CATALYSIS TODAY
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2024
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IF 5.2
Ruiqi Wu,Ning Liu,Chengna Dai,Gangqiang Yu,Ruinian Xu,Biaohua Chen
The propane oxidation dehydrogenation assisted by CO 2 (CO 2 -ODHP) is currently a hot research topic, not only to meet growing demand of propylene but also to favor the CO 2 neutralization. In present work, a series of CrO x @S1-n-1.0 with different Cr contents (n= 2.2, 3.6 and 4.5 wt%) is synthesized based on a small gas molecule directing synthesis strategy, wherein the gaseous CO of 1.0 MPa was in situ introduced in the synthesis system to regulate the interaction and dispersion of CrO x over silicalite-1 (S1) support. The characterization results of XRD , XPS , H 2 -TPR, and Raman indicate that the CO can affect the oxidation state and dispersion of Cr species. As observed, the Cr species were highly dispersed over CrO x @S1–3.6 %-1.0 (in the form of Cr 6+ valance state), which however would aggregate to generate Cr 2 O 3 nanoparticles over the CrO x @S1–3.6 %-0 a prepared by impregnation method in absence of CO. The activity measurement indicates that the CrO x @S1–3.6 %-1.0 possesses the highest activity by displaying an average propane conversion of 50.4 % and CO 2 conversion of 23.6 % at 600 °C, which surpasses most of the literature reports. The CO 2 -ODHP reaction mechanism was further investigated by in situ DRIFTS , which indicates that dissociated H of propane can react with CO 2 to form formate (-COOH), in turn further reacts with H to produce byproducts CO and H 2 O, and the formate species can also react with the CrO 3 active site to form bicarbonate species (HCO - 3 ). Generally, present work has proposed a small gas molecule directing strategy to adjust the dispersions and chemical states of the loaded guest meals over catalytic support. The study of present work would contribute to other highly efficient catalyst design .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Ming Chen,Huan Liu,Ying Wang,Zhiyong Zhong,Yu Zeng,Yuxin Jin,Daiqi Ye,Limin Chen
TiO 2 , ZrO 2 and a series of TiO 2 -ZrO 2 (TxZ1, x means the atomic ratio of Ti/Zr = 10, 5, 1, 0.2 and 0.1) composite oxide supports were prepared through co-precipitation, and then 3 wt% Co was loaded through wetness impregnation methods. The obtained 3 wt% Co/TiO 2 (3CT), 3 wt% Co/ZrO 2 (3CZ) and 3 wt% Co/TxZ1 (3CTxZ1) catalysts were evaluated for the oxidative ethane dehydrogenation reaction with CO 2 (CO 2 -ODHE) as a soft oxidant. 3CT1Z1 catalyst exhibits excellent catalytic properties, with C 2 H 4 yield, C 2 H 6 conversion and CO 2 conversion about 24.5 %, 33.8 % and 18.0 % at 650 °C, respectively. X-Ray Diffraction (XRD), in-situ Raman, UV–vis diffuse reflectance spectra (UV–vis DRS), H 2 temperature-programmed reduction (H 2 -TPR), Electron paramagnetic resonance (EPR) and quasi in-situ X-ray Photoelectron Spectroscopy (XPS) have been utilized to thoroughly characterize the investigated catalysts. The results revealed that 3CT1Z1 produced TiZrO 4 solid solution with more metal defect sites and oxygen vacancies (Ov), promoting the formation of Co 2+ -TiZrO 4 structure. Furthermore, the presence of Ov and Ti 3+ can facilitate the high dispersion and stabilization of Co 2+ , as well as suppressing the severe reduction of Co 2+ , leading to superior ethane oxidative dehydrogenation activity. Besides, less Co 0 is beneficial to ODHE reaction, because of its promotion effects for reverse water gas shift reaction ; however, more Co 0 results in dry reforming reaction (DRE). This work will shed new lights for the design and preparation of highly efficient catalysts for ethylene production.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
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IF 14.7
Zheng Zhe,Wang Yong-Sheng,Wang Miao,Zhao Guo-Hua,Hao Guang-Ping,Lu An-Hui
Removal of confined space carbon dioxide (CO 2 ) that is in low concentration and with coexisting water is necessary but challenging by physical adsorption method. To make the removal process effective, rendering the nanopore surface hydrophobic to resist water is the popular way. Instead of preventing water from occupying the nanopores, in this work, we propose to utilize the guest water for the spatially selective formation of local surface bound water and further induce the preferential CO 2 capture. We observe an anomalous enhancement of CO 2 capture performance under humid conditions over carbon nanopores with spatially selective polar sites. It is evidenced that the surface bound water is formed at non-CO 2 -selective areas of polar carbon nanopores, thus creating additional CO 2 trapping sites. This work may inspire the design of environment tolerable materials for molecular separation and purification under harsh conditions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yifei Ye,Yuanyuan Cui,Li Yang,Jiaxu Zhang,Jianmin Sun
A novel external-skeleton B-containing ionic liquid modified SBA-15 catalyst BBN-Imi-SBA-15-I (BBN denotes borabicyclo[3.3.1]nonane, Imi represents imidazolium ionic liquid) was successfully constructed by a post-modification method for efficiently catalyzing CO 2 -epoxide coupling reaction under both metal- and solvent-free conditions. 5BBN-Imi-SBA-15-I (5 refers to the molar ratio of Si to B), thanks to its synergistic effects of Lewis acid, weak base sites from tertiary amine and quaternary ammonium, hydrogen bond group and nucleophilic group, displayed good catalytic activity with 97 % product yield and 99 % selectivity at 100 °C, 2 MPa in the absence of cocatalyst. The obtained catalyst demonstrated good recyclability during six consecutive catalytic runs, also presented generality for various mono-substitute epoxides. Through in-situ NH 3 diffuse reflectance infrared Fourier transform spectroscopy (NH 3 -DRIFTS) characterization, the Lewis acidity of organo-boron was verified. Besides, kinetics research also proved the positive effect of multiple active components on efficient catalysis under milder conditions over SiO 2 -based metal-free catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Qiang Liu,Zizi Zhang,Xiang Zhang,Junling Chen,Hongwu Ma,Leizhi Zheng,Keliang Wu,Yanlong Tai
The capture and conversion of CO 2 are crucial for achieving carbon reduction targets. Currently, porous carbon is regarded as the most promising material for CO 2 capture, but it is limited by the lack of effective catalytic conversion functional sites. Frustrated Lewis Pairs (FLPs) are considered the most promising metal-free catalysts for CO 2 conversion, but homogeneous catalytic systems fall short of meeting industrial demands. To address this, this paper selected zeolitic imidazolate frameworks (ZIF-8 and ZIF-67) derived N-doped porous carbon (ZIF-8-C and ZIF-67-C) as Lewis base and subsequently introduces B(C 6 F 5 ) 3 to construct B/N-based FLPs, namely ZIF-8-C-FLPs and ZIF-67-C-FLPs. This approach aimed to simultaneously enhance the catalytic conversion ability of porous carbon towards CO 2 and the heterogenization of FLPs. These ZIF-8-C-FLPs and ZIF-67-C-FLPs exhibited exceptional CO 2 capture capacity, with CO 2 adsorption capacities of 57.4 and 41.2 cm 3 /g at 273.15 K and 1 bar, respectively. Additionally, ZIF-8-C-FLPs and ZIF-67-C-FLPs were utilized to catalyze the preparation of benzimidazole and benzoxazole from o-phenylenediamine and o-aminophenol with CO 2 , demonstrating excellent catalytic performance (yields above 86 %) and recyclability (at least 8 cycles).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Lianlong Zhan,Wei Lu,Qin Xiang,Zhiping Chen,Wenlu Luo,Cailin Xu,Renting Huang,Shuagnfei Wang,Hui He
Using biomass for the production of low-energy regenerative carbon capture materials represents an effective strategy to advance carbon dioxide capture and storage technologies. In this study, a low-energy regenerative bagasse-based CO 2 capture material is synthesized through a one-step, rapid crosslinking strategy. In this method, epichlorohydrin is used to crosslink bagasse with temperature sensitive Pluronic® F-127 and polyethyleneimine, thereby addressing the challenge of simultaneously incorporating multiple functional groups into the biomass matrix. The resulting material with abundant amino adsorption sites demonstrates a high adsorption capacity of 4.52 mmol/g. Interestingly, the temperature-sensitive response of the material facilitates the grafted amine chain segments on bagasse to stretch and shrink reversibly within a narrow temperature range of 25 °C for adsorption and 55 °C for desorption. The shrinkage state is conducive to the CO 2 desorption process, resulting in an ultralow regeneration temperature of 55 °C. Additionally, the water contained in the material enhances its cyclic stability in extreme environments, such as pure CO 2 atmosphere at high temperature. Overall, this research not only provides new ideas for enhancing the long-term stability and economic viability of CO 2 capture materials but also offers feasible solutions for combating climate change and promoting sustainable development.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2016
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IF 2.567
Wei He,Fan Zhang,Zhi Wang,Wei Sun,Zhiyong Zhou,Zhongqi Ren
Carbon capture and sequestration (CCS) has become an increasingly important technology for environmental protection and resource utilization. In this work, four task-specific ionic liquids (TSILs), NH2-functionalized IL and three ether-functionalized ILs, were synthesized for CO2 absorption. CO2 absorption experiments of these task-specific ionic liquids (TSILs) showed that the absorption performance of NH2-functionalized IL was higher than that of ether-functionalized ILs. The recycling experiments of CO2 absorption demonstrated a good reusability of synthesized TSILs for CO2 absorption. Supported ionic liquid membranes (SILMs) with synthesized TSILs were prepared, and the CO2/CH4 and CO2/N2 separation performance of SILMs was examined. Results indicated that the SILMs with ether-functionalized ILs have slightly lower permeability but much higher selectivity (up to 9.7) than the SILMs with NH2-functionalized IL. Poly(RTIL)-RTIL composite membranes were prepared using ether-functionalized ILs. The effect of cross-linking monomer content and nonpolymerizable IL (“free” IL) content in poly(RTIL)-RTIL membranes on the CO2/CH4 and CO2/N2 separation performance was investigated. The composite membranes have higher gas permeability with little or no sacrifice in selectivity compared with SILMs. The stability evaluation and comparison of the SILMs and poly(RTIL)-RTIL membranes were conducted, the results of which verified the stronger structural stability of the poly(RTIL)-RTIL membranes. This suggests the potential of poly(RTIL)-RTIL membranes in future CO2-selective membrane separation.
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TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
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2016
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IF 1.34
Ya-hui YANG,Ren-rui XIE,Hang LI,Can-jun LIU,Wen-hua LIU,Fa-qi ZHAN
A novel WO 3– x /TiO 2 film as photoanode was synthesized for photoelectrocatalytic (PEC) reduction of CO 2 into formic acid (HCOOH). The films prepared by doctor blade method were characterized with X-ray diffractometer (XRD), scanning electron microscope (SEM) and transmission electron microscope (TEM). The existence of oxygen vacancies in the WO 3– x was confirmed with an X-ray photoelectron spectroscopy (XPS), and the accurate oxygen index was determined by a modified potentiometric titrimetry method. After 3 h of photoelectrocatalytic reduction, the formic acid yield of the WO 3– x /TiO 2 film is 872 nmol/cm 2 , which is 1.83 times that of the WO 3 /TiO 2 film. The results of PEC performance demonstrate that the introduction of WO 3– x nanoparticles can improve the charge transfer performance so as to enhance the performance of PEC reduction of CO 2 into formic acid.
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JOURNAL OF APPLIED POLYMER SCIENCE
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2016
·Vol. 134
·期 5
·
IF 1.866
Xianwu Jing,Hongsheng Lu,Baogang Wang,Zhiyu Huang
A triblock copolymer, containing a polyethylene glycol (PEG) block and two symmetrical poly(2-(dimethylamino)ethyl methacrylate) (PDM) blocks, was synthesized by using PEG-based macroinitiator with copper-mediated living radical polymerization. The conductivity tests showed that the copolymer exhibited switchable responsiveness to CO 2 , i.e., a relatively high conductivity of solution can be switched on and off by bubbling and removing of CO 2 . According to the nuclear magnetic resonance results, the CO 2 -switchable conductivity variation could be attributed to protonation and deprotonation of tertiary amine groups in PDM blocks. Moreover, at a proper weight concentration 0.5%, the copolymer aqueous solution displayed a CO 2 -switchable viscosity variation. Scanning electron microscopy, cryogenic transmission electron microscopy, and dynamic light scattering characterization jointly demonstrated that the viscosity variation was the result of a CO 2 -switchable vesicle-network aggregate structure transition. This structure transition can actually be attributed to a hairpin-line molecular configuration conversion in terms of the reasonable mechanism discussion. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134 , 44417.
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Science China-Chemistry
·
2016
·Vol. 59
·期 11
·1369-1375
·
IF 2.429
Liu Shunjie,Qin Yusheng,Guo Hongchen,Wang Xianhong,Wang Fosong
Synthesis of polyols from carbon dioxide (CO 2 ) is attractive from the viewpoint of sustainable development of polyurethane industry; it is also interesting to adjust the structure of the CO 2 -polyols for versatile requirement of polyurethane. However, when renewable malonic acid was used as a starter, the copolymerization reaction of CO 2 and propylene oxide (PO) was uncontrollable, since it proceeded slowly (13 h) and produced 40.4 wt% of byproduct propylene carbonate (PC) with a low productivity of 0.34 kg/g. A careful analysis disclosed that the acid value of the copolymerization medium was the key factor for controlling the copolymerization reaction. Therefore, a preactivation approach was developed to dramatically reduce the acid value to ~0.6 mg(KOH)/g by homopolymerization of PO into oligo-ether-diol under the initiation of malonic acid, which ensured the controllable copolymerization, where the copolymerization time could be shortened by 77% from 13 to 3 h, the PC content was reduced by 76% from 40.4 wt% to 9.4 wt%, and the productivity increased by 61% from 0.34 to 0.55 kg/g. Moreover, by means of preactivation approach, the molecular weight as well as the carbonate unit content in the CO 2 -diol was also controllable.
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JOURNAL OF CHEMICAL THERMODYNAMICS
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2016
·
IF 2.196
Dong Fu,LeMeng Wang,ChenLu Mi,Pan Zhang
The absorption capacity of CO 2 in piperazine (PZ) promoted 2-diethylaminoethanol (DEAE) aqueous solution was measured. The viscosities of both CO 2 -unloaded and CO 2 -loaded PZ-DEAE aqueous solutions were measured and then modelled. The temperatures ranged from 303.2 K to 323.2 K. The mass fraction of PZ and DEAE respectively ranged from 0 to 0.075 and 0.3 to 0.5. The temperature and concentration dependences of absorption capacity were determined. The effects of temperature, mass fraction and CO 2 loading on viscosities are demonstrated.
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Journal of CO2 Utilization
·
2016
·
IF 4.764
Xiying Fu,Dagang Zhou,Kai Wang,Huanwang Jing
Pd/C was found to be an excellent catalyst in the coupling reaction of carbon dioxide and epoxides with tetrabutylammonium iodide (TBAI) as cocatalyst and the corresponding cyclic carbonates were obtained in good yields and high selectivities. 3-Chloropropylene carbonate was synthesized under extremely mild conditions of room temperature and atmosphere. The proposed mechanism was also calculated and confirmed by DFT. The palladium catalyst could be simply recycled and reused for 5 times without significant loss of activity.
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