ACS Catalysis
·
2023
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IF 12.9
Meilin Yin,LiPeng Wang,Shaokun Tang
Covalent organic frameworks (COFs) are a class of promising porous crystalline materials for both capturing and converting CO2 into high-value-added products. However, long synthesis time and the need for cocatalyst restrict its potential for CO2 conversion. Herein, bipyridine-based TAPT-BP-COF with high crystallinity as a skeleton is rapidly synthesized within only 1 h by the aid of supercritical CO2 (scCO2) activation. Then, the production of dicationic TAPT-BP2+-COF is accomplished by a quaternization reaction. The CO2 capture capacity of TAPT-BP2+-COF improved by 55.6% due to its CO2-philic groups (imine and triazine groups), polar groups (−OH), charged skeleton, and suitable pore size, thus ensuring sufficient CO2 around the catalytic active sites. Additionally, the outstanding structure-enhanced CO2 conversion performance is observed due to the presence of the synergistic effect between –OH and Br– in the TAPT-BP2+-COF skeleton. The rate-determining step of cycloaddition is significantly accelerated without any solvents and cocatalysts compared to individual TAPT-BP-COF and [OH-BP]2+[Br]2– (BP2+ moiety). Specifically, TAPT-BP2+-COF efficiently generates cyclic carbonate by heterogeneously catalyzing CO2-epoxide cycloaddition with the yield of 99.3% and has excellent stability that can be reused ten times without significant activity reduction. This work provides a novel perspective for the targeted design and rapid synthesis of charged dicationic COF-based catalysts for high efficiency and durability in CO2 capture and conversion.
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高影响因子
Chem
·
2023
·
IF 23.5
Rongming Cai,Mingzi Sun,Fei Yang,Min Ju,Yanpeng Chen,M. Danny Gu,Bolong Huang,Shihe Yang
Summary By leveraging a Cu(OH)F precursor, we construct a disk-like Cu(I)/Cu(0) interface model (P-Cu x /Cu 2 OF) composed of F-stabilized Cu(I) shell and Cu(0) core by one-step pulsed potential conversion. The interfacial region is shown to facilitate ethanol formation, guaranteeing a high FE(C 2+ ) of up to 80.2%. Tuning the Cu(I)/Cu(0) ratio enhances the ethanol yield by 18.5-fold over pure P-Cu, with the corresponding partial current density (j ethanol ) reaching up to 128 mA/cm 2 . This is enabled by a 3.6-fold boost in selectivity for the ethanol product (35.4%) and an overall 7.8-fold boost in activity ( j C 2 + up to 288 mA/cm 2 ). The interactions between P-Cu and Cu 2 OF upshift the d-band center of Cu sites on the interface region, which is critical to asymmetrical C-C coupling to form OCCOH∗, concurrent with a lowered energy barrier for ethanol formation. On the other hand, the ethylene-forming symmetrical C-C coupling occurs primarily on P-Cu away from the Cu(I)/Cu(0) interface.
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Chem Catalysis
·
2023
·
IF 9.4
Guiru Zhang,Ke Ye,Baoxin Ni,Kun Jiang
Using renewable electricity to electrochemically convert CO 2 into value-added chemicals and fuels is a promising way to curb anthropogenic carbon emissions. In past years, exciting achievements have been witnessed on the robust and selective electrochemical CO 2 reduction reaction, via either the delicate design of electrocatalytic materials or the local reaction environment engineering toward a practical system integration. In this perspective, we overview recent advances of extrinsic reaction environment effects in promoting CO 2 -to-C 2+ conversion from three spatial aspects: (1) the chemical and physical surface modification, (2) the electrolyte composition and adjoint concentration gradient for both cations and anions, and (3) the mass transport regulation. Prevailing hypotheses, together with experimental and/or theoretical progress, have been critically assessed along with a deepened mechanism understanding of those extrinsic tuning knobs. Finally, challenges and future opportunities for more efficient C 2+ production are provided in terms of fundamental interface engineering and technical electrolyzer implementation.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Jiaqi Ruan,Yichao Tong,Jingyu Ran,Changlei Qin
A large amount of spent lithium batteries, especially lithium iron phosphate (LiFePO4), is discarded due to their limited lifespan and poses a great threat to the environment. At the same time, the potential application of Li4SiO4, an efficient high-temperature CO2 sorbent, is largely limited by the high cost of lithium resources. Thus, the preparation of Li4SiO4 from spent LiFePO4 batteries has great potential for achieving waste recycling and reducing CO2 capture costs. However, the process of recycling spent LiFePO4 batteries to synthesize Li4SiO4 sorbents still needs to be well investigated. This work proposes to simplify the preparation scheme by combing precipitation, Na doping, and synthesis processes and further optimizing the key variables of pH, Na2CO3 ratio, and heating rate. An optimal condition is determined to be pH = 9, Na2CO3 ratio = 11 wt %, and heating rate = 5 °C/min, and the sorbent prepared shows a superior stable CO2 capacity of 0.24 g/g in 80 adsorption/desorption cycles. The work develops an effective Li4SiO4 preparation scheme from spent LiFePO4 batteries with largely enhanced CO2 adsorption performance and reduced cost and could achieve a win–win situation in waste recycling and CO2 mitigation.
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JOURNAL OF MOLECULAR STRUCTURE
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2023
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IF 3.8
Kaixuan Shen,Han Zhao,Yihao Zhao,Xiaoxiang Wang,Ping Cheng,Congfei Yao,Jie Zhang,Yongpeng Yang,Weijia Huang
With regard to the physical absorbents for CO 2 removal, the alteration of carbon-chain structure may benefit the CO 2 absorption performance. However, the relationship between the carbon-chain structure of ketones absorbents and their CO 2 absorption capacity has rarely been studied, and the related mechanism is unclear. In this study, theoretical calculations and thermodynamic experiments were carried out to explore the effects of the carbon-chain length and isomerism of ketones on their CO 2 absorption performance. The density functional theory (DFT) simulations show that the F-∥ configuration is more stable than the others for the CO 2 +ketone complex in most cases. The followings are obtained according to the experimental results, which are pretty consistent with DFT calculations. The dissolution of CO 2 in the ketone is a typical physical process. As the number of carbon atom increases, the CO 2 absorption capacity of straight-chain ketones increases. Straight-chain ketones exhibit higher CO 2 absorption capacity than branched-chain ones. The effect of increasing carbon-chain length and isomerism on CO 2 absorption capacity are both stronger for the ketones with fewer carbon atoms; the influence mechanism can be attributed to different degrees of weak hydrogen-bond interaction between CO 2 and ketone molecules, suggested by the DFT simulation results. The above conclusions are beneficial for the development of potential CO 2 capture absorbents. In addition, the industrial application feasibility of surveyed ketone absorbents is also discussed.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Yuqi Zhang,Di Zhang,Pengwei Lei,Ziyan Yang,Zhikun Zhang
Metal-organic frameworks (MOFs) are a promising material for CO 2 adsorption because of their great specific surface area, well-ordered porous structures ordered porous structure and various means available for functionalization. In this work, the calcium squarate (UTSA-280) was synthesized from carbide slag without pretreatment at room temperature by a rapid mechanochemical method, and then was further functionalized with tetraethylenepentamine (TEPA) to prepare CO 2 adsorbents. The effects of water content, ball milling frequency, adsorption temperature, and TEPA loading on CO 2 adsorption performance of various adsorbents were investigated. The results showed that the CO 2 adsorption of the synthesized MOFs increased firstly and then decreased with increasing water content and ball milling frequency. The synthesized MOFs with water content of 300 mmol and ball milling frequency of 15 HZ exhibited the best crystallinity. The addition of TEPA provided additional adsorption sites and led to the increase of CO 2 adsorption capacity. The UTSA-280–300-15-40TEPA demonstrated the highest CO 2 adsorption capacity (2.89 mmol/g) at 25 °C. The CO 2 adsorption kinetics analysis showed that the Avrami model fitted well with the experimental results. Furthermore, the UTSA-280–300-15-40TEPA exhibited excellent chemical stability during the adsorption–desorption cycles, with only a 14.53 % decrease in adsorption capacity after 10 cycles. This work demonstrated the possibility of preparing UTSA-280 using carbide slag for effective CO 2 adsorption.
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CHEMISTRY OF MATERIALS
·
2023
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IF 8.6
Xuyang Li,Chengli Jiao,Xiaoqian Zhang,Xinxin Li,Xiangju Song,Yanyu Zhao,Heqing Jiang
Polyamide (PA) membranes show great application potential in the CO2 separation study. However, the PA membranes prepared by the traditional interfacial polymerization (IP) have a dense microstructure and a singularity of functional groups, making it difficult to exhibit both high CO2 permeance and selectivity. Herein, we report a new dual-modulation strategy by preparation method optimization and filler modification to improve the CO2 separation performance of the PA membranes. The PA membranes prepared by vapor–liquid IP have a loose microstructure, which greatly improves the gas permeance. The introduction of mono-(6-ethanediamine-6-deoxy)-beta-cyclodextrin (CD) can better loosen the PA microstructure, and the CO2-philic groups in the CD boost the CO2 selectivity by the facilitated transport effect. Ionic liquid 1-ethyl-3-methylimidazolium tetrafluoroborate is further sealed into PA membranes to remedy the possible microvoids or defects and CD cavities of the membrane microstructure. The prepared membranes display excellent CO2 separation performance with CO2/H2, CO2/CH4, and CO2/N2 selectivity of 8.2, 45.5, and 116.9, as well as a CO2 permeance of about 320 GPU. The proposed strategy provides a facile and effective route to dual-modulated PA membranes for the study of CO2 separation and can be expanded to other macrocyclic molecules and ionic liquid systems.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Yamei Huang,Peiyao Du,Wen-Xiong Shi,Ye Wang,Shuang Yao,Zhi-Ming Zhang,Tong-Bu Lu,Xiaoquan Lu
Solar-driven CO 2 reduction with H 2 O oxidation into liquid fuels is highly desirable for sustainable carbon cycle to achieve carbon neutral, but represents a great challenge for artificial photosynthesis. Herein, bimetallic PdIn nanoclusters are confined in a photosensitizing covalent organic framework (N 3 -COF) to facilely construct Pd x In y @N 3 -COF composites (x:y = 1:0, 0:1, 1:2, 1:1, 2:1). The resulting PdIn@N 3 -COF exhibits excellent activity for CO 2 photoreduction with H 2 O oxidation as the H + and e − source, showing a record-high total yield of 798 μmol g -1 for producing CH 3 OH (74 %) and CH 3 CH 2 OH (26 %) among the framework materials. The synergy in both the bimetallic nanocluster and cluster@N 3 -COF contributes greatly to C C coupling and interfacial charge transfer, thus achieving excellent activity for conversion of CO 2 to C 1 /C 2 alcohols on the non-copper catalysts. This work highlights the amazing potential for constructing bimetallic nanocluster@photosensitizing supports to produce alcohols in artificial photosynthesis with H 2 O oxidation.
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Membranes
·
2021
·Vol. 11
·期 2
·118
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IF 4.106
Chunwei Zhang,Menglong Sheng,Yaoqiang Hu,Ye Yuan,Yulong Kang,Xiao Sun,Tao Wang,Qinghua Li,Xisen Zhao,Zhi Wang
CO2enhanced oil recovery (CO2-EOR) technology is a competitive strategy to improve oil field economic returns and reduce greenhouse gas emissions. However, the arbitrary emissions or combustion of the associated gas, which mainly consists of CO2and CH4, will cause the aggravation of the greenhouse effect and a huge waste of resources. In this paper, the high-performance facilitated transport multilayer composite membrane for CO2/CH4separation was prepared by individually adjusting the membrane structure of each layer. The effect of test conditions on the CO2/CH4separation performance was systematically investigated. The membrane exhibits high CO2permeance of 3.451 × 10−7mol·m−2·s−1·Pa−1and CO2/CH4selectivity of 62 at 298 K and 0.15 MPa feed gas pressure. The cost analysis was investigated by simulating the two-stage system. When the recovery rate and purity of CH4are 98%, the minimum specific cost of separating CO2/CH4(45/55 vol%) can be reduced to 0.046$·Nm−3CH4. The excellent short-to-mid-term stability indicates the great potential of large industrial application in the CH4recovery and CO2reinjection from oilfield associated gas.Keywords:oilfield associated gas;CO2capture;multilayer composite membrane;facilitated transport;CO2/CH4separation
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高影响因子
Journal of Energy Chemistry
·
2021
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IF 9.676
Rui Yang,Zipeng Zeng,Zhen Peng,Jiafang Xie,Yiyin Huang,Yaobing Wang
Currently most of research efforts for selective electrocatalysis CO 2 reduction to C2+ products have relied on crystalline Cu-based catalysts; amorphous Cu with abundant low-coordinated atoms holds greater promise for this conversion yet remains relatively underexplored. Here we report an amorphous urchin-like Cu@nanosilica hybrid synthesized by electrostatic coupling Si polyanions with Cu salt in hydrothermal processes. The Cu@nanosilica electrocatalyst displays excellent CO 2 electroreduction activity and selectivity with a Faradic efficiency of 70.5% for C2+ product production, and higher stability compared to the crystalline Cu counterpart. The solar-driven CO 2 electrolysis yields an energy efficiency of 20% for C2+ product production. Mechanism study reveals that the urchin-like Cu@nanosilica catalyst with amorphous Cu/Cu + dispersion enhances CO 2 adsorption and activation to facilitate generation of CO 2 − * and possible CO* intermediates, and suppresses hydrogen evolution concurrently. The combined effects of both aspects promote efficient C2+ product production from CO 2 electroreduction.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
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IF 7.312
Zhenggang Wang,Jianwei Yuan,Renhao Li,Haipeng Zhu,Jingui Duan,Yanan Guo,Gongping Liu,Wanqin Jin
Compared with traditional separation methods, membrane-based technology shows advantages in energy efficiency for natural gas purification. To overcome the performance trade-off of conventional polymeric membranes, in this study, ZIF-301 MOF was employed as novel filler to fabricate 6FDA-DAM polyimide mixed-matrix membranes (MMMs) for CO 2 /CH 4 separation. A solvent exchange approach was proposed to remove the high-boiling-point solvent used for fabricating the MMMs. The microstructures and physico-chemical properties of the ZIF-301 fillers and ZIF-301/6FDA-DAM MMMs were characterized by SEM, EDX, XRD, IR, TGA, DSC and high-pressure sorption isotherms. The CO 2 /CH 4 transport properties through the MMMs were evaluated by permeation measurement at various feed pressures and analyzed by solution-diffusion model. The results showed that the incorporation of ZIF-301 into 6FDA-DAM enhanced both the CO 2 permeability and CO 2 /CH 4 selectivity, attributing to the preferential CO 2 sorption and aperture molecular sieving effect of the ZIF-301 filler. The MMM with optimal ZIF-301 loading of 20 wt% exhibited CO 2 permeability of 891 barrer and CO 2 /CH 4 of 29.3 that surpassed the 2008 Robeson upper-bound, suggesting that ZIF-301 based membrane could be a potential candidate for natural gas purification.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Shasha Wang,Junfeng Miao,Mengshuai Liu,Lihui Zhang,Zhenfa Liu
Novel microporous carbon xerogels (CX-HMTAs) with different morphologies and well-developed porosity were successfully fabricated. The hierarchical pore, surface structure, and nitrogen content could be easily controlled by adjusting the amount of hexamethylenetetramine (HMTA). The samples as-obtained exhibited high micropore volume and large specific surface area, which were applied as supercapacitor electrodes and CO 2 capture materials. The CX-HMTA4 with a moderate concentration of HMTA (0.72 %) afforded the highest CO 2 adsorption capability with 4.21 mmol g −1 at 273 K and 1 bar, and excellent ideal adsorption solution theory (IAST) selectivity with 70 for CO 2 /N 2 capture at 298 K. Moreover, the CX-HMTA4 were simultaneously conducted as a supercapacitor electrode, and gave a maximum specific capacitance of 161 F g -1 and high stability (retained 99.4 % capacity after 1000 cycles) in 6 M KOH electrolyte at 1 A g -1 , showed a great advance when compared with most reported benchmark carbon materials. The multifunctional porous carbon materials presented herein were facilely prepared without any activation, exhibiting considerable potentials for large-scale gas adsorption/separation and electrochemical energy storage.
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