JOURNAL OF MATERIALS SCIENCE
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2023
·Vol. 58
·期 44
·16891-16904
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IF 4.5
Wu Fanghui,Xu Xudong,Luo Xiangrui,Cheng Yuansheng,Xu Hong,Yuan Guozan,Kang Yanshang,Wei Xianwen,Wang Wenhai,Yan Zhengquan
To alleviate the global warming, it is necessary to transform carbon dioxide (CO 2 ) into carbon monoxide (CO) through an expedient and resultful approach. In this work, a novel kind of Schiff base-cobalt ion complexes (CHE-Co) was constructed with 5-chorosalicylaldehyde, acetylglycine, acetic anhydride and CoCl 3 ·6H 2 O as raw materials. It was discovered that CHE-Co exhibits outstanding photocatalytic activity to reduce CO 2 to CO (selectivity: 91%) in an H 2 O/CH 3 CN solution ( V:V = 1:4) under the irradiation of a LED-simulated solar lamp ( λ > 400 nm, 90 mW cm –2 ). Under the optimized conditions, the yield of CO photo-catalytically reduced from CO 2 can reach 15.92 μmol, with TON value of 1592 and TOF value of 159.2 h −1 . The photo-catalytic mechanism of CHE-Co was proposed that CHE-Co with a positive E onset can drive electrons shift from excited-state photosensitizer [Ru(phen) 3 ] 2+* to CHE-Co via a single-molecule rate control reaction.
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Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Jinghao Hua,Sheng Feng,Changchang Ma,Haitao Huang,Kai Wei,Xiaojun Dai,Kaidi Wu,Haihong Wang,Zhaowei Bian
In this study, a novel 2D/2D Z-scheme Bi 5 O 7 Br/NiFe-LDH photocatalyst was prepared by combining NiFe-LDH with Bi 5 O 7 Br through self-assembly. Under simulated solar irradiation, compared with pure NiFe-LDH and Bi 5 O 7 Br, the 2D/2D Z-scheme Bi 5 O 7 Br/NiFe-LDH photocatalyst revealed a significant improvement in the efficiency of photocatalytic reduction of CO 2 . Z-scheme heterojunction promotes the separation of photo generated charge carriers and 2D/2D structure is conducive to exposing more active site and enhancing the migration rate of interface carriers. The photocatalytic activity experiment revealed that the CH 4 production efficiency of the Bi 5 O 7 Br/NiFe-LDH (37.77 μmol/g/h) after 8 h of light exposure was 2 times and 10 times that of Bi 5 O 7 Br (22.41 μmol/g/h) and NiFe-LDH (3.84 μmol/g/h), respectively. The successful formation of Z-scheme heterojunction was determined through band analysis and related characterization. The advantage of Z-scheme heterojunction is that it has high electron mobility and low resistivity. This work launches a feasible design strategy of special structure photocatalysts to enhance the photocatalytic activity for the CO 2 reduction.
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MACROMOLECULES
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2023
·
IF 5.5
Ke Wang,Jialu Zhang,Meiyu Si,Zilong Wang,Liru An,Guiyan Liu,Yongfei Zeng
A series of temperature/pH/CO2/redox-quadruple-responsive ferrocene-containing homopolymers were prepared for the first time. These homopolymers contain hydrophilic ethoxy group, amino group, and hydrophobic ferrocene (Fc) and were synthesized by reversible addition–fragmentation chain transfer (RAFT) polymerization. They showed four different stimuli responses. (1) They exhibit an upper critical solution temperature (UCST) in n-propyl alcohol and n-butanol, which can be adjusted by the molecular structure, molecular weight, and concentration. (2) They have a critical pH in aqueous solution and are affected by molecular structure, molecular weight, and concentration. (3) The CO2 response of the homopolymers was confirmed by cyclic bubbling CO2/N2 to the solution. (4) The redox response of homopolymers was demonstrated by adding a chemical oxidant (FeCl3)/reductant (VC) or electrical stimulation to the solution of homopolymers. In addition, these homopolymers are amphiphilic, and their self-assembly behavior in solution was investigated. It was found that they have different critical micelle concentrations (cmc) and can form lamella, sphere, and agglomerated sphere in solution, and the morphology can be reversibly changed by applying stimulation. Finally, the release behavior of micelles of the homopolymer was explored by wrapping Nile Red (NR), which proved that they had good release efficiency. These temperature/pH/CO2/redox-quadruple-responsive ferrocene-containing homopolymers expand the types of multistimuli-responsive homopolymers and have excellent application prospects in the fields of self-assembly, drug delivery, and electrode materials.
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Petroleum Science
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2023
·
IF 5.6
Xi-Dao Wu,Peng Xiao,Bei Liu,Guang-Jin Chen,Jian-Hua Pang
CO 2 emulsions used for EOR have received a lot of interest because of its good performance on CO 2 mobility reduction. However, most of them have been focusing on the high quality CO 2 emulsion (high CO 2 fraction), while CO 2 emulsion with high water cut has been rarely researched. In this paper, we carried out a comprehensive experimental study of using high water cut CO 2 /H 2 O emulsion for enhancing oil recovery. Firstly, a nonionic surfactant, alkyl glycosides (APG), was selected to stabilize CO 2 /H 2 O emulsion, and the corresponding morphology and stability were evaluated with a transparent PVT cell. Subsequently, plugging capacity and apparent viscosity of CO 2 /H 2 O emulsion were measured systematically by a sand pack displacement apparatus connected with a 1.95-m long capillary tube. Furthermore, a high water cut (40 vol%) CO 2 /H 2 O emulsion was selected for flooding experiments in a long sand pack and a core sample, and the oil recovery, the rate of oil recovery, and the pressure gradients were analyzed. The results indicated that APG had a good performance on emulsifying and stabilizing CO 2 emulsion. An inversion from H 2 O/CO 2 emulsion to CO 2 /H 2 O emulsion with the increase in water cut was confirmed. CO 2 /H 2 O emulsions with lower water cuts presented higher apparent viscosity, while the optimal plugging capacity of CO 2 /H 2 O emulsion occurred at a certain water cut. Eventually, the displacement using CO 2 /H 2 O emulsion provided 18.98% and 13.36% additional oil recovery than that using pure CO 2 in long sand pack and core tests, respectively. This work may provide guidelines for EOR using CO 2 emulsions with high water cut.
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Haiyan Jiang,Tingting Li,Lu Bai,Jiuli Han,Xiaochun Zhang,Haifeng Dong,Shaojuan Zeng,Shuangjiang Luo,Xiangping Zhang
An efficient separation technology involving ammonia (NH3) and carbon dioxide (CO2) is of great importance for achieving low-carbon economy, environmental protection, and resource utilization. However, directly separating NH3 and CO2 for ammonia-based CO2 capture processes is still a great challenge. Herein, we propose a new strategy for selective separation of NH3 and CO2 by functional hybrid membranes that integrate polyimide (PI) and ionic liquids (ILs). The incorporated protic IL [Bim][NTf2] is confined in the interchain segment of PI, which decreases the fractional free volume and narrows the gas transport channel, benefiting the high separation selectivity of hybrid membranes. At the same time, the confined IL also provides high NH3 affinity for transport channels, promoting NH3 selective and fast transport owing to strong hydrogen bonding interaction between [Bim][NTf2] and NH3 molecules. Thus, the optimal hybrid membrane exhibits an ultrahigh NH3/CO2 ideal selectivity of up to 159 at 30 °C without sacrificing permeability, which is 60 times higher than that of the neat PI membrane and superior to the state-of-the art reported values. Moreover, the introduction of [Bim][NTf2] also reduces the permeation active energy of NH3 and reverses the hybrid membrane toward “NH3 affinity”, as understood by studying the effect of temperature. Also, NH3 molecules are much easier to transport at high temperature, showing great application potential in direct NH3/CO2 separation. Overall, this work provides a promising ultraselective membrane material for ammonia-based CO2 capture processes.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Huicong Zuo,Chunqiang Lu,Lei Jiang,Xianming Cheng,Zhiqiang Li,Yuelun Li,Danyang Li,Hua Wang,Kongzhai Li
Linz-Donawitz converter gas (LDG), an important by-product in the steel industry with CO (55–60 vol%) and CO 2 (15–20 vol%) as the main components, is usually used as fuel for heating or power generation, releasing massive of diluted CO 2 with the concentration lower than 15 % that is difficult to capture. Herein, we propose a method to produce pure H 2 via chemical looping water splitting by using LDG as reducing agent, which can easily concentrate CO 2 for capture. Fe 2 O 3 , one of the most environmentally friendly and low-cost oxides, was chosen as the oxygen carrier to perform this concept. It was found that the addition of small amounts of Ce 0.75 Zr 0.25 O 2 solid solution could strongly improve the activity of Fe 2 O 3 for CO conversion, especially at relatively low temperatures. Compared with pure Fe 2 O 3 , the CO conversion and H 2 yield were increased from 39.5 % and 0.34 mmol·g −1 to 100 % and 2.32 mmol·g −1 at 650 °C, respectively, after adding 5 wt% of Ce 0.75 Zr 0.25 O 2 . The strong interaction between the two oxides contributed to the enhanced performance via promoting CO adsorption and lattice oxygen releasing. Water splitting assisted by air oxidation could fully regenerate the reduced oxygen carrier, and the oxygen carrier was stable during the long-term chemical looping process, with the CO 2 capture rate at ca. 95.8 %. In situ DRIFTS results showed that CO 2 was produced through a direct reaction of lattice oxygen with CO, and the decomposition of carbonate species intermediate by adsorption of CO on the surface of oxygen carriers. This study gave full evidence that it was feasible for achieving H 2 generation and CO 2 capture in one step via chemical looping reforming of reducing exhaust gases (e.g., LDG) from industrial emissions.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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2023
·Vol. 120
·期 44
·e2307320120
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IF 11.1
Yangyang Yu,Ye He,Ping Yan,Shengyao Wang,Fan Dong
The selective photocatalytic conversion of CO2 and H2O to high value-added C2H4 remains a great challenge, mainly attributed to the difficulties in C–C coupling of reaction intermediates and desorption of C2H4* intermediates from the catalyst surface. These two key issues can be simultaneously overcome by alloying Ag with Cu which gives enhanced activity to both reactions. Herein, we developed a facile stepwise photodeposition strategy to load Cu–Ag alloy sub-nanoclusters (ASNCs) on TiO2 for CO2 photoreduction to produce C2H4. The optimized catalyst exhibits a record-high C2H4 formation rate (1110.6 ± 82.5 μmol g−1 h−1) with selectivity of 49.1 ± 1.9%, which is an order-of-magnitude enhancement relative to current work for C2H4 photosynthesis. The in situ FT-IR spectra combined with DFT calculations reveal the synergistic effect of Cu and Ag in Cu–Ag ASNCs, which enable an excellent C–C coupling capability like Ag and promoted C2H4* desorption property like Cu, thus advancing the selective and efficient production of C2H4. The present work provides a deeper understanding on cluster chemistry and C–C coupling mechanism for CO2 reduction on ASNCs and develops a feasible strategy for photoreduction CO2 to C2 fuels or industrial feedstocks.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Xiaohui Liu,Boyu Li,Jiaxiang Liu,Xuanting He,Huachen Liu,Shun Mao,Wenquan Tao,Zhuo Li
Membrane separation technology has been widely used in the separation and capture of CO 2 to reduce carbon emissions. The performances of facilitated hybrid membranes (FHMs) can be improved by properly adding metal-organic framework (MOF)-based nanoparticles (NPs) and modifying polymers to the polymer matrix . Grafting and blending methods are widely used to introduce modifying polymers to improve the compatibility between NPs and the polymer matrix, and the performance of FHMs for CO 2 separation. However, the separation performance of FHMs decreases significantly when the long chains of the polymer infiltrate into the pores of the MOF at the interface between the modifying polymer and MOF. To in-depth understand the nano-scale polymer-NPs interfacial interaction mechanism of the grafting and blending methods, we herein employed molecular dynamic (MD) simulation method combined with experiments to investigate the interface between NPs of Cu-MOF (Cu-BDC) and four commonly used modifying polymers (PEG, polyethylene glycol; PEI , polyethylenimine; PVA , polyvinyl alcohol; PPy, polypyrrole) with PVDF (polyvinylidene difluoride) as the polymer matrix. The results showed that the blending method for modification can effectively avoid the polymer blockage in Cu-BDC pores by using four modifying polymers, while the grafting method caused polymer infiltration for PEG and PEI. The relationship between the polymer diameter and the pore limiting diameter (PLD) of the Cu-BDC was evaluated to analyze the polymer infiltration effect. FHMs of Cu-BDC/PEG@PVDF were synthesized based on the MD simulation results, which showed excellent CO 2 separation performance due to the good compatibility between the Cu-BDC and the modified matrix polymer. This work offers an insight in nano-scale into the interface design between the MOF and the polymer for FHMs separating CO 2 .
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Materials
·
2023
·Vol. 16
·期 21
·7042
·
IF 3.4
Shuling Shen,Xuecong Pan,Jin Wang,Tongyu Bao,Xinjuan Liu,Zhihong Tang,Huixin Xiu,Jing Li
The lateral size of graphene nanosheets plays a critical role in the properties and microstructure of 3D graphene as well as their application as supports of electrocatalysts for CO2reduction reactions (CRRs). Here, graphene oxide (GO) nanosheets with different lateral sizes (1.5, 5, and 14 µm) were utilized as building blocks for 3D graphene aerogel (GA) to research the size effects of GO on the CRR performances of 3D Au/GA catalysts. It was found that GO-L (14 µm) led to the formation of GA with large pores and a low surface area and that GO-S (1.5 µm) induced the formation of GA with a thicker wall and isolated pores, which were not conducive to the mass transfer of CO2or its interaction with catalysts. Au/GA constructed with a suitable-sized GO (5 µm) exhibited a hierarchical porous network and the highest surface area and conductivity. As a result, Au/GA-M exhibited the highest Faradaic efficiency (FE) of CO (FECO= 81%) and CO/H2ratio at −0.82 V (vs. a Reversible Hydrogen Electrode (RHE)). This study indicates that for 3D GA-supported catalysts, there is a balance between the improvement of conductivity, the adsorption capacity of CO2, and the inhibition of the hydrogen evolution reaction (HER) during the CRR, which is related to the lateral size of GO.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Pengchao Zang,Jiyun Tang,Hao Zhang,Xiaozhe Wang,Peiyu Zhao,Lin Cui,Juan Chen,Pei Zhao,Yong Dong
The solid amine adsorbents are potential candidates as materials for post-combustion capture technologies. The type of organic amine and porous material are the key factors influencing the amine-based solid adsorbent performance. Furthermore, there has been relatively little research on the matching mechanism between organic amines and porous materials. This study aims to investigate the effect of the degree of matching between different organic amines and porous materials (X-5 resin) on the performance of CO 2 capture. The results indicated that 30 wt% TETA was the highest matching degree with X-5 and had the maximum CO 2 adsorption of 205.48 mg/g at 30 ℃. The matching degree between the four amines and the X-5 resin followed TETA > TEPA > PEHA > PEI. Since TETA has the simplest molecular structure, it can be conveniently dispersed in the X-5 pores, which not only significantly improves the utilization of active sites but also prevents the phenomena of agglomeration or sintering. Meanwhile, X-5-30TETA has the highest adsorption energy E ads (−85.22 kJ/mol) and the smallest spatial potential resistance, decreasing the mass transfer resistance effectively, thus further increasing the adsorption capacity. Furthermore, the adsorption kinetics results showed that the Avrami model can relatively accurately predict the experimental results of X-5-TPHI CO 2 adsorption. Finally, the in situ DRIFTS indicated that the CO 2 adsorption reaction over X-5-30TETA followed predominantly an amphipathic centipede mechanism. This work provides a new idea for the investigation of the matching mechanism between organic amines and porous materials.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yue Chen,Meigui He,Jianmin Zhang,Yiting Su,Zhe Xue,Chengze He,Yufan Ji,Kecheng Guan,Jing Zhao,Hideto Matsuyama,Wanqin Jin
Cross-linked poly(ethylene oxide) (PEO) is a highly promising membrane material for CO 2 capture, as it allows fast and selective CO 2 transport. However, the facile fabrication of an ultrathin cross-linked PEO selective layer for thin-film composite (TFC) membrane to achieve high CO 2 separation performance remains challenging. To address this issue, we reported the design of a soluble high-permeability cross-linked PEO polymer and the fabrication of it into an ultrathin CO 2 -selective layer through a simple coating technique. The as-synthesized cross-linked PEO polymer contains abundant poly(dimethylsiloxane) (PDMS) segments, leading to highly improved free volume and affinity towards CO 2 , which result in high CO 2 diffusivity, solubility, and consequently high CO 2 permeability (528 Barrer). TFC membranes with an ultrathin selective layer (∼128 nm) were successfully fabricated using the PEO polymer, leading to superior CO 2 capture performance (CO 2 permeance = 2650 GPU, CO 2 /N 2 = 20) for CO 2 /N 2 mixture separation in a long-term stability test, exceeding the target performance for carbon capture. Given their high separation performance, excellent stability, and scalable fabrication route, our PEO-based membranes hold great promise for post-combustion CO 2 capture.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yiting Xu,Xiaobo Yu,Meiling Chen,Yi Sun,Wei Zhang,Yajin Fang,Lanyun Fang,Haining Na,Fei Liu,Jin Zhu
Fabrication of multi-responsive fluorescent sensors for real-time and visual monitoring or detection is practical and challenging. Herein, a novel cellulose-based fluorescent functional material with dual-responsive properties arising from two different functional sites was successfully designed and prepared in a CO 2 switchable solvent. Cellulose was effectively dissolved in this solvent and easily functionalized by successively grafting poly (lactic acid) and 7-hydroxy-4-trifluoromethyl coumarin (HFC) onto the cellulose backbone, resulting in C- g -PLLA/HFC with good processibility and fluorescence quenching response (turn off) towards Fe 3+ due to the coordination of Fe 3+ with the carbonate linkage. Acetylation of HFC under microwave-assisted conditions gave rise to C- g -PLLA/HFC-Ac which showed fluorescence enhancement response (turn on) to various organic amines because of the removal of the acetyl group by aminolysis reaction. Therefore, they could be respectively used for selective identification and detection of Fe 3+ , and real-time, accurate and visual monitoring of aquatic product freshness. Furthermore, an interesting application for irreversible information encryption was demonstrated by combining the dual-responsive property. This study suggests a new strategy for constructing cellulose-based functional material with multiple responsiveness and applications.
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危险品化学品经营许可证（带存储）