RSC Advances
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2018
·Vol. 8
·期 17
·9192-9201
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IF 2.936
Chao Feng,Xianglei Cao,Liugen Zhang,Changyan Guo,Naeem Akram,Jide Wang
Development of heterogeneous catalysts for the cycloaddition of CO2 with epoxides to produce cyclic carbonates is a hot issue in the field of chemical fixation of carbon dioxide. It is fairly promising as production of by-products is quite low. In this study, the [Zn3(BTC)2]/n-Bu4NBr catalytic system was investigated for the solventless cycloaddition of carbon dioxide with epoxides and had an excellent synergetic effect in promoting the reaction. The reaction parameters were moderate i.e. (130 °C and 13 bar CO2 pressure) and were selected by a study of the catalytic system. Under the optimal reaction conditions, the yield of cyclic carbonate reached 99%. A decrease in the yield of cyclic carbonate was not apparent after [Zn3(BTC)2] was reused three times, indicating that [Zn3(BTC)2] was stable. At the same time, the catalytic activity of the catalyst for other epoxides was also verified. The acidic and alkaline nature of the [Zn3(BTC)2] catalyst did not change obviously after recycling the catalyst three times. In this study it is also verified that the [Zn3(BTC)2] catalytic cycloaddition reaction was closely related to the Lewis acid/base distribution. In addition, a plausible mechanism for the synergistic effect of the catalyst (Lewis acid and base properties) and the co-catalyst was suggested.
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CATALYSIS TODAY
·
2024
·
IF 5.2
Ruiqi Wu,Ning Liu,Chengna Dai,Gangqiang Yu,Ruinian Xu,Biaohua Chen
The propane oxidation dehydrogenation assisted by CO 2 (CO 2 -ODHP) is currently a hot research topic, not only to meet growing demand of propylene but also to favor the CO 2 neutralization. In present work, a series of CrO x @S1-n-1.0 with different Cr contents (n= 2.2, 3.6 and 4.5 wt%) is synthesized based on a small gas molecule directing synthesis strategy, wherein the gaseous CO of 1.0 MPa was in situ introduced in the synthesis system to regulate the interaction and dispersion of CrO x over silicalite-1 (S1) support. The characterization results of XRD , XPS , H 2 -TPR, and Raman indicate that the CO can affect the oxidation state and dispersion of Cr species. As observed, the Cr species were highly dispersed over CrO x @S1–3.6 %-1.0 (in the form of Cr 6+ valance state), which however would aggregate to generate Cr 2 O 3 nanoparticles over the CrO x @S1–3.6 %-0 a prepared by impregnation method in absence of CO. The activity measurement indicates that the CrO x @S1–3.6 %-1.0 possesses the highest activity by displaying an average propane conversion of 50.4 % and CO 2 conversion of 23.6 % at 600 °C, which surpasses most of the literature reports. The CO 2 -ODHP reaction mechanism was further investigated by in situ DRIFTS , which indicates that dissociated H of propane can react with CO 2 to form formate (-COOH), in turn further reacts with H to produce byproducts CO and H 2 O, and the formate species can also react with the CrO 3 active site to form bicarbonate species (HCO - 3 ). Generally, present work has proposed a small gas molecule directing strategy to adjust the dispersions and chemical states of the loaded guest meals over catalytic support. The study of present work would contribute to other highly efficient catalyst design .
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APPLIED CATALYSIS B-ENVIRONMENTAL
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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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Research and Practice in Thrombosis and Haemostasis
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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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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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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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APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Miao Sun,Xiao Xu,Shihao Min,Jiaxin He,Kun Li,Longtian Kang
Copper-based metal-organic framework (Cu-MOF) materials with multiple active sites have attracted increasing attention to the electrocatalytic CO 2 reduction reaction (ECR), however, face the huge challenge owing to the poor stability and low C 2 selectivity. Here, the Cu 2 O/Cu-CuTCPP heterojunction (Cu 2 O/CPFs) with three Cu active sites are firstly constructed through in-situ electrodeposition method. The effect of CuSO 4 concentration and electrodeposition conditions on ECR is systematically investigated. The optimized Cu 2 O/CPFs composite achieves the ethylene Faraday efficiency (FE C2H4 ) of 61.8 % at –1.3 V vs. RHE, which is 1.9 and 3.42 times higher than those of CPFs and Cu 2 O, respectively. Meanwhile, the C 2 H 4 partial current density ( j C2H4 ) of –7.96 mA·cm −2 is 2.91 and 4.68 times higher than those of CPFs and Cu 2 O. Further experiments reveals that the formation of Cu 2+ –O–Cu + –O bond between Cu 2 O and Cu–O 4 sites in Cu 2 O/CPF heterojunction is crucial. Consequently, the hydrogen (H 2 ), formic acid (HCOOH) and methane (CH 4 ) evolution reactions are restricted, the C–C coupling reaction of *CHO and *CO intermediates is significantly enhanced, and the Cu–O 4 sites in CPFs are protected. This work provides an effective strategy to stabilize MOF structure and obtain high value-added C 2+ products.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Zhenhui Wang,Hongdong Li,Tian Dong,Yanling Geng,Xiaofeng Tian,Rui Chang,Jianping Lai,Shouhua Feng,Lei Wang
Acidic CO 2 electroreduction has the potential to synthesize low carbon footprint chemicals using renewable electricity. However, proton-rich environments can lead to strong hydrogen evolution reaction (HER) and severe degradation of electrochemical CO 2 reduction reaction (CO 2 RR) performance. Modulating electrode structure plays a critical role in improving the local microenvironment of CO 2 RR electrolytes. Here, by covering the catalyst layer with a hydrophobic silica aerosol layer, the surface of the catalyst is protected from corrosion, thereby increasing the efficiency and stability of the system. In the flow cell, the Sn-C/SiO 2 -3 catalyst has high formic acid (HCOOH) selectivity at high current density (∼90 % at −400 mA cm −2 ). Importantly, the Sn-C/SiO 2 -3 catalyst can operate stably for 45 h at −400 mA cm −2 . Combined in situ infrared analysis reveals that hydrophobic SiO 2 aerosol layer can engineer the local microenvironment over the Sn-C catalyst surface by increasing the coverage of *OCHO to improve the CO 2 RR, which ultimately promotes high-efficiency CO 2 conversion to HCOOH in strong acidic media. This surface coating strategy for adjusting the interface microenvironment can also be used for other electrocatalytic reactions.
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Reaction Kinetics Mechanisms and Catalysis
·
2024
·
IF 1.7
Yu Yue,Chen Xiaolu,He Ping,Xu Zhiwen,Wu Xiao,Chen Hong,Yang Songlin,Yu Jia,Gao Shuang
A number of Ce 1-x Mn x catalysts with different Mn contents were prepared by resol-assisted cationic coordinative co-assembly approach and used for the synthesis of dimethyl carbonate (DMC) from CO 2 and methanol. Multiple characterizations of XRD, FT-IR, TEM, BET, CO 2 -TPD, NH 3 -TPD, H 2 -TPR, XPS analyses were applied to investigate the surface properties of the Ce 1-x Mn x catalysts. It turned out that adjusting the proper concentration of Mn ions not only increased the pore volumes, but also improved the content of medium acidic and medium basic sites. When a small amount of Mn was added, the presence of Mn 2+ on the catalyst surface enhanced, facilitating the conversion of Ce 4+ to Ce 3+ , and leading to higher oxygen vacancy concentration. Consequently, the adsorption and activation of CO 2 and methanol were promoted, and the catalytic efficiency of the reaction was improved. It was found that Ce 0.95 Mn 0.05 catalyst exhibited the best catalytic activity, achieving a high DMC yield of 6.44 mmol/g (120 °C, 6.5 MPa, 4 h). Graphical Abstract
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Small
·
2025
·
IF 12.1
Min Zhu,Ting Zhang,Jinlong Wu,Xiuli Wang,Jin Zhang,Feng Li,Jing Li
Lattice strain is widely recognized as an effective strategy for tuning transition metal catalytic activity, yet its direct impact on electrochemical CO₂ reduction (ECO₂RR) remains not fully understood. In this work, a strategy of Cu-doped Ag is employed to construct a series of AgCu nanosheet structures (NS) with varying lattice compression rates (from −1.90% to −2.75%). Density Functional Theory (DFT) calculations, along with in situ infrared spectroscopic analysis, demonstrate that Cu incorporation efficiently modulates the electronic structure of Ag, promoting enhanced charge transfer. Especially, the changed lattice compression rates can alter the charge density at adsorption sites, thereby ameliorating the surface coverage of CO and adsorption energy of the reaction intermediates ( * COOH and * CO). As a result, the AgCu 5% catalyst exhibits a maximum Faradaic efficiency (FE) of 95.5% for CO production in an H-cell and 98% in a flow cell at −0.8 V RHE , respectively. Simultaneously, the AgCu 5% catalyst achieves FE CO of above 86% in the ultrawide current range of 33–215 mA cm −2 . The work affords an effective way to use a strain compression strategy to improve the CO 2 reduction performance.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Changhong Zhou,Rui Ling,Menglei Wang,Chao Yang,Wentao Qi
Syngas , a mixture of H 2 and CO with adjustable compositional ratios, can be directly produced via H 2 O/CO 2 co-electrolysis in solid oxide electrolysis cells (SOECs). In this study, We have developed a strategy to enhance the catalytic activity of titanate perovskite cathodes by constructing active metal-oxide interfaces through the in-situ growth of Ni x Cu 1-x alloy nanocatalysts (x = 0, 0.25, 0.5, 0.75 and 1) on LST matrix. The evenly distribution of Ni x Cu 1-x alloy nanoparticles (∼30 nm) on the LST substrate has been confirmed through a serious of characterization techniques, including XRD , XPS, SEM and TEM. Specifically, the LSTNi 0.75 Cu 0.25 cathode demonstrated an optimal synergistic effect , achieving high efficiency in the co-electrolysis of H 2 O/CO 2 to syngas. Under an applied voltage of 1.6 V at 800 °C, the syngas production rate reaches 5.43H 2 and 3.48 CO ml min −1 cm −2 with ∼96 % Faradaic efficiency. Furthermore, the composition of the produced syngas can be finely tuned in a broad range from 0.8 to 3.5 b y simply adjusting the inlet gas composition (H 2 O/CO 2 ratio) and the operating temperature. The LSTNi 0.75 Cu 0.25 cathode, when subjected to continuous H 2 O/CO 2 co-electrolysis for 100 h, exhibited remarkable stability, attributing to the robust and active nature of the metal-oxide interfaces.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Lixin Song,Guobin Liu,Zhenping Qu
Cu/ZnAl 2 O 4 spinel is a promising catalyst for CO 2 -to-methanol due to its dual-site H 2 activation. However, controlling surface properties and metal-support interactions (MSI) through the coordination environment of spinel cations remains underexplored. Herein, the occupancy of Zn 2+ and Al 3+ cations in Cu/ZnAl 2 O 4 spinel is fine-tuned by manipulating the calcination atmosphere. More disordered structures (AlO 4 and ZnO 6 ) observed on the CZA-Ar catalyst benefit the creation of oxygen vacancies and surface hydroxyl groups, which facilitate the formation of highly dispersed small-sized Cu species. This enhances MSI and hydrogen spillover effects, thereby boosting CO 2 conversion and the space-time yield (STY) of methanol. High-pressure in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) results reveal that the crucial formate intermediates form at tetrahedral sites in ZnAl 2 O 4 spinel, with more Al-HCOO - species observed on the CZA-Ar catalyst due to the formation of AlO 4 . This work advances the understanding of spinel catalysts in CO 2 hydrogenation to methanol.
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Journal of Environmental Chemical Engineering
·
2025
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IF 7.2
Fangfang Zhang,Yingxuan Wen,Falong Shan,Jingru Dou,Shougui Wang,Jipeng Dong,Guanghui Chen,Fei Gao
In this study, a sequence of pyridine-based hypercrosslinked ionic polymers (HIP-IBy, HIP-IByCA and HIP-IByBA) as heterogeneous catalysts were prepared using a two-step method for the CO 2 cycloaddition reaction. The synthesized pyridine-based HIPs exhibit rich and uniform mesoporous structures, and abundant nucleophilic halide ions and hydrogen bond donors are successfully integrated into the HIPs skeleton. The prepared catalysts show the superior CO 2 selective adsorption performance. In addition, the optimal catalyst HIP-IByBA(1:2) exhibits an excellent catalytic activity for the CO 2 cycloaddition without the metals, cocatalysts and solvents. Especially, under the mild condition (70 °C, 1.0 MPa), the catalyst HIP-IByBA(1:2) also maintains a satisfactory catalytic performance, effectively capturing dilute CO 2 (85 %N 2 /15 %CO 2 ) and converting it into cyclic carbonates. The excellent catalytic activity as well as good recyclability and substrate universality makes prepared pyridine-based HIPs promising heterogeneous catalysts for CO 2 cycloaddition reactions.
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