FUEL
·
2022
·
IF 8.035
Yongtao Zhang,Fulin Chen,Yan He,Fei Wang
CO 2 sequestration based on hydrate technology is considered to be the most promising long-term CO 2 sequestration technology. In this study, a method of using initial stirring to activate CO 2 hydrate formation process was proposed in the aim of saving energy and avoiding the problem of stirring shaft stuck, where the stirring only played a role in activating hydrate formation process. Two amino acids, l -Methionine and d -leucine, were chosen as promoters for improving the formation kinetics of CO 2 hydrates, and l -Methionine presents better than d -leucine. When the concentration of l -methionine solution is equal to or greater than 4 mmol/L, even with the initial stirring of 10 rpm within 8 min, T 90 can be shortened to close to or less than 40 min with a high gas consumption of more than 7.3 mmol gas/mL water, where the promoting effect is similar to the condition of continuous stirring of about 100 min, indicating that about 90 % of the energy consumed for mechanical stirring can be saved. Moreover, an interesting phenomenon was observed that CO 2 hydrates firstly nucleated inside the l -methionine solution, and a large number of small hydrate floccules rapidly formed and filled the entire solution under the action of magnetic stirring, which proved the instantaneous excitation effect of stirring on hydrate formation. This work contributes to rethinking the promoting roles of stirring and promoters in CO 2 hydrate formation.
研究领域:
环境科学
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能源化学
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物理化学
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气体水合物
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碳捕集与封存
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DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2017
·Vol. 134
·期 28
·45046
·
IF 1.86
Fenglei Liu,Shuixia Chen,Yanting Gao,Yufang Xie
A solid amine adsorbent was prepared by modifying a porous polystyrene resin (XAD-4) with chloroacetyl chloride through a Friedel–Crafts acylation reaction, followed by aminating with tetraethylenepentamine (TEPA). The adsorption behavior of CO 2 from a simulated flue gas on the solid amine adsorbent was evaluated. Factors that could determine the CO 2 adsorption performance of the adsorbents such as amine species, adsorption temperature, and moisture were investigated. The experimental results showed that the solid amine adsorbent modified with TEPA (XAD-4-TEPA), which had a longer chain, showed an amine efficiency superior to the other two amine species with shorter chains. The CO 2 adsorption capacity decreased obviously as the temperature increased because the reaction between CO 2 and amine groups was an exothermic reaction, and its adsorption amount reached 1.7 mmol/g at 10 °C in dry conditions. The existence of water could significantly increase the CO 2 adsorption amount of the adsorbent by promoting the chemical adsorption of CO 2 on XAD-4-TEPA. The adsorbent kept almost the same adsorption amount after 10 cycles of adsorption–desorption. All of these results indicated that amine-functionalized XAD-4 resin was a promising CO 2 adsorbent. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134 , 45046.
研究领域:
环境化学
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高分子材料科学
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气体吸附与分离
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碳捕集技术
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DOI
高影响因子
Journal of CO2 Utilization
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2019
·
IF 5.189
Wei Zhang,Fengzhen Zhang,Liping Ma,Jing Yang,Yi Wei,Deqi Kong
In this work, we propose a novel, effective, energy efficient technology to reduce CO 2 emissions and fully use the calcium in the solid waste by-product phosphogypsum (PG), by capturing CO 2 from the PG decomposition product’s hydrolysis solution. Experiments were conducted to investigate the technical feasibility and the influence of temperature and CO 2 partial pressure on CO 2 capture, as well as CO 2 loading on CO 2 sorption capacity. The results showed that > 90 % of the total calcium ions in the solution were converted into calcium carbonate (CaCO 3 ). Furthermore, a decrease in temperature and an increase in CO 2 partial pressure improved CO 2 uptake, with the latter having a greater effect on CO 2 capture capacity than the former. Moreover, kinetic analysis demonstrated that a higher temperature and CO 2 partial pressure increased the absorption rate; and showed that the CO 2 absorption rate is highly affected by the CO 2 loading levels. The thermodynamic analysis indicated that CO 2 absorption heat significantly declined as a function of increasing CO 2 loading. CaO from the calcination of carbonate was added to the hydrolysis solution and significantly enhanced its CO 2 capture ability. Thus, the hydrolyate of PG decomposition products in combination with CaO reinforcement may be a promising method for CO 2 capture.
研究领域:
环境化学
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工业生态学
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固废资源化
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碳捕集与封存
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过程强化
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DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2019
·Vol. 136
·期 27
·47723
·
IF 2.188
Yayun Zheng,Yaofang Hu,Xing Yang,Meng Yuan,Jie Zhang,Yaodong Zhang,Jujie Luo
We synthesized novel polyurethane (PU) membranes from isophorone diisocyanate (IPDI), poly(ethylene glycol) (PEG) with a molecular weight of 2000, aminopropyl-terminated poly(dimethyl siloxane) (PDMS) with a molecular weight of 2000, and 1,4-butanediol (BDO) via a two-step polymerization. The structure of each synthesized membrane was studied through Fourier transform infrared spectroscopy and gel permeation chromatography. The effect of the thermal behavior was determined by differential scanning calorimetry and thermogravimetric analysis. The gas-permeability characteristics of the PU membranes were then tested for a single gas. The results show that the permeability of CO 2 ( P CO2 ) gradually increased with PDMS content. Among these PU membranes, PU-d (PEG/PDMS = 1:1, PEG/PDMS/IPDI/BDO = 1:3:2) showed the best P CO2 (132.6 Barrer) at 25°C and 1 bar pressure. The gas-permeability coefficients of each PU membrane at different operating temperatures were investigated, and the results show that P CO2 reached 302.6 Barrer at 65°C and 1 bar. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136 , 47723.
研究领域:
高分子材料科学
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膜分离技术
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气体分离
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功能高分子
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环境化工
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DOI
高影响因子
GREEN CHEMISTRY
·
2026
·
IF 10.6
Minzhi Ma,Mengge Jia,Shichu Zhao,Zhiqiang Jiang,Kangle Lv,Tongqing Li,Helei Chai,Yan Lei,Jingjing Si,Zhi Zheng,Wenjun Fa
The global imperative for carbon-neutral fuels starkly contrasts with the persistent failure to achieve solar-driven CH4/C2H6 synthesis from CO2/H2O with both high selectivity and yield, as the thermodynamic propensity for CH4/C2H6 formation collides with kinetic bottlenecks inherent in the multi-electron/proton-transfer cascade. The prevailing paradigm has long posited that CH4/C2H6 selectivity is predominantly governed by reaction kinetics rather than thermodynamics, consequently steering catalyst design toward precise modulation of reactant interfacial dynamics at catalytic surfaces. Contrary to previous assumptions, our study demonstrates for the first time that CO2 photoreduction exhibits a characteristic domino-like chain reaction mechanism: when the catalyst amounts in the reaction system reach the threshold, the reaction cascade preferentially proceeds toward thermodynamically favorable CH4 formation through low-barrier pathways, with even C2H6 generation emerging. The universality of this mechanistic paradigm has been rigorously validated across archetypal catalysts (TiO2, MoO3, CeO2, Ni/CeO2, etc.), revealing that low amounts (5.0 mg) selectively yield H2 and CO (＞60 %, 2e- transfer), whereas higher amounts (200.0 mg) drive product distribution toward thermodynamically favorable CH4 (＞50 %, 8e- transfer). To probe this mechanism, the widely utilized Ni/CeO2 was selected as the benchmark photocatalyst, where the primary constituent of the reduction product shifts from CO/H2 (＞80 %) to CH4/C2H6 (＞80 %) upon increasing Ni/CeO2 amounts. Employing quasi in situ XPS and D2O kinetic isotope effects experiments, we unveil that Ni/CeO2 suprathreshold amounts (>150 mg) create electron-enriched microenvironments at interfacial Niδ+ sites, which drive domino photoreduction of CO2 to CH4/C2H6, while kinetically quenching competing CO/H2 evolution via proton-transfer/CO-desorption impedance. Consequently, this study elucidates that the prerequisite for designing catalysts to resolve the persistent activity-selectivity trade-off is to ensure that the photogenerated carrier concentration at the active site reaches the minimum threshold required for CH4/C2+ generation.
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Linkai Wang,Yu Han,Jian Wei,Qingjie Ge,Shijian Lu,Yanpeng Mao,Jian Sun
Hydrogenation of CO 2 into light olefins is an important route to carbon neutrality . Most of traditional researches focus on the catalyst component, structure, and promoter to enhance the selectivity of light olefins while ignoring the diffusion of products. Here, we report a NaFeZr-MOR composite catalyst for light olefin synthesis in CO 2 hydrogenation via pore confinement. The selectivity in hydrocarbons and STY (Space-time yields) of C 2–4 = is gradually increasing maximum up to 51.3% and 12.2 (mmol·g cat −1 . h −1 ), which lie in a high level among reported Fe-based catalysts. Further characterization revealed that the essence of selectivity change period is the accumulation and evolution of carbonaceous species, which causes the change of product diffusion behavior. It suppresses the escape of heavy hydrocarbons from MOR pores, leading to an increased light olefin, especially ethylene, which is called “dynamic confinement”. These findings provide a new insight for controlling low-carbon product selectivity in CO 2 hydrogenation.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Guangping Lei,Guojun Xi,Zihan Liu,Qibin Li,Huiyuan Cheng,Hantao Liu
Efficient capture and separation of CO 2 from flue gas and natural gas are highly promising to reduce carbon emissions and promote fuel calorific value. Here, a novel adsorbent (FeTPPs@Cu-BTC) for CO 2 separation was synthesized by encapsulating 5, 10, 15, 20-tetrakis (4-sulfonatophenyl) porphyrinato iron (III) chloride (FeTPPs) into the cages of Cu-BTC through an in-situ packaging strategy. Such strategy efficiently overcomes the shortcoming of pore clogging and leaching induced by incorporating guest molecules through the wet impregnation method. Meanwhile, more tunable micropores and extra affinity sites for CO 2 adsorption were created after encapsulation of FeTPPs, which preferably enhanced the CO 2 uptakes of FeTPPs@Cu-BTC under low pressures and promoted the separation performances for CO 2 /N 2 (15:85, v/v) and CO 2 /CH 4 (50:50, v/v) mixtures. The corresponding selectivity of FeTPPs@Cu-BTC calculated by ideal adsorbed solution theory (IAST) respectively increase to 57.7 and 14.0 from 36.0 and 10.8 of the pristine Cu-BTC at 273 K and 100 kPa, which also exceeds most reported adsorbents. Grand Canonical Monte Carlo (GCMC) simulations further elucidated that extra interaction with CO 2 and ‘sieve effect’ for N 2 or CH 4 after FeTPPs encapsulation immediately boost CO 2 uptakes and separation performance of FeTPPs@Cu-BTC. This study provides a new design idea for the development of new adsorbent materials.
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Wen-Xiong Shi,Ru-Zhen Ren,Yao Cheng,Fu-Gui Zeng,Xiang-Wei Guo,Zhi-Ming Zhang
Metal–organic framework (MOF) materials have broad application prospects in catalysis because of their ordered structure and molecular adjustability. However, the large volume of bulky MOF usually leads to insufficient exposure of the active sites and the obstruction of charge/mass transfer, which greatly limits their catalytic performance. Herein, we developed a simple graphene oxide (GO) template method to fabricate ultrathin Co-metal–organic layer (2.0 nm) on reduced GO (Co-MOL@r-GO). The as-synthesized hybrid material Co-MOL@r-GO-2 exhibits highly efficient photocatalytic performance for CO2 reduction, and the CO yield can reach as high as 25,442 μmol/gCo-MOL, which is over 20 times higher than that of the bulky Co-MOF. Systematic investigations demonstrate that GO can act as a template for the synthesis of the ultrathin Co-MOL with more active sites and can be used as the electron transport medium between the photosensitizer and the Co-MOL to enhance the catalytic activity for CO2 photoreduction.
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xin Li,Jiale Liu,Guocan Jiang,Xinyu Lin,Jin Wang,Zhengquan Li
Aerogels, especially MXene aerogels, are an ideal multifunctional platform for developing efficient photocatalysts for CO 2 reduction because they are featured by abundant catalytic sites, high electrical conductivity, high gas absorption ability and self-supported structure. However, the pristine MXene aerogel has almost no ability to utilize light, which requires additional photosensitizers to assist it in achieving efficient light harvesting. Herein, we immobilized colloidal CsPbBr 3 nanocrystals (NCs) onto the self-supported Ti 3 C 2 T x (where T x represents surface terminations such as fluorine, oxygen, and hydroxyl groups) MXene aerogels for photocatalytic CO 2 reduction. The resultant CsPbBr 3 /Ti 3 C 2 T x MXene aerogels exhibit a remarkable photocatalytic activity toward CO 2 reduction with total electron consumption rate of 112.6 μmol g -1 h - 1 , which is 6.6-fold higher than that of the pristine CsPbBr 3 NC powders. The improvement of the photocatalytic performance is presumably attributed to the strong light absorption, effective charge separation and CO 2 adsorption in the CsPbBr 3 /Ti 3 C 2 T x MXene aerogels. This work presents an effective perovskite-based photocatalyst in aerogel form and opens a new avenue for their solar-to-fuel conversions.
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Meng Yang,Shujuan Wang,Lizhen Xu
Water vapor in air significantly affects the CO 2 separation performance of solid amine sorbents. Although moisture benefits the CO 2 adsorption process, the co-adsorbed H 2 O in amine sorbents leads to extra regeneration energy consumption, which challenges the application of solid amine sorbents for direct air capture. Reducing H 2 O adsorption and improving the CO 2 /H 2 O selectivity of solid amine sorbents are fundamental solutions. This work clarified the more prominent hydrophilic contribution of polyethylenimine (PEI) layers than support resins for amine-impregnated sorbents. Then, we identified the phenyl group as the preferred additive to enhance the hydrophobic properties of PEI-impregnated sorbents using an orthogonal test. The introduction of hydrophobic phenyl groups reduced the average water vapor adsorption per amine group by more than 50% and increased the CO 2 /H 2 O selectivity of the amine resin sorbents by 68%–89%, resulting in lower heat requirement caused by H 2 O desorption. Despite the modification reduced CO 2 uptake, a modest CO 2 capacity of 1.47–1.6 mmol/g was detected of BZ13.5–40%R20 in a representative air condition (28 °C, relative humidity 50%). In addition, BZ13.5–40%R20 showed stable CO 2 capacity in 10 consecutive temperature swing adsorption cycles (desorption at 70 °C, N 2 stripping) in laboratory.
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yubin Wang,Zifei Yan,Jian Deng,Guangsheng Luo
Microdevices are becoming a hot technology for process intensification of CO 2 capture. However, most microdevices are limited to a small handling capacity, low volume gas to liquid ratio, and cocurrent flow mode. In this context, we proposed a miniaturized annular rotating device ( m -ARD), which has a high handling capacity, can be employed for high volume ratios of gas to liquid, and utilizes a countercurrent flow mode. Variables were investigated to determine the flow characteristic, absorption efficiency of CO 2 , and volume mass transfer coefficient. The gas hold-up and specific surface area in the m -ARD were up to 43.8 % and 1000 m 2 /m 3 , and low pressure drop was observed. Notably, the optimal volume gas to liquid phase ratio, absorption efficiency of CO 2 , and overall volumetric mass transfer coefficient were close to 200 %, 100 %, and 0.53 s −1 , respectively. Furthermore, two dimensionless equations were built to predict the volumetric mass transfer coefficient and gas hold-up. In addition, the contributions of the specific surface area and mass transfer coefficient for enhancing CO 2 absorption were discussed, respectively. This work provides a prospective device for enhancing CO 2 capture and other gas–liquid separation and reaction processes.
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产品关联
DOI
高影响因子
Small
·
2023
·Vol. 19
·期 40
·2303099
·
IF 13.3
Zi Yang,Deguang Ji,Zhi Li,Zidong He,Yang Hu,Jie Yin,Yichao Hou,Pinxian Xi,Chun-Hua Yan
Copper-based electrocatalysts effectively produce multicarbon (C 2+ ) compounds during the electrochemical CO 2 reduction (CO 2 RR). However, big challenges still remain because of the chemically unstable active sites. Here, cerium is used as a self-sacrificing agent to stabilize the Cu + of CuS, due to the facile Ce 3+ /Ce 4+ redox. CeO 2 -modified CuS nanoplates achieve high ethanol selectivity, with FE up to 54% and FE C2+ ≈ 75% in a flow cell. Moreover, in situ Raman spectroscopy and in situ Fourier-transform infrared spectroscopy indicate that the stable Cu + species promote C C coupling step under CO 2 RR. Density functional theory calculations further reveal that the stronger * CO adsorption and lower C C coupling energy, which is conducive to the selective generation of ethanol products. This work provides a facile strategy to convert CO 2 into ethanol by retaining Cu + species.
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产品关联
DOI
PubMed
高影响因子
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