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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PubMed
高影响因子
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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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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DOI
PubMed
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Wei Lu,Xiaoyu Shi,Hang Zhou,Wenlu Luo,Lei Wang,Hui He
Using renewable solar energy sources instead of heat energy to desorb CO 2 from adsorbents is a promising strategy for reducing the energy consumption of adsorbent regeneration. However, the photothermal temperature of adsorbents with high CO 2 adsorption capacity cannot desorb CO 2 efficiently in a real sunlight environment. Here, a novel solar energy-triggered regenerative bionic fiber adsorbent for CO 2 capture was designed via bionic electrostatic and chemical cross-linking assembly of cellulose nanofibers, thermosensitive polymer poly(N-isopropylacrylamide), nano-graphene oxide and polyethyleneimine. Excellent photothermal transformation characteristics, thermosensitivity and high density of amino adsorption sites were synchronously endowed onto cellulose nanofibers with hydroxyl groups. The thermosensitivity and hydroxyl synergy of the adsorbent enables it an ultralow regeneration temperature (60 °C) by preventing the formation of refractory urea. Interestingly, the adsorbent possesses a high CO 2 adsorption capacity (6.52 mmol/g) and can be efficiently regenerated by using renewable solar energy, indicating that it is a promising strategy for greatly reducing the energy consumption for adsorbent regeneration.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Rui Ding,Ziheng Li,Yan Dai,Xiangcun Li,Xuehua Ruan,Jiaming Gao,Wenji Zheng,Gaohong He
The amino functionalization of MOFs has been verified to be effective in improving the selective permeation of CO 2 . However, the introduction of amino groups into ZIF-8 by mixed ligands strategy is hard to achieve due to the high steric hindrance of benzene ring in 2-aminobenzimidazole ligand, resulting in insufficient content of amino groups. Therefore, in this work, polystyrene-acrylate (PSA) template is proposed to provide abundant adsorption and reaction sites for the rapid synthesis of NH 2 -ZIF-8 with high content of 2-aminobenzimidazole. Furthermore, the incomplete etching strategy is used to construct PSA modified hollow NH 2 -ZIF-8 nanospheres (PHNZ). Importantly, the thickness of PSA layer and the hollow size are adjusted by the etching time, as revealed by the SEM and TEM images. In this PHNZ, the modified PSA can provide good interface compatibility between PHNZ and Pebax matrix to enhance the CO 2 selectivity, while the hollow structure can reduce the mass transfer resistance and improve the gas permeability. Moreover, the introduced amino groups can enhance the CO 2 affinity of PHNZ and further improve the CO 2 /N 2 selectivity of the PHNZ-based mixed matrix membranes (MMMs). Benefiting from the synergy of good interface compatibility and enhanced CO 2 affinity from the amino groups, the PHNZ/Pebax MMMs present greatly improved CO 2 /N 2 selectivity in contrast with pure Pebax and NH 2 -ZIF-8 based membranes. Besides, as the etching time increases, the PHNZ-2 and PHNZ-3 based MMMs present a higher CO 2 permeability than that of NH 2 -ZIF-8 based MMM, revealing the significance of the hollow structure. The PHNZ-2/Pebax MMM with filler loading of 10 wt% expresses the best gas separation performance with the CO 2 permeability of 121.9 Barrer and CO 2 /N 2 selectivity of 96.6, respectively, showing an increase of 54.7 % and 98.0 % in contrast with pure Pebax membrane. Meanwhile, this CO 2 separation performance is far beyond the Robeson upper bound in 2008 and close to the McKeown upper bound in 2019, demonstrating that the proposed PHNZ displays a promising and competitive potential in MMM based CO 2 capture.
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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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高影响因子
REACTIVE & FUNCTIONAL POLYMERS
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2022
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IF 4.966
Xiaona Huang,Yinchuan Wang,Xuguang Wang,Xiutian Yang,Hao Zhang,Fan Zhang,Chao Wang,Yungang Bai,Ying Liu,Jiarui Wang,Xinyue Wang,Hui Chi,Chao Zhou,Kun Xu,Pixin Wang
During the completion of a natural gas well , the annular gas migration of the cement paste significantly damages the cement quality. Thus, the cement with self-repairing property has great significance in oil well applications. In this work, chemically cross-linked hydrogels were synthesized by the solution polymerization of acrylamide , acrylic acid , and 2-(dimethylamino)ethyl methacrylate (DMAEMA) with NMBA as cross linker to plug the CO 2 -triggered microcracks in the cement paste. The mechanical strength of the hydrogel (Cu-PMAD) was significantly enhanced by complexation between Cu 2+ and the carboxyl group of the hydrogel network. As a self-healing plugging material, Cu-PMAD hydrogel powder was mixed with cement to prepare self-repairing cement slurry. The amphoteric structure of hydrogel was triggered by CO 2 due to the DMAEMA unit of the hydrogel was protonated, and the hydrogel can swell further by the anti-polyelectrolyte effect under CO 2 of nature gas and formation salt-bearing fluid. The good swelling ability and mechanical properties endowed the Cu-PMAD hydrogel with excellent plugging ability for cement microcracks triggered by CO 2 .
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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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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Jinmiao Sun,Xiaoli Li,Jiamin Li,Manman Mu,Xiaohong Yin
Bi-based semiconductors have been regarded to be an ideal platform in photocatalytic CO 2 reduction to fuels. However, the insufficient charge transfer efficiency greatly restricts their practical application. Herein, we fabricated 1D/2D hierarchical heterostructures by the hybridization of Bi 4 O 5 Br 2 and rod-like MOF-derived MoS 2 anchored in nitrogen-doped porous carbon (NPC-MoS 2 ) using Mo-MOF as a precursor followed by sulfidation and typical solvothermal process. Compared to pristine Bi 4 O 5 Br 2 nanosheet and NPC-MoS 2 nanorod , the 5 wt% NPC-MoS 2 @Bi 4 O 5 Br 2 p-n heterojunction exhibits distinctly enhanced photocatalytic activity under light illumination due to the increased light absorption capability and more effective charge transfer efficiency. X-ray photoelectron spectroscopy and photoelectrochemical analysis imply that a built-in electric field on interfaces is created to form p-n heterojunctions which drive the photoinduced electrons transferred from NPC-MoS 2 to Bi 4 O 5 Br 2 . Finally, the type-II charge transfer mechanism is proposed which promotes separation of the charges and provides suitable conduction band to reduce CO 2 much efficiently. In a word, this work provides a new insight into the establishment of hierarchical p-n heterostructures for photocatalysis .
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高影响因子
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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高影响因子
APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Zhuping Li,Yong Men,Shuang Liu,Jinguo Wang,Keye Qin,Dandan Tian,Tianle Shi,Li Zhang,Wei An
The crystalline phases of support have great influence on their surface and structure properties. Therefore, adjusting the crystalline structure of heterogeneous catalysts imposes a significant impact on the catalytic performance. Herein, a suite of Pd/In 2 O 3 /ZrO 2 catalysts with different crystalline phases of ZrO 2 were prepared and evaluated for CO 2 hydrogenation to CH 3 OH using the same amount of metal loading. The activity data showed the distinct superior reactivity of Pd/In 2 O 3 /ZrO 2 catalyst used mixed monoclinic and tetragonal phases ZrO 2 (Mix-ZrO 2 ) as support as compared to respective single phase of monoclinic ZrO 2 (m-ZrO 2 ) and tetragonal ZrO 2 (t-ZrO 2 ). The catalysts are extensively characterized through BET, XRD, HRTEM, UV–vis, H 2 -TPR, CO 2 /H 2 -TPD and XPS. Combining the characterization results and activity data, the superior activity of Pd/In 2 O 3 /Mix-ZrO 2 catalyst can be correlated with large particle size of Pd nanoparticles, the concentration of oxygen vacancies, and the abundant medium basic sites, which were essential for activation of H 2 and inert CO 2 and enhancement of catalytic performance. The best-performing Pd/In 2 O 3 /Mix-ZrO 2 catalyst exhibited a remarkable reactivity with space time yield (STY) of 0.54 g methanol ·h −1 ·g cat −1 at 573 K and 5 MPa, and stability without noticeable deactivation after 100 h of time on stream, demonstrating its potential as catalyst used in CH 3 OH synthesis from CO 2 hydrogenation.
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FUEL
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2022
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IF 8.035
Huangyu Yan,Guojie Zhang,Ying Wang,Jun Liu,Guoqiang Li,Yuqiong Zhao,Ying Xu,Yongkang Lv
The low-cost of CO 2 adsorbent is crucial for realistic CO 2 adsorption application. In this paper, a series of green CO 2 adsorbents were prepared using tetraethylenepentamine (TEPA) functionalized blast furnace slag (BFS) as raw materials, which not only implemented the recycling of blast furnace slag solid waste, but also realized the low cost of amine adsorbents. A series of characterization analyses were performed on the synthesized hydrotalcite-like and hydrated calcium silicate green support materials. The effects of structures, TEPA loadings and adsorption temperatures on the material properties were investigated. The result shows that BFS10.5-50TEPA with more pores is an ideal adsorbent, its optimum adsorption capacity for CO 2 is 5.64 mmol/g at 80 ℃, and the amine efficiency is as high as 38.42 %. According to CO 2 -TPD analysis, the dominant CO 2 adsorption mechanism of BFS10.5-50TEPA were physisorption and weak chemisorption. Moreover, the adsorption kinetics and regeneration performances also studied. The results indicate that pseudo-first-order model and pseudo-second-order model are both not accurately at predicting experimental results, while the Avrami model can accurately predict the adsorption kinetics of CO 2 at both low adsorption temperature and high adsorption temperature. After 10 adsorption-desorption recycles, the CO 2 adsorption capacity of BFS10.5-50TEPA still maintain 5.02 mmol/g. This study provides a novel method for the preparation of solid amine adsorbents with high adsorption performance from low-cost solid waste.
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高影响因子
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