DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 6
·2526-2533
·
IF 3.5
Jia-Min Lyu,Shen Yu,Zhan Liu,He-You Du,Ming-Hui Sun,Chun-Mu Guo,Yi-Long Wang,Yu Li,Li-Hua Chen,Bao-Lian Su
Excessive emission of CO2 into the atmosphere has severely impacted the global ecological environment. Converting CO2 into valuable chemicals and fuels is of great significance for sustainable development. However, low activity and undesirable selectivity often result from the inherent inertness of CO2. Herein, K- or/and Zn-modified Fe-based catalysts were prepared by an incipient-wetness impregnation method for CO2 hydrogenation via a cascade reaction. The results indicate that K species exist as K2O while Zn species exist as ZnFe2O4. In the CO2 hydrogenation pathway, K2O facilitates the adsorption of CO2 and restrains the adsorption of H2, accelerating the transformation of CO2 into C2–C4 olefins rather than paraffins while Zn species promote the dispersion of Fe species, leading to improved activity. Synergistically, a K- and Zn-modified Fe-based catalyst (2Zn–10K–Fe/Al) shows excellent catalytic CO2 hydrogenation activity, achieving a CO2 conversion of 77% which is 1.8 times that (42%) of the unmodified Fe-based catalyst (Fe/Al). Our catalyst also shows a significantly promoted selectivity to C2–C4 olefins of 17% in comparison with the Fe/Al catalyst (0%). It is envisioned that such a binary effect of elements might contribute to the low-cost and industrial production of Fe-based catalysts for selective CO2 conversion.
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APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Yuanye Zhuang,Shiyang Bai,Meng Ge,Jingjing Sun,Yingying Cheng,Jihong Sun,Yanmin Yu
An environmentally friendly polymer catalyst (PAS) was synthesized via inverse emulsion polymerization using acrylic acid (AA) and 1-vinyl imidazole (VI) as monomers. The excellent catalytic activity of PAS was attributed to the synergistic effects of the carboxyl groups (-COOH) as hydrogen bond donors and N-heterocyclic carbene (NHCs) as electron donor, as well as the swelling properties of the polymer, which can enrich the substrate into the polymer network, increasing the contact between the substrate and active sites. Characterization results from thermogravimetric (TG) analysis and small-angle X-ray scattering (SAXS) showed that the excessive imidazole addition disrupted the polymer's chain-like structure, significantly reducing its swelling properties. And, the catalytic performance is influenced by both the amount of imidazole in PAS and the swelling properties of the polymer. Finally, the reaction mechanism of the CO 2 cycloaddition reaction catalyzed by PAS was proposed and validated through density functional theory (DFT) calculations.
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ChemPlusChem
·
2024
·
IF 3
Hongguang Liang,Xiaoyun Li,Junwei Wang,Qifeng Li,Yuelan Feng,Maoqing Kang,Yingan Zhang
Graphical The efficient utilization of CO 2 into cyclic carbonate as electrolytes and medical intermediates with 100 % atom efficiency is interesting. Employed as catalyst, carbon nitride family with different polymerization degree and pore structure exhibits excellent potential in the cycloaddition reaction. The active amino and hydroxyl groups in the catalyst form interaction with CO 2 molecules and epoxy groups, respectively, generating the synergistic effect to promote the reaction. For the efficient utilization of CO 2 into valuable product, the attractive carbon nitride catalysts have been widely studied. In this work, heptazine-related materials with varying degree of polymerization were designed by an intrinsically modification strategy and employed in the cycloaddition of CO 2 with the bisepoxide 1, 4-butanediol diglycidyl ether (BDODGE). We initially figured out that the sample prepared at 450 °C contained more melem hydrate, exhibiting the best performance. The epoxides conversion and corresponding cyclic carbonates selectivity could achieve 93.1 % and 99.3 % at 140 °C for 20 h without any cocatalyst and solvent, respectively. Results of the catalytic tests suggested that the high catalytic activity was dependent on big size porous structure and the synergetic effect of active amino groups and −OH groups. The role of water in maintaining the specific structure and providing active site has been proved. Moreover, the CN-450-W catalyst exhibited outstanding recycling stability. And finally, a plausible reaction mechanism was proposed.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Hao Yuan,Hanxiang Guo,Zhaosheng Huang,Ping Zhang,Zhe Wang,Chunde Jin
Traditional polyurethane coatings are typically synthesized from non-renewable petrochemical resources, which contradicts modern environmental principles. This paper aims to develop eco-friendly polyurethane wood coatings and enhance coating properties. CO 2 -based polyurethane (PU) was first synthesized by using CO 2 -based polyols instead of petroleum-based polyols and reacting them with isocyanates. The properties of PU coatings such as corrosion resistance, hardness, and adhesion were improved by introducing soybean oil-based polyols (P-ESO) from ring-opening reactions of epoxidized soybean oil (ESO) during the synthesis process. P-ESO-CO 2 -based PU (SPU) wood coatings demonstrated superior tensile strength and adhesion values of 0.77 MPa and 3.66 MPa, respectively, and exhibited a hydrophobicity with a water contact angle of 102°. Hence, SPU holds greater promise and potential for future development in the field of environmentally friendly wood coatings.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xiaofen Wei,Jun Liu,Huangyu Yan,Tianshan Li,Ying Wang,Yuqiong Zhao,Guoqiang Li,Guojie Zhang
Coal gasification fine slag (CGFS), a byproduct of the coal gasification process, is currently being recognized as a resource with significant potential for value addition and sustainable applications, especially in synthesizing CO 2 adsorbents. The overarching challenges in this domain include the attainment of high-efficiency, environmentally benign transformation of CGFS into useful products, and the development of cost-effective adsorbent materials featuring precisely engineered pore structures. In this study, a hierarchical porous nanostructured silica material is synthesized rapidly, efficiently, and cost-effectively through acid leaching and alkaline dissolution-assisted hydrothermal treatment, employing CGFS as the precursor. The mass ratios of sodium hydroxide (NaOH) to CGFS range from 0.4 to 1, resulting in varying morphologies and adsorption properties. Specifically, the sample with the NaOH to CGFS ratio of 0.6 (CGFS-0.6) shows the best adsorption performance. The adsorption capacities are 2.87 mmol/g and 8.49 mmol/g at 20 °C with 15 % and 45 % CO 2 concentration, respectively. The material is characterized by a well-developed pore structure shaped like a bouquet of flowers, with a specific surface area of 457 m 2 /g and pore volume reaching 2.34 cm 3 /g. During the hydrothermal processing, silicate/aluminosilicate entities self-organized into a Si-O-Na/Al network structure, endowing the synthesized adsorbent with optimal internal porosity and silanol functionalities. The adsorption equilibrium is achieved rapidly within 10 min, and CO 2 adsorption stability remains robust across 20 successive cycles. All isothermal models of the adsorbents conform to the Sips model. This study offers a promising pathway for the value-enhanced utilization of coal-derived solid wastes.
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ENERGY
·
2025
·
IF 9.4
Kefei Li,Yue Wu,Yiming Bai,Hai Yan,Yiming Wang,Yuzhe Guan,Liang Li,Guicheng Liu
Reducing the energy consumption of CO 2 regeneration is crucial for enhancing the economic feasibility of CO 2 capture processes. While most studies have focused on developing novel absorbents, the influence of operating parameters on gas-liquid mass transfer behavior and their subsequent impact on energy consumption has received limited attention. This study experimentally investigates the regeneration heat duty (Q reg ) for CO 2 desorption from a 1-(Dimethylamino)-2-propanol (1DMA2P)/2-Methylaminoethanol (MAE) aqueous blend in a lab-scale stripper equipped with high-efficiency Sulzer DX structured packing. The effects of key operating parameters, including rich CO 2 loading, lean CO 2 loading, solution flow rate, amine concentration, and synergistic parameters (Δ α × L and C × L ), on Q reg were systematically analyzed. The experimental results showed that all these factors greatly influenced Q reg . For example, the Q reg decreases as the lean CO 2 loading (α lean ) , rich CO 2 loading (α rich ) , and 1DMA2P/MAE concentration (C) increase, indicating that the Q reg can be reduced by optimizing these operating parameters. Additionally, compared with MEA, 1DMA2P/MAE reduces energy consumption by 51.5 % and decreases the stripper height by 35 %. This study underscores the critical role of operating parameters in reducing CO 2 regeneration energy consumption. The findings provide valuable insights into optimizing stripper performance and demonstrate the advantages of the 1DMA2P/MAE blend as an energy-efficient alternative to MEA-based solvents in industrial CO 2 capture applications.
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ACS Catalysis
·
2025
·
IF 13.1
Zhiwei Liang,Shan Tang,Siyu Chen,Lanqi Ning,Jijie Wang,Can Li
Zinc–zirconium oxides (ZnZrOx) are highly selective and stable catalysts for the hydrogenation of CO2 to CH3OH. However, their catalytic activity has remained relatively moderate, and the influence of the ZnZrOx crystalline phase on performance is not yet fully elucidated. Here, we report a mixed-phase ZnZrOx, comprising coexisting tetragonal and monoclinic domains, and correlate this biphasic architecture with the catalytic performance. At 320 °C, the mixed-phase ZnZrOx catalyst delivers a CO2 conversion of 9.2% coupled with an impressive CH3OH selectivity of 87%, representing a 1.4-fold increase in conversion compared to its purely tetragonal counterpart while maintaining equivalent selectivity. In-depth characterizations attribute this improved performance primarily to the emergence of a two-phase interface, which enhances the dissociation and activation of H2. Density functional theory calculations further reveal that this interfacial region plays a vital role in promoting heterolytic H2 dissociation, boosting the formation of HCOO* and lowering the energy barriers of the rate-determining step for CH3OH formation. This work highlights the effectiveness of the crystal-phase architecture in optimizing ZnZrOx catalysts for CO2 hydrogenation to CH3OH, offering strategic insights for the design of advanced oxide-based hydrogenation systems.
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Carbon Capture Science & Technology
·
2025
·
IF 10.5
Hui Zhou,Yaozu Wang,Yuqi Niu,Yunrong Zhao,Bocheng Yu,Jinyang Xu,Yongqing Xu,Shijie Yu,Xuan Bie,Qinghai Li,Yanguo Zhang,Jingyuan Ma,Shuzhuang Sun,Fei Song
The incorporation of nitrate molten salts has been demonstrated as an effective strategy to enhance the CO 2 uptake of MgO for intermediate-temperature (200–400°C) CO 2 capture. However, the slow carbonation kinetics in flue gas capture, coupled with poor stability, hinder its industrial application. In this study, the addition of Na 2 CO 3 was found to significantly improve the sorption kinetics of MgO in a 15% CO 2 atmosphere, achieving a CO 2 capacity of 19.9 mmol/g at 275°C with a 15 mol% total promoter loading (Na 2 CO 3 /NaNO 3 = 1:4). Mechanistic analysis revealed that Na 2 CO 3 promotes the formation of Na 2 Mg(CO 3 ) 2 , which acts as an effective nucleation site for MgCO 3 formation, accelerating the carbonation rate by a factor of eight. The Hard X-ray photoelectron spectroscopy (HAXPES) revealed that an increased Na/Mg ratio caused subsurface migration and aggregation of molten salts, leading to a permanent rise in local salt concentrations, which negatively affected CO 2 capture performance. These findings offer valuable insights into the structural degradation mechanisms and provide guidance for enhancing the stability of nitrate-enhanced MgO, thereby improving its potential for intermediate-temperature CO 2 capture.
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JOURNAL OF POLYMER RESEARCH
·
2025
·Vol. 32
·期 7
·1-15
·
IF 2.8
Liu Li,Zhao Shuaishuai,Liu Jinxin,Zhan Ende,Wei Jinyun,Xing Mengyi
CO 2 flooding, as an effective method for developing low-permeability heavy oil reservoirs, is often limited by the early gas breakthrough due to the high mobility of the gas. To address this issue, research on enhanced oil recovery using a composite flooding method combining viscosity reducer and CO 2 was conducted. Firstly, a novel low molecular weight viscosity reducer, PAINS, was prepared. Subsequently, the mechanism of viscosity reduction by the viscosity reducer in heavy oil was explored from a molecular simulation perspective. Finally, the oil displacement efficiency of the viscosity reducer-CO 2 combination flooding was studied through core flooding experiments. The results showed that the prepared viscosity reducer exhibited effective viscosity reduction; within the viscosity reducer-heavy oil system, the viscosity reducer achieved its effect by altering the internal structure of the heavy oil. The slug of the viscosity reducer was able to improve the mobility ratio of oil and gas caused by viscosity differences, delaying the breakthrough of CO 2 along gas flow channels. The viscosity reducer-CO 2 combination flooding method increased oil recovery by 14.5% compared to single CO 2 flooding, indicating that the viscosity reducer-CO 2 combination flooding technology has broad application prospects in the development of low-permeability heavy oil reservoirs.
Section
Graphical abstract
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LANGMUIR
·
2025
·
IF 3.9
Yongtao Zhang,Zaizheng Jiang,Zhihe Xin,Qingqi Dong,Fei Wang
Traditional coal burning emits a large amount of pollutants, including sulfur dioxide (SO2), nitrogen oxides, and carbon dioxide (CO2), severely contaminating the environment and exacerbating global warming. In contrast, integrated gasification combined cycle (IGCC) technology, with highly efficient and clean characteristics, significantly reduces pollutant emissions and has a positive impact on environmental protection. It is a simple and effective method to obtain hydrogen (H2) by purifying IGCC fuel gas with the main components of H2 and CO2. Thermodynamic promoter tetra-n-butyl ammonium bromide (TBAB) is widely used in gas separation of IGCC fuel gas by the hydrate method. In this work, polystyrene nanoparticles grafted by –SO3– groups (−SO3–@PSNS) and grafted by –SO3– groups and Ag particles (Ag&–SO3–@PSNS) are used together with TBAB, respectively, to promote the formation of hydrate. The gas separation effect and growth morphology are studied. The experimental results demonstrate that the incorporation of nanopolymer can significantly enhance the separation efficiency (SFr) of a mixture of H2 and CO2. Notably, compared to the reaction solution without nanopolymer, 2 mmol/L –SO3–@PSNS exhibits the most pronounced effect on gas separation, resulting in an impressive gas consumption of 0.755 ± 0.323 mmol/L and a remarkable increase in the separation factor (SF) by 106%. After loading silver nanoparticles, the promoting effect of Ag&–SO3–@PSNS is further strengthened. Under Ag&–SO3–@PSNS-20%, the gas consumption reaches the maximum of 0.775 ± 0.003. Under Ag&–SO3–@PSNS-30%, the SF rises from 32.79 ± 6.27 to 37.92 ± 7.19, indicating an impressive increment of 15.80%. The visualized droplet experiment shows that Ag&–SO3–@PSNS significantly promotes the nucleation of hydrate and the growth rate of hydrate.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2025
·
IF 4.6
Fan Yang,Siqing Liu,Mengdie Yang,Deting Fei,Yunxin Zhang,Panjie Li,Xiaojun Luo,Qiwei Wang
The development of innovative materials capable of detecting heavy metal ions is a crucial goal in the field of environmental remediation. However, achieving high selectivity for specific metal ions remains a challenge. This study designs a novel imine-based COF via Schiff base condensation for efficient detection of cobalt ions (Co 2+ ) in environmental samples. The π-conjugation system provides excellent fluorescence properties. The COF contains tertiary amine and imine structures with nitrogen and oxygen atoms, enabling coordination with Co 2+ as a Lewis base. This interaction disrupts the conjugated structure, causing fluorescence quenching. The experimental results demonstrate that our proposed method stands out in Co 2+ detection, distinguished by its remarkable simplicity, exceptional sensitivity, rapid response time, and easy operability. The novel imine-based COF sensor exhibits high sensitivity (limit of detection = 8.5 × 10 −13 M), excellent selectivity and stability in fluorescence detection, enabling accurate identification of Co 2+ in complex environments. This research not only presents an efficient and practical approach for the detection of Co 2+ but also offers novel theoretical perspectives on the design and application of imine-based COF. The findings lay a solid foundation for the development of COF-based environmental monitoring technologies.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Wang Ruonan,Zhang Mingjia,Liu Jingjing,Wu Xu,Zhang Shule,Zhong Qin,Yao Jianfeng
Scaling up methanol yields by artificial photosynthesis at a modest cost remains thermodynamically challenge. Designing concerted reaction sites to control intermediate evolution and stimulate proton-coupled electron transfer (PCET) is necessary. Here we show a nickel-titanium-based catalyst that achieves near-millimolar hourly methanol yields with 99.79% selectivity and a solar-to-chemical conversion efficiency of 2.23%. This catalyst is synthesized through one-step etching of NiTi-layered double hydroxide, which generates abundant unsaturated sites, along with the in-situ formation of amorphous TiO 2 . Revealed by in-situ characterizations, these defect-rich units effectively suppress the formation of undesirable carbonate while promoting the favorable *COOH intermediate. Furthermore, theoretical simulations confirm this *COOH boost facilitates the production of *CO and accelerates the PCET steps. This work significantly advances efficient methanol production by artificial photosynthesis and offers fundamental insights into controlling reaction pathways for renewable fuel synthesis.
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