INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Shiji Qin,Guangya Wei,Qiuman Zhang,Bowen Liu,Haibao Zhang,Zhongwei Liu
To address the challenges of high energy consumption and insufficient low-temperature activity in conventional thermal catalytic CO 2 methanation, this study reports a new nickel-based catalyst preparation via the solution combustion synthesis (SCS) technique for plasma-catalytic CO 2 methanation. The results demonstrate that the SCS method successfully reconstructed the CaCO 3 support, resulting in a porous structure with a high specific surface area (23.86 m 2 /g) as well as highly dispersed Ni nanoparticles (approximately 9.32 nm), which significantly enhanced the metal-support interaction. Combined density functional theory (DFT) calculations and electron paramagnetic resonance (EPR) analysis revealed that the SCS-reconstructed CaCO 3 surface is rich in oxygen vacancies, markedly enhancing the adsorption capacity for CO 2 and CO (with adsorption energies reaching - 3.83 eV and - 3.56 eV, respectively), thereby providing favorable conditions for the intermediates formation for CO 2 conversion. Under optimized conditions (3 wt% Ni loading, H 2 /CO 2 ratio of 5, discharge power of 28 W, and gas hourly space velocity of 180,000 mL g −1 h −1 ), the CO 2 conversion reached 79.1 % with a CH 4 selectivity of 91.9 % and an energy efficiency of 17.2 %. These performance metrics are significantly superior to those of catalysts prepared by conventional impregnation methods and pure plasma systems. In situ characterizations (plasma DRIFTS and OES) indicated that the basic sites on CaCO 3 preferentially adsorb CO 2 to form carbonate species. The synergistic effect between high-energy electrons generated by the plasma and the Ni active sites promotes the hydrogenation of carbonates to formate intermediates, which are subsequently converted into CH 4 via the formate pathway (HCOO∗ → CO∗ → CH 4 or HCOO∗ → CHO∗ → CH 4 ). The catalyst exhibited good stability during a continuous 24-h operation. This study provides a novel strategy for developing a bionic synergistic catalytic system for low-temperature and highly efficient CO 2 conversion.
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2024
·
IF 3.7
Yunfei Zhao,Hang Sheng,Jiashun Xi,Tingting Jiang,Dong Wang,Jian Zhang,Zheng Li,Bing Wang,Xiaohui Xu,Haifeng Zhang,Bo Yuan,Runlong Hao,Yi Zhao,Tianhao Wang
In the reaction system with NaBH 4 as a hydrogen donor, inhibiting the formation of hydrogen is the key to promote the efficient catalytic hydrogenation of CO 2 . In this study, nanoscale zero-valent nickel supported on carbon nanofibers (Ni 0 /CNFs) was fabricated as a catalyst for CO 2 hydrogenation in aqueous NaBH 4 solution. The characteristics of Ni 0 /CNFs were examined. By SEM, it was observed that spherical nickel nanoparticles were distributed homogeneously on the surface of strip-shaped carbon nanofibers. EDS mappings indicated that elements were evenly distributed on the catalyst, which might contribute to the uniform exposure of active sites. Via XRD, it was determined that all the diffraction peaks corresponded to the crystal face of nickel metal and that the absence of diffraction peaks of carbon nanofibers indicated that the crystallinity of the carrier was low. XPS study showed that nickel existed on the catalyst surface in two forms: zero valence metal and oxidation state. The effects of catalyst addition amount, NaBH 4 concentration, NaOH dosage, stirring rate on the yield of formate and hydrogen generation rate (HGR) were investigated. By optimizing the above parameters, the concentration of formate reached 150 mmol/L and the hydrogen production rate was 10.55 mL/min. Compared with the non-catalytic conditions, the concentration of formate increased by 57 % and the HGR decreased by 78 %. Moreover, the relationship between CO 2 hydrogenation and NaBH 4 hydrolysis was clarified. This research could enhance comprehension of CO 2 hydrogenation in aqueous NaBH 4 solution and contribute to the development of CO 2 capture and utilization storage technology. The significance of this study lies in clarifying the connection between CO 2 hydrogenation and borohydride hydrolysis in CO 2 catalytic hydrogenation technology.
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DOI
高影响因子
JOURNAL OF THE CHINESE CHEMICAL SOCIETY
·
2020
·Vol. 67
·期 10
·1818-1826
·
IF 1.554
Yang Hu,Longchao Du,Cun Li,Jiale Shen,Weiju Zhu,Chenxi Shao
Carbon dioxide (CO 2 ) is an easily available renewable carbon source that can be used as a comonomer in the catalytic ring-opening polymerization of epoxides to form aliphatic polycarbonates. Herein, a series of new Salen-Co(III) bifunctional catalysts were synthesized for the first time, and they were studied to catalyze the copolymerization of CO 2 and propylene oxide (PO)/cyclohexene oxide (CHO). At the same time, the effects of reaction conditions (electronic effect, temperature, time) on catalytic activity and selectivity were investigated. The results show that the Salen-Co(III) complexes with electron-withdrawing groups have higher selectivity and activity for propylene carbonate (PPC)/cyclohexylene carbonate (PCHC). At the same time, the Salen-Co(III) complexes can better catalyze the copolymerization of CHO and CO 2 than that of PO and CO 2 . The catalytic efficiency of the four complexes increased with increasing temperature, and the best reaction condition is 80°C, 30 min and 2 MPa of CO 2 .
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DOI
高影响因子
Catalysis Science & Technology
·
2015
·Vol. 5
·期 5
·2959-2972
·
IF 5.426
Ran Zhang,Li Guo,Chen Chen,Jizhong Chen,Angjun Chen,Xiuge Zhao,Xuerui Liu,Yuhe Xiu,Zhenshan Hou
A novel highly active Mn-doping ceria heterogeneous catalyst (MnOx–CeO2) was prepared and dedicated to the catalytic synthesis of aliphatic carbamates from CO2, aliphatic amines and methanol in one step. The as-obtained catalyst can attain a high yield of carbamate up to 82%, and can also be recycled at least four times through a simple procedure. It was observed that the Mn doping to ceria can alleviate the catalyst deactivation in consecutive catalytic recycles. In this regard, the role of Mn doping in the ceria in the synthesis of the aliphatic carbamates was investigated by means of X-ray diffraction (XRD), Raman spectra, specific surface areas (BET), thermogravimetric analysis (TGA), X-ray photoelectron spectroscopy (XPS), CO2-temperature programmed desorption (CO2-TPD) and in situ diffuse reflectance infrared Fourier transform (DRIFT). The characterization demonstrated that the presence of MnOx in the ceria can not only inhibit the formation of stable carbonate species on the surface of the catalyst but also promote the decomposition/consuming of the carbonaceous species during the synthesis of aliphatic carbamates so as to allow improvement of the recyclability of the catalyst.
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DOI
高影响因子
INORGANIC CHEMISTRY
·
2019
·
IF 4.85
Shikang Yin,Jinze Li,Linlin Sun,Xin Li,Dong Shen,Xianghai Song,Pengwei Huo,Huiqin Wang,Yongsheng Yan
Photocatalytic reduction of CO2 by semiconductors is of great significance in generating value-added fuels. Here, we construct a novel S–C–S heterojunction constituted of MoS2/SnS2/r-GO by a simple solvothermal method. The prepared MoS2/SnS2/r-GO showed significant photoexcitation of photosensitive oxygen (ROS) by electron spin resonance spectroscopy, demonstrating that superoxide radicals (•O2–), pores, and hydroxyl radicals (•OH) are the main active species. The constructed S–C–S heterojunction has a multilevel electron transport mechanism and synergistic effect, which provides the possibility of producing more organic fuel. The photocatalytic materials were characterized by XRD, XPS, SEM, TEM, PL, etc. As a result, the atomic layer MoS2/SnS2/r-GO heterojunction exhibited a CO formation rate of 68.53 μmol g–1 h–1 and a CH4 formation rate of 50.55 μmol g–1 h–1, respectively. This work opens up new prospects for the formation of heterojunctions of chalcogenide transition-metal sulfides.
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DOI
PubMed
高影响因子
Soft Matter
·
2017
·Vol. 13
·期 34
·5704-5713
·
IF 3.889
Cheng Wang,Mengnan Zhang,Wei Li,Xin Huang,Shuang Li,Sen Luan,Xiaojian Hou,Qian Wang
A systematic study on the structural properties and component information of periodic mesoporous organosilicas synthesized by using different nonionic surfactants as templates with compressed CO2 was carried out. Triblock copolymers (F127, F108, and P123), oligomeric alkyl poly(ethylene oxide) (Brij-58 and Brij-76), and alkyl-phenol poly(ethylene oxide) (TX-100) have been employed as templates and BTEB as a bridged organosilica precursor to synthesize PMO materials at 5.90 MPa. The structure and morphology of the obtained materials were investigated by means of transmission electron microscopy (TEM), nitrogen sorption isotherms, solid Si and C NMR, and FTIR. Efforts have also been made to compare the differences in structural and morphological properties among these samples synthesized under similar conditions. We also investigate the synthesis of PMOs using F127 as the template at different CO2 pressures. It was found that the interaction between different organic silica precursors and surfactants with a variety of hydrophilic and hydrophobic chains is the key factor for the disorder degree of mesostructures. On this basis, the possible mechanism of formation of PMOs synthesized using a nonionic surfactant (triblock copolymer) as the template with compressed CO2 is illustrated and discussed.
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高影响因子
RSC Advances
·
2020
·Vol. 10
·期 69
·42408-42412
·
IF 3.119
Yuying Yang,Hong Li,Supeng Pei,Feng Liu,Wei Feng,Yongming Zhang
CO2, the main greenhouse gas, has received considerable attention due to environmental issues. From a scientific perspective, CO2 as a cheap and abundant carbon source, could be applied in synthesizing more valuable chemicals such as urea, formic acid, and cyclic carbonates. However, the high bond energy of CO (750 kJ mol−1) and the non-polarity property make CO2 molecules difficult to activate. In this paper, we have carefully designed a low-cost, stable and, most importantly, highly efficient Co-based heterocatalyst Co@NxC functionalized by nitrogen-doped carbon to activate CO2 molecules and convert it into cyclic carbonates. The CO2 conversion process could be triggered at very mild conditions (60 °C and 1 bar CO2). We carefully adjusted the nitrogen content in the carbon support to enhance the catalytic performance of Co centers via the interface effect. Consequently, the optimal catalyst displayed extraordinary activity toward the cycloaddition of CO2 with styrene oxide as high conversion (92%) and selectivity (>99%) were achieved in 4 h without byproducts.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Qinsheng Wang,Yiyi Fan,Chengliang Wu,Yun Jin,Claudia Li,Jaka Sunarso,Xiuxia Meng,Naitao Yang
Research on gas separation membrane has targeted upon maximizing the selectivity and permeance. The development of 2D materials ( e.g. , MXene) gives a novel avenue to surpass the “trade-off” among the membrane selectivity and permeability. However, randomly stacked nanosheets and the regulation of interlayer spacing for MXene nanosheets hinder the development of MXene membrane. To this end, we designed a Pd-intercalated lamellar MXene membrane to modify the surface chemical properties (H-spillover effect) of MXene (Ti 3 C 2 T x ) and to expand the interlayer spacing (from 2.29 to 3.26 Å) due to the strong interaction between Pd 2+ and MXene nanosheets with negative charge. Here, we performed a single-step etching approach to prepare 2D Pd-MXene membrane and demonstrated its excellent H 2 permeability of 2.66 × 10 −7 mol m −2 s −1 ·Pa −1 and H 2 /CO 2 selectivity of 242 at 25 °C, which greatly exceeds the current benchmark membranes. We also developed single gas transport mathematical mechanism models to interpret and support the experimental results. The combined experimental and modeling results show that interlayer spacing and H-spillover effect of Pd-MXene membrane benefit H 2 /CO 2 separation.
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DOI
高影响因子
ADVANCED MATERIALS
·
2014
·Vol. 26
·期 41
·7027-7031
·
IF 15.409
Li-Li Tan,Haiwei Li,Yanchun Tao,Sean Xiao-An Zhang,Bo Wang,Ying-Wei Yang
Graphical Low-density, solid-state, porous supramolecular organic frameworks are constructed using pillarenes. The frameworks have a honeycomb-like structure, permanent porosity, high thermal stability, and selective and reversible sorption properties toward CO 2 . The exceptionally selective CO 2 -sorption properties (375/1, 339/1) of one framework over N 2 and CH 4 indicate potential applications in CO 2 -capture for post-combustion power plants and natural gas sweetening.
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DOI
PubMed
高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2025
·Vol. 42
·期 8
·1587-1598
·
IF 3.2
Liu Wenhao,Chen Qingcai,Xu Tengfei
To reduce the CO 2 capture cost of solid amine technology, more attention has been paid to the preparation of support materials from solid waste sources. We use basic oxygen furnace steel slag and blast furnace slag as raw materials. To obtain porous support materials, they are treated by acid etching and combined acid-base treatment, respectively. Then modified them using TEPA, finally successfully prepared two types of steel slag-based solid amine materials (BOFS-xTEPA and BFSX-xTEPA). The technologies of XRF, BET and SEM were used to characterize the materials. A homemade static CO 2 adsorption capacity tester was utilized to test the CO 2 adsorption capacity of the composites at 15% CO 2 and 85% air (wet). The optimal CO 2 adsorption capacity was explored by controlling the parameters in the material synthesis process. In terms of mechanism, a rational explanation for the pore formation of the two porous support materials was provided. Finally, the characteristics of the two steel slag-based solid amine preparation routes were analyzed from various perspectives. In comparison with solid amines derived from other solid waste sources, the advantages of this project were elucidated.
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DOI
高影响因子
ChemSusChem
·
2020
·Vol. 13
·期 24
·6594-6601
·
IF 7.962
Biyu Chen,Jiajie Xu,Jiantao Zou,Defei Liu,Yue Situ,Hong Huang
Graphical A hollow victory : The mass transport and reaction process of the CO 2 reduction reaction on copper-tin alloy hollow fibers are investigated. The reason for suppressing hydrogen evolution reaction is revealed by comparing the influence of different gas injection ways. The high performance of formate production on Cu−Sn 45% alloy hollow fiber is attributed to the favorable crystal phase and the unique structure. Electroreduction carbon dioxide into formate has been regarded as a hopeful measure to relieve global warming. Copper-based hollow fibers demonstrated good performances on converting carbon dioxide in previous researches. Herein Cu−Sn alloy hollow fibers were synthesized in an innovative way, combining the structure advantages of hollow fiber and high selectivity towards formate on η′ bronze. Tests under different gas injection conditions were conducted to analyze the contribution of the hollow fiber structure on suppression of hydrogen evolution and promotion on kinetics. Strikingly, Cu−Sn 45 % hollow fiber, the optimal catalyst in this work, achieved a highest faradaic efficiency towards formate of 90.96 % at a lower potential of −0.75 V vs. RHE than most non-noble catalysts, and the FE of H 2 was below 4 %.
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DOI
PubMed
高影响因子
ChemCatChem
·
2022
·Vol. 14
·期 13
·e202200253
·
IF 5.497
Mingsheng Luo,Tong Qin,Qinglong Liu,Zhi Yang,Fengli Wang,Hong Li
Graphical Promoting : A series of Fe-modified CeO 2 catalysts with nanoparticle, nanorod, nanocube and nano-octahedron morphologies were synthesized by the hydrothermal method. The Fe-modified CeO 2 nanorod catalysts exhibit a remarkably promoting effect on the formation of DMC from CO 2 and methanol. A series of Fe-modified CeO 2 catalysts with nanoparticle, nanorod, nanocube and nano-octahedron morphologies were synthesized and applied for direct synthesis of dimethyl carbonate (DMC) from CO 2 and methanol. The Fe-modification shows a remarkably promoting effect on the formation of DMC over Fe-modified CeO 2 nanorod. The DMC yield was improved from 0.202 to 2.568 mmol DMC per g cat by 2 %Fe-modification of CeO 2 nanorod. A synergistic effect among the moderate acid-basic sites, specific surface area and surface composition resulted from Fe-modification was proposed to be crucial to obtaining the high reactivity of DMC formation.
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高影响因子
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