SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yonghong Wang,Zhuo Jin,Xinru Zhang,Jinping Li
The incorporation of lamellar materials into polymer matrix can improve the gas separation performance of mixed matrix membranes (MMMs), which have great potential in chemical separation process. However, few intrinsic selectivity sites on MoS 2 sheets suppress further employment in the membrane separation. In this work, the vacancies and defects-containing MoS 2 sheets were prepared by high temperature oxidation and hydrothermal reaction in NaOH solution, and then L-cysteine-functionalized MoS 2 (Cys-MoS 2 ) was synthesized by a thiol-click chemistry reaction between S vacancies and thiol groups as confirmed by transmission electron microscope (TEM), Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and N 2 absorption. After blending with polyether-block-amide (Pebax), the as-prepared MMMs showed outstanding mechanical properties as a result of the homogeneous dispersion of Cys-MoS 2 and hydrogen bonding between two phases as evidenced by attenuated total reflectance-FTIR, scanning electron microscope (SEM), thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). The highest permeability of 297 Barrer accompanied with a CO 2 /N 2 selectivity of 120 was obtained for MMMs loaded with 1.5 wt% Cys-MoS 2 , which were enhanced by 206.2 % and 124.7 % over the pristine Pebax membrane, respectively. Meanwhile, this value was superior to that of the previously reported Pebax-based MMMs, transcending 2019 upper bound. The enhanced gas separation performance is due to the improved CO 2 adsorption selectivity by the vacancies and defects of Cys-MoS 2 , while the amine groups carrier enhanced CO 2 reactivity selectivity.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Xueyan Chen,Shuo Hu,Xiaoxiao Qin,Min Chen,Jianghao Zhang,Xiaolei Bao,Changbin Zhang
Ag-based catalysts have been extensively investigated in HCHO oxidation on account of the low price of the Ag precursor and their considerable low-temperature activity. It is known that H2 pretreatment has a remarkable promotion effect on Pt- and Pd- catalysts for HCHO oxidation, whereas the effect of H2 reduction on Ag-based catalysts has been rarely reported, probably due to the coexistence of multiple states of Ag species resulting from the high Ag loading. Herein, we prepared a 1% Ag/Al2O3 (Ag/Al-fresh) catalyst with Ag species in a uniform state and then reduced Ag/Al-fresh with H2 at 600 °C to obtain the Ag/Al-600H2 catalyst. We observed that H2 reduction had a significant influence on the performance of Ag/Al2O3 nanocatalysts in HCHO oxidation. In a dry reaction atmosphere, Ag/Al-fresh and Ag/Al-600H2 exhibited comparable HCHO conversion levels, but Ag/Al-600H2 showed much higher CO2 selectivity than Ag/Al-fresh. The presence of water vapor severely suppressed the HCHO conversion of the Ag/Al-fresh catalyst, while Ag/Al-600H2 showed high water resistance, maintaining high HCHO conversion and CO2 selectivity at 35% RH. Characterization results showed that the Ag species on Ag/Al-fresh and Ag/Al-600H2 were single-atom cationic Ag and metallic Ag nanoparticles, respectively. It was revealed that the Ag0 nanoparticles were more conducive than single-atom Ag+ to formate decomposition, as well as O2 and H2O activation, thus accelerating the conversion of HCOO– and CO intermediates to CO2 and contributing to the higher activity and water resistance of the Ag/Al-600H2 catalyst.
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Changzhen Wang,Hao Wu,Xiangyu Jie,Xiaoming Zhang,Yongxiang Zhao,Benzhen Yao,Tiancun Xiao
Well-geometric-confined yolk–shell catalysts can act as nanoreactors that are of benefit for the antisintering of metals and resistance to coke formation in high-temperature reactions such as the CO2 reforming of methane. Notwithstanding the credible advances of core/yolk–shell catalysts, the enlarged shell diffusion effects that occur under high space velocity can deactivate the catalysts and hence pose a hurdle for the potential application of these types of catalysts. Here, we demonstrated the importance of the shell thickness and porosity of small-sized Ni@SiO2 nanoreactor catalysts, which can vary the diffusional paths/rates of the diffusants that directly affect the catalytic activity. The nanoreactor with an ∼4.5 nm shell thickness and rich pores performed the best in tolerating the shell diffusion effects, and importantly, no catalytic deactivation was observed. We further proposed a shell diffusion effect scheme by modifying the Weisz–Prater and blocker model and found that the “gas wall/hard blocker” formed on the openings of the shell pores can cause reversible/irreversible interruption of the shell mass transfer and thus temporarily/permanently deactivate the nanoreactor catalysts. This work highlights the shell diffusion effects, apart from the metal sintering and coke formation, as an important factor that are ascribed to the deactivation of a nanoreactor catalyst.
研究领域:
化学工程
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材料科学
·
催化反应
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Ruiming Fang,Zhongqing Yang,Zukhra C. Kadirova,Ziqiang He,Ziqi Wang,Jingyu Ran,Li Zhang
The visible-light photocatalytic reduction of CO 2 becomes a vital breakthrough to alleviate the greenhouse effect and achieve carbon neutrality. In this paper, ultrathin g-C 3 N 4 nanosheets of 1.74 nm were constructed, and K + was successfully doped between layers. The yields of CO and CH 4 are 1.65 μmol·g −1 ·h −1 and 0.15 μmol·g −1 ·h −1 , which are 4.70 and 7.27 times higher than the original g-C 3 N 4 , respectively. The ultra-thin nano-lamellar structure shortens the carrier transmission distance, and the intercalation of K + not only promotes the electron transport between g-C 3 N 4 layers but also changes the original hybrid mode of the catalytic system, thus shortening the band gap and adjusting the energy band structure. In addition, the CO 2 adsorption center of the K + intercalated g-C 3 N 4 is transferred from the coordinated carbon atom to the center of the triazine unit, and the binding energy is obviously increased, which strengthens the CO 2 adsorption. Finally, through in-situ DRIFT characterization, it is speculated that the reaction enhancement mechanism is that the modified catalyst promotes the adsorption and activation of CO 2 , resulting in the production of more intermediates, especially more hydrocarbon intermediates, which is more conducive to the photocatalytic reduction of CO 2 .
研究领域:
材料科学
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环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Xiaoqi Zhu,Lin Chen,Qisheng Fang,Jianli Cheng,Yuefeng Su,Paula Ratajczak,Francois Beguin,Bin Wang
Li-CO2 batteries with attractive characteristics of high energy density power supply and carbon dioxide fixation have attracted widespread attention. However, the lack of suitable cathode catalysts and their unsatisfactory electrochemical performance have impeded their development as promising Li-CO2 batteries for energy storage. Constructing heterojunctions by interfacial engineering to improve performance is considered one of the effective strategies. Herein, heterostructured CuCo2S4-Co9S8 nanosheets are fabricated by a facile hydrothermal method and employed as efficient cathode catalysts for Li-CO2 batteries. The construction of heterojunctions by interfacial engineering has proved as an effective strategy to enhance the electrochemical performance of the Li-CO2 batteries. The delocalized electrons between CuCo2S4 and Co9S8 contribute to a low median charge potential (∼3.6 V), small polarization (0.62 V), high energy efficiency of up to 83%, and outstanding cycle life (480 h) of the CuCo2S4-Co9S8 cathodes. Meanwhile, as a proof of concept, flexible fiber-shaped Li-CO2 batteries based on these cathodes are fabricated and demonstrate boosted flexibility adaptability and provide a stable power supply at various bending conditions.
研究领域:
材料科学
·
电化学
·
能源存储
·
纳米技术
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Peng Wei,Kaidi Guo,Yahong Xie,Xueli Huang
CO2 foams are of great importance in oil recovery but challenging in some aspects like long-term stabilization and time-separated conflict. In this work, a stability-enhanced switchable foam was fabricated using bis-(2-hydroxyethoxy) olefine amine (BOA) and trace amounts (0.05 wt %) of cationic-modified cellulose nanofibers (CCNFs). The CCNF was developed using sequentially functionalized CNF with diamine groups, which were essential to promote the aqueous dispersibility and a key for strengthening the stabilization of foam. The combination of similarly charged CCNFs and BOA in the presence of CO2 contributed to both surface activity and viscoelasticity. It was demonstrated that CCNFs were entangled and stacked to form the compact films and possessed the ability to costabilize the lamellae, as observed by microscopic studies. In addition, the intermolecular H-bonds were promoted in the binary system after being protonated by CO2 and thus balancing the electrostatic forces, as explored by spectroscopy characterizations. The soft fibrous structure of the CCNF was also capable of wrapping gas bubbles in the form of a functional membrane with both low gas permeability and high surface potential, which slowed down the coarsening and coalescence. Of particular interest is that the reversible protonation state of CCNF-BOA complexes upon the alternate treatment with CO2/N2 led to reversible fast foaming/defoaming, which would be beneficial to construct the steerable plugging in the sand pack. This work is expected to provide a new direction and application of the CO2 responsive foam stabilized by similarly charged nanocellulose fibers in oilfield development.
研究领域:
石油工程
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材料科学
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化学工程
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 8
·3604-3623
·
IF 3.5
Wang Xintong,Yang Jiang,Chen Xu,Wang Yefei,Yang Zhen,Ding Wei
To mitigate CO 2 corrosion in the oil and gas industry, a green non-toxic β -N-butyl amino propionic acid (BAA) was synthesized using a low-energy and zero-waste one-pot method. The effectiveness of BAA as a corrosion inhibitor for N80 steel in CO 2 -saturated brine water was investigated through experimental measurements and theoretical modeling. The results demonstrate that BAA functions as an effective mixed-type corrosion inhibitor. BAA molecules interact with F (1 1 0) with the–COO– and–NH 2 + -moiety in the hydrophilic head group, and the hydrophobic groups are adsorbed on the steel surface in a configuration 45° away from the steel surface. The adsorption is a mixture of physical and chemical processes and is consistent with the Langmuir isothermal adsorption formula. When the concentration is greater than 50 ppm, a complete corrosion inhibitor film with high hydrophobicity can be adsorbed on the steel surface, which can effectively impede the diffusion of corrosive species from brine to the steel surface. Graphical abstract
研究领域:
腐蚀科学
·
材料工程
·
环境化学
·
石油天然气工业
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2022
·
IF 4.654
Shichun Liu,Mingwei Zhao,Yining Wu,Zhibin Gao,Caili Dai,Peng Liu
In order to further increase the temperature and shear resistance of a conventional CO2-sensitive clean fracturing fluid, a novel silica nanoparticle-reinforced CO2-sensitive fracturing fluid system was developed. The system was prepared with the compositions of 2.0 wt % N-[3-(dimethylamino) propyl] oleamide, 1.5 wt % sodium p-toluene sulfonate (NaPts), and 0.025 wt % silica nanoparticles. The rheological properties, temperature resistance, shear resistance, sand-carrying capacity, gel-breaking property, and core damage property of the system were systematically studied and evaluated. Compared with the conventional CO2-sensitive fracturing fluid system, the silica nanoparticle-reinforced CO2-sensitive fracturing fluid system has a better viscosity increase effect, and the zero-shear viscosity increases from 2900 to 3500 mPa·s. By adding and removing CO2, the viscosity of the system can be repeatedly converted from high to low, and the reusable property can be realized. After introducing silica nanoparticles, the temperature resistance ability of the clean fracturing fluid increases from 100 to 130 °C, the sand-carrying effect increases by 23%, rapid and thorough gel breaking occurs, and core damage is less than 13%. We expect that this study can broaden the application of the CO2-sensitive clean fracturing fluid in low permeability, high-temperature reservoirs and provide a theoretical basis for field applications.
研究领域:
石油工程
·
材料科学
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Kai Ma,Yao Luo,Jietao Wang,Xu Chang,Tong Liu,Yao Wang,Mingyue Ding
Developing robust fuel electrodes with high catalytic activity and stability under CO/CO 2 atmospheres is critical for reversible solid oxide fuel cells (RSOFCs). Here, we report a novel A-site-deficient perovskite Sr 1.95 Fe 1.5 Mo 0.3 Ni 0.2 F 0.1 O 6-δ (SFMNF) synthesized via electrospinning, combining Ni 2+ (B-site cation) and F - (anion) co-doping to enhance CO 2 electrolysis and syngas oxidation performance. Physicochemical characterization reveals that F-doping lowers the crystallization temperature, increases oxygen vacancy concentration, and strengthens CO 2 chemisorption. Reduction under H 2 induces exsolution of Ni 3 Fe alloy nanoparticles. The SFMNF electrode achieves a current density of 233 mA cm -2 at 1.3 V and 750°C in CO:CO 2 =2:1 atmosphere, with 36.2% higher activity than the pre-reduced state. Electrochemical impedance and distribution of relaxation time analyses identify CO 2 adsorption/dissociation as the rate-limiting step. The cell demonstrates exceptional durability over 50 redox cycles and 85-hour of operation without carbon deposition. This work highlights dual doping as an effective strategy to tailor perovskite properties for efficient CO 2 utilization in RSOFCs.
研究领域:
能源材料
·
电化学
·
催化
·
纳米技术
·
固体氧化物燃料电池
·
CO2利用
✓ 已验证
DOI
高影响因子
RARE METALS
·
2024
·Vol. 43
·期 4
·1513-1523
·
IF 9.6
Zhang Ze-Yu,Wang Hai-Bin,Zhang Fei-Fei,Li Jing-Wei,Hu Xin-Zhuo,Yan Si-Wei,Bai Yi-Ming,Zhang Xun,Shen Gu-Rong,Yin Peng-Fei,Yang Jing,Dong Cun-Ku,Mao Jing,Liu Hui,Du Xi-Wen
Electrocatalysis of CO 2 reduction reaction is an effective way to convert CO 2 into high value-added products, but the selectivity of Cu-based catalysts for C 2+ products needs to be improved due to the high energy barrier of C–C coupling. Therefore, a viable catalyst design strategy to decrease energy barrier of C–C coupling should be put forward. Here, a nanocavity-enriched CuPd single atom alloy (CuPd SAA) catalyst is designed to promote C–C coupling process. The faradaic efficiency of CuPd SAA for ethylene and C 2+ reaches 75.6% and 85.7% at − 0.7 V versus reversible hydrogen electrode (RHE), respectively. Based on the results given by in situ characterization, the porous hollow structure dramatically increases the ratio of the linear-bond *CO, thus enhancing the faradaic efficiency for ethylene. Density functional theory (DFT) calculation reveals that the Pd doping can regulate the electronic structure of neighboring Cu atoms to decrease the energy barrier of C–C coupling, further improving the faradaic efficiency. This work provides a new idea for designing catalyst with high selectivity for ethylene. Graphical abstract
研究领域:
材料科学
·
化学
·
电化学
·
催化
✓ 已验证
DOI
高影响因子
Processes
·
2025
·Vol. 13
·期 9
·2903
·
IF 2.8
Ping Guo,Yong Li,Yanbao Liu,Yunlong Zou
In this study, a new type of double crosslinked nanospheres (DCNPM-A) was developed to solve the problem of gas channeling caused by fracture development in the process of CO2oil displacement, and the microsphere system with delayed swelling was successfully synthesized by inverse micro lotion polymerization. The microsphere adopts a dual crosslinking structure of stable crosslinking agent (MBA) and unstable crosslinking agent (UCA), achieving intelligent sealing function of shallow low expansion and deep high temperature triggered secondary expansion. The successful preparation of microspheres was verified by characterization methods such as Zeta potential and SEM, and the effects of reaction temperature, time, initiator and crosslinking agent dosage on microsphere properties were systematically studied. The experimental results show that DCNPM-A microspheres exhibit excellent expansion performance, thermal stability, and acid resistance in acidic, high-temperature, and high mineralization environments. Their expansion ratio can reach 13.5 times, and they can maintain stability for more than 60 days in supercritical CO2environments. Core displacement experiments have confirmed that the microspheres have the best sealing performance in matrices with a permeability of 10 × 10−3μm2and fractures with a width of 0.03 mm. The combination of 0.8 PV injection volume, 0.5 mL·min−1injection rate, and continuous injection method significantly improved the plugging rate and recovery rate of CO2flooding. This study provides new technical support for the efficient development of low-permeability fractured reservoirs.
研究领域:
石油工程
·
提高采收率
·
高分子材料科学
·
油藏工程
✓ 已验证
DOI
高影响因子
Carbon Neutrality
·
2024
·Vol. 3
·期 1
·1-20
·
IF 0
Guo Yafei,Gao Yuxuan,Guo Benshuai,Luo Yangna,Zhao Guoyang,Sun Jian,Li Weiling,Wang Ruilin,Zhao Chuanwen
Electrochemical CO 2 reduction (ECR) to value-added products is regarded as a sustainable strategy to mitigate global warming and energy crisis, and designing highly efficient and robust catalysts is essential. In this work, transition metal sulfides (TMS)-decorated CuS microflower-like structures were prepared via the one-pot hydrothermal synthesis method for ECR to CO, and the influence of TMS doping on ECR performance was demonstrated. Characterization of the catalysts was performed using XRD, FESEM-EDS, N 2 physisorption, and XPS, revealing the successful loading of TMS, the formation of microflower-like architectures and the generation of sulfur vacancies. Electrochemical tests demonstrated that doping ZnS, Bi 2 S 3 , CdS and MoS 2 improved the intrinsic CO 2 reduction activity of the CuS catalyst. Particularly, the MoS 2 -CuS composite catalyst with imperfect petal-like structure showed uniform distribution of edge Mo sites, which worked synergistically with the formed grain boundaries (GBs) and undercoordinated S vacancy sites in promoting CO 2 activation, stabilizing * COOH adsorption, facilitating * CO desorption, and lowering the energy barrier of the potential-limiting step for improved CO selectivity. The MoS 2 -CuS catalyst achieved a maximum CO selectivity of 83.2% at –0.6 V versus the reversible hydrogen electrode (RHE) and a high CO cathodic energetic efficiency of 100%. At this potential, the catalyst maintained stable catalytic activity and CO selectivity during a 333-min electrolysis process. The findings will offer a promising avenue for the development of efficient and stable catalysts for CO production from ECR.
研究领域:
材料科学
·
环境科学
·
能源化学
✓ 已验证
DOI
危险品化学品经营许可证（带存储）