SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Menglei Mao,Feixue Sun,Ruqing Chong,Rui Gao,Qiyong Liao,Zihui Meng,Xinlong Fan,Wenfang Liu
Ti 3 C 2 T x as a typical MXene material has a multilayer structure similar to accordion, whose interlayer spacing and specific surface area can be regulated by intercalation and modification. In this work, the effects of several kinds of cation-containing intercalators including NH 4 OH, KOH and NH 4 OH/KCl on the structure of Ti 3 C 2 T x and its application performance in enzymatic CO 2 conversion were investigated for the first time. The results show that Ti 3 C 2 T x intercalated with NH 4 OH/KCl had larger layer spacing (25.25 Å) and specific surface area (20.85 m 2 /g), and better enhancing effect. The initial reaction rate was 0.379 mM/h, which was separately 1.04, 1.42, 1.76 and 5.29 times that of Ti 3 C 2 T x /KOH, Ti 3 C 2 T x /NH 4 OH, Ti 3 C 2 T x and the blank system. Following that, Ti 3 C 2 T x /NH 4 OH/KCl was modified by polyethyleneimine (PEI) and dopamine (DA) and the concentration of modifier was optimized. PEI modified Ti 3 C 2 T x /NH 4 OH/KCl (PEI-Ti 3 C 2 T x ) was superior to PEI/DA modified that in the N content, CO 2 adsorption capacity and application performance. With the addition of 20 mg PEI-Ti 3 C 2 T x , the initial reaction rate was 0.658 mM/h, which was 1.74 and 9.2 times that of before modification and the blank system, respectively. PEI-Ti 3 C 2 T x also exhibited a good reusability and the initial reaction rate was 89.4% of the initial value after 10 cycles.
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ACS Omega
·
2023
·
IF 4.1
Huimei Wu,Yishan Lou,Xiaopeng Zhai,Zhonghui Li,Bin Liu
In this study, we present an innovative intelligent polymer sealant designed to mitigate CO2 leakage during underground geological storage (CCUS). This sealant is formulated by cross-linking CO2-responsive polymers, specifically acrylamide (AM) and N-[3-(dimethylamino) propyl] methacrylamide (DMAPMA), with polyethylenimine (PEI) serving as the cross-linking agent. The polymer sealant’s characteristics were systematically investigated, varying the CO2-responsive polymer content (1.5 wt %) and PEI content (0.1–0.6 wt %). A comprehensive analysis encompassing the rheological properties, thermal behavior, conductivity, and microstructures was conducted. Experimental results indicate that the polymer sealant exhibits excellent injectability, rapid response kinetics, thermal stability, and robust mechanical strength. Upon encountering CO2, the polymer system undergoes a transition from sol to gel state, forming a surface-smooth, uniformly porous three-dimensional (3D) network skeleton structure. Remarkably, the gel’s modulus remains relatively unaffected by the shear frequency. Core fluid displacement experiments demonstrated a substantial sealing efficiency of 73.6% for CO2 and an impressive subsequent injection water sealing rate of 96.2%, underscoring its superior sealing and migration performance. In conclusion, the proposed CO2-responsive gel sealant exhibits an exceptional potential for successful utilization in CCUS operations. This advancement introduces a novel avenue to enhance the effectiveness of CO2-responsive gel sealants, thereby contributing to the advancement of CO2 leakage mitigation strategies in geological storage scenarios.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Hao Jiang,Lizhang Wang,Bai Gao,Yiran Li,Yadan Guo,Mengning Zhuo,Kaixuan Sun,Binyu Lu,Meiyu Jia,Xiaoxia Yu,Huidong Wang,Yongge Li
In order to achieve high energy-conversion efficiency during CO 2 electro-conversion, OH − oxidation was employed as a counter reaction vs . CO 2 electroreduction for formate production on a Tin cathode. The formate faradic efficiency (FE) and production rate were 80.54% and 0.1549 mmol h −1 cm −2 using KOH anolyte at −1.80 V vs . SCE in 8 h operation, which were about 13.71% and 53.03% higher than that for KHSO 4 anolyte, respectively. This is mainly due to alkaline anolyte is beneficial to stabilize the catholyte pH, thus avoiding the competitive hydrogen evolution reaction, while maintaining fast electron transfer rate for the formation of CO 2* − . Moreover, KOH anolyte achieved the lowest power consumption (4.81 kWh kg −1 formate) compared with KHCO 3 and KHSO 4 . Polarization and electrochemical impedance spectroscopy measurements indicated that such energy-saving performance enhancement originated from low equilibrium potential and fast oxidation kinetics associated with the conversion of OH − to H 2 O, which reduced the anode potential and cell voltage. This study puts forward another insight for cost-effective CO 2 reduction, which is of great value to improve the balance of energy input and output during CO 2 conversion, thus having implication in enriching strategy in the field of electroreduction.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-10
·
IF 14.919
Xu Xiaozhi,Wang Jiajie,Zhou Awu,Dong Siyuan,Shi Kaiqiang,Li Biao,Han Jingbin,O’Hare Dermot
Membrane-based gas separation exhibits many advantages over other conventional techniques; however, the construction of membranes with simultaneous high selectivity and permeability remains a major challenge. Herein, (LDH/FAS) n -PDMS hybrid membranes, containing two-dimensional sub-nanometre channels were fabricated via self-assembly of unilamellar layered double hydroxide (LDH) nanosheets and formamidine sulfinic acid (FAS), followed by spray-coating with a poly(dimethylsiloxane) (PDMS) layer. A CO 2 transmission rate for (LDH/FAS) 25 -PDMS of 7748 GPU together with CO 2 selectivity factors (SF) for SF(CO 2 /H 2 ), SF(CO 2 /N 2 ) and SF(CO 2 /CH 4 ) mixtures as high as 43, 86 and 62 respectively are observed. The CO 2 permselectivity outperforms most reported systems and is higher than the Robeson or Freeman upper bound limits. These (LDH/FAS) n -PDMS membranes are both thermally and mechanically robust maintaining their highly selective CO 2 separation performance during long-term operational testing. We believe this highly-efficient CO 2 separation performance is based on the synergy of enhanced solubility, diffusivity and chemical affinity for CO 2 in the sub-nanometre channels.
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JOURNAL OF POLYMER SCIENCE
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2021
·Vol. 59
·期 14
·1528-1539
·
IF 0
Yao Chen,Wenchuan Wang,Dong Xie,Lili Wu,Chaocan Zhang
TPPAlCl-PPN + Cl − binary catalyst (where TPPAlCl is 5,10,15,20-tetraphenylporphyrin aluminum chloride, PPN + Cl − is bis[triphenylphosphine] iminium chloride, the molar ratio of TPPAlCl to PPN + Cl − is 1 to 0.5) can initiate the effective one-pot/one-step ternary copolymerization of CO 2 , lactide and 4-vinyl-1-cyclohexene-1,2-epoxide, and the quaternary copolymerization of CO 2 , propylene oxide, lactide, 4-vinyl-1-cyclohexene-1,2-epoxide, to form multiblock poly(carbonate-co-lactide) products with pendant vinyl group. The ternary copolymerization product composes of polylactide (PLA) block and poy(vinylcyclohexylene carbonate) (PVCHC) block, and the quaternary copolymerization product composes of poy(propylene carbonate) (PPC) block, PLA block and PVCHC block, which are verified by 1 H NMR, 13 C NMR, 1 H- 1 H cosy, hetero-nuclear multiple bond correlation, DTG, and Gel permeation chromatography analysis. The functionality and glass-transition temperature of the products can be easily adjusted by the copolymerization variables, such as the molar ratio of comonomers, copolymerization temperature, pressure of CO 2 , the concentration of the catalyst. Graphical
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Pan Li,Haifeng Hu,Gan Luo,Shuang Zhu,Lingju Guo,Peng Qu,Qi Shen,Tao He
Crystal facet engineering provides a promising approach to tailor the performance of catalysts because of the close relationship between the photocatalytic activity and the surface atomic and electronic structures. An in-depth understanding mechanism of crystal facet-dependent CO2 photoreduction is still an open question. Herein, two different types of porous ZnO nanocatalysts are used as model photocatalysts for the investigation, which are, respectively, with exposed {110} and {001} facets. The porous ZnO with an exposed {110} facet exhibits superior photocatalytic activity to the one with the {001} facet. Various influencing factors have been thoroughly studied both theoretically and/or experimentally, including light harvesting (i.e., band gap), reduction capability (potential of conduction band), crystallinity, CO2 adsorption ability, CO2 activation, and charge separation. The major influencing factors are eventually figured out based on the experimental and calculation results. The product selectivity and the influence of the hole scavenger can be explained too. Our work may pave a way for directing the future rational design of efficient photocatalysts for CO2 reduction.
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ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 30
·期 27
·2001619
·
IF 16.836
Jiaxin Li,Lie Wang,Yang Zhao,Shangyu Li,Xuemei Fu,Bingjie Wang,Huisheng Peng
Lithium-carbon dioxide (Li-CO 2 ) batteries are considered promising energy-storage systems in extreme environments with ultra-high CO 2 concentrations, such as Mars with 96% CO 2 in the atmosphere, due to their potentially high specific energy densities. However, besides having ultra-high CO 2 concentration, another vital but seemingly overlooked fact lies in that Mars is an extremely cold planet with an average temperature of approximately −60 °C. The existing Li-CO 2 batteries could work at room temperature or higher, but they will face severe performance degradation or even a complete failure once the ambient temperature falls below 0 °C. Herein, ultra-low-temperature Li-CO 2 batteries are demonstrated by designing 1,3-dioxolane-based electrolyte and iridium-based cathode, which show both a high deep discharge capacity of 8976 mAh g −1 and a long lifespan of 150 cycles (1500 h) with a fixed 500 mAh g −1 capacity per cycle at −60 °C. The easy-to-decompose discharge products in small size on the cathode and the suppressed parasitic reactions both in the electrolyte and on the Li anode at low temperatures together contribute to the above high electrochemical performances.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
·
IF 3.99
Ying Zhang,Dongfang Liu,Baogang Wang,Hongsheng Lu,Zhiyu Huang
Due to the limitation of anhydrous conditions, the research on anhydrous microemulsion has been developed rapidly. In this paper, CO 2 /N 2 -responsive ILs was used as a polar phase instead of water to prepare anhydrous surfactant-free microemulsion (SFME) with ethanol and n-hexane. This research group has previously studied the preparation process and CO 2 /N 2 responsiveness of the ILs. Then the boundary between multi-phase zone and single-phase zone of surfactant free microemulsion system was determined by drop addition. And the single-phase region was divided into three regions: O/W, B.C and W/O by conductivity and uv–vis. N 2 was introduced into SFME system at 30℃. Interestingly, we found that there was no separation of oil and water. Through the study on DLS , pH and the mutual solubility of Dipropylamine, ethanol and n-hexane, it was found that demulsification occurred in the system, and the absence of oil-water separation was due to the formation of uniform and transparent mixed solution in the system. Finally, It is found that changing the temperature can make the boundary of the multi-phase zone and the single-phase zone in the three-phase diagram of SFME system move. In addition, temperature also had an effect on the particle size of SFME system.
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Science Bulletin
·
2020
·
IF 9.511
Dong-Rui Yang,Ling Liu,Qian Zhang,Yi Shi,Yue Zhou,Chungen Liu,Feng-Bin Wang,Xing-Hua Xia
Electrochemical conversion of CO 2 into fuels is a promising means to solve greenhouse effect and recycle chemical energy. However, the CO 2 reduction reaction (CO 2 RR) is limited by the high overpotential, slow kinetics and the accompanied side reaction of hydrogen evolution reaction. Au nanocatalysts exhibit high activity and selectivity toward the reduction of CO 2 into CO. Here, we explore the Faradaic efficiency (FE) of CO 2 RR catalyzed by 50 nm gold colloid and trisoctahedron. It is found that the maximum FE for CO formation on Au trisoctahedron reaches 88.80% at −0.6 V, which is 1.5 times as high as that on Au colloids (59.04% at −0.7 V). The particle-size effect of Au trisoctahedron has also been investigated, showing that the FE for CO decreases almost linearly to 62.13% when the particle diameter increases to 100 nm. The X-ray diffraction characterizations together with the computational hydrogen electrode (CHE) analyses reveal that the (2 2 1) facets on Au trisoctahedron are more feasible than the (1 1 1) facets on Au colloids in stabilizing the critical intermediate COOH*, which are responsible for the higher FE and lower overpotential observed on Au trisoctahedron.
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JOURNAL OF MOLECULAR LIQUIDS
·
2021
·
IF 6.165
Mi Zhang,Xiaolong Ma,Weiguang Yang,Fangjunchuan Wang,Hao Yu,Aixin Song
We reported the dual-responsive Pickering emulsion systems with a reversible transition between the oil-in-water emulsified form and separated oil/water phase. The Pickering emulsions were prepared using negatively charged Fe 3 O 4 nanoparticles in combination with 1-dodecyl-1H-imidazole (abbreviated as C 12 mim) as stabilizers. By blowing CO 2 , C 12 mim was protonated to be [C 12 mim] + , inducing the modification of negatively charged Fe 3 O 4 nanoparticles through electrostatic attraction and further the generation of emulsions. Moreover, the emulsions exhibited excellent stability at different oil/water ratios and high ionic strength. The reversible process, demulsification, could be realized by bubbling N 2 to remove CO 2 . Being ascribed to the magnetism of the Fe 3 O 4 nanoparticles, the complete demulsification process could also be triggered in several minutes under an external magnetic field. In addition, due to the avoidance of the extra additives in response, the emulsions can maintain their initial performance in theory after the transition between emulsification and demulsification, and can be adequately recycled after removing the original oil and adding fresh oil, being conformed to the principle of green and energy-saving processing.
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ULTRASONICS SONOCHEMISTRY
·
2021
·
IF 7.491
Hanyang Gao,Kunkun Pei,Dong Lei,Guoxin Hu,Yan Chao,Aihua Meng,Hongcheng Wang,Wei Shentu
Due to the tunability in mass transfer, solvation and solubility, gas-expanded liquids show advantages over traditional organic solvents in many characteristics. Ultrasonication is a commonly used method to promote heat and mass transfer. The introduction of ultrasonic technology into the gas-expanded liquid system can promote the polymerization of polymer monomers, enhance extraction efficiency, and control the growth size of nanocrystals, etc. Although acoustic cavitation has been extensively explored in aqueous solutions, there are still few studies on cavitation in organic liquids, especially in gas-expanded liquid systems. In this article, the development of cavitation bubble cloud structure in CO 2 -expanded N, N-dimethylformamide (DMF) was observed by a high-speed camera, and the cavitation intensity was recorded using a spherical hydrophone. It was found that the magnitude of the transient cavitation energy was not only related to input power, but also closely related to CO 2 content. The combination of ultrasound (causing a rapid alternation of gas solubility) and gas-expanded liquid system (causing a decrease in viscosity and surface tension of liquids) is expected to provide a perfect platform for high-speed mass transfer.
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ADVANCED MATERIALS
·
2019
·Vol. 31
·期 17
·1807807
·
IF 25.809
Xueyuan Wang,Jiafang Xie,Muhammad Arsalan Ghausi,Jiangquan Lv,Yiyin Huang,Maoxiang Wu,Yaobing Wang,Jiannian Yao
Metal–CO 2 batteries represent a promising priority for sustainable energy and the environment. However, CO 2 utilization in nonaqueous electrolytes mostly involves difficult CO 2 electrochemistry, leading to poor selectivity and limited cycle performance. Herein, an aqueous rechargeable Zn–CO 2 electrochemical cell that tunably produced CO fuel gas (90% Faradaic efficiency) during cell discharge (cathodic reaction: CO 2 + 2e − + 2H + → CO + H 2 O) and O 2 during cell charge at ≈2 V (cathodic reaction: H 2 O → 1/2O 2 + 2e − + 2H + ), mimicking the separate steps of CO 2 fixation and water oxidation during photosynthesis while exhibiting the advantages of high efficiency, tunable products, and operation independent of sunlight is proposed and realized. The cell achieves a remarkable energy efficiency of 68% with fuel generation, providing an alternative for the green, efficient, and safe utilization of CO 2 by metal–CO 2 batteries.
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