ADVANCED ENGINEERING MATERIALS
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2025
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IF 3.3
Wenxiang Wang,Hongxin Guo,Yutong Ding,Zhou Chen,Ling Yu,Songdi Wu,Tairong Kuang
Polymer foams, particularly those prepared using supercritical carbon dioxide (Sc-CO 2 ), are extensively utilized in diverse applications like thermal insulation and packaging due to their lightweight and efficient properties. However, the effectiveness of Sc-CO 2 foaming is often limited by low cell density and large cell size, mainly resulting from insufficient nucleation control and inadequate gas management. In this study, hollow metal-organic frameworks (MOFs) (HZIF-8) were introduced as effective nucleating agents in Sc-CO 2 -assisted polystyrene (PS) foaming. Owing to their unique hollow structure and high internal surface area, HZIF-8 significantly enhances gas adsorption and storage capacity, thereby improving nucleation efficiency during the foaming process. The results show that incorporating HZIF-8 into PS significantly increases the cell density (up to 1.4 × 10 9 cells cm −3 ) and decreases the average cell size (to 8.6 μm) under optimal foaming conditions (13.8 MPa, 100 °C). Compared to conventional ZIF-8 nanoparticles, the hollow structure of HZIF-8 facilitates more efficient CO 2 uptake, leading to a finer microcellular morphology, more stable foam expansion, and enhanced mechanical properties. These results demonstrate the potential of hollow MOFs in creating high-performance microcellular foams, with promising applications in energy-efficient insulation, lightweight packaging, and functional materials.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Zhicheng Liu,Manli Wang,Ming Hou,Yun Zhao,Wenbin Yang,Yangkai Han,Zhigang Shao
In traditional CO 2 electrolysis systems, oxygen evolution reaction (OER) consumes 90 % of the electricity input, whereas the product of oxygen holds minimal value. Moreover, the use of different electrocatalysts for the anode and cathode remains a challenge due to high capital costs of the electrolysis system. Substituting the OER with thermodynamically advantageous value-added anodic reactions and developing bifunctional electrocatalysts are crucial for the advancement of CO 2 electrolysis. In this study, for the first time, we present an innovative CO 2 electrolysis system that integrates CO 2 electroreduction reaction (CO 2 RR) with SO 2 electrooxidation reaction (SO 2 OR) and employ Ni-N-C as the bifunctional electrocatalysts to produce CO and H 2 SO 4 simultaneously. Notably, the novel CO 2 electrolysis system can reduce the cell voltage by 1.05 V, resulting in nearly 50 % reduction in energy consumption. This is also the first attempt to use Ni-N-C to catalyze SO 2 OR, showing markedly superior performance compared to commercial 20 % Pt/C. In-situ ATR-SEIRAS and DFT calculations demonstrate that the NiN 4 sites in Ni-N-C catalysts augment the direct conversion of *SO 2 to *HSO 4 - , identified as the rate-determining step for the SO 2 OR. This work provides guidance for the design of novel CO 2 electrolysis systems, the construction of bifunctional electrocatalysts, as well as the mechanistic investigation of the SO 2 OR.
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Catalysis Science & Technology
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2025
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IF 4.2
Longhao Xu,Wenhao Zhang,Liang Shen,Minghui Zhu,Yi-Fan Han
Despite the substantial efforts in the conversion of carbon dioxide (CO2) into high value-added products, directly transforming CO2 into CH4 at low temperatures still poses a formidable challenge. In this study, we report a bottom-up strategy to synthesize supported Ni catalysts on a doped Al2O3 support. LaAl mixed oxide was first synthesized via a co-precipitation method, followed by Ni species loaded using a deposition precipitation method. The CO2 conversion of the Ni/LaAl catalyst is found to be greatly enhanced, two times higher than that of the Ni/Al2O3 catalyst at 250 °C. The characterization results show that the introduction of La promotes the dispersion of Ni, reduces the reduction temperature of NiO and facilitates the adsorption of CO2 by increasing the basic sites. Temperature-programmed reduction with H2 demonstrated that La2O3 promotes the reducibility of NiO. Furthermore, kinetic analysis, in situ DRIFTS and CO methanation tests evidenced that La2O3 promotes the activation of CO2 and accelerates the CO hydrogenation step.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Zilei Zhang,Dagang Li,Dongxiang Zhang,Haocun Tan,Fengqi Zhang,Jinzheng Hou,Runchao Tan,Jinying Li,Xiyan Xu
Adsorption technology is a promising strategy for efficient CO 2 capture, especially when adsorbents feature three-dimensional interconnected pore structures that enable rapid gas transport. Polyaniline (PANI), a nitrogen-rich and cost-effective polymer, holds the potential for CO 2 adsorption. However, strong hydrogen bonding between PANI molecular chains often leads to significant aggregation, hindering dispersion and reducing the density of accessible adsorption sites. In this study, we present an innovative cryo-polymerization approach to fabricate CO 2 adsorbents 3D-(PANI@PAM) gel, where PANI is “self-assembled” onto the surface of a three-dimensional interconnected polyacrylamide (PAM) medium. This method enables the ordered “stereoscopic printing” of PANI on PAM pore surfaces, effectively preventing PANI aggregation. After activation treatment, the resulting nitrogen-rich aerogel exhibits uniform nitrogen distribution and a high nitrogen content. The resulting hierarchical pore structure (0.54–0.64 nm) significantly enhances CO 2 affinity. The optimized aerogel achieves an exceptional CO 2 adsorption capacity of 6.04 mmol·g −1 at 0 °C and 101 kPa, surpassing comparable materials. Furthermore, the aerogel demonstrates a CO 2 /N 2 selectivity of 23.07. These findings underscore the unique advantages and significant potential of carbon aerogels in CO 2 capture, providing a novel and effective pathway for designing high-capacity polymer-based carbon materials.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yuhang Zheng,Jiayi Wu,Liji Zhang,Yafei Guo,Zhihao Xu,Yu Huang,Pu Huang,Jubing Zhang,Chuanwen Zhao
Alkali metal salts (AMS) promoted MgO with high CO 2 uptakes represents a promising adsorbent candidate for CO 2 capture. The AMS-MgO composite adsorbents are facing the challenges of increased pressure drop or elutriation when employed in dual fixed-bed reactor or twin circulating fluidized-bed configurations. Granulation by the extrusion-spheronization technique represents an effective problem-solving strategy. However, textural properties and CO 2 uptakes of MgO-based adsorbent pellets might be adversely affected by the granulation process. In this work, AMS-MgO composite adsorbent pellets were prepared by the extrusion-spheronization method. Citric acid (CA), ammonium bicarbonate (AB), urea (UA) and microcrystalline cellulose (MC) were employed as pore-forming templates to improve the porous structures and CO 2 uptakes of the AMS-MgO pellets. CO 2 uptakes and adsorption kinetics of the adsorbent pellets were studied using a fixed-bed reactor. Effects of granulation and pore templating on the structure-performance relationships of the AMS-MgO pellets were unraveled. Granulation had resulted in the remarkable decrease in CO 2 uptake from 10.87 to 4.24 mmol CO 2 /g due to the impaired textural parameters. The employed sacrificial templates endowed the AMS-MgO pellets with enhanced CO 2 uptakes and improved carbonation kinetics. This was associated with extended surface area and expanded pore structures due to gas liberation in the pyrolysis of templates, which had facilitated the kinetics of CO 2 bulk diffusion. The desired AMS-MgO-MC pellet modified with MC template showed a high CO 2 uptake of 7.54 mmol CO 2 /g in 50%CO 2 at 340 °C, and its CO 2 uptake was stabilized around 5.0 mmol CO 2 /g within 20 cycles. Besides, the AMS-MgO-MC pellet also exhibited good mechanical properties. The results will guide the rational design of highly efficient and robust MgO-based adsorbent pellets for CO 2 capture applications.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yuqi Zhang,Yaxuan Zhen,Chunying Zhu,Taotao Fu,Youguang Ma
Chemical absorption has become the most mature and widely used CO 2 capture technology to address CO 2 emissions. Phase change absorbents based on mixed amines combine the advantages of individual amines and reduce regeneration energy consumption. A novel phase change absorbent system based on mixed amine was developed in this study and its CO 2 capture and desorption performance was investigated. The system comprises monoethanolamine (MEA), N-methyldiethanolamine (MDEA), n-butanol and water. Gas-liquid absorption experiments in the microchannel revealed that the flow patterns of the rich phase changed successively through homogeneous flow, irregular droplet flow, tubular-droplet flow and liquid slug flow as the gas-liquid ratio was increased. This transition was influenced by internal circulation, phase change and viscosity, causing the absorption rate to rise initially, then increase slowly before eventually declining. The desorption performance of the saturated rich phase in the MEA-MDEA-n-butanol-H 2 O system was significantly superior to that of the 30 wt% MEA aqueous solution. Comprehensively, the optimal mass ratio of MEA-MDEA-n-butanol-H 2 O was identified as 1.2:1.8:4:3, achieving a higher desorption rate and lower energy consumption. Desorption efficiency and cyclic capacity were 1.8 times those of the 30 wt% MEA aqueous solution, indicating promising application potential.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Shihui Wang,Futang Liu,Xiaole Dong,Dongmei Lv,Guodong Zhang,Xiaokun Li,Jinkai Pan,Qingmei Meng,Xinpeng Liu
In this study, composite carbon dioxide (CO 2 ) absorbents were developed following a transferable design strategy involving a polyamine-rich ionic liquid (IL) scaffold, microstructure control via synthesis pathway, and optional nanofluid construction to tailor transport properties. Specifically, absorbents based on [TEPA·Lys] IL and deep eutectic solvents (DESs) were prepared. The effects of mass ratio, temperature, and other factors on absorption/regeneration performance were investigated. The results showed that the composite absorbent of [TEPA·Lys] and [EG/ChCl] with a mass ratio of 4:6 exhibited the optimal performance. At 298.15 K, the absorption capacity reached 102.55 mg CO 2 /g absorbent. However, the [TEPA·Lys][EG/ChCl] absorbent exhibited suboptimal cyclic regeneration performance. In order to seek effective ways of regeneration enhancement, the methods of altering the synthesis sequence and adding nanoparticles have been explored. The synthesis of [TEPA·Lys]@ChCl+EG showed relatively stable regeneration performance under optimal conditions. The results of density functional theory (DFT) calculations showed that [TEPA·Lys][EG/ChCl] has stronger CO 2 binding energy and lower absorption energy barrier, which is beneficial to the initial absorption. The [TEPA·Lys]@ChCl+EG has a lower desorption energy barrier, which is conducive to regeneration. As for the performance of nanofluids, it was found that the addition of 0.05 wt% carbon nanotubes (CNTs) can increase the absorption capacity of [TEPA·Lys][EG/ChCl] by 5.2 %, but the degree of regeneration enhancement was lower than the effect of synthesis sequence. This study provides experimental and theoretical insights for developing effective regeneration enhancement approaches for CO 2 absorbents.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120635
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IF 7.2
Nan Xiang,Huajun Sun,Guifeng Tang,Na Zhang,Chuanhui Gao,Yuetao Liu,Chuanxing Wang,Junwei Ding,Li Ding
Photocatalytic conversion of CO 2 into solar fuels presents a promising strategy for mitigating greenhouse gas emissions. The reduction of CO 2 to methanol not only enables carbon resource recycling but also facilitates the production of sustainable fuels. In this study, a litchi-shell-like TiO 2 /WO 3 -5 hollow heterojunction catalyst was constructed, featuring surface alkalization and abundant oxygen vacancies. This unique architecture provides a high specific surface area and plentiful active sites, thereby significantly enhancing CO 2 adsorption capacity. Under neutral conditions (pH = 7), the TiO 2 /WO 3 -5 catalyst achieves a remarkable methanol production rate of 780 μmol·g⁻¹ ·h⁻¹ with a high selectivity of 88.6 %, substantially outperforming its individual counterparts, pure TiO 2 and WO 3 . Furthermore, the catalyst demonstrates excellent stability over multiple reaction cycles. A series of characterizations, including EPR, PL, TRPL, and in situ DRIFTS, collectively verify the formation of a Z-type heterojunction, which effectively promotes the spatial separation of photoinduced charge carriers and suppresses the formation of CO and CH 4 . This work underscores the crucial synergy between Z-type heterojunction engineering and surface defect manipulation in enhancing reaction selectivity and efficiency. The TiO 2 /WO 3 -5 catalyst offers a prospective platform for CO 2 -to-fuel conversion and provides valuable guidance for the design of advanced photocatalysts.
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ACS Sustainable Chemistry & Engineering
·
2025
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IF 7.3
Tianzi Bi,Yuxuan Wei,Jiabin You,Guiru Zhang,Yongjian Su,Xiaojing Cheng,Xiaohui Yan,Huiyuan Li,Shuiyun Shen,Junliang Zhang
Cobalt phthalocyanine (CoPc) is a widely utilized molecular catalyst for converting CO2 to CO in the CO2 reduction reaction (CO2RR). However, achieving high selectivity at high current densities remains significant challenges, such as mass transport and interfacial microenvironment. In this study, CoPc-based gas diffusion electrodes with thermal induction treatments are investigated to reach high performance and stability. At a current density of 300 mA/cm2, the cell voltage is 2.9 V, with a CO selectivity of 95%, representing nearly a 5-fold improvement compared to the pristine electrode. Additionally, at a current density of 150 mA/cm2, the electrode demonstrates long-term durability, maintaining stable performance for 45 h. The structural changes and underlying mechanisms of the Nafion ionomer induced by thermal treatment are investigated via microscopic characterization and molecular dynamics simulations. It is revealed that thermal induction at temperatures slightly above Nafion’s glass transition point could enhance ionomer phase separation, resulting in the formation of additional hydrophilic–hydrophobic interfaces that facilitate CO2 mass transport. Moreover, the rearrangement of Nafion chains during thermal induction produces a denser structure that restricts OH– release. This localized retention of OH– raises the pH near the catalyst, thereby improving the efficiency of the CO2RR. This work offers valuable insights into the design of CoPc-based gas diffusion electrodes with high selectivity at elevated current densities and provides guidance for post-treatment processes in the field of CO2RR.
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Separations
·
2025
·Vol. 12
·期 12
·342
·
IF 2.7
Guangjie Chen,Guangying Chen,Li Sze Lai,Zhiwei Zhang,Xiaodi Chen,Yun Hin Taufiq-Yap
Mixed amine/sulfolane (TMS) biphasic solutions have gained attention for their adjustable structure–activity relationships and lower regeneration energy. In this study, monoethanolamine (MEA) is employed as the main absorbent and polyamine as the co-absorbent, which are subsequently mixed with the phase separation promoter sulfolane (TMS) to form ternary biphasic solvent systems. Polyamine co-absorbents include 3-Dimethylaminopropylamine (DMAPA), 3-Diethylaminopropylamine (DEAPA), and Diethylenetriamine (DETA). Phase separation, absorption, and desorption performances were systematically studied. Reaction and phase separation mechanisms were elucidated through13C nuclear magnetic resonance (NMR) spectroscopy. The overall mass transfer coefficients (KG) were measured using a wetted wall column (WWC). Variations in the amine-to-sulfolane concentration ratio showed minimal impact on phase volume, while temperature and solvent composition significantly influenced phase separation behavior. All three solvents exhibited superior CO2capture performance, with CO2loadings in the rich phases ranging from 4.09 to 4.71 mol/L and over 96.82% of CO2concentrated in them, cyclic capacities reached or exceeded 3 mol/L, and regeneration energy consumption was 29.63–55.51% lower than 5 M MEA.13C NMR analysis indicated that multiple N atoms in polyamines promoted the formation of additional ionic species during CO2absorption, thereby enhancing phase separation completeness. Furthermore, KGvalues for the ternary systems exceeded that of conventional MEA, with the MEA/DEAPA/TMS system exhibiting a 1.7-fold increase. These findings demonstrated the industrial potential of MEA/polyamine/TMS biphasic solvents for efficient CO2capture.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Jiaqi Ruan,Chang Gao,Tao Deng,Changlei Qin
Li 4 SiO 4 sorbent attracts wide attention due to its high and stable CO 2 adsorption. However, the process of CO 2 capture is significantly affected by various impurities under the circumstance of industrial applications, and water vapor is one such impurity that needs to be well studied. Herein, we aim to evaluate the effect of water vapor on physicochemical characteristics of Li 4 SiO 4 -based sorbents during cyclic CO 2 adsorption and desorption and to understand the action mechanism of H 2 O molecules on CO 2 adsorption by Li 4 SiO 4 . Reaction tests show that water vapor can significantly enhance CO 2 adsorption performance of sorbents, but the promotion effect varies with the different presence of water vapor during reactions. Material characterization and DFT calculation reveal that although the presence of water vapor leads to deterioration of internal pore structure of the sorbent, H 2 O molecule will form OH – on the surface of Li 4 SiO 4 and further react with CO 2 to generate HCO 3 – , thus the adsorption energy with water vapor presenting is increased with an observation of promoted CO 2 adsorption.
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Catalysts
·
2024
·Vol. 14
·期 12
·859
·
IF 3.8
Lingji Zhang,Mengke Shi,Shuo Zhang,Feng Yue,Cairong Yang,Yang Meng,Wen Li,Cong Li,Mario Berrettoni,Silvia Zamponi,Yongpeng Ma,Hongzhong Zhang
In response to growing concerns about the greenhouse effect, the direct conversion of atmospheric CO2has become a pivotal research focus. This research utilizes hydrothermal synthesis to develop Bi2WO6/MXene(Ti3C2Tx), which efficiently reduces CO2directly at the gas–solid interface through photothermal synergy, without requiring additional sacrificial agents or alkaline absorption solutions. The results indicate that the CO formation rate is about 216.9 μmol·g−1h−1. Notably, this system demonstrates exceptional selectivity for reducing CO2to CO. The outstanding photothermal catalytic efficiency is attributed to the introduction of MXene, which serves as an efficient and economical co-catalyst. The integration of MXene improves the composite material’s specific surface area and pore structure, enhances its CO2adsorption capacity, and results in the Bi2WO6/MXene hybrid having a shorter charge transfer distance and a larger interface contact area. This ensures superior charge transfer capabilities, ultimately leading to a significant enhancement in the catalytic efficiency of the composite. This study presents a straightforward and highly selective method for capturing and converting atmospheric CO2, offering fresh insights for developing efficient photothermal catalytic materials.
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