ADSORPTION SCIENCE & TECHNOLOGY
·
2022
·
IF 4.373
Zhijuan Zhang,Pengwei Li,Ting Zhao,Yuanhan Xia
The ZIF-8 crystals were successfully postsynthetically modified using methylamine (MA), ethylenediamine (ED), and N, N-dimethylethylenediamine (MMEN) to improve their adsorption performance toward CO2. Results showed that, compared with the original ZIF-8, the BET specific surface area of MA-ZIF-8, MMEN-ZIF-8, and ED-ZIF-8 has increased by 118.2%, 92.0%, and 29.8%, respectively. In addition, their total pore volume increased separately by 130.8%, 100%, and 48.7%. The adsorption capacities of CO2 on the amine-modified ZIF-8 samples followed the order . The CO2 adsorption capacities at 298 K on MA-ZIF-8, MMEN-ZIF-8, and ED-ZIF-8 were increased by 118.2%, 90.2%, and 29.8%, respectively. What is more, the CO2/N2 selectivities calculated using an IAST model of the amine@ZIF-8 samples at 0.01 bar and 298 K were also significantly improved and followed the order , which increased by 173.0%, 121.4%, and 22.6%, respectively. The isosteric heat of CO2 adsorption () on the MA-ZIF-8, MMEN-ZIF-8, and ED-ZIF-8 all becomes higher, while of N2 on these samples was slightly lower in comparison with that on the ZIF-8. Furthermore, after six recycle runs of gravimetric CO2 adsorption-desorption on MA-ZIF-8, the adsorption performance of CO2 is still very good, indicating that the MA-ZIF-8 sample has good regeneration performance and can be applied into industrial CO2 adsorption and separation.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Wenqian Yang,Ziqian Xue,Jun Yang,Jiahui Xian,Qinglin Liu,Yanan Fan,Kai Zheng,Peiqin Liao,Hui Su,Qinghua Liu,Guangqin Li,Cheng-Yong Su
The selective electrochemical reduction of CO 2 to CO is a promising solution for the design of carbon-neutral, sustainable processes. Achieving a highly selective single reduction product is still challenging because of the energetically favorable competing hydrogen evolution reaction. We report the fabrication of N-doped sponge-like porous graphitic carbon structures embedded with Fe nanoparticles (Fe@NPC) via the pre-modification of a metal-organic framework (IRMOF-3(Zn)) with carboxyferrocene, followed by pyrolysis . The as-prepared Fe@NPC exhibited a 96.4% CO Faradaic efficiency at –0.5 V RHE and good stability. The exceptional CO 2 reduction performance is attributed to the unique structure of the composite catalyst, which provides abundant hierarchical pores that increase CO 2 adsorption and mass transfer, and active Fe sites that synergistically accelerate the kinetics of CO generation. The in situ attenuated total reflectance-Fourier transform infrared analysis provided proof of the improved ability of Fe@NPC to accumulate the crucial intermediate *COOH compared with other pyrolyzed porous carbons. Fe@NPC was used in a Zn-CO 2 battery that delivered a maximum power density of 3.0 mW cm –2 , evidencing its potential for application in energy-converting devices.
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Yining Wu,Qixin Liu,Dayu Liu,Xiao Peng Cao,Bin Yuan,Mingwei Zhao
Considerable research efforts have been devoted to finding and developing the oil locked within low-permeability reservoirs. The oil-rock interaction exacerbated in tiny pores and heterogeneities in formation epitomize the challenges accompanying the development of low-permeability reservoirs. CO 2 flooding has become a promising treatment to increase displacement efficiency and formation energy for enhanced oil recovery. Nevertheless, due to the mismatch in the viscosity of CO 2 with that of the crude oil and the intrinsic heterogeneity of the reservoir, gas channeling is inevitable, resulting in low oil recovery and low CO 2 storage efficiency. This paper is motivated to fabricate CO 2 intelligent responsive hydrogel that exhibits a delayed swelling: the hydrogel will uptake water and swell when encountering CO 2 or H + , to strengthen the plugging capacity for the gas channeling. A two-step method was used to prepare CO 2 responsive (CR) hydrogel which has good injection performance and can form gel in-situ to control the gas channeling in low-permeability reservoirs. To achieve the above functions, CR polymer with acrylamide (AM) and N-[3-(Dimethylamino) propyl] methacrylamide (DMAPMA) was synthesized by aqueous free-radical copolymerization. CR hydrogel was prepared by crosslinking CR polymer with polyethyleneimine (PEI). Then 1.2 wt% CR polymer and 0.2 ∼ 0.4 wt% PEI were determined as the optimal synthetic formulation of CR hydrogel which is capable of maintaining stability at 80 ℃ for more than 30 days without dehydration. The gelation time was more than 24 h indicating that the CR hydrogel has good injection and in-depth migration ability. Also, the swelling behaviors of CR hydrogel were studied, and the hydrogel can expand more than 10 times in acidic conditions (pH ∼ 4.5) with respect to about 2 times in neutral conditions (pH ∼ 7). The expansion mechanism is further revealed and proved to be feasible for CO 2 channeling control.
研究领域:
化学工程
·
材料科学
·
石油工程
✓ 已验证
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Wang Mengjun,Jia Jun,Xia Jing,Peng Chun-Kuo,He Jinxin,Qiu Yueming,He Yuting,Gao Le,Xue Fei,Lin Yan-Gu,Zhan Guowu,Guo Yuzheng,Huang Xiaoqing,Xu Yong
Carbon dioxide (CO 2 ) conversion to liquid fuels has attracted great attention due to the current environmental concerns and energy crisis. However, the selective conversion of CO 2 to target liquids is formidably challenging due to the chemical inertness of CO 2 . We theoretically and experimentally confirm that the bending of Pd−Pd bond can breaks the asymmetric potential well and facilitate CO 2 adsorption. We have successfully synthesized a new class of Pd nanoneedles via a “close edges and open corners” process, with a magic angle of 60 o between the main trunk and branch, and realized the selective CO 2 hydrogenation to formic acid (HCOOH) at room temperature in water. Impressively, a HCOOH productivity of ~250 mmol g −1 in 100 h while maintaining HCOOH selectivity over 99%. This work bridges nanostructure design and catalytic application, which may open a new avenue for selective CO 2 conversion in an elegant manner.
研究领域:
催化
·
纳米技术
·
环境化学
·
能量转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yongxiao Tuo,Wanli Liu,Qing Lu,Xingzhao Wang,Jiabing Luo,Shutao Wang,Yan Zhou,Min Wang,Xiaohui Sun,Xiang Feng,Mingbo Wu,De Chen,Jun Zhang
The most difficulty of efficient CO 2 electroreduction lies in the activation step that turns CO 2 into the CO 2 − radicals or other intermediates that can be further converted. To overcome this bottleneck, many efforts have been devoted to develop electrocatalysts to lower the overpotential of CO 2 activation, but they inevitably involve complicated or/and unscalable synthesis methods. Here we reported that the SO 4 2− ion modified metal foils, including Zn, Ag, Au and Cu, demonstrated ∼6.5, 1.4, 14 and 2.5 times of CO faradaic efficiency in K 2 SO 4 electrolyte compared to KHCO 3 electrolyte at −1.05 V vs. RHE. According to both experimental and DFT studies, the electron-rich metal-SO 4 adlayer can activate CO 2 by bending the linear molecule of CO 2 through donating electrons to the antibonding orbital of CO 2 , thus facilitating the formation of key intermediate *CO 2 − . Moreover, the adsorption of H + on metal sites is restrained by the metal-SO 4 adlayer, leading to a suppressed H 2 evolution activity. From a broader perspective, many catalysts can benefit from this approach to achieve more efficient CO 2 electrochemical reduction.
研究领域:
材料科学
·
电化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of CO2 Utilization
·
2018
·
IF 5.503
Zhengfeng Huang,Peimei Dong,Yanzhao Zhang,Xiaoxiao Nie,Xiya Wang,Xiwen Zhang
A strategy of coupling a photocatalyst with a high CO 2 adsorption capacity material was proposed in order to integrate CO 2 capture and photoreduction processes into a single system. TiO 2 and ZIF-8 were selected for their high photoactivity and CO 2 adsorption capacity respectively. We employed a facile in-situ growth strategy to inlay ZIF-8 into the TiO 2 film grid. X-ray diffraction and scanning electron microscopy revealed that ZIF-8 was successfully prepared and inlaid into the TiO 2 film. X-ray photoelectron spectroscopy and photoluminescence spectra suggested that the TiO 2 and ZIF-8 were coupled by chemical bonding. The ZIF-8 decorated TiO 2 film exhibited excellent CO 2 capture capacity and showed remarkably enhanced yield for reducing CO 2 to CO and CH 4 when compared with pure TiO 2 film. The probable mechanism of the photoreduction process is also discussed.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 34
·16566-16573
·
IF 9.931
Danke Chen,Wensen Wang,Wen Ying,Yi Guo,Donghui Meng,Youguo Yan,Rongxin Yan,Xinsheng Peng
The modern global climate change and global warming of Earth make it an urgent need to develop emerging CO2 capture and storage techniques. Herein, we first reported the use of WS2 nanosheets to construct laminated membranes for CO2 separation. However, the WS2 membrane showed poor CO2 separation performance with Knudsen selectivities for N2/CO2 (1.28), CH4/CO2 (1.72) and H2/CO2 (4.96). To improve the performance, an ionic liquid (IL) 1-butyl-3-methyl imidazolium tetrafluoroborate ([BMIM][BF4]) with high CO2 solubility and practically no vapour pressure was used for filling the nanochannels of the WS2 membrane. Compared to the bulk IL, the nanoconfined IL exhibits higher freezing temperature, shift of vibration bands and higher interaction energy between CO2 and ILs. Besides, the prepared WS2 laminated membrane with the nanoconfined ionic liquid shows excellent selectivities for CO2/N2 (153.21), CO2/CH4 (68.81) and CO2/H2 (13.56) in single gas measurements as well as good CO2 permeance due to the nanoconfinement of the IL. The simulation results further confirmed and explained the CO2 separation mechanism. It indicates that the nanoconfinement of ILs into the nanochannels of two-dimensional materials is a novel way to achieve CO2-philic membranes to efficiently separate CO2 from other light gases.
研究领域:
材料科学
·
环境工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Membranes
·
2021
·Vol. 11
·期 2
·118
·
IF 4.106
Chunwei Zhang,Menglong Sheng,Yaoqiang Hu,Ye Yuan,Yulong Kang,Xiao Sun,Tao Wang,Qinghua Li,Xisen Zhao,Zhi Wang
CO2enhanced oil recovery (CO2-EOR) technology is a competitive strategy to improve oil field economic returns and reduce greenhouse gas emissions. However, the arbitrary emissions or combustion of the associated gas, which mainly consists of CO2and CH4, will cause the aggravation of the greenhouse effect and a huge waste of resources. In this paper, the high-performance facilitated transport multilayer composite membrane for CO2/CH4separation was prepared by individually adjusting the membrane structure of each layer. The effect of test conditions on the CO2/CH4separation performance was systematically investigated. The membrane exhibits high CO2permeance of 3.451 × 10−7mol·m−2·s−1·Pa−1and CO2/CH4selectivity of 62 at 298 K and 0.15 MPa feed gas pressure. The cost analysis was investigated by simulating the two-stage system. When the recovery rate and purity of CH4are 98%, the minimum specific cost of separating CO2/CH4(45/55 vol%) can be reduced to 0.046$·Nm−3CH4. The excellent short-to-mid-term stability indicates the great potential of large industrial application in the CH4recovery and CO2reinjection from oilfield associated gas.Keywords:oilfield associated gas;CO2capture;multilayer composite membrane;facilitated transport;CO2/CH4separation
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Hong-Nan Chen,Yi-Fei Sun,Ming-Long Wang,Jin-Rong Zhong,Dan Rao,Chang-Yu Sun,Guang-Jin Chen
CO 2 hydrate provides an important alternative solution for CO 2 geological sequestration. However, fingering flow of liquid CO 2 and hydrate membrane effect can severely restrict flowing CO 2 conversion to hydrate. Here we report an enhanced CO 2 hydrate sequestration method via CO 2 -H 2 O emulsion injection, and its effectiveness has been proven in a three-dimensional system. Compared to liquid injection, emulsion injection demonstrated higher displacement efficiency of pore water and larger sweep area, finally increasing CO 2 sequestration density by 142 %. The highly dispersed CO 2 micro-droplets significantly increase CO 2 -H 2 O contact capability and weakens the hydrate membrane effect, thereby greatly increasing the rate and quantity of hydrate conversion. For different water contents, the highest CO 2 sequestration density of 148 kg/m 3 is achieved at 40 % water content, with hydrated CO 2 accounting for 71.45 %. The excellent performance of CO 2 -H 2 O emulsion provides a green and high-efficient approach to CO 2 hydrate sequestration.
研究领域:
环境科学
·
地质学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2022
·
IF 4.654
Xianhang Jin,Enze Ren,Yun Yang
Nonaqueous absorbents for CO2 capture have attracted great attention in research institutes recently because of their many advantages, such as energy efficiency and noncorrosiveness. Novel nonaqueous single-phase and biphasic absorbents have been developed. In this work, to satisfy application requirements, the effects of solvents on nonaqueous absorbents’ phase separation behavior and CO2 solubility were clarified. The nonaqueous absorbents comprising MEA and 26 kinds of solvents were investigated. The phase separation behavior after CO2 absorption, CO2 solubility, and CO2 cyclic capacity of nonaqueous absorbents were studied. The solvent polarity parameter ET(30) and the dielectric constant of solvents mainly affected the phase separation behavior and CO2 solubility of nonaqueous absorbents, respectively. The nonaqueous absorbent comprising a solvent with an ET(30) value larger than 50 kcal/mol maintained a single phase after CO2 absorption. The CO2 solubility of nonaqueous absorbents had a good positive relation with the dielectric constant of solvents. Moreover, nonaqueous absorbents comprising ethylene glycol monoethyl ether exhibited the optimal CO2 cyclic capacity and heat of CO2 absorption. In comparison to 30% MEA/H2O, the CO2 cyclic capacity of the nonaqueous absorbent increased by 51.8%, and the heat of CO2 absorption decreased by 35.4%.
研究领域:
化学工程
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy Materials
·
2024
·
IF 24.4
Xiecheng Yang,Dantong Zhang,Lanqing Zhao,Chao Peng,Kun Ren,Changfan Xu,Pan Liu,Yingjie Zhou,Yong Lei,Bin Yang,Dongfeng Xue,Feng Liang
Rechargeable Na-CO 2 batteries are considered to be an effective way to address the energy crisis and greenhouse effect due to their dual functions of CO 2 fixation/utilization and energy storage. However, the insolubility and irreversibility of solid discharge products lead to poor discharge capacity and poor cycle performance. Herein, a novel strategy is proposed to enhance the electrochemical performance of hybrid Na-CO 2 batteries, using water-in-salt electrolyte (WiSE) to establish an optimal reaction environment, regulate the CO 2 reduction pathway, and ultimately convert the discharge product of the battery from Na 2 CO 3 to formic acid (HCOOH). This strategy effectively resolves the issue of poor reversibility, allowing the battery to exhibit excellent cycle performance (over 1200 cycles at 30 °C), especially under low-temperature conditions (2534 cycles at −20 °C). Furthermore, density functional theory (DFT) calculations and experiments indicate that by adjusting the relative concentration of H/O atoms at the electrolyte/catalyst interface, the CO 2 reduction pathway in the battery can be regulated, thus effectively enhancing CO 2 capture capability and consequently achieving an ultra-high discharge specific capacity of 148.1 mAh cm −2 . This work effectively promotes the practical application of hybrid Na-CO 2 batteries and shall provide a guidance for converting CO 2 into products with high-value-added chemicals.
研究领域:
能源存储
·
电化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xuebi Du,Shichao Feng,Jianquan Luo,Yongbing Zhuang,Weijie Song,Xuewei Li,Yinhua Wan
Amine-functionalized and metal doped metal–organic frameworks (MOFs) will enable further enhancement of CO 2 adsorption, which holds great promise in mixed matrix membranes (MMMs) for CO 2 /N 2 separation. Four kinds of UiO66 with different sizes have been successfully fabricated by introduction of Ce and/or amino groups in UiO66. The influence of Ce doping on the UiO66 is greatly related to the ligand. Compared with ZrUiO66, the CeZrUiO66 has bigger particle size, lower BET specific surface area and pore volume and a worse CO 2 adsorption capacity. Interestingly, the tendency of Ce-doped ZrUiO66-NH 2 is contrary to the aforementioned. In particular, bimetallic CeZrUiO66-NH 2 has an ultramicroporous structure, small particle size, rich crystal defect, superb CO 2 capture capacity and high CO 2 /N 2 adsorption selectivity, suggesting that the simultaneous introduction of Ce and amino groups is conducive to the enhancement of CO 2 separation. The intrinsic ultramicroporous structure of CeZrUiO66-NH 2 not only offers fast and low resistance transport channels for CO 2 , but also supplies more sites for CO 2 adsorption owning to the doping of Ce and the amino groups. As a result, Pebax/CeZrUiO66-NH 2 (3 wt%) MMMs show the CO 2 permeability of 100.7 Barrer and the CO 2 /N 2 ideal selectivity of 76.4, which is close to Robeson upper bound from 2008. Meanwhile, the Pebax/CeZrUiO66-NH 2 (3 wt%) MMMs present relatively good pressure resistance, which would be advantageous in terms of industrial application.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子