CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Kaifang Wang,Danlin Chen,Jiali Tang,Zihao Hong,Zhongtai Zhu,Ziyi Yuan,Zhihong Lin,Yuqi Liu,Raphael Semiat,Xuezhong He
Membrane gas separation technologies have emerged as highly prospective avenues for the selective separation of CO 2 . In this research, a novel array of mixed-matrix membranes (MMMs) was engineered, integrating two-dimensional nanosheets of MXene, specifically Ti 3 C 2 T x , into polymers of intrinsic microporosity (PIMs) to selectively separate CO 2 from N 2 . The inclusion of Ti 3 C 2 T x nanosheets, rich in polar functional groups, significantly increases the affinity between CO 2 molecules and the fabricated MMMs. Additionally, the precise modulation of the molecular diffusion channels for CO 2 and N 2 is achievable due to the interlayer spacing between MXene layers (∼0.35 nm) within the PIM-1 matrix. This innovation is predicated on the synergistic effect of solution-diffusion and molecular sieving mechanisms that underpin the gas separation process, leading to a marked improvement in both selectivity for CO 2 over N 2 and the permeability of CO 2 . Among the series, the MMMs with a 0.5 wt% MXene display exceptional separation efficiency, achieving a CO 2 permeability of 12475.3 barrer and a CO 2 /N 2 selectivity of 32.7. Notably, all the PIM-1/MXene membranes prepared with different compositions in this study exceed the Robeson upper bound defined in 2019, indicating their substantial promise for CO 2 separation and capture in industrial applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Zongze Lv,Junqiang Han,Tao Deng,Chang Gao,Jianan Li,Changlei Qin
Integrated CO 2 capture and utilization (ICCU) is an emerging technology to reduce CO 2 emissions by greatly simplifying the processes of conventional CO 2 capture and utilization. In particular, ICCU-methanation could directly convert the low-concentration CO 2 into CH 4 using hydrogen from new energy electricity, representing an efficient Power-to-Gas route. CO 2 adsorption/catalytic materials play a crucial role for the operation of ICCU-methanation, and it is more feasible to scale up material production and avoid components interference by directly combining the sorbent and catalyst. However, it is necessary to reveal the effect of different arrangements of sorbent and catalyst on reaction characteristics of ICCU-methanation. In the work, the matching of K 2 CO 3 -doped Li 4 SiO 4 sorbent with various supported Ni-based catalyst was tested and four arrangements of sorbent and catalyst particles in a fixed-bed were investigated to understand the influences on ICCU-methanation. Results show that the presence of catalyst accelerates CO 2 supply by sorbent and achieves quicker methanation, and the promotion effect becomes more obvious with a closer contact between the sorbent and catalyst. Under optimized conditions, ICCU-methanation of uniformly mixed K-Li 4 SiO 4 and Ni/Al 2 O 3 shows an excellent performance with very stable CO 2 conversion of 95.58% and CH 4 selectivity of 93.29% during cyclic reactions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
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IF 21.1
Tinghui An,Nan Wang,Jiaqi Li,Yuhao Wang,Zongxuan Bai,Dong Xiang,Kedi Cai
Cu-based electrocatalysts possesses superior potential to produce energy-dense fuels and value-added chemicals in electrocatalytic CO 2 reduction reaction (eCO 2 RR). Nevertheless, the desperately desired target C 2 selectivity is fundamentally constrained by inevitable hydrogen evolution reaction (HER), C 1 products competition and sluggish reaction kinetics, especially for ethanol. Herein, the strategy of introducing Mg on CuO is proposed to aim at modulating adsorption energetics of oxygen-associated active species, which can effectively suppress competing pathways while boosting ethanol production. Benefitting from the modified electronic structure and lattice compressive strain induced by Mg-doping, Mg 0.34 @CuO exhibited 77.5 % of C 2 FE with remarkable stability, in which FE C2H5OH could reach 48.5 % with total current density of 245.5 mA cm −2 . Density functional theory (DFT) calculation revealed that Mg-doped Cu surface exhibits multiple catalytic function, such as suppressed HER, increased surface CO coverage and accelerated H 2 O dissociation, which can be conducive to promote ethanol production. Incorporation of Mg significantly reduces the energy barrier for asymmetric CO-CHO coupling reaction and stabilizes C-O bond in *CH 2 CHO intermediate (shared by ethylene (C 2 H 4 ) and ethanol (C 2 H 5 OH)) by enhancing d-p orbital coupling, thus prioritizing C 2 H 5 OH pathway. Furthermore, it could achieve a high discharge capacity of 14944 mAh g −1 and stable charge-discharge operation of 153 cycles in Li-CO 2 batteries that utilize Mg 0.34 @CuO as cathode material. This work demonstrates a generalizable approach to regulate eCO 2 RR activity and selectivity, and meanwhile shows great application potential in rechargeable Li-CO 2 batteries.
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LANGMUIR
·
2018
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IF 3.789
Dongfang Liu,Zhiyu Huang,Yuxin Suo,Peiyao Zhu,Jiang Tan,Hongsheng Lu
A surfactant-free microemulsion (SFME) with CO2 stimuli responsive properties was prepared. The oil and the water phases were N,N-dimethylcyclohexylamine (DMCHA) and deionized water, respectively, and N,N-dimethylethanolamine was used as an amphisolvent. The single-phase and multiphase zones were measured by the ternary-phase diagram, and the microstructure of the SFME was determined by measuring the change trend of the electrical conductivity of the system with increasing DMCHA content. While using methyl orange as a probe, the microstructure of the SFME was further confirmed by an UV–visible spectrometer. The microstructures of water-in-oil (SFME-I) and oil-in-water (SFME-II) microemulsions were obtained by changing the DMCHA content in the system. The SFME-I system has a significant phase separation after the action of CO2. However, with the continuous introduction of CO2, the upper phase of DMCHA is gradually protonated and dissolves in the aqueous phase, resulting in a gradual decrease in the volume of the upper phase, and eventually in an aqueous solution of ammonium bicarbonate. For SFME-II, CO2 does not directly cause phase separation, but eventually it becomes an aqueous solution of ammonium bicarbonate with the addition of CO2. Both the water-in-oil structure SFME-I and the oil-in-water structure SFME-II have excellent CO2 stimuli responsive performance.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jiaqi Ruan,Zongze Lv,Yong He,Xin Huang,Jingyu Ran,Changlei Qin
High-temperature CO 2 adsorption has an attractive prospect in reducing CO 2 emissions efficiently. As the core of CO 2 adsorption technology, sorbents suffer from a well-known problem of capacity degradation as a result of sintering during cyclic CO 2 adsorption and desorption at high temperatures. This work aims to understand the microstructural evolution of Li 4 SiO 4 , one of the most typical and promising sorbents, during CO 2 capture. In-situ Transmission Electron Microscopy was used to directly capture the morphological variation of Li 4 SiO 4 sorbents. Comprehensive characterization techniques were adopted to quantify microstructural parameters of Li 4 SiO 4 under different conditions . The real-time shrinkage of Li 4 SiO 4 particles was demonstrated and equations on grain growth, specific surface area reduction, and pore volume evolution were established. The work can not only reveal the reason for the reduction of CO 2 capacity, but provide a theoretical guidance for the development of sintering-resistant CO 2 sorbents.
研究领域:
材料科学
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环境科学
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Small Science
·
2025
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IF 8.3
Muhammad Kashif Aslam,Iftikhar Hussain,Sidra Hameed,Liang Wang,Muhammad Ehtasham ul Haq,Ali H. Al-Marzouqi,Maowen Xu
This study investigates the synergistic interaction of CuO and SnO 2 in a heterostructure catalyst (CuO@SnO 2 ) for the conversion of C1 carbon dioxide (CO 2 ) reduction products to C2 products and its application in high-performance aqueous Zn-CO 2 batteries. This synergistic combination enhances the Faradaic efficiency (FE) for ethanol production from 12.5% to 41.8%, shifting the selectivity from C1 to C2 products. The flow-type aqueous Zn-CO 2 battery exhibits an ultrahigh power density of 6.5 mW cm −2 , demonstrates a high discharge voltage of 0.9 V, and maintains stable operation over 140 cycles, underscoring the catalyst's exceptional reversibility and durability. During battery discharge, the system achieves a FE of 36.86% for ethanol production. These results highlight the pivotal role of the CuO@SnO 2 synergy in optimizing CO 2 conversion efficiency while generating electrical energy. The findings advance the development of dual-function energy storage systems that integrate renewable electricity generation with sustainable CO 2 utilization, paving the way for industrial-scale applications.
研究领域:
电化学
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能量存储
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二氧化碳利用
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催化
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材料科学
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Energy & Environmental Materials
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2026
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IF 13.8
Eunchae Oh,Jaewon Jang,Yoon Kyeung Lee,Junghoon Yang,Byung-Joo Kim,Jungpil Kim
The direct conversion of CO 2 into high-quality carbon nanotubes (CNTs) remains a formidable challenge, primarily due to the oxidation of metal catalyst by the oxidative nature of CO 2 . To overcome this limitation, a tandem catalytic system was implemented, in which CO 2 was converted to produce CH 4 on Ni catalysts in the primary reactor, and the CNT was synthesized from CH 4 on an Fe catalyst in the secondary reactor. Nevertheless, unreacted CO 2 was introduced into the secondary reactor, where the Fe catalysts were oxidized and thus failed to produce any solid carbon. To prevent the oxidation of Fe catalysts, a bimetallic Fe–Mo catalyst was employed instead of pure Fe. Mo was partially converted to Mo 2 C by reacting with unreacted CO 2 , which effectively suppressed the oxidation of Fe, thereby stabilizing the active Fe phase. This transformation was further corroborated by XPS analysis, where the Mo 3d spectra exhibited an increased Mo 2+ peak intensity, whereas the Fe 2p spectra showed a stronger metallic Fe signal, confirming that Mo incorporation inhibited Fe oxidation. However, excessive Mo loading resulted in the formation of multi-walled CNTs instead of single-walled CNTs, as evidenced by the reduced selectivity toward radial breathing modes in the Raman spectra and the broader diameter distribution observed in TEM measurements. These findings underscore the critical role of Mo in preserving Fe activity under oxidizing conditions and highlight the importance of optimizing its content, as an appropriate Mo level enables the selective synthesis of high-quality single-walled CNTs from CO 2 via a dual-step tandem process.
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FUEL
·
2022
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IF 8.035
Qixin Yuan,Yongsheng Zhang,Tao Wang,Jiawei Wang,Carlos E. Romero
The accelerated mineralization of fly ash is a potential way to achieve CO 2 emissions reduction. However, the slow reaction at the diffusion control stage is the bottleneck. Due to the strong diffusion of supercritical CO 2 , it has been to strengthen mineralization, but the degree of improvement in mineralization efficiency and the changes that take place in the transition from non-supercritical to supercritical CO 2 are not clear. In the mineralization process, CaO in the ash reacts with CO 2 to form CaCO 3 . In order to exclude the influence of other alkaline oxides, powdered and block CaO were used to research the mechanism, and experiments were then carried out on samples of fly ash with different CaO content. Firstly, powdered CaO was used to conduct dry and wet mineralization experiments. In dry mineralization, the mineralization efficiency of the process changes in two stages as the pressure increases, first undergoing a gentle-increase and then a rapid one. Diffusion depth experiments on block CaO show that the supercritical diffusion depth is higher than the non-supercritical diffusion depth by a factor of 1.22, indicating that supercritical CO 2 can improve the degree of mineralization in diffusion stage. The presence of water could promote mineralization. In wet mineralization, the efficiency of the process changes in three stages as the pressure increases, with first a gentle increase then a more rapid one and finally an attenuated rate of increase. The supercritical mineralization efficiency at 8 MPa was 55.27%, a factor of 2.09 larger than for non-supercritical mineralization at 3 MPa (26.39%). This is because that supercritical CO 2 has increased the diffusion and greatly improved solubility in water. The results of DFT calculations show that H 2 O can promote the adsorption of CO 2 by CaO, which is one of the reasons why water promotes mineralization. Finally, wet mineralization experiments on fly ash show that at 8 MPa, the mineralization efficiencies of HB, SD, SX and YN fly ashes are 1.94, 1.30, 2.03 and 1.62 times their values at 3 MPa. Although the difference in efficiency is affected by the CaO content, supercritical CO 2 can effectively improve the mineralization efficiency.
研究领域:
环境科学
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碳捕集与封存
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材料化学
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PETROLEUM CHEMISTRY
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2025
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IF 1.1
Jiang Ning,Mao Min,Wang Qingyin,Wang Gongying
MOF-5 is a classic metal-organic framework (MOF) crystal. However, synthesis of high-quality crystals usually requires an expensive N , N ′-diethylformamide (DEF) solvent, and a high molar ratio of a raw material (Zn 2+ : BDC 2– = 3‒5 : 1). More critically, its extreme instability against water vapor has caused researchers to do not use it. In this study, we achieved some important breakthroughs by using inexpensive N , N ′-dimethylformamide (DMF) solvent and meticulously optimizing synthesis parameters combined with a specialized micro-open solvothermal method. With a reduced molar ratio of a raw material (1.47 : 1), we successfully synthesized crystals exhibiting excellent phase structure and morphology, high surface area, out standing water vapor stability, and strong CO 2 adsorption capacity. The results show that the DEF replacement with DMF and reduction of the raw material molar ratio from 3 : 1 to 1.47 : 1 provides an increase of the BET surface area from ~935 to 2388 m 2 /g, and an improvement of the CO 2 adsorption capacity from ~0.8 to 2.5 mmol/g (298 K, 100 kPa). Breakthrough curves reveal that in simulated separation experiments for the flue gas and natural gas containing low CO 2 concentrations (10‒20%), the dynamic separation selectivity for CO 2 /N 2 reaches 22, while that for CO 2 /CH 4 remains stable at 4. Notably, the selectivity remained nearly unaffected by the pressure variation; this phenomenon is promising for enhancing the capture and purification of a low-concentration CO 2 from the flue gas and natural gas. It is important that the improved MOF-5 crystals prepared under optimal synthetic conditions maintained the stable phase structure and morphology even after 14-day exposure to humid air (relative humidity >70%), successfully overcoming the challenge posed by a water vapor.
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CHINESE JOURNAL OF CATALYSIS
·
2026
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IF 17.2
Junyan Liu,Tao Shao,Xun Peng,Shengwei Liu
Electrochemical CO 2 reduction reaction (CO 2 RR) is a potential strategy for mitigating severe greenhouse effect. Despite its potential, CO 2 RR encounters critical challenges to convert low CO 2 concentrations in practical scenarios, due to the CO 2 mass transfer limitations. Herein, we prepared a reduced 2-aminoterephthalic acid modified bismuth coordination compound (Re-BiBDC-NH 2 ) for CO 2 RR in low CO 2 concentrations. Retained amino groups after in situ reduction induce abundant unsaturated coordination sites, enhancing CO 2 adsorption and enabling localized concentration enhancement even under low CO 2 supply concentrations. As such, the optimized Re-BiBDC-NH 2 achieves a Faradaic efficiency for formate (FE formate ) of > 80% at a wide potential range of 700 mV, FE formate of >75% across 15%–100% CO 2 concentrations. Furthermore, in a flow cell at a current density of 300 mA cm⁻ 2 and across a wide pH range (pH = 1.7, 7, and 14), the Re-BiBDC-NH 2 catalyst achieved FE formate > 95%, with a single-pass carbon efficiency (SPCE) reaching 71.6% in acidic electrolyte (pH = 1.7). In situ spectroscopies and Density functional theory calculations reveal that dynamically frustrated Lewis pairs formed by amino groups and defects concentrate CO 2 , and stabilize *OCHO intermediates to reduce energy barriers, thereby not only enhancing the CO 2 RR performance but also allowing reaction to operate under low CO 2 concentrations. This work presents a promising ligand-defect synergistic catalyst for low-concentration CO 2 RR, offering insights for bridging catalyst research and practical CO 2 conversion.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Yifan Zhang,Longchun Zhong,Rashid M.Othman,George P. Lithoxoos,Ali Nabeeh Shakhs,Faiz Almansour,Xi Zeng,Wei-Ping Pan
This study evaluated zeolite-templated carbon (ZTC) and soft-templated carbon (STC) for direct air capture (DAC) of CO 2 , examining their synthesis, structural features, adsorption performance, and potential for industrial use. ZTC was produced through chemical vapor deposition using 13× zeolite, revealing a microporous structure (0.72–1.41 nm) and a specific surface area of 2815 m 2 /g. Conversely, STC prepared via a dual-template glucose system demonstrated a hierarchical pore structure (0.69 nm ultra-micropores and 3.05 nm mesopores) with a surface area of 838 m 2 /g. Under pure CO 2 conditions, both materials had similar adsorption capacities (2.16 mmol/g and 2.09 mmol/g, respectively). However, at 400 ppm CO 2 , STC outperformed ZTC (0.013 mmol/g vs. 0.0107 mmol/g) due to its radially oriented pores and hollow cavities, which created an “adsorption-enrichment” pathway, thereby improving low-concentration CO 2 uptake. Under humid conditions (RH = 75%), both materials exhibited two-stage adsorption kinetics, starting with rapid physical adsorption of CO 2 , followed by a water-driven carbonation reaction. Water blocking the hierarchical pores and cavities reduced the adsorption efficiency of STC due to its hydrophilic surface. In contrast, ZTC maintained strong physical adsorption and carbonation reactions in humid environments. Additionally, ZTC's lower cost ($29.60/kg vs. $44.36/kg for STC), scalability, and humidity tolerance make it more suitable for industrial CO 2 capture.
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INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Peng Zhu,Yi Guo,Ying Zhang,Siqi Wu,Rongyuan Wang,Zhanbo Si,Xiaojie She,Yilin Deng,Qing Yu
The electrocatalytic reduction of industrially diluted CO2 streams (5–30%) represents a pivotal avenue for carbon resource utilization. However, its practical implementation has long been hindered by mass transfer limitations and competitive hydrogen evolution reactions under low CO2 concentrations. Current research has largely focused on pure CO2 systems, overlooking the mechanistic intricacies of *CO intermediate dynamics and C–C coupling efficiency in CO2-deficient environments. To address this challenge, this study developed compositionally tunable core–shell Ag@(Cu2O)x catalysts via a seed-mediated growth approach, enabling precise modulation of the Cu2O/Ag ratio (x = 0.14–5.0) to optimize the interplay between *CO intermediates and C–C coupling under diluted conditions. Notably, experimental results demonstrate that the Ag-rich Ag@(Cu2O)0.75 catalyst achieves a Faradaic efficiency for ethylene (FEC2H4) exceeding 45% under 25% CO2. While the Cu2O-rich Ag@(Cu2O)3.0 catalyst, although optimal in pure CO2 systems, fails under the same diluted conditions due to insufficient *CO supply. This discovery underscores the pivotal role of *CO supply in dictating the overall catalytic efficiency and product distribution pathways during low-concentration CO2 electrocatalytic processes.
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