CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Feiyu Zhu,Yudong Ding,Xinglu Feng,Yujia Gan,Xun Zhu,Min Cheng,Qiang Liao
Hydrophobic DES integrates CO 2 cycloaddition and catalyst recycling. • Polarity evolution drives aqueous extraction of carbonate products. • Water extraction gives 93% recovery and > 97% yield over five cycles. • DFT reveals a water-tolerant decanol-assisted ring-opening pathway. • Catalyst-as-raffinate design enables reaction–separation integration. Homogeneous catalysts offer high activity for CO 2 fixation, yet their separation from polar carbonate products remains a persistent barrier to catalyst recycling. Here, we report an integrated catalysis–separation system based on a catalyst-as-raffinate strategy, exploiting the polarity increase inherent to the CO 2 cycloaddition of epoxides. A hydrophobic deep eutectic solvent composed of trioctylmethylammonium bromide and decanol was constructed as both the catalytic medium and the recyclable low-polarity raffinate phase. During the conversion of glycidol to glycerol carbonate, the reaction-induced polarity shift promotes product partitioning into water during extraction, while retaining the catalyst in the hydrophobic phase. Product extraction reached 93%, and the recovered catalyst maintained glycerol carbonate yields above 97% over five consecutive catalytic–extraction cycles. DFT and energy-decomposition analyses show that residual water is thermodynamically accommodated within the hydrogen-bonding catalytic network, whereas the decanol-assisted ring-opening pathway remains kinetically favored by avoiding excessive exchange repulsion in the rate-determining transition state. These features enable stable catalytic performance during aqueous recycling. Across different epoxides, extraction efficiency correlates with the product–DES polarity difference. This work establishes reaction-induced polarity evolution as a design principle for coupling homogeneous catalysis with product separation and catalyst recycling. Download: Download high-res image (101KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Jing Fan,Pengfei Jin,Guohua Wu,Fenhong Song,Long Ma
Twelve ternary DESs were prepared for efficient and regenerable CO 2 capture. • AA-PZ-EG (1:1:8) reached 0.18876 mol mol −1 at 303.15 K and 810 kPa. • CO 2 solubility was accurately correlated with a maximum AAD of 0.299%. • FTIR verified physical dissolution coupled with amine-assisted chemical capture. • DES2 retained >80% regeneration efficiency after three capture-release cycles. To address the greenhouse effect and climate change caused by excessive CO 2 emissions, the development of efficient, green, and regenerable CO 2 absorbents has become a major research focus in the fields of energy and environmental science. In this study, twelve ternary deep eutectic solvents (DESs) were synthesized from acetamide, piperazine, 1,4-diazabicyclo[2.2.2]octane (DABCO), ethylene glycol, and diethylene glycol via a one-step heating and stirring method. The density, viscosity, potential ecotoxicity of the constituent components, CO 2 absorption performance, and short-term cyclic performance were systematically investigated. With increasing temperature, the prepared DESs exhibited an approximately linear decrease in density, while their viscosity displayed a temperature-dependent reduction consistent with Arrhenius behavior. Ecological Structure-Activity Relationships (ECOSAR) screening suggested relatively low predicted aquatic toxicity for most of the individual components, whereas the ecotoxicity of the complete DES mixtures remains to be assessed experimentally. Among the twelve ternary DESs, DES2, which exhibits combined physical dissolution and reversible chemical interactions at the PZ sites, showed the best CO 2 absorption performances, with a CO 2 uptake of 0.1294 g CO 2 /g DES at 303.15 K and 810 kPa. The CO 2 solubility data were correlated using the Jou and Mather equation within the investigated temperature and pressure ranges, and the model showed good agreement with the experimental data. Moreover, DES2 (AA:PZ:EG = 1:1:8) retained over 80% of its initial CO 2 absorption capacity after three consecutive absorption–desorption cycles, indicating favorable short-term cyclic performance. Download: Download high-res image (162KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
AICHE JOURNAL
·
2026
·
IF 4.4
Xin Ta,Qiang Sun,Min Xiao,Zhiwu Liang,Hongxia Gao
Phase-separating absorbents show promise for reducing energy consumption, as desorption requires heating only the CO 2 -enriched phase. This study investigates triethylene glycol monobutyl ether (TGBE) as a phase-separation promoter for the N-methylaminoethanol (MAE)–water system. The role of TGBE in restructuring hydrogen-bond networks and promoting rich-phase aggregation was analyzed using gas–liquid–liquid equilibrium, 13 C NMR, gas chromatography, and molecular dynamics (MD) simulations. Experimental results demonstrate that TGBE significantly reduces rich-phase volume while achieving CO 2 equilibrium loadings of 3.59 mol/kg for water-containing systems and 4.73 mol/kg for water-free systems. MD simulations reveal that CO 2 absorption redistributes intermolecular interactions, where strengthened hydrogen bonds between water and ionic species drive polar rich-phase aggregation. Furthermore, an empirical model, a GBDT-based predictive model, and a modified Deshmukh–Mather framework were developed to describe phase behavior with AARDs of 2.81%, 4.58%, and 6.61%, respectively. These findings provide a theoretical foundation for designing energy-efficient CO 2 capture systems.
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122807
·
IF 7.5
Xiao Lin,Zhenxing Zhou,Xiuxiu Zhang,Chongqing Wang
Indirect mineralization is a promising technology for carbon capture, utilization, and storage that enables CO 2 sequestration while simultaneously producing high-purity CaCO 3 . There remains a research gap in the regulation of the CaCO 3 product in the CO 2 mineralization process. This work innovatively compared CO 2 mineralization in different systems. Ca leaching from titanium gypsum was conducted using ammonium citrate, and then CO 2 mineralization was performed in Ca-rich solution (CRS) and calcium citrate precipitate (CCP) systems. The effects of key parameters including ammonia dosage, CO 2 flow rate, and temperature were studied, and the mineralization conversion rate and mineralization products were investigated. Ammonia dosage significantly influenced the mineralization conversion rate and the crystal form of CaCO 3 , and the conversion rate was 95% at 50 mL/L ammonia for CCP and 85% at 100 mL/L ammonia for CRS. Notably, increasing ammonia dosage promoted the vaterite formation in the CCP system. Temperature exhibited a pronounced impact on the mineralization conversion rate. As the temperature increased, the time required to attain the maximum conversion rate decreased markedly from 20 min to 5 min for CRS and from 60 min to 10 min for CCP. Temperature also influenced particle size and morphology, with both systems producing larger particles at higher temperatures. As to the growth mechanism of CaCO 3 , the CRS exhibited a gas–liquid interface dominated by homogeneous nucleation, while the CCP system proceeded through a gas–liquid–solid mechanism governed by heterogeneous nucleation. The high-quality CaCO 3 product (93.53% purity and 96.40% whiteness for CRS; 95.32% purity and 97.80% whiteness for CCP) meeting the standards of commercial CaCO 3 indicated promising economic benefits.
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yali Wang,Leibing Chen,Jing Mei,Guoying Li,Feng Zhang,Jiaxing Lu,Huan Wang
“Bimetallic-molecular” interface strategy constructs CuxAg1-x-SPyz catalysts for efficient CO 2 -to-methanol. • Cu 0.3 Ag 0.7 -Spy 0.05 achieves 46.8% methanol FE and 117 mA cm −2 partial current in a flow cell. • DFT calculations confirm Cu-Ag optimizes *CO adsorption, while pyridine modification lowers the *CO → *CHO barrier by 0.27 eV. The design of highly selective catalysts for direct methanol production via CO 2 electrolysis remains challenging due to its complex pathways and intense hydrogen evolution competition. This study employed a “bimetallic-molecular” interface synergy strategy to construct Cu x Ag 1-x -SPy z catalysts by in situ anchoring mercaptopyridine on the CuAg bimetallic surface. Experimental results indicate that the Cu 0.3 Ag 0.7 -Spy 0.05 catalyst in an H-cell exhibits a maximum Faradaic efficiency (FE) of 45.3% for methanol at −1.13 V (vs. RHE), while the FE for methanol in a flow cell reached 46.8% with a partial current density of 117 mA cm −2 , outperforming unmodified Cu Ag and existing mainstream catalysts. In situ ATR-FTIR spectroscopy simultaneously captured *COOH, *CO, *CHO, *OCH 2 , and *OCH 3 intermediates. Combined with DFT calculations, it was confirmed that Cu Ag synergistically optimized *CO adsorption energy, while the modified pyridine acted as a proton relay, lowering the *CO → *CHO energy barrier by 0.27 eV to achieve directional regulation of the methanol pathway. This study establishes a scalable molecular interface engineering paradigm for highly selective CO 2 methanolation and expands novel approaches to “metal-ligand” synergistic design in complex multi-electron reactions. Anchored by metal‑sulfur bonds, a mercaptopyridine modified copper‑silver bimetallic composite material Cu 0.3 Ag 0.7 -SPy 0.05 is prepared. The synergistic interaction between silver and copper bimetallic sites enhances the generation and adsorption of *CO, while the pyridine groups accelerate the effective protonation of *CO to methanol. It delivers a Faradaic efficiency of 46.8% with a partial current density of 117 mA cm −2 for methanol. Download: Download high-res image (179KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Yuqing Sui,Jinlong Li,Xue Yang,Dongxuan Guo,Mingna Chu,Guozhe Sui
ZIF-67-derived Co 3 O 4 /MXene Schottky heterojunction is constructed successfully. • MXene concentrates CO 2 molecules and participates in surface redox reactions. • Schottky heterointerface improves photogenerated carrier separation. • Co 3 O 4 /MXene Schottky heterojunction achieves effectively photocatalytic CO 2 reduction to CO. The escalating emission of carbon dioxide necessitates the urgent development of efficient CO 2 conversion technologies. Herein, a novel Co 3 O 4 /MXene Schottky heterojunction photocatalyst was rationally designed and synthesized, where Co 3 O 4 is derived from ZIF-67 and anchored onto MXene nanosheets. The composite demonstrates high activity in photocatalytic CO 2 reduction, achieving a yield rate of 58 μmol g −1 h −1 for CO using triethanolamine (TEOA) as an electron donor, while maintaining excellent stability over multiple cycles. The enhanced performance stems from the Schottky junction between Co 3 O 4 and MXene, which establishes a built-in electric field that drives efficient charge separation and directional carrier flow. Additionally, MXene acts as a cocatalyst that not only concentrates CO 2 molecules near active sites but also participates in surface redox reactions. This work offers an effective strategy for designing high-performance photocatalysts for sustainable solar fuel production. Download: Download high-res image (368KB) Download: Download full-size image A novel ZIF-67-derived Co 3 O 4 /MXene Schottky heterojunction exhibits photocatalytic CO 2 reduction to CO with production rate of 58 μmol g −1 h −1 .
✓ 已验证
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2026
·
IF 9.2
Liju Bai,Xiaotong Jiang,Can Lv,Yaxing Zhang,Wenwei Wu,Zixuan Hao,Jianchao Luo,Yimin Deng,Tejraj M. Aminabhavi,Helei Liu
High thermal stability amine solvents are critical for post-combustion CO 2 capture. For this, two novel ternary blended amine systems, AMP-AEP-MDEA and AMP-HMDA-MDEA were developed to overcome the limitations of traditional monoethanolamine (MEA) due to its poor thermal stability. The results demonstrated that both the chosen ternary systems exhibited superior CO 2 absorption-desorption performance compared to 30 wt% MEA due to synergistic kinetic effects and high molar amine density, emphasizing the importance of environmental management. To rigorously evaluate long-term durability, accelerated thermal degradation tests were conducted at 150 °C for 28 days to demonstrate AMP-AEP-MDEA had the highest thermal stability with a degradation rate of 25.1%, significantly lower than those of AMP-HMDA-MDEA (29.4%) and MEA (39.6%). Mechanistic investigations using 13 C NMR and GC-MS elucidated distinct degradation pathways. AMP undergoes independent intramolecular cyclization to form oxazolidinones, while stability of the activators dictates the overall system robustness. Rigid heterocyclic nature of AEP that restricts deep fragmentation, limiting the degradation of the side-chain cleavage. In contrast, flexible linear HMDA chains are susceptible to C-C bond breakage and dehydrogenation, leading to the formation of irreversible aromatic byproducts such as methylpyridine. The research highlights the critical role of molecular topology in solvent stability, suggesting AMP-AEP-MDEA as a promising candidate for large scale CO 2 capture to provide clean environment.
✓ 已验证
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122721
·
IF 7.5
Nitin Goyal,Peng Gao,Liying Liu,Haoran Liu,Zhe Wang,Shuwen Cheng,Gang Li
The development of efficient and scalable solid sorbents is crucial for advancing CO 2 capture technologies. While commercial activated carbons are inexpensive and porous, they typically exhibit low CO 2 selectivity. This study demonstrates a facile two-step strategy to significantly enhance the CO 2 capture performance of a commercial granulated activated carbon (DGAC). The carbon was first oxidized with nitric acid to create anchoring sites, and then impregnated with the amine-rich polymer polyethylenimine (PEI). Comprehensive characterization like SEM-EDS, XPS, BET confirmed the successful incorporation of PEI onto the oxidized surface. The modified adsorbent (O-DGAC@PEI) achieved a remarkable CO 2 adsorption capacity of 4.67 mmol/g at 273 K and 1 bar, nearly double that of the pristine DGAC (2.6 mmol/g). More importantly, it exhibited exceptional CO 2 /N 2 selectivity of 349 (for a 15/85 CO 2 /N 2 mixture), as calculated by the Ideal Adsorption Solution Theory (IAST). The high isosteric heat of adsorption of 73.63 kJ/mol confirms chemisorption as the dominant mechanism, facilitated by the introduced amine groups. The adsorption process was spontaneous and well-described by the Dual-site Langmuir model. Thus, O-DGAC@PEI offers a favorable balance of high adsorption capacity, strong humidity resistance, and stable cyclic performance, distinguishing it from previously reported systems and demonstrating its potential for practical CO 2 capture applications.
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Jiasen He,Ruimin Zhao,Xuran Li,Qiannan Wang,Yumeng Xiao,Yue Wu,Tony D. James,Lidong Wang,Meng Li
The catalytic conversion of CO 2 into value-added chemicals via epoxide cycloaddition represents a promising route for sustainable carbon utilization. Herein, a facile one-pot doping strategy is developed to fabricate a robust and cost-effective catalyst from biomass waste rice husk. The N-doped carbon dots (CDs) are in situ synthesized and simultaneously doped within a mesoporous silica network via covalent C-O-Si bonds, followed by Cu(II) ions coordinating doping. The incorporation of hydrogen bond donor (such as hydroxyl groups) and Lewis base sites (nitrogen groups) on the CDs within the silica network synergistically activate the epoxides and CO 2 molecules, meanwhile the Si O protective layer promotes the catalytic stability. Furthermore, density functional theory (DFT) calculations reveal that Cu N complexes lower the energy barrier by facilitating epoxide activation. The resulting multi-confined catalyst delivers a 99% yield within 15 h at 80 °C and 1 atm CO 2 , retaining its activity after ten cycles. Life cycle and techno-economic analyses reveal that the prepared catalyst produces less CO 2 emissions and reduces the cost of styrene carbonate production to $31.3 per kg, below the commercial value ($100 per kg). This work paves a new way for sustainable and economical CO 2 valorization via highly efficient and stable catalyst.
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Zhiliang Guo,Huiyu Liu,Bo Jin,Rufang Peng,Qingchun Zhang
A practical strategy was proposed to prepare interlayer Ni-Co DACs. • The Ni-Co DACs achieve a high FE CO of 97% at −0.7 V. • The interlayer Ni-Co DACs possess superior catalytic activity, selectivity, and durability. Developing highly efficient, selective, and stable electrocatalysts for the electrochemical CO 2 reduction reaction (CO 2 RR) is crucial for mitigating energy and environmental challenges. This work presents a practical strategy for synthesizing spatially discrete yet strongly synergistic interlayer dual-metal atom catalysts (DACs) with a Ni-Co configuration through pyrolysis of core-shell zeolite imidazolate frameworks (ZIFs). The resulting CoNC@NiNC catalyst features a core-shell structure where CoNC is encapsulated within NiNC. The strong interaction between the layers of NiNC and CoNC increases the density of active sites, ensures the stability of the structure, facilitates mass or charge transfer, and may produce synergistic interaction between the active sites in core and shell, which can effectively catalyze the conversion of CO 2 to CO. Benefiting from the unique interlayer Ni-Co configuration, the CoNC@NiNC electrocatalyst achieved minimal onset overpotential, high CO Faraday efficiency (FE CO = 97%), and robust operational stability at −0.7 V vs. reversible hydrogen electrode ( vs. RHE). This study demonstrates the promising potential of interlayer DACs for efficient CO 2 RR, more importantly, establishes a viable method for developing interlayer DACs, utilizes the strong interlayer interactions to drive this complex reaction, and inspires further exploration of interlayer DACs in energy conversion and beyond. Download: Download high-res image (152KB) Download: Download full-size image The interlayer dual-metal atom catalysts (DACs) with controlled local coordination environments and three-dimensional spatial structures can efficiently convert CO 2 into high-value chemicals or fuels. Herein, a practical strategy was proposed to prepare interlayer Ni-Co DACs, which have core-shell structure consisted of CoNC encapsulated within NiNC (denoted as CoNC@NiNC), by self-assembly and high-temperature pyrolysis core-shell zeolite imidazolate frameworks (ZIFs) precursor. The practice reveal that the interlayer Ni-Co DACs possess superior catalytic activity, selectivity, and durability, which demonstrates the great potential as highly efficient catalysts for CO 2 RR.
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Xiangyun Liao,Chengdong Kong,Yanchi Jiang,Xiaojiang Wu,Zhongxiao Zhang
Chemical absorption with amines offers an attractive solution for large-scale carbon mitigation, but its practical application is impeded by high regeneration energy consumption. Despite extensive efforts to accelerate regeneration through chemical catalysis, inefficient gas-liquid mass transfer during desorption remains a major bottleneck. Herein, we report a microcavity-engineered desorption packing fabricated via nanosecond laser etching to promote bubble nucleation and release. Benefiting from the enhanced mass transfer, the optimized desorption packing enhances the maximum desorption rate by 92.2% and reduces the relative heat duty by 35.8% compared to the blank case, without significant performance degradation after multiple desorption cycles. Mechanistic studies show that the laser-induced microcavities can entrap gas to form stable gas nuclei sites, reducing the supersaturation barrier for bubble nucleation and thus accelerating the amine regeneration. The universality of this microcavity engineering strategy is demonstrated by its successful implementation on different substrate materials, including Ni, Ti, and Fe. This study provides new ideas for the design and fabrication of highly efficient desorption packings.
✓ 已验证
DOI
高影响因子
GREEN CHEMISTRY
·
2026
·
IF 10.6
Yangyang Jiang,Yuxin Liu,Yuanli Qi,Yurou Shao,Dong Wang,Benshuai Guo,Jingyan Zhao,Zhibin Zhou,Yuntao Lei,Lili Jin
The capture and utilization of carbon dioxide (CO2) from the post-combustion of fossil fuels has been identified as a highly effective strategy for reducing carbon emissions. Herein, a series of novel substituted benzenesulfonamide ionic liquids (BSA-ILs) were designed and synthesized via facile acid–base neutralization reactions for the purpose of achieving reversible CO2 capture and catalyzing CO2 chemical fixation. Addressing the inherently high viscosity of neat BSA-ILs (551.2–7785.7 mPa s), propylene carbonate (PC), a green product derived from CO2 chemical fixation, was selected as a diluent to form BSA-IL mixed absorbents (BSA-IL-MAs). The optimized system exhibited a high CO2 uptake capacity of 1.38 mol of CO2 per mol BSA-IL, an excellent CO2/N2 selectivity of 18.36, and a remarkable 99.0% conversion of epichlorohydrin under mild, solvent-free, metal-free, halogen-free, co-catalyst-free and atmospheric pressure conditions. Meanwhile, the findings demonstrated a certain positive correlation between the CO2 uptake capacity/conversion and the pKa of the substituted BSA. Notably, the BSA-IL system retained nearly intact CO2 capture performance and catalytic activity after five consecutive absorption–desorption and catalytic cycles, with an extremely low E-factor of 0.11. Spectroscopic characterization confirmed the formation of a new carbonyl moiety peak in CO2-saturated BSA-ILs, indicating that chemisorption dominated the CO2 uptake process. NMR investigations and DFT calculations further elucidated the interactions between BSA-ILs, CO2 and epoxide substrates, validating the feasibility of the proposed reaction pathways. This work provides a sustainable, efficient and industrially feasible integrated platform for CO2 capture and utilization, offering a paradigm for low-carbon catalytic conversion systems.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）