CHEMISTRY-A EUROPEAN JOURNAL
·
2020
·Vol. 26
·期 35
·7918-7922
·
IF 4.857
Yichen Zhou,Mingmin Jia,Xiongfei Zhang,Jianfeng Yao
Graphical Filling the voids : Etched ZIF-8 (ZIF-8-E) crystals permeated by open through pores of size about 100 nm have been introduced into a polyethersulfone membrane matrix. The resulting material shows enhanced CO 2 /N 2 separation performance (see scheme). Zeolite ZIF-8 has been etched with acid to form microporous ZIF-8-E crystals. These were then introduced into a polyethersulfone (PES) membrane matrix to enhance its CO 2 /N 2 separation performance. Open through pores of size about 100 nm formed in the ZIF-8 crystals allow the ingrowth of polyethersulfone chains, ensuring a reduction in the number of nonselective voids, thereby achieving better interaction between ZIF-8-E and PES. As a result, the CO 2 /N 2 separation performance of the ZIF-8-E/PES membrane increased significantly, showing a CO 2 permeability of 15.7 Barrer and a CO 2 /N 2 ideal selectivity of 6.5.
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Hainan Shi,Saran Long,Shen Hu,Jungang Hou,Wenjun Ni,Chunshan Song,Keyan Li,Gagik G. Gurzadyan,Xinwen Guo
Two-dimensional graphitic carbon nitride (g-C 3 N 4 ) has been widely explored as a promising photocatalyst for solar CO 2 conversion. However, rapid charge recombination and low visible-light utilization are severely detrimental to photocatalytic CO 2 conversion. Zero-dimensional/two-dimensional (0D/2D) heterostructures are considered the promising materials with size tunability and enhanced charge separation efficiency for photocatalysis. Herein, a 0D/2D heterostructure of oxygen vacancy-rich TiO 2 quantum dots confined in g-C 3 N 4 nanosheets (TiO 2- x /g-C 3 N 4 ) was prepared by in-situ pyrolysis of NH 2 -MIL-125 (Ti) and melamine. Charge dynamics analysis by time-resolved photoluminescence (tr-PL) and femtosecond and nanosecond pump-probed transient absorption (TA) spectra revealed that charges transfer occured from 2D-g-C 3 N 4 to 0D-TiO 2 at an ultrafast subpicosecond time scale (<1 ps) through the intimate interface. The overall fast decay of the charge carriers was attributed to interfacial charge transfer, which was accompanied by recombination relaxation mediated by shallow trapped sites. Ultrafast interfacial charge transfer greatly promoted charge separation and electrons in shallow trapped sites were easily trapped by CO 2 . In addition, combining with the synergetic advantage of strong visible light absorption, high CO 2 adsorption and large surface area, TiO 2- x /g-C 3 N 4 exhibited a superior CO evolution rate of 77.8 μmol g −1 h −1 , roughly 5 times that of pristine g-C 3 N 4 (15.1 μmol g −1 h −1 ). This work provides in-depth insights into optimizing the heterojunction for robust solar CO 2 conversion.
✓ 已验证
DOI
高影响因子
Carbon Neutralization
·
2024
·
IF 0
Hua-Wei Guo,Ya-Jun Wang,Huan Liu,Ya-Nan Zeng,Wei-Jie Wang,Tian-Ji Liu,Le-Le Kang,Rui Ji,Yi-Tong Wang,Jun-Guo Li,Zhen Fang
Metallurgical slag such as solid waste generated in the steel industry carries environmental pollution risks, but it is rich in nutrients required by microalgae. Metallurgical slag used for carbon capture and biomass energy conversion has multiple benefits: (i) reduction and harmless treatment of metallurgical solid waste, (ii) assisting in carbon neutrality by efficient carbon fixation, and (iii) production of biodiesel from CO 2 . In this study, AOD, BOF, BFS, HVS, and VTS slag were applied to culture Chlorella pyrenoidosa ( C. pyrenoidosa ) with the regulation of growth, carbon fixation, and lipid synthesis. An excellent fixed amount of CO 2 with 94.59 mg is obtained from C. pyrenoidosa biomass at BOF slag added (mass ratio of CO 2 captured/microalgae/slag with 1.99/1.00/10.53) since high Ca/Mg mass ratio of 419 (8.38 mg/L Ca and 0.02 mg/L Mg), no Cr and low concentration of Al (0.04 mg/L) contribute to regulating antioxidant enzyme activity (SOD and POD) to resist ROS and improving PEPC activity to reduce carbon flux toward lipid to promote biomass synthesis. Both metal concentrations from Ca (5.86 mg/L), Mg (0.05 mg/L), Al (0.42 mg/L), and Cr (0.006 mg/L) and suitable pH (10.53) in AOD leaching solution at solid/liquid ratio of 0.5 g/L change carbon flow toward efficient lipid synthesis (47.07 wt%) by continuously providing raw materials and energy by regulating ACC, ME, and PEPC activities. High value-added biodiesel with high concentrations of C16 and C18 methyl esters from lipid of C. pyrenoidosa is achieved, following other ecological and economic benefits including 197 mg CO 2 captured and 2198 mg AOD applied with harmless. In this study, C. pyrenoidosa is cultured with elements from metallurgical slag solid waste, which promotes C. pyrenoidosa efficient carbon fixation to assist in carbon neutrality, and provides guidance for CO 2 conversion to high-value-added products with low cost.
✓ 已验证
DOI
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Guo-Cui Mao,Xiao-Tian Kan,Ming-Xiu Xiao,Wen-Long Liu,Bao-Xia Dong,Yun-Lei Teng
CaO is promising to be widely used to capture CO2. The produced CaCO3 can be considered as solid CO2, which is also a plentiful, convenient, and useful carbon resource. Here, for the first time, we report that an alkaline earth metal can selectively induce the hydrogenation of the CaO-captured CO2 (namely, the produced CaCO3) to CH4 under room-temperature ball-milling conditions. The effects of ball-milling conditions and different catalysts on the methanation performance were studied. The results show that the CH4 yield can reach 56.1%, and the CH4 selectivity is 100%. When adding metal Ni, the CH4 yield can be further increased. The experimental and density functional theory calculation results indicate that the in situ formed metal hydride plays a key role in the process of methanation. This work provides a novel and energy-saving method to convert the metal oxide-captured CO2/carbonate to CH4 at room temperature.
✓ 已验证
DOI
高影响因子
Journal of CO2 Utilization
·
2022
·
IF 8.321
Jiahui Li,Keyan Li,Jun Du,Hong Yang,Chunshan Song,Xinwen Guo
Incorporation of transition metals in polymeric carbon nitride (CN) is an effective strategy to enhance its photocatalytic CO 2 reduction activity, however, the difference of activity enhancement by incorporating different metals is not well understood. Herein, CN is modified with different transition metals by pyrolyzing the mixtures of urea and metal-organic frameworks (MOFs) to obtain MCN (M = Cu, Co, Ti or Fe). For each given type of metal-modified CN, the photocatalytic CO 2 reduction activity is optimized by controlling the content of MOF precursor during pyrolysis . The optimized MCN delivers significantly enhanced CO evolution rate than pure CN, in the order of CN (83 μmol g −1 h −1 ) < CuCN (246 μmol g −1 h −1 ) < CoCN ( 326 μmol g −1 h −1 ) < TiCN (454 μmol g −1 h −1 ) < FeCN (490 μmol g −1 h −1 ). It is revealed that for CuCN and CoCN, Cu and Co are doped in CN. In contrast, for TiCN and FeCN, Ti and Fe exist as TiO 2 and Fe 2 O 3 forming Z-scheme heterojunctions with CN. The progressively improved photocatalytic activity corresponds to the increased specific surface area , CO 2 adsorption capacity, visible light absorption as well as charge separation and transfer efficiency. Furthermore, we design and prepare bimetal incorporated CN through combining metal doping with heterojunction construction strategies, i.e., Cu doped CN/TiO 2 and Co doped CN/Fe 2 O 3 , which exhibit further enhanced CO 2 photoreduction performance with CO evolution rates of 613 and 718 μmol g −1 h −1 , respectively. This work provides insight into the design and preparation of highly efficient CN-based photocatalytic materials.
✓ 已验证
DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2021
·
IF 9.811
Xiangyang Yao,Kaihong Chen,Li-Qi Qiu,Zhi-Wen Yang,Liang-Nian He
Visible light-induced photocatalytic CO2 reduction reaction (CO2RR) is a feasible and promising option to tackle the greenhouse effect and energy crisis. Herein, two ferric porphyrin-based porous organic polymer semiconductors, hereafter referred to as POPn-Fe (porous organic polymers, n = 1 or 2, corresponding to a benzene/biphenyl unit as a linker between porphyrin units), are synthesized for the visible light-driven CO2RR to produce syngas. The CO/H2 evolution rates for POP2-Fe under irradiation >420 nm are found to successfully reach up to 3043 and 3753 μmol g–1 h–1, respectively. Interestingly, the experiment results imply that the ferric porphyrin site could be responsible for CO evolution and the uncoordinated porphyrin unit in POPn or POPn-Fe semiconductors may be obligate for H2 formation. Furthermore, as evidenced by Mott–Schottky plots, the extended π-conjugation with the biphenyl linker makes POP2-Fe a lower conduction band potential, which helps the ferric porphyrin sites capture electrons from the photosensitizer, thus producing more CO to realize selectivity control. Also, the efficient catalytic activity of POP2-Fe is presumably attributed to the accelerated charge transfer as well as facilitates photogenerated electron and hole separation. This work offers an elegant strategy to design and optimize earth-abundant metal visible light photocatalysis for CO2 reduction to syngas with CO/H2 ratio control.
✓ 已验证
DOI
高影响因子
HIGH PERFORMANCE POLYMERS
·
2022
·
IF 1.73
Shuo Yan,Haibin Yu,Zan Chen
Membranes with both good permeation and selectivity are highly desired for gas separations. In this study, we synthesized a new 6FDA-type polyimide copolymer 6FDA-BDTA-ODA, and then an organic polymer of poly (N-vinylimidazole) was doped into the polyimide to prepare mixed matrix membranes (MMMs). We also studied the effect of poly (N-vinylimidazole) contents on the separation performance of MMMs. The results showed that the ideal selectivity for CO2/CH4 was improved by adding the poly (N-vinylimidazole) filler. The ideal selectivity reached 63.5 with 6 wt% poly (N-vinylimidazole) loading with the permeability of 29.2 Barrer. The highly permeable MMMs showed a considerably enhanced performance for CO2/CH4 that close to the 2008 Robeson upper-bound. The gas separation performance of the prepared MMMs for CO2/CH4 was improved compared to that of the pure polymer membrane, indicating that the copolyimide/poly (N-vinylimidazole) MMMs have promising applications in CO2/CH4 gas separation.
✓ 已验证
DOI
高影响因子
CARBOHYDRATE POLYMERS
·
2018
·
IF 5.158
Xiang Li,Qinqin Xu,Hongwei Shen,Yuanlong Guo,Mouyi Wu,Ya Peng,Lihua Zhang,Zongbao Kent Zhao,Yu Liu,Haibo Xie
To overcome the natural recalcitrance of cellulose for glucose production in aqueous media catalyzed by enzyme, in this study, a dissolution pretreatment strategy was developed by using in situ formed CO 2 -based reversible ionic compounds (RICs)/DMSO mixed organic electrolytes under mild conditions. The influences of the constitution of RICs, CO 2 pressure, dissolution pretreatment time on the physic-chemical structure of cellulose were investigated systematically by FTIR, XRD, SEM, AFM towards in-depth understanding of the correlations between the pretreatment conditions, micro-scale structure and enzymatic saccharification of cellulose. The results showed that the tetramethyl guanidine (TMG) based RICs solvent system [TMGH] 2 + [O 2 COCH 2 CH 2 OCO 2 ] 2− /DMSO (X RICs = 0.1, X RICs : the mole fraction of the formed RICs in the mixture) presented the best performance, which was evidenced by 100% glucose yield after the dissolution-regeneration pretreatment strategy under mild conditions (T = 60 °C, Pco 2 = 2.0 MPa, t = 2 h). Furthermore, the solvent system have good recyclability and usability.
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2021
·
IF 8.742
Nan Li,Zhi Wang,Jixiao Wang
Developing efficient membrane technology for CO 2 capture has aroused wide interest for environment conservation and emission reduction. Developing facilitated transport membranes is a potential strategy for improving CO 2 permeance and CO 2 /N 2 selectivity synchronously, based on the reversible reactions among carriers and CO 2 molecules. The reaction activity can be optimized by tuning the carrier mobility due to the enhanced water-swelling capacity. Here, thin-film composite (TFC) membranes containing water-swelling carboxymethyl chitosan (CMC) chains were prepared via interfacial polymerization process, aiming to improve CO 2 separation performance. As-prepared TFC membranes with different CMC loading have exhibited different Turing nanostructures , such as corrugated structures, octopus-branched structures and nodular structures. Water can enhance the activity of carriers in reversible reaction for facilitated transport membranes. TFC membranes with CMC have exhibited the enhanced water-swelling capacity, showing high CO 2 permeance of 1278 GPU together with CO 2 /N 2 selectivity of 89. This work put forward a simple and effective method to tune the membrane structure and enhance the facilitated transport.
✓ 已验证
DOI
高影响因子
Polymer Chemistry
·
2024
·Vol. 15
·期 27
·2780-2789
·
IF 4.1
Ke Wang,Zilong Wang,Meiyu Si,Xiaofang Liu,Guiyan Liu,Yongfei Zeng
Three novel temperature/pH/CO2-triple-responsive homopolymers namely P(Et-N-EO2MA), P(THP-N-EO2MA) and P(Ph-N-EO2MA) were prepared by reversible addition–fragmentation chain transfer (RAFT) polymerization. They have the same backbone structure but different types of end substituents i.e., ethyl, tetrahydropyran, and the benzene ring, respectively. Subsequently, their responsive properties were studied. P(Et-N-EO2MA) has a lower critical solution temperature (LCST)-type cloud point (CP) in aqueous solution and is affected by many factors such as the molecular structure and weight, concentration, additives, pH and CO2. P(THP-N-EO2MA) is soluble in water, but in different buffer solutions, it shows a soluble–LCST–insoluble transition, and its LCST-type CP can also be adjusted by molecular weight and concentration. P(Ph-N-EO2MA) is insoluble in water, but reversible phase transformation can be achieved by adjusting the pH of the solution or injecting CO2, and it also shows different properties in buffer solutions and an upper critical solution temperature (UCST)-type CP in n-butanol. In addition, since P(Ph-N-EO2MA) is amphiphilic, it can be self-assembled in solution, and the release of Nile Red (NR) can be achieved under the stimulation of acid. The different properties of these homopolymers show the effect of substituents on the responsiveness of multistimuli-responsive polymers, which provides ideas for the design of stimuli-responsive polymers, and have good application prospects in the fields of self-assembly and controlled release.
✓ 已验证
DOI
高影响因子
NANO
·
2024
·
IF 1
Xuecong Ma,Linlin Geng,Yu Li,Jianwen Wei,Lei Liao,Dunqiu Wang
Micro/mesoporous materials are low-cost functional materials with the potential for CO 2 adsorption. Modifying micro/mesoporous materials is significant for enhancing CO 2 adsorption and their high-value utilization. Herein, the micro/mesoporous material of composite molecular sieve ZSM-5/MCM-48 (ZM) was synthesized by a two-step crystallization method using cetyltrimethylammonium bromide as a template, tetraethyl orthosilicate as a silicon source and ZSM-5 seed as part of silicon aluminum source. Tetraethylenepentamine (TEPA) and polyethyleneimine (PEI) were used as impregnation modifiers to modify ZM with amine groups. The results showed that with the increase of amine loadings, both ZM-T60 (Impregnated with TEPA) and ZM-P60 (Impregnated with PEI) functionalized adsorbents exhibited the best adsorption capacities of 4 . 9 7 mmol ⋅ g − 1 and 3 . 2 8 mmol ⋅ g − 1 at 60, respectively, when the loading of ZM sample was 60%. The adsorption kinetic analysis showed that the adsorption of CO 2 by ZM-T60 and ZM-P60 was a chemisorption-dominated process accompanied by physical adsorption. After 10 adsorption/desorption cycles, the CO 2 adsorption capacity of ZM-T60 and ZM-P60 decreased by 8.7% and 2.6%, respectively. This work demonstrates that impregnation modification of the composite molecular sieve to achieve efficient CO 2 adsorption has practical application significance.
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 14
·21267-21278
·
IF 0
Zhao Dongling,Geng Linlin,Jia Yanfei,Wei Jianwen,Zhou Xiaobin,Liao Lei
High-temperature solid adsorbent Li 4 SiO 4 has received broad attention due to its high theoretical adsorption capacity, high regeneration capacity, and wide range of raw materials for preparation. In this paper, a Li 4 SiO 4 adsorbent was prepared by MCM-48 as the silica precursor and modified by doping with metal ions (Ca 2+ and Na + ) for high-temperature capture of low-concentration CO 2 . The results showed that the surface of the Ca-doped (or Na-doped) Li 4 SiO 4 adsorbent developed some particles that are primarily composed by Li 2 CaSiO 4 (or Li 3 NaSiO 4 ). Furthermore, the grains of the adsorbents became finer, effectively increasing the specific surface area and enhancing adsorption performance. Under 15 vol% CO 2 , the maximum CO 2 adsorption was 25.63 wt% and 32.86 wt% when the Ca 2+ doping amount was 0.06 and the Na + doping amount was 0.12, respectively. These values were both higher than the adsorption capacity before the metal ion doping. After 10 adsorption/desorption cycles, the adsorption capacity of Na-doped Li 4 SiO 4 increased by 9.68 wt%, while that of Ca-doped Li 4 SiO 4 decreased by 7.98 wt%. This difference could be attributed to the easy sintering of the Ca-containing adsorbent. Furthermore, a biexponential model was used to fit the CO 2 adsorption curve of the adsorbent in order to study the adsorption kinetics. Compared to the conventional Li 4 SiO 4 , the Ca/Na-doped adsorbent offers several advantages, such as a high CO 2 adsorption capacity and stable cycling ability.
✓ 已验证
DOI
危险品化学品经营许可证（带存储）