MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Meng Rong,Liangrong Yang,Chao Yang,Jiemiao Yu,Huizhou Liu
Herein, a new tetraphenyladamantane-cored triazine-based multiamine (TPADT) was designed and synthesized. Its bulky molecular volume, strong rigidity, and high amine functionality enable it easy to prop up the polymer backbone and form a high hypercrosslinking degree to obtain high microporosity. A series of highly microporous tetraphenyladamantane-based polyaminals (Ad-MALPs) were prepared through the catalyst-free copolymerization of TPADT and commercial aromatic aldehydes. By changing the strut length and functionality of aldehyde monomers , the resulting polymers exhibit tailored BET surface area (1541–1779 m 2 /g) and narrow ultramicropore size distribution (0.52–0.93 nm). Ad-MALP-2 with the largest microporosity possesses the highest CO 2 uptake (21.1 wt %, 273 K/1.0 bar) and CO 2 /N 2 adsorption selectivity (35.2). Interestingly, Ad-MALP-3 shows the highest H 2 uptake (2.26 wt%, 77 K/1.0 bar) due to larger total pore volume . In addition, highly microporous Ad-MALPs simultaneously contain aromatic and cycloaliphatic components, and thus show exceptionally large aromatic and cycloaliphatic organic vapor adsorption capacity under low pressure. At P/P 0 = 0.1, the benzene and cyclohexane vapor uptakes of Ad-MALPs are up to 44.8 wt% and 39.0 wt %, far exceeding that of most previously reported porous organic polymers . Considering that Ad-MALPs have outstanding gas adsorption performance, simple preparation, good stability, and cycle ability, they are expected to be promising adsorbent materials for CO 2 adsorption/separation, H 2 storage and low-concentration volatile organic vapors capture.
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Tianqinji Qi,Weizuo Li,Hong Li,Ke Ji,Shaoyun Chen,Yongchun Zhang
Revealing the origin of the enhanced performance on yttria (Y 2 O 3 ) promoted Cu/ZnO based catalyst for methanol synthesis via CO 2 hydrogenation is still challenging. To shed light upon the promotion effect of Y 2 O 3 modifier on binary Cu/ZnO catalyst for CO 2 hydrogenation reaction, a ternary Cu/ZnO/Y 2 O 3 catalyst was synthesized via a citric acid coordination-assisted strategy. The developed Cu/ZnO/Y 2 O 3 catalyst exhibited a remarkably higher Weight-time yeild of methanol (236.8 g MeOH g cat −1 ∙ h − 1 ) and methanol selectivity (81.1%) in comparison to Cu/ZnO catalyst (159.6 g MeOH g cat −1 ∙ h − 1 and 73.9%, respectively). Various characterizations results have uncovered the enhanced catalytic activity of Cu/ZnO/Y 2 O 3 catalyst for methanol synthesis was associated with small size and highly dispersed Cu species and abundant surface adsorption sites as well as more Cu-ZnO interfaces with strong interaction. Moreover, the Cu/ZnO/Y 2 O 3 catalyst displayed a superior weight-time yield of methanol with a time-on-stream of 100 h in comparison with classic Cu/ZnO catalyst. We anticipate that this basic design strategy will provide a novel alternative to expand opportunities to explore scalable, cost-effective catalysts for industrial methanol synthesis.
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2020
·
IF 3.421
Cui-Ping Ye,Rui-Nan Wang,Xia Gao,Wen-Ying Li
To screen the efficient media for CO2 capture of flue gas from power plants, a strategy for improving the CO2 capture capacity by dual functionalized ionic liquids (ILs) with multiple active sites is proposed. Three phosphonium dual functionalized ILs ([aP4443][2-Np], [aP4443][2-Op], and [aP4443][Triz]) have been prepared. The sorption capacities of the synthesized ILs under pure CO2 atmosphere and the supported ILs under different loading amounts from 10 to 50%, temperatures of 30–80 °C, and CO2 partial pressure varied from 10 to 15% were determined. Fourier transform infrared (FTIR) spectroscopy was applied to reveal the interaction between CO2 and ILs, and the pseudo-second-order model and the intraparticle diffusion model were used for a better understanding of the CO2 adsorption behavior. The results showed that a high capacity up to 1.88 mol of CO2/mol of IL for [aP4443][2-Np] is achieved, and 30% IL–MCM-41 can reach 3.19 mmol/g with excellent reversibility under the atmosphere of CO2:N2 (15%:85%) at 30 °C and 0.1 MPa. Raising the temperature or decreasing the CO2 concentration is not conducive to improving the CO2 capacity. FTIR spectroscopy demonstrated that the amino and hydroxyl react with CO2 to form NHCOO– or CO3–. Combined with the activation energy calculation, the kinetic analysis revealed that the CO2 capture of supported ILs is an internal diffusion controlled physical adsorption.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2020
·
IF 7.216
Hui Ning,Dianliang Guo,Xiaoshan Wang,Zhonghao Tan,Wenhang Wang,Zhongxue Yang,Linqing Li,Qingshan Zhao,Jian Hao,Mingbo Wu
Developing of economic and efficient catalysts is critical for the application of electroreduction of carbon dioxide to highly valuable chemicals. Herein, we present a facile method to synthesize N-doped hieratically porous carbon through pyrolysis of petroleum pitch followed by ammonia etching. We found mesopores are favored formation by removing of asphaltene from petroleum pitch during the carbonation process. Simultaneously, ammonia etching can not only increase the pyridinic-N content, but also upgrade the ratio of meso- to micro- pores of carbon materials. Using the N-doped hieratically porous carbon as catalyst for carbon dioxide electroreduction, the Faradaic efficiency of carbon monoxide reaches 83% at −0.9 V vs. the reversible hydrogen electrode (RHE) in 0.1 M KHCO 3 . This superior performance is attributed to the synergistic effects of highly pyridinic-N content in conjunction with the hieratically porous architecture, rendering abundant exposed and accessible active sites for electroreduction of CO 2 . Our work provides a new strategy for the large-scale preparation of high-performance, low-cost catalysts for CO 2 electroreduction.
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 30
·期 39
·2002092
·
IF 16.836
Facai Wei,Tingting Wang,Xiaolin Jiang,Yan Ai,Anyang Cui,Jing Cui,Jianwei Fu,Jiangong Cheng,Lecheng Lei,Yang Hou,Shaohua Liu
Currently, the precise control of the architecture and surface of functional materials for high-performance still remains a great challenge. Here, a feasible approach is presented to synchronously manipulate mesoporous surface and dimensionality of SnO 2 catalysts into hierarchically mesoporous nanosheets and nanospheres within one simple reaction system. By adjustment of the hydrophobic chain length of different fluorinated surfactants, 0D SnO 2 nanospheres with average size of 165 nm, and 2D SnO 2 ulthrathin nanosheets with thickness of 22.5 nm with the distinct dimensionalities are separately obtained (one stone, two birds), both of which are well decorated with ordered mesopore arrays on their surfaces (pore size of 16 nm). The following calcination gave rise to the formation of hierarchically mesopores (5 and 16 nm, respectively) with high crystallization and improved surface area (96.8 m 2 g −1 ). The resultant mesoporous SnO 2 nanosheets as catalyst for CO 2 electroreduction reaction (CO 2 RR) exhibit excellent selectivity, with a high Faraday efficiency (FE) of HCOOH reaching up to 90.0% at −1.3 V and C 1 FE of 97.4% at −1.2 V versus reversible hydrogen electrode, as well as long-term stability, which is among the best performance compared to reported SnO 2 materials, thanks to the collective contributions of the unique architecture and mesoporous structure.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Ge Xie,Nuoya Zhou,Yujie Gao,Shuo Du,Hongyao Du,Juan Tao,Lianbin Zhang,Jintao Zhu
Acceleration of skin wound healing is an important aspect of wound treatment. The use of carbon dioxide (CO 2 ) has been recognized as one of the most effective ways to improve microcirculation and to benefit wound healing, while the need of the specialized equipment and the uncontrollable delivery of gas CO 2 might restrict such strategy in wide applications. Herein, we develop a photothermal hydrogel for the on-demand and localized delivery of CO 2 to accelerate skin wound healing by combining thermoresponsive block copolymer (BCP) of Pluronic F127 and carbon nanoparticles (CNPs) with amino groups, which can be used for loading CO 2 precursor of bicarbonate for controlled release. We show that by rationally optimizing the content of the thermoresponsive BCP in the photothermal hydrogel, a liquid-to-solid transition triggered by the body temperature can be achieved. Under light irradiation, the CNPs can convert light into heat, triggering the decomposition of the bicarbonate, and the photothermal hydrogel can thus locally release CO 2 in the wound site. Wound healing can be accelerated by improving local microcirculation disturbance and increasing tissue oxygen concentration. This study provides a new opportunity for local CO 2 supplement for accelerating wound healing.
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2020
·
IF 2.627
Bo-Yun Liu,Min-Jie Chen,Liang Yang,Bo Zhao,Tao Xia,Gang-Gang Chang
The engineering of highly efficient and stable heterogeneous catalysts for catalytic conversion of CO 2 to high value-added products is highly desirable but presents a great challenge. Herein, we reported the synthesis of a series of multifunctional IL@H-Zn/Co-ZIF composite catalysts with a unique porous hollow capsule structure and encapsulated amino-functionalized ionic liquids (ILs). The unique hollow capsule structure of IL@H-Zn/Co-ZIF provides sufficient space for loading active ILs ([C 2 NH 2 Mim + ][Br − ]) and fast mass transfer of substrate molecules during catalysis. Furthermore, the microporous Zn-ZIF shell can effectively avoid the leaching of active ILs. Benefiting from the unique hollow structure, the resultant IL@H-Zn/Co-ZIF demonstrated excellent catalytic performance (>95% yield), and good recyclability (still remained about 90% activities after 5 cycles) when applied in the CO 2 cycloaddition reaction under solvent and co-catalyst free conditions.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Xuandong Wang,Jie He,Liang Mao,Xiaoyan Cai,Chuanzhi Sun,Mingshan Zhu
Photocatalytic CO 2 conversion to valuable fossil fuels has been demonstrated to be a promising approach to reduce emissions of CO 2 and produce renewable energy, which primarily depends on developing the high efficiency of charge separation photocatalysts. Herein, CsPbBr 3 , one typical kind of all-inorganic perovskite nanocrystal, is immobilized on monolayer MoS 2 nanosheets to construct a new and ideal CsPbBr 3 /MoS 2 photocatalyst in the application of CO 2 photoreduction. In comparison with pure CsPbBr 3 , CsPbBr 3 /MoS 2 heterostructures possessed a specific electric field to more efficiently separate charges and generated more active sites for facilitating CO 2 activation, resulting in 3.0 and 2.4 times yields for CO 2 photoreduction to CH 4 and CO, respectively. Detailed characterization methods such as photoluminescence, surface photovoltage spectroscopy and theory calculations indicate the vivid illustrations of photogenerated carries separation which contributes to improving photocatalytic CO 2 conversion efficiency. The present investigation is anticipated to provide a new way for fabricating highly efficient perovskite-based photocatalyst in solar-energy-driven applications.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Ke Guo,Xiaoli Zhu,Lianlian Peng,Yanghe Fu,Rui Ma,Xinqing Lu,Fumin Zhang,Weidong Zhu,Maohong Fan
The conversion of CO 2 into valuable chemicals utilizing solar energy is one of the most promising approaches to solve the problems associated with global warming and energy shortage. Considering more and more covalent organic frameworks (COFs) that have been reported, the great potential of COFs as photocatalysts for CO 2 reduction is still appreciated to a limited extent. In the current work, Ru nanoparticles (NPs) loaded ketoamine-based COF (TpPa-1) catalysts, named Ru/TpPa-1, were developed for the photocatalytic reduction of CO 2 upon visible-light irradiation for the first time. Compared with TpPa-1, Ru/TpPa-1 catalysts exhibit a significantly enhanced activity for the photoreduction of CO 2 . In combination with the results from some extensive characterizations, it is found that the interactions between the Ru NPs and TpPa-1 can enhance the visible-light harvesting and create a new way to extend the service life of photo-generated charge carriers via facilitating the electron transfer through the loaded Ru NPs. The current investigation, therefore, provides a photocatalytic approach for CO 2 fixation, enriches the theory of photocatalysis, and enlarges the application of COF-based materials.
✓ 已验证
产品关联
DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2020
·Vol. 132
·期 1
·417-429
·
IF 1.52
Xie Qi,Miao Changxi,Lei Tianqi,Hua Weiming,Yue Yinghong,Gao Zi
Dehydrogenation of ethane assisted by CO 2 has been investigated over Au catalyst supported on Y-doped CeO 2 nanorod. The catalysts were characterized by XRD, TEM, N 2 adsorption, XPS, TG, H 2 -TPR and Raman spectroscopy. Enhanced activity can be obtained after the proper Y doping. The optimal catalyst Au/Ce 0.9 Y 0.1 exhibits an ethane conversion of 20.9% and nearly 100% selectivity to ethylene without any evident tendency of deactivation in 50 h. The reducibility of surface oxygen species is found to play a key role in the dehydrogenation assisted by CO 2 , which can be improved by proper Y doping into CeO 2 nanorod. The promoting effect of CO 2 on activity is evident over Au/Ce 0.9 Y 0.1 catalyst, due to the quick transformation of H 2 product into H 2 O by the reverse water gas shift reaction. The catalyst stability is also improved by the addition of CO 2 , attributed to the elimination of coke by Bouduoard reaction.
✓ 已验证
产品关联
DOI
高影响因子
ENERGY
·
2020
·
IF 6.082
Rujie Wang,Shanshan Liu,Qiangwei Li,Shihan Zhang,Lidong Wang,Shanlong An
Blended amine solvents are considered potential alternatives to monoethanolamine for CO 2 capture, for the fast absorption kinetics of primary/secondary amine and low regeneration penalty of tertiary amine. In this research, blended amine solvents comprising N,N-dimethylcyclohexylamine (DMCA) and N-methylcyclohexyamine (MCA) were proposed. CO 2 absorption increased the polarity of the products and ensured the absorbent remained homogenous throughout the absorption/desorption cycles. Through quantum chemical calculation, the low stability of MCA-carbamate was confirmed by a ΔΔG 3 value of −6.41 kcal/mol, and a possible reaction route from carbamate to bicarbonate was revealed. Thus, the CO 2 capacity of DMCA-MCA reached 0.875–0.985 mol CO 2 /mol amine. Moreover, MCA exhibited considerably low forward energy barrier for zwitterion formation (2.7 kcal/mol), and the CO 2 absorption of DMCA could be accelerated through the proton transfer reaction with the MCA-zwitterion. Accordingly, the total mass transfer coefficient of CO 2 in DMCA-MCA approached 2.02 × 10 −10 mol/cm 2 s Pa, which was 1.2-fold higher than that of 5 M MEA. The total regeneration energy of DMCA-MCA blend was estimated at 2.20 GJ/t CO 2 , which was 44.9% lower than 5 M MEA. This study developed a novel DMCA-MCA blended solvent with rapid absorption rate, huge CO 2 capacity and efficient regeneration for CO 2 capture.
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Tingting Zhai,Caihong Wang,Fengjuan Gu,Zi-hui Meng,Wenfang Liu,Yanzi Wang
Enzymatic conversion of CO2 to high-value chemicals is a green route of resource reutilization, which is limited by low solubility of CO2 in mild conditions. Here, silica microspheres were first modified by the co-deposition of polyethyleneimine (PEI) and dopamine and the resultant polydopamine (PDA)/PEI-SiO2 was then used as the strengthening material of the enzymatic conversion of CO2 to formate. The initial reaction rate increased from 13.4 to 27.2 times with the loading amount of PDA/PEI-SiO2 increasing from 0.1 to 0.4 g. Following that, PDA/PEI-SiO2 was used as the carrier for the immobilization of carbonic anhydrase (CA). As a result of synergism, the formate synthesis was accelerated up to 48.6 times with a low loading amount of 0.2 g of PDA/PEI-SiO2-CA. Although the promoting effect of PDA/PEI-SiO2 retained only 56.1% after being used once, PDA/PEI-SiO2-CA retained 95.1% activity after 10 cycles of use. It was presumed that CA boosted the impact and reusability of PDA/PEI-SiO2 by improving CO2 desorption. This work is much significant in providing a simple and high-efficiency strategy for process intensification of enzymatic CO2 conversion.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）