Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Wenhan Wang,Wenqiang Li,Zijian Wang,Bo Liu,Bing Wang,Jingui Duan,Rongfei Zhou
Carbon dioxide capture is an effective method to mitigate climate change . Highly CO 2 -selective and highly moisture-resistant absorbent is essential for energy-efficient carbon capture by absorption. Herein, a highly CO 2 -selective and high-silica CHA zeolite in a pure lithium form (Li-SSZ-13) was synthesized using a direct synthesis method for the first time. The effects of gel n (SiO 2 )/ n (Al 2 O 3 ) ratio, gel n (SiO 2 )/ n (Li 2 O) ratio and synthesis time on the crystallinity , yield, micropore volume and CO 2 loading of the crystals were systematically investigated. The adsorption isotherms of CO 2 and N 2 were measured for directly synthesized Li-SSZ-13, conventional Na-SSZ-13 and ion-exchanged Li-Na-SSZ-13 zeolites. The dynamic breakthrough adsorption properties were measured for Li-SSZ-13 in comparison with Na-SSZ-13 and Li-Na-SSZ-13. The obtained Li-SSZ-13 exhibited a high CO 2 adsorption capacity of 4.48 mmol/g and a high CO 2 /N 2 IAST selectivity of 310 at 100 kPa and 273 K, which were 45.0 % and 441 % higher than Na-SSZ-13 zeolite, 24.8 % and 179 % higher than Li-Na-SSZ-13 zeolite, respectively. It suggests that directly synthesized Li-SSZ-13 zeolite has great potential for efficient CO 2 capture from flue gas .
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Science China-Chemistry
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2024
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IF 10.4
Chen Zhi-Wei,Wang Hong-Juan,Liu Chang,Lu Xiu-Li,Lu Tong-Bu
Nitrogen-doped carbon materials have been widely used for the constructions of single-atom catalysts, while the effect of different species of doped nitrogen on the catalytic activity of CO 2 electroreduction has rarely been investigated. Here we found that pyrrolic-N coordinated Ni 2+ catalysts display much higher electrocatalytic CO 2 -to-CO activity and selectivity than the corresponding pyridinic-N coordinated low valent Ni (0−+2) catalysts, and pyrrolic-N coordinated Ni 2 dual-atoms catalyst of Ni 2 /N-CNTs exhibits the best electrocatalytic performance, with over 90% Faradaic efficiencies in a broad potentials from −0.6 to −1.2 V vs. reversible hydrogen electrode, as well as an outstanding CO specific current of 56.2 A/mg Ni and high turnover frequency of 6.2 × 10 4 h −1 , over 7-times higher than those of pyridinic-N coordinated Ni catalysts. Electrochemical results indicate the weak electron-donor nature of pyrrolic-N facilitates the generation of a reduced active site at low overpotential for boosting CO 2 electroreduction. Density functional theory calculations reveal that the reaction free energy for the *COOH formation on pyrrolic-N coordinated Ni catalysts are lower than those on pyridinic-N coordinated Ni catalysts, and a H 2 O-adsorbed Ni 2 /N-CNTs displays the optimized reaction free energy for both *COOH formation and CO desorption, which derive the best catalytic performance.
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ACS Applied Optical Materials
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2024
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IF 0
Zhiwei Wang,Qiuying Wang,Qin Liu,Suwit Suthirakun,Wongsathorn Kaewraung,Peng Jiang,Hang Zhao,Xin Xin,M. A. Subramanian
Blue pigments and blue glazes play crucial roles in our daily life. Ongoing research into blue pigments aims at environmentally friendly compositions with a lower cost. In this work, Co-doped BaAl2Si2O8 pigments were synthesized by a solid-state method. The blue color of the pigments is due to the 4A2(4F) → 4T1(4P) transitions allowed by doped Co2+ in the tetrahedral coordination of the structure. The pigments exhibit excellent stability under both acidic and alkaline conditions. When combined with transparent glazes, BaAl2–xCoxSi2O8 demonstrates satisfied compatibility, resulting in blue glazes with a significant reduction in Co content compared with existing formulations. Furthermore, BaAl2–xCoxSi2O8 blue glazes possess a simple production route, commendable color performance, and cost-effectiveness.
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Nature Communications
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2025
·Vol. 16
·期 1
·1-9
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IF 15.7
Wei Shilei,Hua Hang,Zhao Yuxuan,Luo Jingshan
Zero-gap membrane electrode assembly (MEA) CO 2 electrolysers offer high energy efficiency and promise for industrial application. However, the transport of carbonates within an anion exchange membrane (AEM) electrolyser leads to CO 2 loss, thereby limiting carbon utilization efficiency. Emerging acidic anolyte electrolysers using cation exchange membrane (CEM) can address this challenge but face critical stability issues, including accelerated hydrogen evolution reaction (HER) and persistent salt precipitation. Here, we propose a porous membrane (PM) as an alternative to the CEM in acidic anolyte electrolysers. The system demonstrates continuous operation at 100 mA cm −2 for 200 h without salt precipitation, while maintaining nearly 100% CO selectivity. Furthermore, large-scale device (100 cm 2 ) also shows stable performance. Mechanism analysis suggests that enhanced water permeation and bidirectional ion transfer are critical for achieving stable performance in acidic anolyte electrolysers. These findings offer a feasible approach for high-performance, stable and scalable acidic MEA CO 2 electrolysers.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Li Wang,Zhangmiao Ye,Caihong Lin,Yugao Wang,Jinping Li,Jiangfeng Yang
N2O/CO2 separation in the tail gas of adipic acid presents a significant challenge due to the closely resembling physical characteristics exhibited by CO2 and N2O. Herein, adsorption and separation performances of CO2 and N2O on FAU-type zeolite Y with different cations (Na+ and Ag+) were studied comprehensively. After Ag+ exchange, zeolite Y changes from a CO2-selective adsorbent to a N2O-selective adsorbent. AgY shows high N2O uptake (95.7 cm3/g) but relatively low adsorption heat (23.1 kJ/mol), making it suitable for N2O/CO2 separation. In situ Fourier transform infrared spectrometry indicates that N2O is successfully adsorbed on AgY. The breakthrough experiment reveals that AgY exhibits superior performance in the separation of N2O/CO2 at a flow rate of 20 mL/min while also exhibiting a favorable retention time and ratio of retention time with CO2 breakthrough time, which can reach up to 4.1 min and 0.24, respectively, which makes it an optimum N2O/CO2 separation material reported so far.
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CHEMICAL ENGINEERING SCIENCE
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2024
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IF 4.1
Wenlong Chen,Yuting Chen,Runwei Mo,Jiannong Wang
To reduce the amount of carbon dioxide (CO 2 ) already emitted into the atmosphere, various carbon capture, utilization, and storage (CCUS) technologies have been developed for climate and economic reasons in recent years. However, the state of art CCUS techniques suffer from deficiencies such as high cost, low yield, and harsh and discontinuous production conditions. In this work, we report a new thermal reduction method for continuously conversing CO 2 to methane (CH 4 ) by introducing sodium borohydride (NaBH 4 ) as a reductant under catalyst-free conditions. Experimental results show that CO 2 can be fully captured and converted to CH 4 and carbon monoxide (CO) and the selectivity efficiency of CO 2 to CH 4 can be achieved to be as high as 90% with the optimization of experimental conditions. Such a result originates from the high activity of NaBH 4 and high selectivity of the thermal reduction of CO 2 . To demonstrate one of the potential usages of the reduction products, we integrated the thermal reduction of CO 2 with the production of carbon nanotubes (CNTs). As long as CO 2 is supplied at the source end, the reduction products can undergo catalytic decomposition to produce a CNT fiber or film continuously at the final end. The present technique is featured with simple equipment setup, low cost, and continuous thermal reduction, thus providing a new pathway for the large-scale conversion of CO 2 into high-valued products for wide applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Zeyou Meng,Yuhao Hu,Xin Ye,Xiao Sun,Jun Hu,Zhen Wang,Jiabao Qiang,Sanping Chen,Gang Xie
To address the limitation of mono-pore mode SBA-15 on adsorption efficiency and the aggregation of amine groups within the confined pores, an innovative TEOS hydrolysis-driven dual-pore strategy to fabricate SBA-15-Dual-Mesopore (SBA-DMP) structure with covalent-grafted of 3-trimethoxysilylpropan-1-amine (APTMS) is proposed. Structural and thermodynamic characterizations reveal that this dual-mesopore design provides more CO 2 adsorption sites, and the larger mesopores exhibit a strong affinity for tetraethylenepentamine (TEPA) that significantly enhances its dispersion and incorporation efficiency. Of noted, for the first time, electron paramagnetic resonance (EPR) spectroscopy is employed to study the electronic interactions within amine-functionalized materials, indicating that APTMS-induced surface hydrogen bonds facilitate lone pair electron delocalization through electronic rearrangement, improving the local electronic density around secondary amines. Microcalorimetric studies, along with temperature-programmed desorption (TPD) and density functional theory (DFT) calculations, confirm that hydrogen bonding significantly enhances the reactivity of secondary amines, leading to a high CO 2 adsorption capacity of 5.83 mmol g −1 at 70 °C under 10 % CO 2 (60 % RH). The comprehensive evaluation of the SBA-DMP material demonstrates an excellent amine efficiency, adsorption stability, recyclability, and selectivity, highlighting its suitability for practical CO 2 capture. The dual-mesopore design with surface hydrogen bonding collectively advances CO 2 adsorption efficiency, offering a practical and effective solution for carbon capture.
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CHEMICAL ENGINEERING SCIENCE
·
2025
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IF 4.3
Lidong Wang,Chensheng Ma,Qin Dai,Kangkang Li,Kaiqi Jiang
Solvent degradation is the most critical challenge of amine-based CO 2 capture technology, which necessitates the development of chemically stable amine/amine blends to mitigate the absorbent degradation for industrial application. This study experimentally examined fourteen structurally different amines, namely the relatively stable cyclic, sterically hindered, and tertiary amines, to reveal the relationship between amine structure and chemical stability. The cyclic amines with a symmetrical ring structure greatly promote their oxidative stability, whilst the asymmetrical ring structure exhibited poor performance due to its relatively high C-N bond flexibility. The potential intramolecular interaction between the parent ring and the branched chain also reduced the stability of cyclic amines. While sterically hindered amines showed desirable oxidative stability thanks to the C-N bond protection by substitutions adjacent to amino group, their stability was very sensitive to the number of chain and the type of functional group surrounding to the amino group. Thermal stability of sterically hindered amines was also less satisfactory. It is observed that the amines with a rigid C-N bond, a longer branched chain connected to parent ring, and a preferable steric hinderance substantially promote the oxidative stability, with approximately 20 times less degradation compared to the benchmark MEA. Quantum calculation of bond dissociation energies (BDEs) of hydrogen-containing bonds were performed to reveal the atom position of radical formation that initiates the amine degradation. The potential degradation pathways were further predicted based on the positions of radical formation and the calculation of reaction Gibbs energy for possible degradation reactions. The analysis of heat stable salts products and the nitrogen distribution in the degraded solutions confirmed the bond cleavage position induced by radical formation and the reaction pathways, which clarified the potential amine oxidation mechanism. This work is anticipated to provide the generic principles to evaluate and develop the chemically stable amine solvent towards long-term operation of the amine process.
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JOURNAL OF ORGANIC CHEMISTRY
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2024
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IF 3.3
Tianyu Zhu,Yue Xu,Zhenjiang Li,Jun He,Xin Yuan,Dong Qian,Tong Chang,Longlin Lu,Bo Chi,Kai Guo
A halide-free ionic pair organocatalyst was proposed for the cycloaddition of CO2 into epoxide reactions. Cholinium pyridinolate ionic pairs with three different substitution positions were designed. Under conditions of temperature of 120 °C, pressure of 1 MPa CO2, and catalyst loading of 5 mol %, the optimal catalyst cholinium 4-pyridinolate ([Ch]+[4-OP]−) was employed. After a reaction time of 12 h, styrene oxide was successfully converted into the corresponding cyclic carbonate, and its selectivity was improved to 90%. A series of terminal epoxides were converted into cyclic carbonates within 12 h, with yields ranging from 80 to 99%. The proposed mechanism was verified by 1H NMR and 13C NMR titrations. Cholinium cations act as a hydrogen bond donor to activate epoxides, and pyridinolate anions combine with carbon dioxide to form intermediate carbonate anions that attack epoxides as nucleophiles and lead to ring opening. In summary, a halide-free ionic pair organocatalyst was designed and the catalytic mechanism in the cycloaddition of CO2 into epoxides reactions was proposed.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Ning Zhang,Yingmei Meng,Zhiying Li,Chuanlong Jin,Junjiang Bao,Xiaopeng Zhang,Gaohong He
High free-volume microporous membranes constructed by intrinsically microporous polymers (PIMs) are up-and-coming in efficient carbon capture, but their practical applications are limited by plasticization and physical aging issues. This work we proposed a CO 2 -solution-compensated cross-linking strategy to construct microporous membranes with both crosslinking network and enhanced CO 2 solubility via the Hoffmann alkylation reaction between the bromomethylated PIM matrix and Ethylenediamine (EDA) only at 80 °C. The enhanced CO 2 solubility could compensate the reduced CO 2 diffusion by the crosslinking network. Accordingly, the crosslinked microporous membranes with CO 2 -solubility compensation achieved a superior decarbonization from natrual gas (CO 2 permeability of 898.9 Barrer, CO 2 /CH 4 separation factors of 204.1) surpassing the 2019 Robeson upper and excellent anti-plasticization (plasticizing pressure up to 0.8 MPa) and anti-aging (CO 2 permeability loss < 10 % after 30 days) performance. The CO 2 -solubility-compensation crosslinking strategy will promote the development of high-performance microporous membrane for efficient decarbonization.
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Nature Communications
·
2025
·
IF 15.7
Han Songyue,He Linhai,Chen Nan,Fan Dong,Tian Peng,Liu Zhongmin
Selective hydrogenation of CO 2 into high-value C 2+ oxygenates, such as acetic acid (AA), methyl acetate (MA), and ethanol, is highly attractive yet remains a significant challenge. This study demonstrates an innovative tandem catalysis system for converting CO 2 to AA and MA, employing GaZrO x and hydrophobically modified MOR-8-C1@PC (PTFE+CNTs) catalysts. The upstream GaZrO x drives CO 2 hydrogenation to produce an effluent gas with a controlled CO/(DME + CH 3 OH) ratio of approximately 4, facilitating the subsequent carbonylation reaction over the MOR-based catalyst. For the downstream catalyst, surface silanization of MOR zeolite combined with a hydrophobic promoter effectively prevents water (generated during CO₂ hydrogenation) from entering the zeolite channels and greatly enhances the carbonylation activity and catalyst stability. Results show that at a CO 2 conversion of 27%, the selectivity towards AA and MA in the organics reaches up to 78%, with no catalyst deactivation observed over 50 hours. This strategy offers an efficient approach for converting CO 2 into C 2+ oxygenates, with promising implications for sustainable chemical production.
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THERMOCHIMICA ACTA
·
2017
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IF 2.236
Zhongyun Zhou,Ke Wang,Zeguang Yin,Pengfei Zhao,Zhen Su,Ji Sun
Highly efficient K 2 CO 3 -doped lithium orthosilicate (Li 4 SiO 4 ) sorbents were synthesized using acid treatment to overcome the typical kinetic limitations of sorbents at low CO 2 concentrations. The effects of K 2 CO 3 on the structure and absorption properties were characterized using various morphological characterization techniques, differential scanning calorimetry (DSC) and thermogravimetric analysis (dynamic and isothermal). The results showed that different amounts of K 2 CO 3 greatly affected the physical-chemical properties and absorption kinetics of the sorbents. On one hand, K 2 CO 3 formed a solid solution with Li 4 SiO 4 and generated favorable characteristics (a smaller crystal size, corrugated morphology, larger surface area and higher surface concentration of Li 2 O), significantly facilitating the chemisorption processes. On the other hand, a higher amount of doped K 2 CO 3 was located on the surface, which induced molten phases during CO 2 absorption, remarkably decreasing the diffusion processes. Therefore, 0.1 M K 2 CO 3 doped sorbent obtained noticeable absorption capacity and good regenerability in 15 vol.% CO 2 .
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