Greenhouse Gases-Science and Technology
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2022
·Vol. 12
·期 3
·362-375
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IF 2.518
Jinxiu Li,Yu Li,Chen Li,Rui Tu,Pengfei Xie,Yi He,Yao Shi
While nonaqueous organic-amine absorbents have great potential in reducing energy consumption of CO 2 capture, their absorption/desorption behaviors are still poorly understood when high-concentration polyamines are used. On the other hand, large scale CO 2 capture demands the use of high-concentration polyamines absorbents. Therefore, we investigated the absorption and microwave regeneration behavior of high-concentration triethylenetetramine (TETA) in three typical organic solvents, including polyethylene glycol 200 (PEG200), diethylene glycol (DEG), and ethylene glycol (EG). The results showed that high-concentration TETA nonaqueous absorbents demonstrate advantages in absorption rate and regeneration energy consumption. The average absorption rate of 2.0 and 5.0 mol/L TETA/EG was 2.84 and 4.70 times that of 0.6 mol/L, respectively. The energy consumption of TETA/EG and TETA/DEG decreased by 29.4 and 25.6% as the concentration increased from 0.6 to 5.0 mol/L. In addition, the high-concentration TETA/PEG200 absorbent demonstrated observable tolerance for water vapor, which usually exists in flue gas. Results also showed that microwave regeneration was superior to conventional conduction heating especially when high-concentration TETA/PEG200 absorbent were used. The energy consumption of microwave regeneration of the absorbent with a concentration of 0.6, 2.0, and 5.0 mol/L was reduced by 65.9, 81.2, and 86.0%, respectively when compared with conduction heating. © 2022 Society of Chemical Industry and John Wiley & Sons, Ltd.
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EUROPEAN POLYMER JOURNAL
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2022
·
IF 5.546
Yiming Chen,Xuening Hu,Jun Guo,Zhiyong Guo,Hongbing Zhan,Shaowu Du
Covalent triazine framework (CTF) is widely utilized in lots of porosity related applications such as gas storage, molecule separation and heterogenous catalysis. The permanent porosity and high nitrogen content in the CTF material will greatly promote the affinity between gas molecules and the skeleton. In this work, four covalent triazine framework materials (denoted as Py-CTF-400, Py-CTF-500, TPPy-CTF-400 and TPPy-CTF-500) with high BET surface areas had been successfully constructed by pyrene-based building block under ionothermal reaction conditions using anhydrous ZnCl 2 as the polycyclotrimerization catalyst. The surface area, pore volume/size of CTFs can be simply tuned by varying the synthesis temperature. Among the four CTFs, TPPy-CTF-400 display high specific surface area up to 1753 m 2 /g. The high surface area and nitrogen rich scaffold enable these CTFs to facilitate in CO 2 /N 2 , CO 2 /CH 4 separation. Impressively, the CO 2 /N 2 selectivity of Py-CTF-500 is up to 45.3 (298 K, 1 bar), which is comparable to the highest value calculated by ideal adsorption solution theory (IAST) among CTF based materials. More importantly, as the building units of these CTFs extending from 1,3,6,8-tetracyanopyrene (TPy) to 1,3,6,8-tetrakis(4-cyanophenyl) pyrene (TPPy), their CO 2 /N 2 , CO 2 /CH 4 separation efficiency decreased, which is probably ascribed to the decrescent size of the corresponding pore aperture.
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LANGMUIR
·
2022
·
IF 4.331
Yangguan Chen,Guorong Lin,Haorui Liu,Jinrui Zhang,Shuixia Chen
Solid amine adsorbents are promising materials to mitigate global warming. In this study, a commercially available melamine-formaldehyde sponge was adopted as a support to prepare a kind of solid amine adsorbent using polyethylenimine as a functional component and ethylene glycol diglycidyl ether as a cross-linker. The adsorbent, with abundant tunnels and a high amine loading amount, had a high adsorption capacity. When the amine loading was 89.6 wt%, the as-prepared adsorbent showed a high adsorption capacity of 7.29 mmol/g at 20 °C in the presence of water. The spent adsorbent could be easily regenerated by heating it at 90 °C, resulting in lower energy consumption. It has been proved by the Avrami model that physical and chemical adsorption coexist in the adsorption of CO2 on this adsorbent. Simulation with the intraparticle diffusion model has revealed that the rate-controlling step in the adsorption process was the gas film diffusion period when the adsorption temperature was below 30 °C, while it was the adsorption equilibrium period when the adsorption temperature was above 30 °C.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Baoqiang Wang,Xiaochun Chen,Guangren Yu
A new class of biphasic system composed of tetraethylene pentaamine (TEPA), organic solvents and water is developed for capturing CO 2 , among which TEPA/Diethyleneglycolmonomethylether (DGME)/Water shows the best performance. When the TEPA/DGME/Water with mass ratio 3:3:4 is at 25 °C and atmospheric pressure, CO 2 absorption capacity reaches 1.89 mol CO 2 /mol amine (2.99 mol CO 2 /kg) after 50 mins, in which CO 2 rich phase accounts for 73%. The CO 2 desorption efficiency reaches about 97% at 130 °C and the CO 2 desorption energy consumption is 53.2%, 27.4% and 3% lower than that of MEA, TEEA/DEEA/Water and 0.5D1.5A3P respectively. The CO 2 cycle capacity is approximately 60% higher than that of traditional monoethanolamine (MEA)/1-propanol/Water biphasic absorbent. Compared with previously reported biphasic system, even with similar absorbent masses, the absorption equilibrium time is significantly shortened with competitive absorption capacity. This is a class of promising absorbent for capturing CO 2 .
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Yang Li,Zhaojian Zeng,Yuanming Zhang,Yong Chen,Wenjing Wang,Xiaoming Xu,Mengyang Du,Zhaosheng Li,Zhigang Zou
Photothermal catalytic reduction of CO2 is a powerful way to promote carbon neutralization goals. However, there are few reports on the deactivation of the photothermal CO2 reduction reaction. Here, we observed an interesting deactivation phenomenon of photothermal CO2 conversion over TiO2–xHx (black TiO2). Despite the presence of a reducing atmosphere of H2, the oxygen vacancy concentration of TiO2–xHx is reduced, resulting in the deactivation of photothermal CO2 reduction. After Ni is modified onto TiO2–xHx, Ni can activate H2 to form Hs, and the oxygen vacancy concentration of Ni/TiO2–xHx may be maintained, thus solving the deactivation problem in photothermal CO2 hydrogenation.
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ACS Omega
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2022
·
IF 4.132
Longlong Chen,Xinwei Liao,Shanfa Tang,Shuyun Feng,Ruijia Tang,Shaojing Jiang,Yuanwu Dong
Tight oil reservoirs have poor physical properties, insufficient formation energy, and low natural productivity. CO2 flooding is an important technical mean that enhances the oil recovery of dense reservoirs and achieves effective CO2 sequestration, but strong heterogeneity of the tight oil reservoir usually results in gas channeling and poor enhanced oil recovery effect. The existing methods to prevent gas channeling are mainly to use the small-molecule amine system and the polymer gel system to plug fracture and high permeability channels. The small-molecular amine system has low flash points and pollutes the environment and the polymer gel has poor injectivity and great damage to the formation, which limit their large-scale application. Therefore, a new viewpoint of CO2-low interfacial tension viscoelastic fluid synergistic flooding for enhanced oil recovery in a tight oil reservoir was made. The performance of low interfacial tension viscoelastic fluid (GOBT) was studied. The injectivity and oil displacement effect of CO2-GOBT synergistic flooding were evaluated, and the mechanism of CO2-GOBT synergistic flooding was discussed. The experimental results showed that 0.4% GOBT is a low interfacial tension viscoelastic fluid, which has strong adaptability to the salinity water of tight oil reservoirs (6788–80,000 mg/L), good viscosity stability at different pHs, excellent capacity to emulsify crude oil, and the ability to improve reservoir water wettability. CO2 alternating 0.4% GOBT flooding has good injection ability in cores (Ka = 0.249 mD), and injecting 0.4% GOBT can effectively increase the injection pressure of subsequent CO2 flooding. CO2 alternating 0.4% GOBT flooding can effectively improve water flooding recovery in tight sandstone reservoirs, which is better than CO2 flooding and 0.4% GOBT flooding in both homogeneous and heterogeneous conditions. The mechanisms of CO2 alternating 0.4% GOBT flooding to enhance the oil recovery include that GOBT and CO2 foam block high permeability layers, shunt and sweep low permeability layers, and GOBT emulsify and wash oil. CO2 partially dissolving in GOBT synergistically enhances the core water wettability, which improves GOBT injectability, emulsification, and stripping ability to residual oil.
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JOURNAL OF MATERIALS RESEARCH
·
2022
·Vol. 37
·期 2
·543-553
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IF 2.909
Jia Yanfei,Wei Jianwen,Yuan Yuan,Geng Linlin,Chen Siqi,Liao Lei
A stable and effective amine-modified adsorbent for CO 2 capture was prepared with the impregnation method using the ZSM-5/SBA-16 (ZS) as support and the tetraethylenepentamine (TEPA) as modifier. The CO 2 adsorption performance was investigated by thermal gravimetric analysis (TGA) in mixed gases (15% CO 2 and 85% N 2 ) at 30–90 °C. At 60 °C, the ZS displayed the highest CO 2 adsorption capacity of 2.80 mmol g −1 at 60% TEPA loading. The adsorption kinetics analysis showed that the adsorption process of amine-modified ZS was dominated by both physical and chemical adsorptions. After five cycles of adsorption/desorption, ZS-T-60 kept better stability with the equilibrium adsorption capacity of the composite material was 2.486 mmol g −1 , which was 11.1% lower than the original adsorption capacity. The composite material ZS showed good CO 2 capture ability, indicating the promising future of these adsorbents for CO 2 adsorption from actual flue gas after desulfurization. Graphical abstract
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hailong Liao,Heping Xie,Shuo Zhai,Ling Fu,Yuan Zhang,Senran Hao,Bin Chen,Chuanxin He,Zongping Shao
Aqueous Zn-CO 2 batteries are a new technology for reducing carbon dioxide emissions and converting CO 2 into valuable products. The development of high-performance catalysts is crucial for improving the efficiency of the CO 2 reduction reaction(CO 2 RR) in these batteries. The technical challenges of CO 2 RR catalysts include high cost, complicated synthesis and low Faraday efficiency. In this study, we developed an efficient and cost-effective CO 2 RR perovskite catalyst, by partially substituting Fe to the B site of precious metal-free La 0.5 Sr 0.5 MnO 3 (LSM) perovskite. Comprehensive investigation into the Structure, morphology, coordination information and electrochemical performance of pristine La 0.5 Sr 0.5 MnO 3 (LSM) and substituted La 0.5 Sr 0.5 Fe 0.6 MnO 3 (LSF 0.6 M) catalysts were conducted, LSF 0.6 M catalyst shows enhanced electrochemical performance, Faraday efficiency, battery durability and battery power density than LSM. Specifically, the Fe-doped catalyst shows a significant improvement in CO 2 reduction reaction (CO 2 RR) performance, with an 80% increase in current density, an 82% Faraday efficiency, and a 50% increase in power density of Zn-CO 2 battery. Characterization experimental results and DFT calculation reveal that Fe substitution can increase the perovskite lattice size to favor CO 2 absorption and *COOH formation, thus the improved CO yields. These analyses provided insights into the underlying mechanisms of the catalyst's performance in CO 2 RR within the battery system. These results highlight LSF 0.6 M perovskite as a very promising CO 2 RR electrocatalyst for Zn-CO 2 battery.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Debo He,Wenji Ruan,Jibiao Li,Jiupai Ni,Chengsheng Ni
The large-scale integration of intermittent renewable energies into the power grid could reduce the CO 2 emission from the combustion of fossil fuel, but it requires energy storage techniques to balance the energy production and demand. The electrolysis of CO 2 that converting electricity into chemicals/fuels provides a sustainable way of energy storage and CO 2 reduction. Solid oxide electrolysis cell (SOEC) operating at around 800 °C was able to provide highly efficient transformation of CO 2 because the high temperature was able to decrease the energy demand and increase the activation of CO 2 than room temperature electrolysis. In this study, Mo-doped ferrite perovskite , La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 , was studied as the cathode of an SOEC for the direct electrolysis of CO 2 at 800 °C. Cell with La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 cathode showed a significantly higher current density during CO 2 electrolysis than the one with La 0.55 Sr 0.45 FeO 3 cathode. Compared with the parent La 0.55 Sr 0.45 FeO 3 cathode that will subject to a superficial decomposition into Fe 0 and SrO or SrCO 3 at an elongated cathodic bias of − 1.4 V, Mo-doping will induce the production of Ruddlesden-Popper phase ( e.g. (La,Sr) 2 (Mo,Fe)O 4 , Fe-Mo-O oxides and Fe 0 ). La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 cathode was found to an unobvious current decrease at − 1.1 V, but a cell degradation was found under a high bias of − 1.4 V. During the 97 h’ aging under a cathodic bias (−1.4 V), the reduced molybdenum cation in La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 was found to be less mobile than Fe 3+/2+ , La 3+ or Sr 2+ , and the perovskite with Fe-deficit region were also found to be important for the activation of CO 2 and dissociation of CO in the electrochemical process.
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Advanced Science
·
2021
·Vol. 9
·期 4
·2104138
·
IF 16.806
Aya Gomaa Abdelkader Mohamed,Enbo Zhou,Zipeng Zeng,Jiafang Xie,Dunfeng Gao,Yaobing Wang
Electrochemical CO 2 reduction (ECR) is one of the promising CO 2 recycling technologies sustaining the natural carbon cycle and offering more sustainable higher-energy chemicals. Zn- and Pb-based catalysts have improved formate selectivity, but they suffer from relatively low current activities considering the competitive CO selectivity on Zn. Here, lead-doped zinc (Zn(Pb)) electrocatalyst is optimized to efficiently reduce CO 2 to formate, while CO evolution selectivity is largely controlled. Selective formate is detected with Faradaic efficiency (FE HCOOH ) of ≈95% at an outstanding partial current density of 47 mA cm –2 in a conventional H-Cell. Zn(Pb) is further investigated in an electrolyte-fed device achieving a superior conversion rate of ≈100 mA cm –2 representing a step closer to practical electrocatalysis. The in situ analysis demonstrates that the Pb incorporation plays a crucial role in CO suppression stem from the generation of the Pb–O–C–O–Zn structure rather than the CO-boosted Pb–O–C–Zn. Density functional theory (DFT) calculations reveal that the alloying effect tunes the adsorption energetics and consequently modifies the electronic structure of the system for an optimized asymmetric oxo-bridged intermediate. The alloying effect between Zn and Pb controls CO selectivity and achieves a superior activity for a selective CO 2 -to-formate reduction.
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ChemSusChem
·
2021
·Vol. 15
·期 1
·e202102010
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IF 8.928
Han Zhang,Yu Yang,Yongxiang Liang,Jun Li,An Zhang,Han Zheng,Zhigang Geng,Fengwang Li,Jie Zeng
Graphical Lend me your EORs : Electrochemical oxidation-reduction (EOR) processing of a Cu-based metal-organic framework results in the formation of sub-nanometer Cu clusters that retains the organic linkers for highly selective and durable electrosynthesis of methane from the electrochemical CO 2 reduction reaction. Electrochemical CO 2 methanation powered by renewable electricity provides a promising approach to utilizing CO 2 in the form of a high-energy-density, clean fuel. Cu nanoclusters have been predicted by theoretical calculations to improve methane selectivity. Direct electrochemical reduction of Cu-based metal-organic frameworks (MOFs) results in large-size Cu nanoparticles which favor multi-carbon products. This study concerns an electrochemical oxidation-reduction method to prepare Cu clusters from MOFs. The derived Cu clusters exhibit a faradaic efficiency of 51.2 % for CH 4 with a partial current density of >150 mA cm −2 . High-resolution microscopy, in situ X-ray absorption spectroscopy, in situ Raman spectroscopy, and a range of ex situ spectroscopies indicate that the distinctive CH 4 selectivity is due to the sub-nanometer size of the derived materials, as well as stabilization of the clusters by residual ligands of the pristine MOF. This work offers a new insight into steering product selectivity of Cu by an electrochemical processing method.
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CATALYSIS LETTERS
·
2023
·
IF 2.8
Ji Yaxiong,Lin Shuang,Xu Guihong,Chen Tianen,Gong Jianchao,Meng Fanbin,Wang Yuanhao
Abstract Catalytic conversion of CO 2 to methanol with H 2 from renewable energy has attracted increasing interest as a promising strategy for reducing excessive CO 2 emissions. However, the performance of reported various catalysts still suffers from low methanol yield with a passable CO 2 conversion. In this work, Cu–ZnO–La 2 O 3 interfaces are constructed with various La 2 O 3 mole ratio. Compared to Cu/ZnO, the optimized catalyst (i.e., Cu 0.6 Zn 0.2 La 0.4 ) exhibits a much higher mass-specific methanol formation rate (159.3 g MeOH /kg cat /h) at 240 °C and 3 MPa. A series of ex-situ and in-situ characterizations, such as X-ray diffractometer (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), N 2 O titration measurements, and in-situ diffuse reflectance Fourier transform infrared spectroscopy ( in-situ DRIFTS) study, are used to investigate its structure and mechanism study. The dispersion of Cu over Cu/ZnO/La 2 O 3 catalyst is significantly enhanced, forming more Cu–ZnO–La 2 O 3 interfaces. LaO x species favor CO 2 activation and generate more carbon intermediates species for CO 2 hydrogenation. Furthermore, more Cu + is bonded, which stabilizes the key intermediate, inhibits its desorption, and facilitates its further hydrogenation to methanol. This work is expected to offer an effective strategy to develop new catalysts with high performance for CO 2 hydrogenation to methanol. Graphical Abstract
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