SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Jianfei Xiao,Xiaofang Yuan,Tian C. Zhang,Like Ouyang,Shaojun Yuan
Heteroatomic doped porous carbon (HPCs) is a promising advanced material, showing great application potential in greenhouse gas capture. Here, in-situ N-doped porous carbon (NPC) was developed via a novel and readily scalable strategy − one-step solvent-free melt polycondensation assisted by organic potassium salts, followed by pyrolysis and activation. As both a template and an activator, the added C 6 H 5 K 3 O 7 played an important role to create abundant microporous structure. The as-fabricated NPC-650–0.5 showed a rich N content (6.11 at.%), abundant narrow micro-porosity (0.3437 cm 3 ·g −1 ), and a high surface area (1209.37 m 2 ·g −1 ) and delivered an excellent CO 2 static adsorption capacity (4.16 mmol·g −1 and 8.40 mmol·g −1 at 100 and 500 kPa), a fast adsorption kinetics (circa 98% of balance capacity in 12 min), moderate heat of adsorption (25 to 30 kJ/mol), high selectivity of CO 2 /N 2 , and outstanding uninterrupted recyclability. Both the narrow micropore volume and N-doping sites had strong effects on the CO 2 adsorption capacity, indicating a physical and chemical adsorption process with the mechanism being multi-layer adsorption by the micropore filling. This work highlights the great potential of the NPC-650–0.5 for capturing CO 2 and offers new insights into a green activator and a simple and easy-to-scale method for preparing HPCs.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Ya Liu,Yunfeng Zhao,Ning Jiang,Wei Cheng,Dongwei Lu,Tao Zhang
Oil-in-water (O/W) emulsion is one type of oily wastewater produced by many industries. The treatment of and resource recovery from O/W emulsions are very challenging. Unlike bulk or floating oil, which can be successfully abstracted from wastewater by hydrophobic/oleophilic materials, the abstraction of emulsified oil is not easy because of its highly hydrophilic surface composed of dense surfactants. Separate reclamation of miscible oil and surfactant through a green approach is even more difficult. Here, we report that a CO2-responsive material can abstract emulsified oil and demulsify the oil droplets. Moreover, it can release the abstracted oil and surfactant separately. This material exhibited a very high adsorption capacity for emulsified oil (14 g g–1). Upon switching the surface wettability of the material under CO2 or synthetic flue gas sparging, coalesced oil was reclaimed while the surfactant was retained inside the pores. The hydrophobic character of the material was retrieved when CO2 was purged with nitrogen sparging or air heating. Then, the surfactant was reclaimed by elution with diluted alkali/ethanol. Oil and surfactant were thus separately reclaimed from the O/W emulsion. High rates of oil removal, oil recovery, and surfactant recovery were maintained during repeated adsorption/desorption operations. This work provides a potentially sustainable and green way for O/W emulsion treatment and resource recovery.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Yunxia Bai,Mei Li,Xuemei Liu,Jinyu Han,Xinli Zhu,Qingfeng Ge,Hua Wang
Photocatalytic CO2 reduction is a promising route to simultaneously address two critical issues related to the energy and environment. Herein, a direct Z-scheme photocatalytic system, Ti3+ defective TiO2/CdS nanoflowers, was fabricated to enhance the production of C1–C3 products from CO2 reduction. First, nanoflower-like TiO2 (NF-TiO2) is prepared using a TiB2 precursor to build in Ti3+ defects. Then, the NF-TiO2/CdS heterojunctions are constructed via the sulfurization of TiO2/Cd-MOF. Importantly, the optimal heterojunction photocatalyst NF-TiO2/CdS0.6 exhibits a highly promoted CO2 reduction activity not only for CO and CH4 but also for C2–C3 hydrocarbons. The cumulative yields of CO and CH4 are 1007.0 μmol/g and 83.5 μmol/g (2.5 h), respectively, and a yield of 55.3 μmol/g (2.5 h) of C2–C3 hydrocarbons is obtained. This enhanced yield of C1–C3 products is attributed to the synergistic effects of abundant Ti3+ defects that increase adsorption and activation of CO2, the large surface area that provides sufficient active sites, and a direct Z-scheme heterojunction with a good intimate contact interface that effectively separates charge carriers and accumulates electrons with strong reducibility. Moreover, the photoluminescence analysis of hydroxyl radicals was conducted to provide evidence for the direct Z-scheme mechanism. This work provides a facile method for the construction of a TiO2-based direct Z-scheme photocatalytic system for improving photocatalytic performance toward CO2 reduction.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2022
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IF 3.898
Yuxin Wu,Zhuo Chen,Xiaohui Zhang,Jian Chen,Yundong Wang,Jianhong Xu
Carbon dioxide (CO 2 ) utilization and fixation have become one of the most important research areas nowadays due to the increase of global greenhouse effect. Cyclic carbonate, which is widely used in various fields, can be synthesized by fixation of CO 2 with epoxide in industry. Moreover, the synthesis of cyclic carbonate is a 100% atom economical reaction, which makes it eco-friendly and promising. To enhance the reaction efficiency and safety, a microreaction system was used as the platform for cycloaddition reaction. In this work, tetrabutylammonium bromide (TBAB) was chosen as catalyst, and propylene oxide (PO) as a mode substrate. Interestingly, the addition of water can increase the propylene carbonate (PC) yield and decrease the activation energy considerably, proving water as catalyst promoter for PC synthesis. PC yield and selectivity could reach 91.6% and 99.8%, respectively. The Influence factors and kinetic equation for CO 2 cycloaddition were obtained as well.
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ELECTROANALYSIS
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2022
·Vol. 35
·期 1
·e202200158
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IF 3.077
Liangyin Zhou,Hongji Li,Dandan Wang,Wei Jiang,Yuanyuan Wu,Liaofang Shang,Chunyi Guo,Chunbo Liu,Baixiang Ren
Zeolitic Imidazolate Frameworks (ZIFs) are considered as a novel porous material combining high stability in inorganic zeolites with high porosity and organic functionality of MOFs. The cage-like structure selectively and efficiently traps CO 2 , which is an indispensable and critical step for Electrocatalytic CO 2 Reduction Reaction (CO 2 RR). In this work, ultrasmall ZIF-8 nanomaterials are synthesized by tuning the molar ratio of the feedstock and used as electrocatalysts for the selective reduction of CO 2 to CO. The catalytic activity of the ultra-small size ZIF-8 material for the electrocatalytic reduction of CO 2 can reach satisfactory results with a Faraday efficiency of 91 % for CO and a stability of 12.5 h at a high applied potential of −1.8 V vs. RHE. The investigation can provide a new idea to explore for the design and improvement of catalysts for CO 2 RR.
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CHEMICAL ENGINEERING SCIENCE
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2022
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IF 4.889
Qinlan Luo,Qiang Sun,Qi Liu,Sen Liu,Min Xiao,Mengjie Chen,Yuanyuan Li,Hongxia Gao,Zhiwu Liang
The kinetics of CO 2 absorption in ethanolamine (MEA) + H 2 O + ethanol systems was investigated using stopped-flow apparatus. The first-order reaction rate constant ( k 0 ) values were tested with varying H 2 O and MEA concentrations. Transiting from the aqueous to non-aqueous solvents, the k 0 decreases and the reaction order for MEA shifts from 1.05 to 1.88. The zwitterion mechanism with the rate-limiting step of deprotonation was used to explore the role of water and its effect. Results showed that water could impact reactions through direct involvement and changing solvation environment. An improved kinetic model based on the zwitterion mechanism was obtained to indicate the quantitative influence of H 2 O concentration on the reaction kinetics of MEA + H 2 O + ethanol systems. The predicted values from the model well agreed to the experimental data with the average absolute relative difference of 6.73%. This study highlights the important effects of water on the reaction kinetics of CO 2 absorption into water-lean amine solutions.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
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IF 6.76
Liwei Sun,Meilin Yin,Zhen Li,Shaokun Tang
To alleviate environment issues derived from CO 2 emission, developing effective and economical methods for CO 2 capture has attracted much attention for decades. Metal-organic frameworks possess high porosity and stability, which is favorable to the adsorption of small molecules. Herein, an aluminum-based MOF, aluminum terephthalate [MIL-53(Al)], was synthesized with H 2 O and N , N′ -dimethylformamide as co-solvent via microwave-assisted method for CO 2 adsorption. The parameters including pre-mixing mode, microwave temperature, microwave power and reaction time were varied to study their influences on crystal structure, morphology and CO 2 adsorption capacity of MW-MIL-53(Al). Wherein, MW-MIL-53(Al) prepared with pre-mixing mode of stirring at 130 °C, 200 W and 3 h presents high crystallinity and rod-like morphology. The synthesized MW-MIL-53(Al) possesses relatively high BET surface area (961 m 2 /g), pore volume (0.46 cm 3 /g) and thermal stability (up to 480 °C), and its CO 2 adsorption capacity is 2.16 mmol CO 2 /g adsorbent under 25 °C and 0.1 MPa, which is higher than CS-MIL-53(Al) synthesized via conventional solvothermal method at 130 °C for 48 h.
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Su Liu,Mingqiang Tang,Jun Pang,Jintao Hu,Weijie Chen,Jie Cheng,Zewei Liu,Haihong Zhao,Rong Tan
Water-soluble single-chain polymeric nanoparticles (SCPNs), which isolated catalytic sites within a hydrophobic interior, made water-incompatible organometallic catalysis highly efficient in water. However, it is still a great challenge to conveniently control their hydrophilicity, so as to combine reactivity and recovery of the catalytic SCPNs in aqueous systems. Herein, we have developed a series of catalytic SCPNs, which possessed CO2-switchable hydrophilic/hydrophobic behavior, to realize the gas-controlled reaction and separation for asymmetric sulfa-Michael addition (SMA) in water. A novel series of CO2-switchable random copolymers were thus synthesized by copolymerization of CO2-responsive amidine derivatives with hydrophobic chiral salen FeIII monomers via reversible addition-fragmentation chain transfer polymerization. Characterization suggested their CO2-controlled self-collapse behavior in water due to CO2-switched change in hydrophilicity/hydrophobicity of the amidine moiety. The resultant CO2-switchable SCPNs provided hydrophobic, catalytic compartments for asymmetric SMA in water upon CO2 addition, giving various chiral β-keto sulfides with almost quantitative yields (90–98%) and high enantioselectivities (93–99%). When CO2 is removed by N2 bubbling, they were collapsed and spontaneously precipitated from the aqueous system for steady reuse. The gas-controlled reaction-separation approach provides an energy-efficient way to combine reactivity and recovery of catalytic SCPNs in aqueous systems, which should be quite practical in large-scale industrial applications.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Yanyong Sun,Minmin Gou
Based on the one-dimensional tubular structure of halloysite nanotubes (HNTs), plant polyphenols and polyamines were used for in situ polymerization on the surface of HNTs to form amino-rich polymers, which were then removed as templates to synthesize polymer nanotubes. These nanotubes were then incorporated into a Pebax matrix to prepare mixed-matrix membranes (MMMs) for CO 2 /CH 4 gas separation. The removal of the HNT template increased the lumen diameter of the filler and significantly improved its gas permeability . And the amino groups on the inner surface of the polymer nanotubes were exposed. Further, the number of CO 2 reaction sites increased, which improved the reaction selectivity of CO 2 . In addition, the presence of amine groups on the inner and outer surfaces of the polymer nanotubes provided various transfer channels for CO 2 , which were conducive for CO 2 gas transfer in the membrane. When the CC-PEINT content was 8 wt%, the CO 2 permeability was 710 Barrer and CO 2 /CH 4 selectivity was 60. The CO 2 permeability and CO 2 /CH 4 selectivity of the Pebax/CC-PEINTs membranes increased by 163% and 132%, respectively, compared with those of the pure Pebax membrane.
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Science Bulletin
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2022
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IF 20.577
Qi Hao,Qi Tang,Hai-Xia Zhong,Jia-Zhi Wang,Dong-Xue Liu,Xin-Bo Zhang
Single-atom catalysts (SACs) have attracted increasing concerns in electrocatalysis because of their maximal metal atom utilization, distinctive electronic properties, and catalytic performance. However, the isolated single sites are disadvantageous for reactions that require simultaneously activating different reactants/intermediates. Fully exposed metal cluster catalyst (FECC), inheriting the merits of SACs and metallic nanoparticles , can synergistically adsorb and activate reactants/intermediates on their multi-atomic sites, demonstrating great promise in electrocatalytic reactions . Here a facile method to regulate the atomic dispersion of Ni species from cluster to single-atom scale for efficient CO 2 reduction was developed. The obtained Ni FECC exhibits high Faradaic efficiency of CO up to 99%, high CO partial current density of 347.2 mA cm −2 , and robust durability under 20 h electrolysis. Theoretical calculations illuminate that the ensemble of multiple Ni atoms regulated by sulfur atoms accelerates the reaction kinetics and thus improves CO production.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Yun Long,Jian Sun,Changnian Mo,Xiangyao She,Pengxin Zeng,Hongqiang Xia,Jubing Zhang,Zijian Zhou,Xinming Nie,Chuanwen Zhao
Calcium looping (CaL) belongs to a promising high-temperature CO 2 capture technology because of adopting cheap and extensive source CaO-based sorbents . However, CaO-based sorbents are prone to occur the issues of sintering and elutriation in the fluidized-bed reactors. To further enhance the practicability, the Zr-supported, CaO-based sorbent pellets were produced using the graphite-moulding method. Different synthesis modes (i.e., sol-gel, hydration-mixing, and wet-mixing) were compared for preparing CaO-based composite slurry before pelletization. Sol-gel is the promising synthesis mode to prepare Zr-supported, CaO-based pellets with outstanding CO 2 capture performance due to achieving a more uniform distribution of inert CaZrO 3 spacer. Moreover, the Zr-based stabilizer content within sorbent pellets produced by the combined method of sol-gel and graphite-moulding was further studied. The higher content of Zr-based stabilizer promotes the enhancement of cyclic stability and mechanical strength of Zr-supported, CaO-based pellets. After 17 cycles, the sorbent pellets containing 20 wt% of Zr-based stabilizer display a high CaO carbonation conversion of 74.1 %. Moreover, CaO-based pellets with 20 wt% of Zr-based stabilizer possess a higher compression strength of 4.84 ± 1.08 MPa, which is as high as 1.8 times that of the pellets with 5 wt% of Zr-based stabilizer.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Tianle Shi,Yong Men,Shuang Liu,Jinguo Wang,Zhuping Li,Keye Qin,Dandan Tian,Wei An,Xiaoli Pan,Lin Li
Hydrogenation of CO 2 to methanol is an achievable way for “methanol economy” and “liquid sunshine” visions. Owing to highly tunable properties containing different morphologies, exposed crystal facets and oxygen vacancies , In 2 O 3 has become a promising material for CO 2 hydrogenation. Here we successfully introduced highly dispersed Pt 2+ species into three different morphologies In 2 O 3 supports by controllable precipitation method. The dominant exposed crystal facets of In 2 O 3 supports during the research are discovered to greatly affect the dispersion of active Pt 2+ species and the number of oxygen vacancies, as analyzed by diverse characterization techniques, and closely correlated with the catalytic performance. Compared with Pt/In 2 O 3 whcih mainly exposing (222) or (104) facet, Pt/In 2 O 3 which primarily exposed (211) facet obtained higher catalytic activity, including a CO 2 conversion of 11.7% and methanol selectivity of 74.8% with a space time yield of methanol of 0.63 g MeOH h −1 gcat −1 at 300 °C, 5 MPa, and 21,000 cm 3 h −1 g −1 . The highly enhanced activity of 1.5Pt/C-In 2 O 3 -S catalyst was ascribed to its more abundant oxygen vacancies and well-dispersed Pt 2+ species, which derived from the interaction between Pt 2+ and the underlying In 2 O 3 (211) facet. The special interface structure enabled the activation of CO 2 and hydrogenation of key intermediates effectively. Exposing the highly active crystal face of the In 2 O 3 supports is proved to be an effective strategy to enhance catalytic performance of Pt/In 2 O 3 catalyst for methanol synthesis .
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