AICHE JOURNAL
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2023
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IF 3.7
Jiajin Huang,Liang Yu,Qichen Fan,Jinze Yao,Yongsheng Huang,Haoyuan Luo,Baoyu Liu,Hao Wang,Qibin Xia
The purification of gaseous olefins, such as C 2 H 4 and C 3 H 6 , requires the efficient removal of trace CO 2 impurities. However, the development of ideal adsorbents with high CO 2 /olefin selectivity has remained a challenge. In this study, we synthesized a novel adsorbent, denoted as PEI/DEA@FS, by modifying fumed silica (FS) with a combination of polyethylenimine (PEI) and diethanolamine (DEA). At 298 K and 0.0004 bar, PEI/DEA@FS presented the highest CO 2 adsorption capacity among previously studied adsorbents, with a value of 2.12 mmol/g. Notably, PEI/DEA@FS demonstrated very high ideal adsorption solution theory selectivity for CO 2 /C 2 H 4 (>10 10 ) and CO 2 /C 3 H 6 (>10 7 ) at 298 K and 0.01 bar. Breakthrough experiments revealed its excellent separation performance, producing olefins (C 2 H 4 and C 3 H 6 ) with ultra-high purity (>99.9%) from a CO 2 /olefin (1/99) mixture. Moreover, PEI/DEA@FS exhibited outstanding stability over 20 adsorption and desorption cycles, and its CO 2 adsorption performance remained almost unchanged under 75% relative humidity in the feed stream.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Ying Zhang,Linlin Zang,Shuting Zhao,Weipeng Cheng,Long Zhang,Liguo Sun
Covalent organic frameworks (COFs) have great potential for photocatalytic CO 2 reduction, owing to their adjustable structures, porous characteristics, and highly ordered nature. However, poor light absorption, fast recombination of photogenerated electron-hole pairs, and suboptimal coordination conditions have contributed to the hindered efficiency and selectivity observed in photocatalytic CO 2 reduction processes. In this work, the integration of bromine (Br) atoms into COFs was achieved through the synthesis process involving nickel (II) tetraaminophthalocyanine (NiTAPc) and 3,6-dibromopyromellitic dianhydride (BPMDA) using a solvothermal approach. The coupling of a porous framework structure alongside the incorporation of Br atoms yields a significant enhancement in photoelectric properties compared to bromine-free COFs. Meanwhile, X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations revealed that the introduction of Br atoms can facilitate the adjustment of the electron configuration around the phthalocyanine unit and diminish the required energy for the photocatalytic reaction. When subjected to visible light irradiation, the NiTAPc-BPMDA COF showcased a CO yield of 148.25 μmol g −1 over a 5-hour period, accompanied by an impressive selectivity of 98%. This work highlights the collaborative influence of phthalocyanines and Br atoms within COF-based photocatalysts, offering an alternative approach for designing and constructing high-performance photocatalysts with elevated yield and selectivity. The synergistic role of phthalocyanines and Br atoms within the COF-based photocatalysts provides an alternative strategy for photocatalysts with high yield and selectivity in the future.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ganghua Zhou,Longyun Zhang,Yu Xia,Hangmin Xu,Weiqin Yin,Shengsen Wang,Jianjian Yi,Xingwang Zhu,Xin Ning,Xiaozhi Wang
Solar-driven conversion of CO 2 into high-value-added chemicals is considered as one of the effective strategies to address global climate change. However, the sluggish charge separation kinetics and poor product selectivity remain the two major bottlenecks restricting photocatalytic CO 2 conversion. Herein, we developed an anatase surface modified atomically dispersed Cu (Cu anchored on N-doped carbon skeleton) photocatalyst (TiO 2 /Cu 1 NC) based on a “reflux + calcination” method for CO 2 photoreduction. Under full spectral illumination, the as-synthesized TiO 2 /Cu 1 NC displayed a brilliant CO production rate of 2.59 μmol h −1 (mass of photocatalyst: 5 mg), high selectivity (∼98.5%), and excellent durability using [Ru(bpy) 3 ]Cl 2 ·6H 2 O as the photosensitizer and triethanolamine as an electron donor. Experiments and density functionalized theory calculations synergistically confirm that the surface-constructed atomically dispersed Cu 1 NC active sites can accelerate the separation and transfer of photogenerated charge carriers, optimize CO 2 adsorption and activation, reduce the formation energy barrier of the key intermediate *COOH during the CO 2 RR process, and thus enhance the activity and selectivity of CO 2 RR. This work provides new insights into the surface engineering of atomically dispersed active sites to improve the activity and CO selectivity of CO 2 photoreduction.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Lang Pei,Xusheng Wang,Heng Zhu,He Yu,Sateesh Bandaru,Shicheng Yan,Zhigang Zou
Photothermal catalysis, which combines light promotion and thermal activation, is a promising approach for converting CO2 into fuels. However, the development of photothermal catalysts with effective light-to-heat conversion, strong charge transfer ability, and suitable active sites remains a challenge. Herein, the photothermal effect- and interfacial N–Ni/Ta–O bond-modulated heterostructure composed of oxygen vacancy-rich NiOx and Ta3N5 was rationally fabricated for efficient photothermal catalytic CO2 reduction. Beyond the charge separation capability conferred by the NiOx/Ta3N5 heterojunction, we observed that the N–Ni and Ta–O bonds linking NiOx and Ta3N5 form a spatial charge transfer channel, which enhances the interfacial electron transfer. Additionally, the presence of surface oxygen vacancies in NiOx induced nonradiative relaxation, resulting in a pronounced photothermal effect that locally heated the catalyst and accelerated the reaction kinetically. Leveraging these favorable factors, the NiOx/Ta3N5 hybrids exhibit remarkably elevated activity (≈32.3 μmol·g–1·h–1) in the conversion of CO2 to CH4 with near-unity selectivity, surpassing the performance of bare Ta3N5 by over 14 times. This study unveils the synergistic effect of photothermal and interfacial chemical bonds in the photothermal–photocatalytic heterojunction system, offering a novel approach to enhance the reaction kinetics of various catalysts.
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ENERGY
·
2023
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IF 9
Run Qi,Zhaohao Li,Hongyuan Zhang,Hongming Fu,Heng Zhang,Dan Gao,Haiping Chen
Membrane absorption is a promising CO 2 capture technology, which is limited by the high cost of membrane materials. Coal fly ash (CFA)-based ceramic membrane as an alternative material for membrane modules can effectively reduce the preparation cost. In this study, CFA-based ceramic membrane with superhydrophobic properties is prepared by depositing SiO 2 nanoparticles and grafting 1H, 1H, 2H, 2H-perfluorooctyltriethoxysilane (POTS). Characters including pore size distribution, porosity and N 2 flux of superhydrophobic membrane are performed. The superhydrophobic modified ceramic membrane is applied to CO 2 capture experiments using ethanolamine (MEA) solution as the absorbent. The result shows that the contact angle of the modified ceramic membrane reaches 155.0°, which significantly improves the anti-wetting properties of the membrane surface . The CO 2 capture experiment demonstrates a maximum capture efficiency of 97.45% and a mass transfer rate of 21.17 mol/(m 2 ·h). In addition, the superhydrophobic modified ceramic membrane exhibits excellent thermal and chemical stability, sustaining high performance even after 8 h of continuous operation. This study provides the theoretical and empirical foundation for the application of CFA-based superhydrophobic ceramic membranes in CO 2 capture.
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Polymers
·
2023
·Vol. 15
·期 19
·3886
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IF 5
Xin Chen,Yiqiang Li,Xiaoguang Sun,Zheyu Liu,Jianbin Liu,Shun Liu
CO2flooding is a favorable technical means for the efficient development of low-permeability reservoirs, and it can also contribute to the realization of net-zero CO2emissions. However, due to the unfavorable viscosity ratio and gravity overriding effect, CO2channeling will inevitably occur, seriously affecting its storage and displacement effects. This paper conducts a systematic study on the application of polymer-assisted CO2flooding in low-permeability reservoirs. Firstly, the polymer agent suitable for low-permeability reservoirs is optimized through the viscosity-increasing, rheological, and temperature- and salt-resistant properties of the solution. Then, the injectivity performance, resistance-increasing ability, and profile-improving effect of the polymer solution were evaluated through core experiments, and the optimum concentration was optimized. Finally, the enhanced oil recovery (EOR) effects of polymer-assisted and water-assisted CO2flooding were compared. The results show that the temperature-resistant polymer surfactant (TRPS) has a certain viscosity-increasing performance, good temperature resistance performance, and can react with CO2to increase the solution viscosity significantly. Meanwhile, TRPS has good injection performance and resistance-increasing effect. The resistance increasing factor (ηandη′) of TRPS-assisted CO2flooding increases with increased permeability, the concentration of TRPS solution, and injection rounds. Consideringη′ and the profile improvement effect comprehensively, the application concentration of TRPS should be 1000 mg/L. The EOR effect of TRPS-assisted CO2flooding is 8.21% higher than that of water-assisted CO2flooding. The main effective period is in the first and second rounds, and the best injection round is three. The research content of this paper can provide data support for the field application of polymer-assisted CO2flooding in low-permeability reservoirs.
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ELECTROCHIMICA ACTA
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2023
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IF 6.6
Zhihong Xu,Yunxi Han,Jiuyi Sun,Meng Xu,Wenli Zhao,Qingfa Wang
Electrochemical CO 2 reduction (ECR) to C 2+ products is an efficient method to accomplish intermittent energy storage and CO 2 utilization. Developing high-selectivity electrocatalysts for C 2+ products, especially C 2+ alcohols, have attracted more attention but still remains a major challenge. Here, three kinds of short nanotube (<100 nm), long nanotube (>100 nm), and long nanotube-assembled hollow sphere CuSiO 3 catalysts with different confined space are fabricated for boosting the ECR to produce C 2+ products selectivity. Long CuSiO 3 nanotubes exhibit a higher yield of C 2+ alcohols (26.8 %) and more satisfactory Faraday efficiency (FE) of 69.5 % for C 2+ products than short nanotubes and nanotube-assembled hollow spheres. The confinement effect of long CuSiO 3 nanotubes is conducive to promoting the dimerization of the key reaction intermediate (*CO), inhibiting the diffusion of protons and the side-reaction hydrogen evolution reaction (HER). The formed Cu 0 /Cu + interfaces in CuSiO 3 nanotubes promote the dimerization reactions of adsorbed *CO. The synergistic effect of nanotubes confinement and Cu 0 /Cu + interfaces facilitate the C C coupling reaction to C 2+ products via ECR.
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ENERGY & FUELS
·
2023
·
IF 5.3
Jinrui Zhang,Xiaoqiong Wang,Shixun Chen,Haorui Liu,Shuixia Chen
The adsorption capacity of a solid amine adsorbent for CO2 adsorption is often limited by the number of amino groups on the adsorbent surface. In this paper, a kind of ultrafine solid amine fiber (PSN) was prepared by direct electrospinning of polyethylenimine blends, which could provide plentiful amino groups on the fiber surface without further modification and would improve the CO2 adsorption capacity and amino utilization efficiency of the fibrous adsorbent. The effects of the adsorbent structure on the CO2 adsorption performance of PSN was investigated. The results indicated that the fibrous structure and higher outer surface area of PSN can greatly improve its adsorption capacity and adsorption rate for CO2. Under the simulated flue gas conditions (90% N2/10% CO2) at 25 °C, the CO2 adsorption capacity of PSN fiber is 2.10 mmol/g, and its CO2 adsorption capacity could reach 4.98 mmol/g at 75 °C. The diameter of the fiber obviously affects the CO2 adsorption behavior of the solid amine adsorbents; an increase of the fiber diameter would result in the decrease of the adsorption capacity of the adsorbents. PSN has good regeneration stability, and its CO2 adsorption performance remained almost unchanged after a number of regeneration cycles.
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FUEL
·
2023
·
IF 7.4
Anbang He,Yong Yang,Shuhui Tao,Xubing Zhou,An Wu,Qian Zhang,Changyuan Tao,Jun Du
Co 3 O 4 -based catalysts emerged as promising candidates for electrocatalytic CO 2 reduction reaction (eCO 2 RR), while the unclear active sites and poor stability are challenging for the application of Co 3 O 4 as an electrocatalyst. Here, we developed a feasible method to in situ encapsulate Co 3 O 4 nanoparticles (NPs) into self-grown CNTs . Co 3 O 4 NPs were elaborately controlled to terminate with the occupation Co 2+ Th /Co 3+ Oh sites (with Co 2+ and Co 3+ in the center of tetrahedral/octahedral cells). The well-dispersed Co atoms derived from ZIF-67 catalyzed the in situ assembly of CNTs, allowing controlled oxidation and growth into Co 3 O 4 nanoparticles spatially confined by CNTs, resulting in Co 3 O 4 highly-dispersed into hollow CNTs and well-protected. The enhanced electrocatalytic performance of Co 2+ Th was revealed with an onset potential of −0.24 V, and the CO production rate (131 μmol/s·g·cm 2 , −0.85 V vs. RHE) on Th-Co 3 O 4 /CNTs (exposed with Co 2+ Th sites) is 3.1 times of that on Oh-Co 3 O 4 /CNTs (exposed with Co 3+ Oh sites). DFT calculations demonstrated a significant reduction in the rate-limiting activation barrier of CO 2 , and Co 2+ Th was proved to be more active than Co 3+ Oh with elongated *CO-OH bonds. In situ ATR-SEIRAS confirmed that the enhanced CO 2 adsorption and rapid formation of *COOH on Th-Co 3 O 4 /CNTs were key factors leading to efficient CO production. This work introduced a clear understanding of the eCO 2 RR performance of Co 2+ Th /Co 3+ Oh sites, along with a feasible approach for catalyst construction and protection.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xiaochen Xiang,Jiao Wang,Qinglong Ru,Sumin Li,Ke Zhao,Yifei Zhu,Zhenpan Chen,Liangliang Liu,Guangqin Gu,Yu Jia,Bao Zhang,Gang Cheng,Zuliang Du
As the single electron transfer of CO 2 to CO 2 − ions is the critical step in the CO 2 activation, it is very important to develop appropriate strategies to construct efficient catalytic systems. Herein, we constructed a coupled catalytic system consisting of mechanical-energy-driven triboelectric plasma and indium oxide rich in oxygen vacancies to achieve CO 2 reduction to CO at room temperature and atmospheric pressure. At the discharge distance of 0.6 mm, the indium oxide with more oxygen vacancies exhibited an optimal catalytic activity of 0.20 mmol·g −1 ·h −1 for CO evolution rate, and the conversion efficiency from electrical to chemical energy was 10.8 %. Electron paramagnetic resonance experiments showed that a large amount of CO 2 − ions were generated in the triboelectric plasma. The introduction of oxygen vacancies could increase the density of states near the Fermi level of indium oxide catalysts, stabilize highly active CO 2 − ions, and reduce the energy barrier of CO 2 − decomposition.
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JOURNAL OF MOLECULAR STRUCTURE
·
2023
·
IF 3.8
Dongxue Xiang,Feng Niu,Jing Ji,Junhui Liang,Huayu Chen,Laishun Qin,Yuexiang Huang,Da Chen
Lead halide perovskites (LHPs) quantum dots (QDs) has been deemed as a promising material for photocatalytic conversion (e.g., CO 2 reduction or water splitting) due to their remarkable photoelectrical properties. However, the severe carrier recombination and low charge transfer efficiency largely restrain their photocatalytic performance. Herein, a series of graphene supported dual-phase perovskite QDs photocatalysts were designed by a facile hot-injection strategy for highly efficient photocatalytic CO 2 reduction. Catalytic results showed that under a 5 W white LED irradiation, the CsPbBr 3 /Cs 4 PbBr 6 @G 5% composite with 5 wt% graphene loading exhibited an optimum CO yield of 18.76 μmol g −1 with a selectivity of 52.99% towards the product of CO for photocatalytic CO 2 reduction. The enhanced photocatalytic CO 2 reduction performance over the composites compared with that of CsPbBr 3 , Cs 4 PbBr 6 and CsPbBr 3 /Cs 4 PbBr 6 QDs could be ascribed to the type-I heterojunction structure and graphene support as the electron acceptor in the composite, which could stepwise accelerate the charge separation, suppresses recombination process, and provide more active sites for CO 2 adsorption and reaction. This work would bring new insight in designing novel efficient perovskite-based catalysts for photocatalytic CO 2 transformation.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2023
·
IF 8.7
Xingyuan Wang,Jiamin Qi,Hengxi Zhu,Jiancheng Wang,Heping Zeng,Bin Li,Si Yan
The aluminum industry is facing severe economic and environmental problems due to increasing carbon emissions and growing stockpiles of red mud (RM). RM is a strongly alkaline, high-emission solid waste from the alumina industry with potential for CO 2 sequestration. However, the effectiveness of RM carbon sequestration is poor, and the mechanism behind it is not well understood. In this study, the effect of microwave and tube furnace activation of RM on CO 2 sequestration in alumina was first investigated at different temperatures. The result showed that the CO 2 sequestration capacity of unmodified RM (URM) was only 14.35 mg/g at ambient temperature and pressure, and the CO 2 sequestration capacity could be increased to 52.89 mg/g after high-temperature activation and modification. Besides, high-temperature activation and modification will effectively improve the carbon sequestration capacity of RM. The carbonized RM was characterized by FT-IR, SEM, XRD , laser particle size, TG-DSC, and pH measurements. In addition, the mechanism of RM capturing CO 2 was also proposed, which shows that CO 2 was finally sequestered in the RM as CaCO 3 . The change in particle size distribution and the mineral phase in the RM indicated that high-temperature activation modification positively affects the application of RM to the sequestration of CO 2 . This study can provide a promising technology for the low-carbon and green development of the aluminum industry, as well as achieving the waste treatment and utilization objective.
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