ENERGY & FUELS
·
2024
·
IF 5.2
Qian Xue,Faping Liu,Zunzhao Li,Xiaolin Wang,Wei Wang,Mingrui Liu,Jing Yang,Shuanshi Fan,Xuemei Lang
To increase the calorific value and energy density of biogas, the removal of CO2 gas is required to purify biogas. In this work, a tubular loop reactor was designed to enhance the formation of semiclathrate hydrate and separate simulated biogas of 50.0 mol % CO2/50.0 mol % CH4. In the separation process of simulated biogas, the gas hydration ratio was increased to 52.81% with the increase of initial pressure, but the fierce competition between CH4 and CO2 molecules in the hydrate cages prevented CO2 molecules to enter the hydrate cages at high initial pressure, which reduced CO2 separation factor significantly. The CO2 separation factor and CH4 concentration in the gas phase reached optimized values of 7.43 and 72.00%, respectively, at an initial pressure of 3.0 MPa. In addition, the CO2 concentration in the hydrate phase and the CH4 recovery ratio at 5.0 K were more than those at a higher driving force due to the formation of more CO2 hydrate at a low driving force. Through the determination of the sapphire window and the online particle analyzer, the size of hydrate particles and stable flow were observed. In the period of hydrate nucleation and slow growth, the average particle size D50 was 18.9 and 50.2 μm, respectively.
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高影响因子
Membranes
·
2025
·Vol. 15
·期 1
·26
·
IF 3.6
Rujing Hou,Junwei Xie,Yawei Gu,Lei Wang,Yichang Pan
Membrane technology is a promising methodology for carbon dioxide separation due to its benefit of a small carbon footprint. However, the trade-off relationship between gas permeability and selectivity is one obstacle to limiting its application. Herein, branched polyethyleneimine (BPEI) containing a rich amino group was successfully grafted on the surface of the metal–organic framework (MOF) of AIFFIVE-1-Ni (KAUST-8) through coordination between N in BPEI and open metal sites in the MOF and with the resultant maintained BET surface area and pore volume. Both the strengthened CO 2 solubility coefficients coming from the additional CO 2 adsorption sites of amino groups in BPEI and the reinforced CO 2 diffusivity coefficients originating from the fast transport channels created by KAUST-8 led to the promising CO 2 separation performance for KAUST-8@BPEI/Pebax-1074 MMM. With 5 wt.% KAUST-8@BPEI loading, the MMM showed the CO 2 permeability of 156.5 Barrer and CO 2 /N 2 selectivity of 16.1, while the KAUST-8-incorporated MMM (5 wt.% loading) only exhibited the CO 2 permeability of 86.9 Barrer and CO 2 /N 2 selectivity of 13.0. Such enhancement is superior to most of the reported Pebax-1074-based MMMs for CO 2 separation indicating a wide application for the coordination method for MOF fillers with open metal sites.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Lingjia Ma,Jiongliang Yuan,Zhaotao Liu,Yiqing Luo,Yuning Su,Kunye Zhu,Zefeng Feng,Huihua Niu,Shuaishuai Xiao,Jianjun Wei,Xu Xiang
The electrocatalytic synthesis of high-value-added urea by activating N2 and CO2 is a green synthesis technology that has achieved carbon neutrality. However, the chemical adsorption and C–N coupling ability of N2 and CO2 on the surface of the catalyst are generally poor, greatly limiting the improvement of electrocatalytic activity and selectivity in electrocatalytic urea synthesis. Herein, novel hierarchical mesoporous CeO2/Co3O4 heterostructures are fabricated, and at an ultralow applied voltage of −0.2 V, the urea yield rate reaches 5.81 mmol g–1 h–1, with a corresponding Faraday efficiency of 30.05%. The hierarchical mesoporous material effectively reduces the mass transfer resistance of reactants and intermediates, making it easier for them to access active centers. The emerging space-charge regions at the heterointerface generate local electrophilic and nucleophilic regions, facilitating CO2 targeted adsorption in the electrophilic region and activation to produce *CO intermediates and N2 targeted adsorption in the nucleophilic region and activation to generate *N ═ N* intermediates. Then, the electrons in the σ orbitals of *N ═ N* intermediates can be easily accepted by the empty eg orbitals of Co3+ in CeO2/Co3O4, which presents a low-spin state (LS: t2g6eg0). Subsequently, *CO couples with *N ═ N* to produce the key intermediate *NCON*. Interestingly, it was discovered through in situ Raman spectroscopy that the CeO2/Co3O4 catalyst has a reversible spinel structure before and after the electrocatalytic reaction, which is due to the surface reconstruction of the catalyst during the electrocatalytic reaction process, producing amorphous active cobalt oxides, which is beneficial for improving electrocatalytic activity.
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PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Bowen Tan,Danru Xu,Mengmeng Jin,Bolun Yang,Zhun Hu,Jingjun Liu
Cerium dioxide (CeO2) with different morphologies was synthesized via a hydrothermal method and applied to the carbonylation of glycerol with CO2. Subsequent characterization through H2-TPR and catalytic activity tests demonstrated that CeO2 nanorods exhibited the highest oxygen storage/release capacity as well as enhanced catalytic performance compared to other morphologies. CeO2 nanorods were thus further modified through hydrogen reduction at varying temperatures, aiming to tune the density of the oxygen vacancies. Characterization via BET, NH3-TPD, CO2-TPD, XPS, and ESR indicated that variations in morphology and reduction temperature influenced the microstructural characteristics and the strength of the acid–base sites of the catalysts. Notably, hydrogen reduction created more oxygen vacancies in the CeO2 nanorods, with the concentration of these vacancies increasing with higher reduction temperatures. Furthermore, the catalytic activity of CeO2 in glycerol carbonylation with CO2 showed a positive correlation with the concentration of oxygen vacancies. Optimizing CeO2 catalysts can enhance its performance in activating CO2, providing new ideas for industrial CO2 resource utilization and carbon capture technology development.
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高影响因子
Catalysis Science & Technology
·
2024
·Vol. 14
·期 14
·4019-4028
·
IF 4.4
Yang Yang,Liqiang Zhang,Jiaben Wang,Hao Song,Xiao Zhang,Xiang Gao
Indium oxide is widely used in the photothermal catalytic reduction of CO2. However, the high bandgap and relative low CO2 adsorption capacity limit its application. Herein, we report a simple and cost-effective strategy to modify In2O3 with hydrogen treatment and Cu doping to form a Cu–In2O3−x catalyst with a lower bandgap and enhanced CO2 adsorption properties. The catalyst can absorb more visible light and effectively reduce the activation energy of the intermediate in the CO2 reduction route, thus demonstrating superior performance in the photothermal catalytic reduction of CO2. Moreover, the Cu–In2O3−x catalyst can maintain almost 100% product selectivity over a wide range of reaction conditions and reaches the highest yield compared to other doping noble metals (Ru, Pt, and Rh). This catalyst synthesis strategy provides practical application prospects for CO green manufacturing, as well as inspiration for the performance improvement of other catalytic materials.
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SEPARATION SCIENCE AND TECHNOLOGY
·
2024
·
IF 2.3
Chengpeng Zhang,Hongjing Liu,Hanyu Qiu,Wei Zhao,Xu Zhao,Xiaochun Jing,Hui Yao
Nano-organic hybrid materials (Al2O3-NOHMs) were synthesized with nano-alumina as the core, γ-(2,3-epoxypropyl) propyl trimethoxysiane (KH560) as the corona, and three of polyetheramine M2070, D2000, M1000 as the canopy, respectively. Al2O3-NOHMs were used as fillers to prepare MMMs with Pebax as substrate to improve the CO2 separation performance. The Al2O3-NOHMs were characterized by TEM and rheological properties. The results showed that the synthesized Al2O3-NOHMs were liquid-like and had a core-shell structure, which can effectively reduce Al2O3 agglomeration in the membrane. FT-IR analysis of MMMs showed that Al2O3-NOHMs and Pebax were physically blended, TGA indicated that Al2O3-NOHMs do not affect the thermal stability of the membrane, and XRD indicated that the addition of Al2O3-NOHMs destroyed the interchain hydrogen bond of Pebax and reduced the crystallinity of MMMs. The gas permeability of the membrane was tested under ideal gas conditions, compared with pure membrane, the CO2 permeability of Al2O3-NOHM(M2070)/Pebax MMMs and Al2O3-NOHM(D2000)/Pebax MMMs reached 137.15 Barrer (24.68%) and 147.52 Barrer (34.11%), and the selectivity of CO2/N2 reached 77.82 (58.84%) and 72.31 (47.59%) at 30°C and 0.3 MPa, respectively, surpassing 2008 Robeson upper bound.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jian He,Yifan Liang,Wenting Xiang,Changjun Liu,Pan Wu,Wei Jiang
Liquid marbles(LMs) are formed by encapsulating liquid with hydrophobic particles showed potential application in capturing CO 2 . However, conventional LMs are mostly millimeter scale and easily deformed by extrusion. This study aimed to enhance the mechanical stability by controlling the particle size to prepare “dry water” type LMs (DWLMs). The N-methyldiethanolamine (MDEA) solution was used as the core in constructing DWLMs, and SiO 2 /graphene(GPE) was used as the shell material. The incorporation of GPE can endow DWLMs with photothermal conversion properties, with a particle size distribution around 100 ∼ 250 μm occupying the largest volume fraction. These DWLMs exhibited good flow ability and mechanical stability. Moreover, the effects of MDEA concentration, and content of SiO 2 / GPE on the preparation of DWLMs were investigated. Under an illumination intensity of 1 × 10 6 Lux, the temperature of DWLMs reached above 95 °C. Subsequently, the absorption performance was examined by a fixed-bed absorption tower, and it was found that decreasing the droplet size can increase the gas–liquid mass transfer area to reduce the mass transfer resistance. The height of the fixed bed constructed by DWLMs was higher than 7 cm, and the bottom particles can still maintain stability without agglomeration and blocking the supporting mesh. The breakthrough point (t 0.5 and t 0.95 ) of large-DWLMs (L-DWLMs) were greater than that of tiny-DWLMs (T-DWLMs). The absorption kinetics have validated that chemisorption is the primary mode of CO 2 absorption. In desorption process, the results showed that the desorption of CO 2 was realized by photothermic desorption, and the desorbed DWLMs were regenerated and recycled, which could prevent the corrosion of the device as well as utilize the energy provided by the sunlight.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Yafei Sang,Xiaolong Jia,Pengpeng Wu,Xiangquan Yan,Xiaotao Kuang,Quan Feng,Jiahao Qiao,Min Chen,Jian Zhang,Xiuli Yan,Tao Chang
The porous organic polymers HIP-Br-1 and HIP-Br-2 rich in bromine anions were prepared by quaternization one-pot method. The contents of N and Br in HIP-Br-1 reached 15.93 wt% and 6.94 wt% respectively. These high content of bromine ions combined with rich mesoporous and macroporous structures gave the materials good catalytic ability. The material has moderate adsorption heat (28-36 kJ/mol). The catalytic experiment shows that HIP-Br-1 has good catalytic performance. Under the mild conditions of 0.4 MPa CO2, 60 oC, and 9 h, without any cocatalyst and solvent, 93% of propylene oxide can be converted to cyclic carbonate. The catalyst has good repeatability, and the conversion efficiency to cyclic carbonate did not significantly decrease after four catalytic experiments. Density functional theory (DFT) shows that HIP-Br-1 can effectively activate PO and CO2, thereby enhancing the catalytic activity of cycloaddition reactions. This work explores the one-step synthesis of ion-type porous organic polymers rich in nitrogen atoms.
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高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Xiaoqian Peng,Shaojun Liu,Jing Zhang,Xu Zhang,Xiaochan Liu,Zhipeng Yuan,Guoran Liu,Xibin Yi,Serguei Filatov
It is well known that adsorbent material is the key to determine the CO 2 adsorption performance. Herein, ZIF-8 derived porous carbon (ZIF-8-C) is anchored into the framework of a novel composite aerogel (ZCPx), which utilizes chitosan (CS) and polyvinyl alcohol (PVA) as raw materials. By controlling the ratio of ZIF-8-C, the developed hierarchical porous structures combine the advantages of micropores, mesopores, and macropores. Besides, the ligand material of ZIF-8-C and the amino group from CS are two sources of the high nitrogen content of ZCPx. The optimized sample ZCP4 shows a high nitrogen content of 6.78 %, which can create more active centers and supply basic sites, thereby enhancing the CO 2 adsorption capacity. Moreover, ZCP4 composite aerogel presents a CO 2 adsorption capacity of 2.26 mmol·g −1 (298 K, 1 bar (equivalent to 100 kPa)) and CO 2 /N 2 selectivity (S CO2/N2 ) can reach 20.02, and the dynamic breakthrough experiment is performed to confirm the feasibility of CO 2 /N 2 actual separation performance, proving that the composite aerogel is potential candidates for CO 2 adsorption.
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高影响因子
ACS Applied Polymer Materials
·
2024
·
IF 4.4
Qingping Xin,Tao Huang,Shuo Li,Ningning Gao,Huimin Jin,Hao Chen,Lei Zhang,Hui Ye,Hong Li,Yuzhong Zhang
The membrane separation approach has garnered considerable interest in the area of CO2 separation due to its advantages of requiring little electricity and a wide range of applications. Here, we report the preparation of pSBMA@Ti3C2Tx nanosheets functionalized with poly(amphiphilic poly(methacryloyloxyethylsulfobetaine) (pSBMA)) by precipitation distillation, weighing of pSBMA@Ti3C2Tx nanosheets with different mass ratios to be added into cross-linked poly(ethylene oxide) (XLPEO), and preparation of a continuous, thin mixed-matrix membrane (MMM). Under gas humidification, the membrane showed the best permeation performance. Due to the richness of hydrophilic organosulfate groups (−SO3–) and quaternary amine groups [−N+(CH3)3] in pSBMA, the overall water content of the MMMs is increased, which greatly improves the CO2 permeability. Enhancing the ratio of bound water augments the membrane’s capacity to segregate CO2/N2. Under coordination of water molecules, quaternary amine groups effectively promote the quick delivery of CO2 in the membrane. In the wet state, the XLPEO/pSBMA@Ti3C2Tx-0.2 membrane has a CO2/N2 selectivity of 27.5 and a CO2 permeability of 4953 barrer, an improvement of 87% and 109%, respectively, compared to those of the XLPEO pure membrane, breaking the 2008 Robeson upper limit and approaching the 2019 upper limit. We also studied the change of the gas separation performance of the membrane under different pressures.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Qiaoshan Chen,Yueling Chen,Mingfei Yu,Bin Xu,Houyi Wu,Liuyi Li,Jinhong Bi
A metal–insulator-semiconductor (MIS) ternary photo-system was intricately crafted through precise amalgamation polyvinylpyrrolidone (PVP)-capped metal Cu with typical covalent triazine framework CTF-1 via electrostatic self-assembly. The 2 % Cu-PVP-CTF exhibited an impressive CH 4 yield of 80.7 μmol·g −1 ·h −1 with selectivity of 96.8 % under visible light, representing a 2.3-fold and 112-fold improvement over Schottky-type Cu-CTF and pristine CTF-1, respectively. In-situ XPS and VASP-diff calculations unfolded that the ultrathin PVP insulating layer significantly expedited interfacial charges tunneling, corroborated by smaller lifetime τ 2 determined via femtosecond transient absorption spectroscopy. The intermediates of paramount importance in CO 2 reduction like *COOH and *HCHO were meticulously monitored by in-situ Fourier infrared spectroscopy. DFT calculations elucidated that Cu-PVP-CTF was notably more adept at facillitating the rate-determining step (*COOH → *CO) to produce CH 4 than Cu-CTF. This work tamps the groundwork for conceptional roadmap in designing novel MIS photo-system for CO 2 conversion.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yunzhe Wang,Wanyue Qian,Ganghua Zhou,Sai Zhang,Xianglin Zhu,Li Li,Xingwang Zhu,Xiaozhi Wang,Xiguang Han,Jianjian Yi
Crystal phase engineering emerges as a powerful strategy to enhance photocatalytic activity, yet controlled phase-selective synthesis and phase-dependent performance understanding remain challenging. In this study, we introduce a method for synthesizing phase-engineered In 2 O 3 via the pyrolysis of metal–organic frameworks (MOFs). We demonstrate that the functional group and pyrolysis temperatures of MOFs are critical for phase-selective synthesis. Specifically, pyrolysis of MIL-68(ln)–NH 2 at optimal temperatures yields In 2 O 3 with rhombohedral (rh-In 2 O 3 ), cubic (c-In 2 O 3 ), and rhombohedral/cubic heterophase (rh/c-In 2 O 3 ) structures. The photocatalytic CO 2 reduction tests reveal that c-In 2 O 3 outperforms rh-In 2 O 3 and rh/c-In 2 O 3 , achieving a CO production rate of 29.19 μmol g -1 h −1 with 94.47 % selectivity. Spectroscopic and theoretical analyses show that c-In 2 O 3 has superior charge transfer efficiency and lower reaction energy barriers, particularly for the rate-determining *CO intermediate, which exhibits a lower Gibbs free energy on its surface. This work provides a significant advancement in optimizing photocatalytic CO 2 reduction efficiency through precise phase engineering, underscoring the vital role of phase control in enhancing catalytic performance.
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