POWDER TECHNOLOGY
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2023
·
IF 5.2
Duanlian Tang,Xiaoying Lyu,Zhixian Huang,Renwei Xu,Jie Chen,Ting Qiu
Nitrogen-doped microporous carbon, which features a uniquely tunable porosity, exhibits promisingly high adsorption prospects in the greenhouse gas capture and water treatment. Herein, we propose a series of novel N-doped microporous carbons (CMPA n -C1000), and precisely tune their porosities via a direct pyrolysis of rigid conjugated microporous poly(aniline)s (CMPA n , n = 1, 2, 3) with pore size difference in a molecular level, as achieved by simply tuning their linkers with varying sizes, planarity, and symmetry. The CMPA3-C1000, with a satisfactory amount of nitrogen heteroatoms , high S BET of ∼800 m 2 g −1 , and large ultra-micropore volume of 0.25 cm 3 g −1 , has excellent CO 2 capture ability ( i.e. , 5.1 mmol g −1 at 273 K, 1 atm) and Hg(II) adsorption performance ( i.e. , Q e = 571 mg g −1 ; k 2 = 0.0031 g mg −1 min −1 ), respectively. CMPA3-C1000 might perform chemisorption towards Hg(II), according to calculations using density functional theory and experimental data; nitrogen atoms in porous carbon contributed to this excellent Hg(II) adsorption.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 25
·67290-67302
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IF 5.8
Chen Zewen,Zhi Yunfei,Li Wenlong,Li Shuangjiang,Liu Yi,Tang Xiaoning,Hu Tianding,Shi Lan,Shan Shaoyun
Nitrogen-rich organic polymer poly(chloride triazole) (PCTs) was synthesized by a one-step method as metal-halogen-free heterogeneous catalyst for the solvent-free CO 2 cycloaddition. PCTs had abundant nitrogen sites and hydrogen bond donors, exhibited great activity for the cycloaddition of CO 2 and epichlorohydrin, and achieved 99.6% yield of chloropropene carbonate under the conditions of 110 ℃, 6 h, and 0.5 MPa CO 2 . The activation of epoxides and CO 2 by hydrogen bond donor and nitrogen sites was further explained by density functional theory (DFT) calculations. In summary, this study showed that nitrogen-rich organic polymer is a versatile platform for CO 2 cycloaddition, and this paper provides a reference for the design of CO 2 cycloaddition catalysts. Graphical abstract
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Huangying Wang,Haiyang Yan,Kang Peng,Junying Yan,Rong Fu,Ruirui Li,Baoying Wang,Chenxiao Jiang,Yaoming Wang,Tongwen Xu
The growth of CO 2 emissions is a critical challenge to the global ecological system. Meanwhile, the rising use of evaporation units in industrial wastewater treatment plants has generated a large number of salts with low values for further valorization. In this study, a direct electrochemical substitution electrodialytic system is proposed for the conversion of CO 2 and Na 2 SO 4 into high value-added NaHCO 3 and H 2 SO 4 . The CO 2 is absorbed with polyethyleneimine and further metathesized with inorganic salts in an electrodialytic reactor. This unique system achieves soda preparation by avoiding the use of ammonia as a feedstock and demonstrates the ability to capture and convert CO 2 at a specific energy consumption of 1.2 kWh/kg NaHCO 3 and a current efficiency of 83%. This proof-of-concept study provides a highly effective technological pathway for the conversion of notorious wastes into valuable resources, creating possibilities for concurrent carbon reduction and wasted salt utilization.
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Molecular Catalysis
·
2023
·
IF 4.6
Junqiang Li,Weifeng Huang,Zhuoyue Wang,Xiao Xu,Miao Sun,Longtian Kang
The carbon-based materials with metal-N-C active sites have been widely studied on the electrocatalysis for carbon dioxide reduction reaction (CO 2 RR), however, they were investigated a few for the photocatalytic CO 2 RR. Here, cobalt phthalocyanine (CoPc) molecules with intrinsic Co-N 4 -C moiety are successfully dispersed on graphene oxide (GO) as the CO 2 RR photocatalyst. The morphology, structure, and component of CoPc/GO composites with the different ratio of GO to CoPc are systematically characterized, confirming the existence of Co-O-C axial coordination bond between CoPc and GO. The optical, photoelectric, and electrical properties of CoPc/GO composites are carefully investigated, indicating their synergistic role of CoPc and GO in photocatalysis. With the optimal CoPc/GO sample as photocatalyst, a ∼1500 μmol⋅g − 1 ⋅h − 1 evolution rate and ∼ 85% selectivity of CO and CH 4 can be achieved, which is much higher than those performances of CoPc. After the reduction of CoPc/GO to CoPc/rGO, the rate of CO 2 RR to CO and CH 4 is reduced to 916 μmol⋅g − 1 ⋅h − 1 , indicating the important role of Co-O-C axial bond in the CO 2 RR. This work provides a simple way to prepare the single-molecule catalyst for CO 2 RR.
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RARE METALS
·
2023
·Vol. 42
·期 7
·2284-2293
·
IF 8.8
Du Juan,Lin Qin-Yan,Zhang Jian-Qi,Hou Sen-Lin,Chen Ai-Bing
Herein, we successfully prepare highly dispersed and uniform small nano-size nickel nanoparticles embedded on core–shell carbon spheres by confined-deposition method. The mesoporous silica layer containing surfactant coated on the surface of the polymer sphere provides confined space and effectively controls the growth of nickel nanoparticles during pyrolysis. At the same time, the introduction of nickel species has an impact on structure of the obtained carbon spheres, and it can promote the deposition of carbon to realize the adjustment from hollow to core–shell and then to solid spheres. Owing to the uniform distribution of Ni nanoparticles with small size, mesoporous structure, N-doping groups, high specified surface areas, and core–shell structure, the obtained catalyst shows exciting ability for the production of CO by reduction of CO 2 with a maximum CO Faradaic efficiency of 98%, indicating its promising prospect in electro-reduction of CO 2 . Graphical Abstract
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JOURNAL OF POLYMER SCIENCE
·
2023
·Vol. 61
·期 17
·2025-2036
·
IF 3.4
Tao Li,Zhijian Liu,Yao Chen,Na Sun,Haozhou Shu,Lili Wu,Chaocan Zhang,Dong Xie
Two-component catalysts composed of tetra ( para -X substituted) phenylporphyrin aluminum (III) chloride, T ( p -X-P)PAlCl, (where X = H, F, Cl, Br, CH 3 , OCH 3 , tert -butyl), and cocatalyst bis(triphenylphosphine)imminium chloride (PPN + Cl − ), could initiate the polymerization of propylene oxide (PO). And they could react with rac -lactide, ( rac -LA), in the presence of propylene oxide (PO), to yield chains of enriched isotactic polylactide (PLA) with trace polyether segment. Also, these catalysts displayed different catalytic activity in the copolymerization of CO 2 and PO, resulting in poly(carbonate-co-ether) copolymer with different carbonate unit content (CU%). Further, these catalysts could initiate one-pot regio- and stereo- selective terpolymerization of rac -LA, CO 2 and rac -PO, resulting in multi-blocky poly(carbonate-co-lactide) with trace polyether segment. The structure of the products was verified by 1 H NMR, 13 C NMR, GPC, and DSC analysis, and it was found that variation of substitution groups in the periphery of porphyrin ligand would affect on the catalytic efficiency of ter-polymerization, and the relative polymerization reaction ratio of the ring-opening polymerization of LA (ROP) to the ring-opening copolymerization of PO and CO 2 (ROCOP), resulting in ter-polymer with different contents of PLA segment and PPC segment. However, H-T % in polycarbonate unit and P i % in polylactide unit did not vary much with the change of catalysts. Graphical
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Journal of CO2 Utilization
·
2023
·
IF 7.7
Qin Fang,Huanda Zheng,Shengnan Li,Tao Cai,Fuer Zheng,Laijiu Zheng
Large degree of orientation, crystallinity, and high glass transition temperature of aramid make the fibers exhibit ultra-high strength, high modulus, high temperature resistance, acid and alkali resistance, light weight and other excellent properties. However, the resulting poor dyeability and water pollution problems of aramid greatly limits its application in protective areas. An eco-friendly supercritical CO 2 assisted printing strategy for meta-aramid was developed firstly in this study. The effects of treatment temperature, time, pressure and dye concentration on the printing properties were investigated. The obtained results showed that the K/S values of the printed meta-aramid increased with the enhancing of CO 2 temperature, treatment time and CO 2 pressure. Compared to tradition printing, higher color depth can be obtained by supercritical CO 2 assisted printing with 40% sodium carboxymethyl cellulose and 20% guar gum as original paste. The K/S values of the meta-aramid with Cationic Pink X-FG in supercritical CO 2 was 12.18 while that of the samples with Cationic Yellow 5GL was 5.42. Washing and rubbing colorfastness rated above 4 were reached at 180 °C for Cationic Pink X-FG and at 160 °C for Cationic Yellow 5GL in supercritical CO 2 . In addition, up to 99% outline sharpness and acceptable stiffness, air permeability and mechanical properties was obtained, which demonstrated that the meta-aramid fabrics with supercritical assisted printing could better meet the wearability requirements.
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AICHE JOURNAL
·
2023
·Vol. 69
·期 9
·e18126
·
IF 3.7
TingTing Wang,Biao Meng,Yang Zhou,Yuan Wang,Lei Wang,Lifeng Ding,Yu Zhou,Jun Wang
High tunability of both ionic liquids (ILs) and metal organic frameworks (MOFs) enables great opportunity in the rational designation of IL/MOF composites for physical adsorption and separation. Traditionally, cations and anions of ILs as an entirety are combined with MOFs either inside or outside the microchannels. Herein, organic cations of ILs were confined into Cu-BTC and the champion adsorbent is obtained by using 1-propionic acid-3-vinylimidazole bromide as the precursor with a moderate loading amount, exhibiting higher CO 2 uptakes of 8/5 mmol g −1 than Cu-BTC (6.0/3.5 mmol g −1 ) at 273/298 K and 100 kPa, associating with significantly improved CO 2 /N 2 (CH 4 ) selectivities. The organic cations are interacted with two adjacent CuII 2 (CRO 2 ) 2 paddle wheel units of Cu-BTC, expanding the Cu O bond to strengthen the CO 2 affinity of open Cu sites and also serving as an additive CO 2 adsorptive site. The promotion of CO 2 capture ability is further reflected in the dynamic column breakthrough experiment.
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POLYMER
·
2023
·
IF 4.6
Ke Wang,Liru An,Ganghui Lu,Jialu Zhang,Zilong Wang,Meiyu Si,Guiyan Liu,Yongfei Zeng
A series of novel thermo/pH/CO 2 -triple responsive homopolymers were synthesized by reversible addition-fragmentation chain transfer (RAFT) polymerization. These homopolymers contain ethoxy groups , and the end substituents are pyrrolidine , piperidine , N -methylpiperazine, morpholine and thiomorpholine , respectively. The effects of different heterocyclic substituents on the responsiveness of temperature, pH and CO 2 were studied. For temperature-response, it was found that the lower critical solution temperature (LCST)-type cloud point (CP) temperature decreased as the number of carbon atoms increases, while the solubility of the polymers changed greatly with the introduction of oxygen, nitrogen and sulfur atoms. And the CP of the polymers can be adjusted by molecular weight , concentration and salt. Furthermore, some of these polymers present upper critical solution temperature (UCST) behavior in alcohols. For pH-response, the initial pH of the polymer solution is different, their critical pH changed accordingly, and is affected by temperature; in addition, changing the pH of solution can also affect the CP. For CO 2 -response, all of the polymers were completely soluble after pumping with CO 2 , and their LCST behavior recovered after N 2 was pumped in, but there was a gap with the initial CP. The study of these properties reveals the influence of different heterocyclic substituents on the responsiveness of polymers, which is of great significance for understanding the stimulation response properties of polymers and provides ideas for the design of new stimuli-responsive polymers.
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ENERGY
·
2023
·
IF 9
Xingxing Zhao,Yudong Ding,Lijiao Ma,Xun Zhu,Hong Wang,Min Cheng,Qiang Liao
Porous liquids (PLs) is a new material with two seemingly unrelated characteristics: porosity and liquidity. In this study, an amine functionalized strategy was proposed to enhance the CO 2 absorption of Type III Porous Liquids. 2-Methylimidazole zinc salt (ZIF-8) modified by tetraethylenepentamine (TEPA) was chosen for providing porosities and the 1-Ethyl-3-methylimidazolium Bis(trifluoro-methanesulfonyl)-imide ([EMlm][NTf 2 ]) was chosen as sterically hindered solvent, an amine-functionalized type Ⅲ porous liquids were reported. First, amine groups were successfully loaded on the ZIF-8. Then, the effect of amine loading on ZIF-8 was investigated. It was found the 30 TEPA@ZIF-8 nanoparticles were the optimum candidates based on CO 2 absorption capacity and micropore analysis. Subsequently, the CO 2 absorption capacity of absorbent was studied. 5-30TEPA@ZIF-8/[EMlm][NTf 2 ] had a CO 2 absorption capacity of 0.124 mmol g −1 , which was 4.43 times higher than 5-0TEPA@ZIF-8/[EMlm][NTf 2 ]. And the corresponding absorption rate increased by 745%. Three kinetics models were used for describing the absorption process, and the result showed the fractional-order kinetic model was the most accurate. Finally, the absorbent had a low heat absorption with a value of −1.38 kJ/mol. The CO 2 absorption capacity lost just 4.3% after five cycles. All the results indicate the prepared porous liquids had an application potential in CO 2 capture.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xiaohong Ma,Danyang Li,Huacheng Jin,Xi Zeng,Jian Qi,Zongxian Yang,Feifei You,Fangli Yuan
Herein, an urchin-like Fe 2 O 3 @In 2 S 3 hybrid composite is designed and synthesized using a facile process. The composite efficiently harvests light in both the ultraviolet and visible regions, and the unique hierarchical structure provides several advantages for photocatalytic applications: (i) a suitable band-matching structure and broadband-light absorbing capacity enable the reduction of CO 2 into hydrocarbon, (ii) the extensive network of interfacial contact between nano-sized Fe 2 O 3 and In 2 S 3 significantly increases the separation of charge carriers and enhances the utilization of photogenerated electron-hole pairs, and (iii) an abundance of surface oxygen vacancies provide numerous active sites for CO 2 molecule adsorption. The optimized Fe 2 O 3 @In 2 S 3 composite generated CO from the photocatalytic reduction of CO 2 at a rate of 42.83 μmol·g −1 ·h −1 , and no signs of deactivation were observed during continued testing for 32 h under 300 W Xe lamp irradiation.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2023
·
IF 3.9
Zijian Wang,Liying Liu,Guo Tian,Tingsheng Ren,Zhi Qi,Gang Kevin Li
Globally, fossil fuel combustion from various industrial processes has caused a significant increase in CO 2 emissions, exacerbating the greenhouse effect and climate change. Therefore, effective CO 2 capture technologies must be urgently developed. Vacuum temperature swing adsorption (VTSA) is an efficient technique for CO 2 capture. The presence of water vapor, H 2 S, etc., is an important factor that affects the performance of CO 2 adsorption, and they are usually removed prior to the adsorption separation process. However, volatile organic compounds (VOCs), a common component of industrial flue gas , can also affect the adsorption and capture of CO 2 , which is often ignored. Thus, in this study, the effect of isopropanol (IPA), one of the most common VOCs used in industry, on the CO 2 removal performance is examined using an in-house VTSA device with activated carbon (AC) as the adsorbent. The effect of IPA on the CO 2 adsorption performance of AC under varying IPA concentration, IPA content in AC, feed flow rate , and adsorption/desorption temperature is comprehensively investigated. The results verify that the impact of VOCs in the industrial exhaust gases on CO 2 capture by adsorption cannot be disregarded.
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