Surfaces and Interfaces
·
2024
·
IF 5.7
Pengfei Zhu,Mengrong Geng,Shuang Qin,Heyang Cao,Zhenhong He,Xinhua Gao,Chuanyi Wang
The conversion of CO 2 into chemical products or fuels of great value always remains an outstanding challenge. Here, we report a heterojunction Fe@C/Ni 2 P composite catalyst obtained by preparing MIL-100(Fe) derived Fe@C confined Ni 2 P nanoparticles, which is applied to photothermal catalytic CO 2 hydrogenation with H 2 O. Without adding any sacrificial agents or co-catalysts, the optimal Fe@C/Ni 2 P sample shows higher yields for CO 2 -to-C 2 H 6 and CO 2 -to-CO yield of 5.83 μmol g −1 h −1 and 179.9 μmol g −1 h −1 than that of pristine Fe@C and Ni 2 P, respectively. The experimental results indicated that the obtained Fe@C/Ni 2 P can act as catalytic sites to adsorb, activate, and convert CO 2 under low-intensity LED light irradiation (420 nm) with a temperature of 200 ℃. The physical structure, photochemical properties and energy band structure of the Fe@C/Ni 2 P composite catalysts were investigated by XRD, XPS, FT-IR, TEM, BET, respectively. Furthermore, the reaction pathway of Fe@C/Ni 2 P photothermal catalytic CO 2 hydrogenation with H 2 O to C2 products and CO were systematically analyzed by in situ infrared spectroscopy (DRIFTS).
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lijian Jin,Xueyan Hou,Lingxiao Zhan,Shangzhi Xie,Lina Gu,Hangqi Yang,Xin Wang,Xinfeng Qian,Jianchong Shen,Linjun Yang
In order to ameliorate the issues of corrosion and high regeneration energy associated with traditional biphasic solvents, a nonaqueous biphasic solvent has been proposed as a potential alternative. This study introduces Tetramethylethylenediamine (TMEDA) as a phase splitter within the Ethanolamine (MEA)/Dimethyl sulfoxide (DMSO) system, resulting in a novel nonaqueous biphasic solvent, TMEDA/MEA/DMSO. Compared with other screened phase splitters, the appropriate polar size and intermolecular interaction force of TMEDA are the key factors that make it comply with the screening of nonaqueous biphasic solvent. When the mass ratio of TMEDA/MEA/DMSO is maintained at 3:3:4, the CO 2 loading attains 0.54 mol (CO 2 )/mol (MEA), with the rich phase comprising 75 % of the total. 13 C NMR and FT-IR characteristics showed that the absorbent product is mainly in the form of MEACOO − /MEAH + . Absorption and phase separation mechanisms of absorbent elucidated by DFT calculations and molecular dynamics simulations. The limited opportunity for TMEDA to interact with MEA molecules emerges as the primary reason for its reduced involvement in the reaction, with the inclusion of TMEDA intensifying the aggregation of MEACOO − /MEAH + and triggering phase transition. In comparison to a 30 wt% MEA water-based absorbent, TMEDA/MEA/DMSO exhibits a 40 % reduction in regeneration energy (estimate) and possesses energy-saving attributes, rendering it a promising candidate for CO 2 capture.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Chengming Guo,Pengtao Guo,Youbin Zhou,Xin Yan,Huifang Li,Dahuan Liu
Porous adsorbents are widely used for the adsorptive separation of carbon dioxide (CO 2 ) from gas mixtures, offering a promising solution to address both the energy crisis and environmental issues. However, developing highly efficient CO 2 selective adsorbents has been challenging due to the similar physicochemical properties of CO 2 and other gases. To overcome this challenge, we herein have developed a core–shell composite utilizing ionic liquids (ILs) and metal–organic frameworks (MOFs) based on the dissolution-diffusion mechanism. The unique solubility differences of ILs for various gas molecules, particularly their strong solubility for CO 2 , allow only CO 2 to be adsorbed while excluding other gases. As a result, the composite exhibits a remarkable separation selectivity for CO 2 /C 2 H 2 , CO 2 /CH 4 and CO 2 /N 2 . Breakthrough experiments have verified the outstanding performance of this core–shell composite in separating gas mixtures containing CO 2 impurities. Remarkably, this composite can be synthesized by a simple method, which is more practical for large-scale production.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Jiepeng Zhao,Yifei Ma,Zhaomin Tong,Mei Wang,Liantuan Xiao,Suotang Jia,Xuyuan Chen
Engineering photocatalyst crystal facets and constructing heterojunctions are effective strategies to improve photocatalytic activity. The amino-modified titanium-based metal–organic framework (MOF) NH 2 -MIL-125(Ti) (NM) has drawn extensive attention as a photocatalyst by virtue of its high specific surface area, abundant pore structure, and narrow bandgap. However, its catalytic activity is hindered by fast electron-hole recombination and limited light absorption. This study synthesizes NM with engineered crystal facets and Co 3 O 4 @NH 2 -MIL-125(Ti) (C-NM) composites with varying Co 3 O 4 loadings using a facile hydrothermal method. The impact of heterojunctions and facet design on photocatalytic CO 2 reduction under visible light is also studied. Results show that the C-NM, with exposed {111} facets and optimal Co 3 O 4 loading, demonstrates superior photocatalytic CO and CH 4 production rates of 21.64 μmol h −1 g −1 and 3.99 μmol h −1 g −1 , 2.1 and 1.6 times higher than those of NM {001} , respectively. Experimental characterization and density functional theory (DFT) analyses attribute the improved photocatalytic activity to several mechanisms. First, crystal facet modulation can optimize the active sites and specific surface area of the photocatalysts. Second, by loading the narrow-bandgap Co 3 O 4 nanoparticles, bandgap of the C-NM photocatalyst is further reduced, thereby enhancing the absorption and utilization of visible light. Finally, the NM/Co 3 O 4 heterostructure minimizes electron-hole recombination, significantly boosting CO 2 reduction efficiency.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Haiqian Zhao,Jiuyang Jia,Jiaxin Ying,Mingqi He,Zekun Sun,Xing Zhang,Zhonghua Wang,Wei Zhou
Utilizing flue gas as feedstock for CO 2 electro−reduction systems is a promising technology to address problems caused by excessive CO 2 emissions. However, the O 2 contained in the flue gas has a significant adverse effect on the CO 2 reduction. Herein, a facile strategy was proposed to suppress the influence of O 2 by constructing a CO 2 −enriched region. N−doping was demonstrated to be an efficient way to enhance CO 2 adsorption selectivity over O 2 on activated carbon. The N−doped activated carbon achieved 3.7 times increase in CO 2 adsorption selectivity over O 2 than that before modification under simulated flue gas atmosphere (75 %N 2 + 15 %CO 2 + 10 %O 2 ). The distinction in adsorption mechanism between CO 2 and O 2 was revealed by quantum chemistry study. The increased polarity of the carbon materials favored CO 2 adsorption and had less impact on O 2 adsorption. The electrostatic interaction between CO 2 and carbon material was demonstrated to be enhanced after the introduction of pyridinic N and pyrrolic N, which led to an improvement in the CO 2 adsorption capacity. The dispersion interaction, which fully regulated O 2 adsorption, was weakened due to the deviation of the O 2 adsorption position. This study provided a reference for the subsequent development of CO 2 selective adsorption materials.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Jiaqi Feng,Yanlin Wang,Guilin Li,Qizhou Xue,Min Wang,Xiaofu Sun,Shaojuan Zeng,Xiangping Zhang
Copper-based catalysts hold promise for electrochemical reduction of CO 2 to multi-carbon (C 2+ ) products, but achieving high selectivity and ampere-level current density remains challenging. A key hurdle lies in stabilizing Cu + species under reducing conditions, which are crucial for C-C coupling reaction. Herein, we modified Cu 2 O with sodium citrate through the coordination interaction between Cu atoms and carboxyl group. In situ spectroscopy analysis and theoretical studies revealed that the modification induced electron transfer from Cu 2 O to the citrate anion, stabilizing Cu + species under reduction conditions. Additionally, the presence of sodium citrate facilitated the hydrogenation of *CO to *CHO, with *CHO being more prone to C-C coupling reactions. Thereby, the as-prepared catalyst showed an C 2+ products Faradaic efficiency (FE) of 88.1 % at − 0.9 V vs reversible hydrogen electrode (RHE) with a C 2+ products partial current density ( j C2+ ) of 825.94 mA cm −2 and maintained over 80 % FE at − 1.1 V vs RHE with j C2+ of 1239.92 mA cm −2 . This work suggests that surface modification of Cu 2 O via carboxyl group is an effective strategy for altering the surface electronic structure of Cu 2 O and regulating the C-C coupling pathway, encouraging the exploration of more carboxyl-containing molecules for modifying copper-based catalysts to further enhance electrocatalytic performance.
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FUEL
·
2025
·
IF 7.5
Zhengyu Yang,Jianmin Li,Yubin Wang,Mengyao Shi,Jide Wang,Changyan Guo
Zeolitic imidazolate frameworks (ZIFs) are rich in accessible and active Lewis acid-base sites and hierarchical pores, making them effective catalysts for the cycloaddition of CO 2 to epoxides under mild conditions. In this study, a facile defect-engineering strategy using acid etching and ligand exchange was developed to convert three-dimensional ZIF-L into layered Br-ZIF-L with a tire-like surface, abundant active sites, and a structure optimized for efficient mass diffusion. This modification enabled the rapid cycloaddition of CO 2 to propylene oxide under mild conditions (1 MPa and 100 °C for 2 h). The resulting cyclic carbonate was obtained in 92 % yield and 100 % selectivity. Additionally, Br-ZIF-L exhibited excellent chemical stability without a loss of catalytic activity after six consecutive cycles, highlighting its potential as a high-performance catalyst for CO 2 conversion. The developed catalytic system exhibited a conversion rate of >90 % for five different substituted epoxides. This study introduces an efficient approach for synthesizing cyclic carbonates via CO 2 fixation under mild conditions.
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Research and Practice in Thrombosis and Haemostasis
·
2025
·
IF 3.4
Shunli Gu,Jinmei Xu,Erxiong Liu,Xuejia Hou,Ning An,Yaozhen Chen,Zhixin Liu,Wenting Wang,Xingbin Hu,Wen Yin
Background The timely administration of platelet transfusions is critical for patient survival, and the clinical demand for platelet transfusions has been steadily increasing. However, platelet storage lesion (PSL) that develops during in vitro preservation exacerbate these shortages. The PSL is significantly influenced by various factors, including temperature, gas composition, and buffering systems. Strategies to mitigate PSL and improve platelet storage have been actively explored in recent years. Objectives This study aimed to investigate whether elevated carbon dioxide (CO 2 ) levels improve platelet quality and functionality during storage. Methods Platelet concentrates from 28 donors were stored under control or 3% CO 2 conditions at 22 ± 2°C for up to 7 days. Platelet quality was evaluated through scanning electron microscopy, adhesion, aggregation, clot contraction, activation, apoptosis assays, blood gas, ATP, metabolomics analyses, and in vivo thrombosis and survival tests. Results Our findings indicate that increasing the CO 2 concentration in the storage environment mitigates PSL and improves platelet quality. Conclusions Our study highlights the potential benefits of utilizing a high-CO 2 storage environment to improve platelet preservation, offering a promising method to address clinical platelet shortages.
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Shuting Zhang,Jianwen Wei,Linlin Geng,Lin Ge,Lei Liao
Novel bifunctionalized amine-based protic ionic liquid/KIT-6 composite adsorbents for carbon dioxide (CO 2 ) adsorption have been prepared by impregnating amine-based protic ionic liquids of different types (tetraethylenepentamine nitrate, [TEPA][NO 3 ], or tetraethylenepentamine lysinate, [TEPA][Lys]) and concentrations (20, 30, 40, and 50 wt%) onto N-[3-(trimethoxysilyl)propyl]ethylenediamine-grafted KIT-6. These innovative hybrid adsorbents exhibited remarkable CO 2 adsorption performance and thermal stability. In particular, the adsorbent with 40 wt% [TEPA][Lys] loading exhibited the highest adsorption capacity at 90 ℃ (3.670 mmol·g −1 ), which was almost 5 times higher than that of the original carrier KIT-6 (0.850 mmol·g −1 ). This excellent adsorption performance can be ascribed to the synergistic effect of strong affinity between the amine groups and CO 2 and high porosity of the support. After five adsorption/desorption cycles, the CO 2 adsorption by the adsorbents demonstrated significant regeneration, and the saturated adsorption capacities of 2N-K6-P30 and 2N-K6-L40 were only 8.98 % and 7.77 % lower than those of the original ones, respectively. In addition, the infrared results revealed that CO 2 adsorption is a synergistic process of physical and chemical adsorption, in which chemisorption is dominated, and the CO 2 adsorption mechanism is consistent with the zwitterion mechanism. In conclusion, the bifunctionalized amine-based protic ionic liquid/KIT-6 adsorbents can be suggested as potential/recyclable materials for efficient removal of CO 2 from industrial flue gases after desulfurization.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 45
·19220-19228
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IF 2.7
Peng Lu,Qianwen Hu,Kui Wang,Shiyong Chen,Zongxiao Li,Xinjie Chen,Chuang Xing,Yanhong Wang,Ce Du
The efficient CO2 conversion to light olefins through hydrogenation is a feasible strategy to achieve carbon neutrality goals. Herein, a series of bimetallic Zn–Zr/supports are synthesized by a conventional impregnation method. We demonstrate that different supports endow catalysts with various specific surface areas, pore sizes, chemical adsorption performances, and acid densities. The effects of different support-loaded Zn–Zr coupled with SAPO-34 on CO2 hydrogenation to light olefins are investigated systematically. The CO2 conversion of Zn–Zr/Q10-SAPO-34, Zn–Zr/Q50-SAPO-34, Zn–Zr/γAl2O3-SAPO-34, Zn–Zr/MgO-SAPO-34 and Zn–Zr/S-1-SAPO-34 is 11.4%, 9.2%, 24.0%, 8.8%, and 16.2%, respectively, with corresponding light olefin selectivity of 39.0%, 28.1%, 30.4%, 4.8%, and 14.7%, respectively. Significantly, γAl2O3 is more conducive to CO2 conversion, while Q10 tends to produce light olefins. This work provides an effective reference for support selection in CO2 hydrogenation to light olefins.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Haonan Liu,Francesco Barzagli,Li Luo,Xin Zhou,Jiaofei Geng,Chao’en Li,Min Xiao,Rui Zhang
The combination of primary and tertiary amines represents a promising approach to improve sorbent performance in CO 2 capture by enhancing absorption efficiency and reducing regeneration energy. This study focuses on investigating the absorption performance of binary mixtures of ethanolamine (MEA) and N,N-dimethylethanolamine (DMEA) at temperatures between 298–323 K and CO 2 partial pressures between 5–60 kPa. The species generated during the absorption were analyzed using 13 C NMR spectroscopy, to clarify the intricate role of MEA and DMEA in the capture process. A developed excess property model for MEA-DMEA, based on excess CO 2 loading, predicted equilibrium CO 2 solubility data with an average absolute relative deviation (AARD) of 1.6 %. Additionally, the machine learning models XGBoost, RBFNN, and SVR were applied, providing AARD values between 0.86 % and 1.28 %, demonstrating strong agreement between experimental and predicted outcomes. These comprehensive findings enhance our understanding of mixed amines’ mechanisms and practical applications, contributing to ongoing research development.
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高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Xiangqian Guo,Chenhui Qiu,Zhiqiang Zhang,Jie Zhang,Lei Wang,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Photocatalytic CO 2 reduction plays an important role in solving environmental issues and alleviating the energy crisis. However, it is still challenging to distribute the surface-active site on photocatalysts with efficient separation of carriers in rational. Herein, the Cu species loaded SrTiO 3 nanofiber was constructed through coaxial electrospinning which could realize the dispersion of the Cu site on the one-dimensional (1D) nanofiber structure. The 1D nanofiber with Cu site exhibited superior performance on photocatalytic CO 2 reduction based on the excellent ability of charge separation. The Cu 2 O and CuO were determined to be located on the surface of 1D SrTiO 3 nanofiber by the TEM and XPS. The work functions of SrTiO 3 , Cu 2 O, and CuO were calculated to be 5.26, 5.47, and 5.51 eV, respectively, suggesting that the carriers could transfer from SrTiO 3 nanofiber to the Cu species. The yield of CH 3 OH with the optimized 8%Cu-SrTiO 3 catalyst could reach 8.08 ± 0.03 µmol⋅g −1 ⋅h −1 . This work provided a coaxial electrospinning strategy to load the Cu species active site on the surface of 1D SrTiO 3 nanofiber for enhancing photoreduction CO 2 .
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