FUEL
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2025
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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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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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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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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
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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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Qiang Liu,Zizi Zhang,Xiang Zhang,Junling Chen,Hongwu Ma,Leizhi Zheng,Keliang Wu,Yanlong Tai
The capture and conversion of CO 2 are crucial for achieving carbon reduction targets. Currently, porous carbon is regarded as the most promising material for CO 2 capture, but it is limited by the lack of effective catalytic conversion functional sites. Frustrated Lewis Pairs (FLPs) are considered the most promising metal-free catalysts for CO 2 conversion, but homogeneous catalytic systems fall short of meeting industrial demands. To address this, this paper selected zeolitic imidazolate frameworks (ZIF-8 and ZIF-67) derived N-doped porous carbon (ZIF-8-C and ZIF-67-C) as Lewis base and subsequently introduces B(C 6 F 5 ) 3 to construct B/N-based FLPs, namely ZIF-8-C-FLPs and ZIF-67-C-FLPs. This approach aimed to simultaneously enhance the catalytic conversion ability of porous carbon towards CO 2 and the heterogenization of FLPs. These ZIF-8-C-FLPs and ZIF-67-C-FLPs exhibited exceptional CO 2 capture capacity, with CO 2 adsorption capacities of 57.4 and 41.2 cm 3 /g at 273.15 K and 1 bar, respectively. Additionally, ZIF-8-C-FLPs and ZIF-67-C-FLPs were utilized to catalyze the preparation of benzimidazole and benzoxazole from o-phenylenediamine and o-aminophenol with CO 2 , demonstrating excellent catalytic performance (yields above 86 %) and recyclability (at least 8 cycles).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Lianlong Zhan,Wei Lu,Qin Xiang,Zhiping Chen,Wenlu Luo,Cailin Xu,Renting Huang,Shuagnfei Wang,Hui He
Using biomass for the production of low-energy regenerative carbon capture materials represents an effective strategy to advance carbon dioxide capture and storage technologies. In this study, a low-energy regenerative bagasse-based CO 2 capture material is synthesized through a one-step, rapid crosslinking strategy. In this method, epichlorohydrin is used to crosslink bagasse with temperature sensitive Pluronic® F-127 and polyethyleneimine, thereby addressing the challenge of simultaneously incorporating multiple functional groups into the biomass matrix. The resulting material with abundant amino adsorption sites demonstrates a high adsorption capacity of 4.52 mmol/g. Interestingly, the temperature-sensitive response of the material facilitates the grafted amine chain segments on bagasse to stretch and shrink reversibly within a narrow temperature range of 25 °C for adsorption and 55 °C for desorption. The shrinkage state is conducive to the CO 2 desorption process, resulting in an ultralow regeneration temperature of 55 °C. Additionally, the water contained in the material enhances its cyclic stability in extreme environments, such as pure CO 2 atmosphere at high temperature. Overall, this research not only provides new ideas for enhancing the long-term stability and economic viability of CO 2 capture materials but also offers feasible solutions for combating climate change and promoting sustainable development.
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PubMed
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Minglun Cheng,Sibo Shen,Zhiwei Zhang,Kui Niu,Ning Wang
Electroreduction of CO2 to value-added low-carbon chemicals is a promising way for carbon neutrality and CO2 utilization. It was found that the diiron complex [(μ-bdt)Fe2(CO)6] (bdt = benzene-1,2-dithiolate) has high catalytic activity for electrocatalytic CO2 reduction. To further study the effect of the S-to-S bridge on the catalytic performances of diiron complexes for electrochemical CO2 reduction, four diiron complexes 1–4 with different rigid and conjugated S-to-S bridges were either selected or designed. The electrocatalytic studies showed that under optimal conditions, 2 with a 2,3-naphthalenedithiolato bridge exhibited the lowest catalytic onset potential (Eonset = −1.75 V vs Fc+/0), while 4 with a diphenyl-1,2-vinylidene bridge displayed the highest catalytic activity (TOFmax = 295 s–1), which is 1.5 times that of [(μ-bdt)Fe2(CO)6]. The controlled potential electrolysis experiments of 4 in 0.1 M MeOH/MeCN at −2.35 V vs Fc+/0 gave a total faradaic yield close to 100%, with selectivities of 77%, 9%, and 14% for HCOOH, CO, and H2, respectively. The mechanism for CO2 reduction was studied using density functional theory, IR spectroelectrochemistry, and electrochemical methods. The results indicate that modifying the structure of the S-to-S bridge is an effective strategy to improve the catalytic performance of diiron complexes for electrocatalytic CO2 reduction.
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iScience
·
2024
·
IF 4.6
Junfu Zhou,Yuting Miao,Hongxin Ding,Yuanhang Ren,Lin Ye,Bin Yue,Heyong He
Direct and stable conversion of CO 2 to aromatics (CTA) is an attractive route for reducing CO 2 emissions. However, due to the chemical inertness of CO 2 , direct CTA reaction with high aromatics selectivity is still challenging. In this work, a tandem catalyst Zn 0.1 Ti 0.9 O x /HZSM-5 with appropriate density and strength of acid sites exhibits a high aromatics selectivity of 67.2% and long-term stability over 100 h. Furthermore, the total selectivity of benzene, toluene, and xylene achieves 24.1% over Zn 0.1 Ti 0.9 O x /HZSM-5 with a modified hydrophilic surface. In addition, the CTA via the formate route has been determined in this reaction system.
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高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Lyu Wenyuan,Liu Yang,Chen Datong,Wang Fengliang,Li Yingwei
Photocatalytic conversion of CO 2 into syngas is highly appealing, yet still suffers from the undesirable product yield due to the sluggish carrier transfer and the uncontrollable affinity between catalytic sites and intermediates. Here we report the fabrication of Co sites with tunable electron localization capability on two dimensional (2D) nanosheets assembled three dimensional (3D) ordered macroporous framework (3DOM-NS). The as-prepared Co-based 3DOM-NS catalysts exhibit attractive photocatalytic performances toward CO 2 reduction, among which the cobalt sulfide one (3DOM Co-SNS) shows the highest syngas generation rate up to 347.3 μmol h −1 under the irradiation of visible light and delivers a remarkable catalytic activity (1150.7 μmol h −1 ) in a flow reaction system under natural sunlight. Mechanism studies reveal that the high electron localization of metal sites in 3DOM Co-SNS strengthens the interaction between Co and HCOO* via the orbital interactions of d yz / d xz - p and s - s , thus facilitating the cleaving process of C-O bond. Additionally, the ordered macroporous framework with nanosheet subunits elevates the transfer efficiency of photoexcited electrons, which contributes to its high activity.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Pengfei Lin,Xiwei Qu,Bhaskar Jyoti Deka,Chao Hu,Lei Zhao,Dongyun Wu,Chunhai Yi,Min Wei Boey,Muhammad Usman Farid,Alicia Kyoungjin An,Jiaxin Guo
The photocatalytic Metal-organic frameworks (MOFs) membrane addresses challenges faced by MOF powders in practical applications such as aggregation and difficult recovery, but its current application is mainly confined to wastewater treatment. Expanding the application of MOFs membranes to CO 2 reduction could unleash their greater potential in energy conversion and storage field. In this study, ZIF-67 was deposited on polyacrylonitrile (PAN) nanofiber membranes (NFMs) using an in-situ growth technique, followed by thermal stabilization to produce SZIF-67/PAN NFMs for photocatalytic CO 2 reduction. ZIF-67 was uniformly and densely distributed on the NFMs, with a mass loading of up to 8 wt%. The thermal stabilization process significantly enhanced the photothermal conversion capability and solvent resistance of the NFMs, enabling SZIF-67/PAN NFMs to exhibit outstanding photocatalytic activity even under mild environmental conditions, with a remarkable CO generation rate of 39,250 μmol g −1 h −1 . Furthermore, the performance remained at 70 % even after five consecutive tests. This study presents a novel and effective method for preparing MOF NFMs with excellent photocatalytic CO 2 reduction performance, offering valuable insights for advancing the practical application of MOF materials.
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Carbon Capture Science & Technology
·
2024
·
IF 10.4
Yangna Luo,Xianglin Chen,Xiang Liu,Yafei Guo,Yuxuan Gao,Guoyang Zhao,Chuanwen Zhao
Electrochemical CO 2 reduction to synthetic fuels and commodity chemicals using renewable energy offers a promising approach to mitigate CO 2 emissions and alleviate energy crisis. Copper-based catalysts show potential for electrochemical CO 2 reduction applications, while they face the key challenges of high potential, sluggish kinetics, and poor selectivity. In this work, Cu-Zn, Cu-Co, Cu-Cd, and Cu-In bimetallic catalysts are synthesized via the electrodeposition method for electrochemical CO 2 reduction to syngas with adjustable CO/H 2 ratios. The bimetallic catalysts are characterized using various techniques to reveal their crystalline structures, morphologies, and elemental compositions. The structure-property-activity relationships of these catalysts are investigated to identify optimal candidates for electrochemical CO 2 reduction applications. The findings reveal that the bare Cu mesh catalyst exhibits poor CO 2 reduction activity, and the products are dominated by hydrogen evolution reaction (HER). The bimetallic catalysts exhibit improved CO 2 reduction performance, with the Cu-Zn and Cu-Cd catalysts showing excellent activity, and the CO/H 2 ratio in syngas can be tuned over a wide range by adjusting the applied potential. The Cu-Zn and Cu-Cd catalysts demonstrate outstanding performance with Faradic efficiencies of ∼90 % and ∼80 % towards syngas production with CO/H 2 ratios of ∼2.0 and ∼1.5 at −0.81 and −1.01 V vs. RHE, respectively, making the produced syngas suitable for various industrial applications. Stability tests over 450 min show that the Cu-Zn and Cu-Cd catalysts maintain stable catalytic activity, syngas selectivity and CO/H 2 ratio, making them robust candidates for syngas production. The results will provide valuable insights into the design of robust catalysts for electrochemical CO 2 reduction, offering a promising path toward sustainable syngas production.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Yulan Xu,Minxian Wu,Xinlei Cheng,Shiying Wang,Dan Wang,Wenchang Wang,Naotoshi Mitsuzaki,Zhidong Chen
Gallium-based liquid metals are considered as promising catalysts for electrochemical CO 2 reduction due to their ability to effectively prevent the adhesion of byproduct carbon, which leads to the deactivation of electrode materials. In order to increase the specific area of liquid alloys, Ga-Sn thin liquid films were electrodeposited from a deep eutectic solvent composed of acetamide and dimethyl sulfone. Electrodeposition of Ga-Sn thin films with varying compositions that follow normal deposition behavior achieved, resulting in Sn rich in overall composition. To obtain Ga-rich thin liquid films, a straight forward and efficient two-step electrodeposition approach was employed. A layer of Ga thin film was firstly electrodeposited on the substrate, followed by electrodepositing a Sn layer. The prepared Ga-Sn thin films were applied for electrochemical reduction of CO 2 in a CO 2 -saturated 0.1 M KHCO 3 solution. Ga-Sn alloy with 91.6 at% Ga was in the liquid state at 25℃ and showed an excellent performance in reduction CO 2 to formate. The Faradaic efficiency reached 80 % and the partial current density was 46 mA cm −2 .
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