared was carried out. © 2012 American Institute of Chemical Engineers AIChE J, 59: 215–228, 2013

✓ 已验证 DOI 高影响因子
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Materials · 2024 ·Vol. 17 ·期 9 ·1946 · IF 3.1

Adsorption of Co2+ and Cr3+ in Industrial Wastewater by Magnesium Silicate Nanomaterials

Jing Bao,Yongjun Feng,Yong Pan,Juncheng Jiang

In this paper, two flower-like magnesium silicate nanomaterials were prepared. These and another two commercial magnesium silicate materials were characterized using a scanning electron microscope, the N2adsorption–desorption method, and other methods. The structure–activity relationship between the adsorption performance of these four magnesium silicate materials and their specific surface area, pore size distribution, and pore structure was compared. The results showed that the 3-FMS modified by sodium dodecyl sulfonate (SDS) had the largest specific surface area and pore size, the best adsorption performance, and the largest experimental equilibrium adsorption capacity (qe,exp) for Co2+, reaching 190.01 mg/g, and Cr3+, reaching 208.89 mg/g. The adsorption behavior of the four materials for Co2+and Cr3+both fitted the pseudo-second-order kinetic model and Langmuir adsorption model, indicating that chemical monolayer uniform adsorption was the dominant adsorption process. Among them, the theoretical adsorption capacity (qm) of 3-FMS was the highest, reaching 207.62 mg/g for Co2+and 230.85 mg/g for Cr3+. Through further research, it was found that the four materials mainly removed Co2+and Cr3+through electrostatic adsorption, surface metal ions (Mg2+), and acidic groups (-OH and -SO3H) exchanging with ions in solution. The adsorption performance of two self-made flower-like magnesium silicate materials for Co2+and Cr3+was superior to that of two commercial magnesium silicates.

✓ 已验证 DOI PubMed 高影响因子
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Science China-Materials · 2025 · IF 7.4

Crystal defects engineering of BiOI elevated photocatalytic CO2 to C2 conversion performance

Huang Fuxia,Liu Yifei,Wang Feng,Liu Ya,Guo Liejin

BiOI materials show significant potential for photocatalytic CO 2 reduction, but their limited CO 2 activation and poor charge carrier properties hinder conversion efficiency. In this study, we engineered BiOI-based photocatalysts with abundant crystal defects to enhance performance. X-ray diffraction (XRD), Raman spectroscopy, and high-resolution transmission electron microscopy (HRTEM) revealed lattice distortions and twin crystals in BiOI-LD and BiOI-TC. Ultraviolet-visible spectroscopy, micropore and chemisorption analyses, and photoluminescence spectroscopy demonstrated that crystal defects improved light absorption, CO 2 adsorption, charge transfer efficiency, and carrier lifetime. Electron paramagnetic resonance (EPR) spectroscopy showed increased superoxide radical generation in BiOI-TC, suggesting higher reactivity. Consequently, BiOI achieved a CH 3 CH 2 OH generation rate of 6.2 µmol g −1 h −1 with 100% selectivity. Key intermediates (*CO, *COCO, *CHO, *CH 2 ) for CH 3 CH 2 OH production were identified, and C 2 H 6 formation in BiOI-LD was linked to the generation of *CH 3 .

✓ 已验证 产品关联 DOI 高影响因子
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ACS Sustainable Chemistry & Engineering · 2025 · IF 7.3

Unveiling the Size-Dependent Photothermal Synergy of TiO2 in Catalytic CO2 Reduction

Haodong Zhang,Min Chen,Weiming Qian,Jianghao Zhang,Xueyan Chen,Xiaoxiao Qin,Minmin Liang,Changbin Zhang

The hydrogenation of CO2 to produce valuable chemicals through photocatalytic or photothermal technologies represents a viable path toward carbon neutrality. However, typical nanosemiconductor materials, such as TiO2, often exhibit limited activity, necessitating the optimization of their performance as a key research priority. Here, we demonstrate that the size of anatase TiO2 significantly influences its performance in the selective photocatalytic and photothermal reduction of CO2 to CO. The small-sized TiO2 (S-TiO2, 15 nm) exhibits a low CO yield of 32.7 μmol g–1 h–1 and shows almost no photothermal synergy. In contrast, the large-sized TiO2 (L-TiO2, 160 nm) demonstrates a high CO yield of 185.3 μmol g–1 h–1 and significant photothermal synergy, with the CO yield reaching 438.7 μmol g–1 h–1. We reveal that L-TiO2 is well-crystallized and has a higher conduction band position compared to the S-TiO2. This results in a higher charge separation efficiency and more effective photoexcited electrons for CO2 reduction. Additionally, the external heating primarily enhances the charge separation in L-TiO2, significantly improving the conversion of CO2 to CO. This work provides insights into the relationship between the structure and activity of TiO2 in photocatalytic and photothermal CO2 reduction.

✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Fe-TiO2-x/TiO2 S-scheme homojunction for efficient photocatalytic CO2 reduction

Ya-Nan Jing,Xing-Liang Yin,Lei-Lei Li,Yan-Lan Wang,Jia Xue,Ze-Feng Xu,Da-Qiang Liu,Chuan-Wu Chen,Xiao-Jie Liu,Er-Kang Liu

CO 2 -to-high value-added chemicals via a photocatalytic route is of interest but strangled by the low efficiency. Herein, a novel Fe-TiO 2-x /TiO 2 S-scheme homojunction was designed and constructed by using a facile surface modification approach whereby oxygen vacancy (OV) and Fe introducing on the TiO 2 nanorod surface. The as-synthesized Fe-TiO 2-x /TiO 2 S-scheme homojunction exhibits positive properties on promoting photocatalytic CO 2 reduction: i) the nanorod structure provides numerous active sites and a radical charge transfer path; ii) the doped Fe and OV not only synergistically enhance light utilization but also promote CO 2 adsorption; iii) the Fe-TiO 2-x /TiO 2 S-scheme homojunction benefits photoexcited charge separation and retains stronger redox capacity. Thanks to those good characters, the Fe-TiO 2-x /TiO 2 homojunction exhibits superior CO 2 reduction performances with optimized CO/CH 4 generation rates of 122/22 μmol g -1 h −1 which exceed those of pure TiO 2 by more than 9.4/7.3 folds and most currently reported catalytic systems. This manuscript develops a facile and universal approach to synthesize well-defined homojunction and may inspire the construction of other more high-efficiency photocatalysts toward CO 2 reduction and beyond.

✓ 已验证 DOI PubMed 高影响因子
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INTERNATIONAL JOURNAL OF FOOD MICROBIOLOGY · 2015 · IF 3.082

Inactivation of Bacillus subtilis spores by high pressure CO2 with high temperature

Lei Rao,Zhenzhen Xu,Yongtao Wang,Feng Zhao,Xiaosong Hu,Xiaojun Liao

The objective of this study was to investigate the inactivation of the Bacillus subtilis spores by high pressure CO 2 combined with high temperature (HPCD   +   HT) and to analyze the clumping effect of the spores on their HPCD   +   HT resistance. The spores of B . subtilis were subjected to heat at 0.1   MPa and HPCD at 6.5–25   MPa, and 82   °C, 86   °C, and 91   °C for 0–120   min. The spores were effectively inactivated by HPCD   +   HT, but a protective effect on the spores was also found, which was closely correlated to the pressure, temperature and time. The spores treated by HPCD   +   HT at 6.5 and 10   MPa exhibited a two-stage inactivation curve of shoulder and log-linear regions whereas the spores at 15–25   MPa exhibited a three-stage inactivation curve of shoulder, log-linear and tailing regions, and these curves were well fitted to the Geeraerd model. Approximately 90% of pyridine-2,6-dicarboxylic acid (DPA) was released after HPCD   +   HT and the 90% DPA release time depend on the pressure and temperature. Moreover, the spore clumping in suspensions was examined by dynamic light scattering. The particle size of the spore suspensions increased with the increase of pressure, temperature and time, indicating the spore clumping. 0.1% Tween 80 as a surfactant inhibited the spore clumping and increased the inactivation ratio of the spores by HPCD   +   HT. These results indicated that the spore clumping enhanced the spores' resistance to HPCD   +   HT and induced a protective effect.

CAS / MDL: 13798-24-8
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