JOURNAL OF APPLIED POLYMER SCIENCE
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2019
·Vol. 136
·期 27
·47723
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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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GREEN CHEMISTRY
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2026
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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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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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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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CHEMICAL ENGINEERING JOURNAL
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2023
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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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INORGANIC CHEMISTRY
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2023
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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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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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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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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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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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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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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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Small
·
2023
·Vol. 19
·期 40
·2303099
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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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Materials Chemistry Frontiers
·
2023
·Vol. 7
·期 16
·3382-3389
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IF 7
Gaoming Sun,Chong Zou,Wen Sun,Ying Fang,Shuijian He,Yana Liu,Jiguang Zhang,Yunfeng Zhu,Jun Wang
The electrochemical reduction of CO2 to value-added products represents a promising strategy to store renewable energy and realize global carbon neutrality. Bi-based materials have attracted extensive attention for formate production from CO2 reduction. Herein, we employ BiPbO2Br nanosheets as the bimetallic oxyhalide precursor to prepare a reconstructed Bi–Pb composite catalyst by electroreduction. The resultant catalyst exhibits impressive performance for formate production, including a high partial current density (40 mA cm−2 at −1.0 V), a high faradaic efficiency (96.6% at −0.9 V), a high energy conversion efficiency (>50% from −0.8 to −1.1 V), and good stability. As compared with the monometallic Bi and Pb counterparts, the Bi–Pb composite catalyst demonstrates superior intrinsic performance, which is attributed to the multiphase composites and abundant heterogeneous interfaces derived from electroreduction induced structural reconstruction of BiPbO2Br. This work offers an attractive strategy to further improve the performance of Bi catalysts for CO2 reduction to formate.
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ADVANCED MATERIALS
·
2023
·Vol. 35
·期 33
·2302325
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IF 29.4
Chang Guo,Fuli Zhang,Xiao Han,Lipeng Zhang,Qian Hou,Lele Gong,Jincheng Wang,Zhenhai Xia,Jianhua Hao,Keyu Xie
To date, the effect of noble metal (NM) electronic structures on CO 2 reaction activity remains unknown, and explicit screening criteria are still lacking for designing highly efficient catalysts in CO 2 -breathing batteries. Herein, by preferentially considering the decomposition of key intermediate Li 2 CO 3 , an intrinsic descriptor constituted of the d x 2 − y 2 ${{\rm{d}}}_{{x}^2 - {y}^2}$ orbital states and the electronegativity for predicting high-performance cathode material are discovered. As a demonstration, a series of graphene-supported noble metals (NM@G) as cathodes are fabricated via a fast laser scribing technique. Consistent with the preliminary prediction, Pd@G exhibits an ultralow overpotential (0.41 V), along with superior cycling performance up to 1400 h. Moreover, the overall thermodynamic reaction pathways on NM@G confirm the reliability of the established intrinsic descriptor. This basic finding of the relationship between the electronic properties of noble metal cathodes and the performance of Li-CO 2 batteries provides a novel avenue for designing remarkably efficient cathode materials for metal-CO 2 batteries.
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Journal of Physical Chemistry C
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2023
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IF 3.7
Minglu Li,Siyu Kuang,Hai Liu,Qun Fan,Sheng Zhang,Xinbin Ma
Significant efforts have been devoted to the investigation of catalysts for converting CO2 into C2+ products. Cu catalysts are attractive for their initial selectivities but limited by the low stability over time. Herein we investigated the stability of Cu catalysts in an operating CO2RR environment. Hydroxides in electrolytes were found to play a key role in morphology evolution of Cu catalysts and thus result in decreasing Faradaic efficiencies of C2+ products. To this end, we deposited a porous carbon overlay on Cu catalysts through a thermal annealing method. Physical characterizations and electrochemical measurements showed that the morphology of Cu catalysts and Faradaic efficiencies of products were well maintained during the reaction. As evidenced by Fourier transform infrared spectroscopy with phenolphthalein as a probe, the added carbon overlay could effectively resist the influence of hydroxide corrosion on Cu catalysts. This study provides an efficient strategy to improve the stability of copper catalysts toward electrochemical CO2 reduction.
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