CHEMICAL ENGINEERING SCIENCE
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2021
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IF 4.311
Zhongliang Huang,Yujia Yuan,Miaomiao Song,Zhimian Hao,Jingran Xiao,Dongren Cai,Abdul-Rauf Ibrahim,Guowu Zhan
Herein, we fabricated a series of bimetallic Pt-Ni catalysts supported on mesoporous silica nanorods ( m SNR, specific BET surface area of 1802 m 2 g −1 ) to study the effect of Ni/Pt ratio on the product selectivity in CO 2 hydrogenation. Both monometallic Pt/ m SNR and Ni 50 Pt 50 / m SNR catalysts revealed negligible methane selectivity. However, methane became the major product only when increasing the Ni/Pt ratio up to 9. X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma (ICP) characterizations showed that the Pt/Ni ratio on the catalyst surface was appreciably higher than the bulk composition, suggesting the enrichment of Pt on the surface ( e.g. , Pt/Ni of 61/39 for Ni 50 Pt 50 / m SNR catalyst). The Pt/Ni ratio was crucial in determining the CH 4 /CO selectivity, and the addition of a tiny amount of Pt could improve the catalytic performance and stability of Ni/ m SNR. Among the different catalysts, Ni 98 Pt 2 / m SNR showed the best CO 2 conversion (59%) and CH 4 selectivity (96%) at 400 °C, 0.1 MPa, 9600 mL h −1 g cat −1 , and H 2 /CO 2 of 3. In-situ DRIFTS and temperature-programmed surface experiments suggested that the dissociated adsorption of CO 2 on the Pt site led to CO*, but the strongly adsorbed CO* cannot be further hydrogenated to CH 4 over the Pt site. In contrast, CO* could be further hydrogenated into CH 4 via CH x O* intermediates on adjacent Ni sites.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Xiaodi Zhang,Guojie Zhang,Xiaowei Qin,Jun Liu,Guoqiang Li,Ying Xu,Yongkang Lv
A series of nitrogen doped biomass carbon catalysts were prepared through two different nitrogen doped methods by using soybean meal as the raw material, melamine as nitrogen source and KOH as the activators. The catalysts were characterized by BET, SEM , CO 2 -TPD, EA , FTIR , XPS and Raman. The catalytic performances of CH 4 –CO 2 reforming over different samples were also studied. The results show that the preparation method of the catalyst significantly affects the structural characteristics, N content and N species type of the catalyst. The characterization results also show the proportion of pyrrolic-N in the catalyst prepared by in-situ nitrogen doped method (Y-NC) is higher than that in prepared by the post-treatment method (H-NC). Pyrrole-N is more conducive to the adsorption and activation of CO 2 . So, the catalyst prepared by in-situ nitrogen doped method has good catalytic activity and stability. The conversion of CH 4 and CO 2 were respectively 40% and 65% at 900 °C after 50 h of CH 4 –CO 2 reforming reaction .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
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IF 5.816
Sheng Li,Guojie Zhang,Jiming Wang,Jun Liu,Yongkang Lv
Carbon materials are widely used as catalysts or supports due to their excellent properties. In this paper, the tungsten carbide-activated carbon (WC-AC) composite support was successfully prepared by in-situ carburizing on AC matrix, which is characterized by the covalent anchoring of WC on the AC support. The active metal Co was supported on WC-AC for dry reforming of methane (DRM). Samples were analyzed by N 2 physisorption measurements, XRD , XPS , H 2 -TPR, H 2 -TPD, CH 4 &CO 2 -TPSR, TG-DTG. The WC-AC stabilizes the disturbance of C in AC, alleviates the gasification effect of CO 2 and increases the active sites for CH 4 cracking. Moreover, WC provides a resistance-less bridge suitable for the Co 3+ → Co 2+ , resulting in a high Co 2+ /Co 3+ ratio on the catalyst surface . This enhances the interaction between the Co species and the WC-AC, thereby enhancing the CH 4 activation. In the process of WC-AC promoting Co 3+ →Co 2+ , the catalyst surface is accompanied by the generation of oxygen vacancies . This can enhance the dissociative adsorption of CO 2 on surface of the WC-cobalt oxide, and at the same time increase the relative proportion of adsorbed oxygen on the catalyst surface, thereby effectively inhibiting the formation of coke. However, the small amount of graphitic carbon generated due to the strong coupling of WC and Co is the main reason for deactivation of Co/WC-AC.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Daofei Lv,JiaYu Chen,Kexin Yang,Houxiao Wu,Yongwei Chen,Chongxiong Duan,Ying Wu,Jing Xiao,Hongxia Xi,Zhong Li,Qibin Xia
Using porous materials to selectively adsorb CO 2 from flue gas or natural gas is a promising method for mitigating CO 2 emission and purifying methane. Here, we synthesized an L-aspartic acid based microporous metal-organic framework (MIP-202) and studied its adsorptive separation performance for CO 2 /CH 4 and CO 2 /N 2 mixtures. Results show that MIP-202 had ultrahigh CO 2 /CH 4 (72.9 and 241.5 for CO 2 /CH 4 = 50/50 and 10/90, respectively) and CO 2 /N 2 (1,950,000 and 2129.1 for CO 2 /N 2 = 50/50 and 15/85, respectively) IAST selectivities at 298 K and 100 kPa. The high selectivity was verified by the calculations of Henery’s law selectivity and breakthrough experiments. Metropolis Monte Carlo simulation calculations show that CO 2 with greater polarizability and quadruple moment tends to occupy the pore walls of large cages with higher polarity, while the less polar CH 4 or N 2 majorly being adsorbed in the pore walls of small cages with lower polarity, resulting in the ultrahigh CO 2 /CH 4 and CO 2 /N 2 separation selectivities. MIP-202 exhibits low CO 2 adsorption enthalpy (17.2–30.7 kJ/mol), superior persistent reusability after five cyclic adsorption experiments, easy desorption performance at 298 K, moderate water and moisture stability, good stability under dry and humid SO 2 atmosphere, and low ligand cost ($36/kg). MIP-202 extrudates were prepared by an extrusion molding method using hydroxypropyl cellulose (HPC) as the binder and they retained 97.35% CO 2 uptake of MIP-202 powder at room temperature and pressure. This work shows that MIP-202 is an industrially promising material for the separation of CO 2 /CH 4 and CO 2 /N 2 mixtures.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2015
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IF 2.037
Qiaobei Dong,Yan Sun,Wei Su,Jia Liu
The use of hydrate formation in porous media is an effective method for gas storage and separation. The equilibrium isotherms of CH4 and N2 in CMK-3, a mesoporous carbon material, were measured under different tetrahydrofuran (THF) concentrations and temperatures. The higher is the temperature required, the greater is the formation pressure needed, but the presence of THF significantly reduces the hydrate formation pressure. When THF exists, both CH4 and N2 form structure II (sII) hydrate; however, the amount of hydrate generation is lower than the theoretical value. As the operating pressure increases, some of the sII CH4 hydrate may transform into structure I (sI) and the amount of hydrate generation increases. The desorption isotherms showed that the gas hydrate decomposed completely when the operating pressure was below the hydrate decomposition pressure. In addition, it is feasible to separate gas mixtures via hydrate formation using the different gas hydrate formation pressures.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Run-Jing You,Kuan Wang,Huan Ma,Xin-Peng Li,Zhe Cao,Zhen-Hong He,Huan Wang,Weitao Wang,Xiaojuan Lai,Zhao-Tie Liu
The utilization of solar energy in photocatalytic CO 2 reduction technology has demonstrated a significant potential in addressing the challenges of environmental pollution and energy shortage issues. Precise modulating of the photoreduction CO 2 pathway to achieve desired products is of particular interest, while the design of cost-effective and robust catalysts remains crucial. Herein, a series of BiOBr-based photocatalysts with different Co species were synthesized through a facile simple hydrothermal method in combination with the mechanical mixing. The Co species, which can be precisely modulated from Co 3 O 4 to CoOOH by adjusting the concentration of H 2 O 2 , were anchored into the BiOBr nanospheres to establish rich Z-scheme heterojunction interfaces. The Co species modulating of BiOBr-based Z-scheme heterojunction can achieve the transform photoreduction CO 2 products from CO to CH 4 . The CO selectivity in CO 2 photoreduction to reached 98.10 % (54.10 μmol·g −1 ·h −1 ), while the CH 4 selectivity over CoOOH/BiOBr reached 72.59 % (20.06 μmol·g −1 ·h −1 ). The outstanding photocatalytic performance and selective regulation of products are ascribed to the modulation of Co species in the BiOBr-based heterojunctions, which enables the customization of the photoreduction CO 2 pathway to achieve the desired products transformation from CO to CH 4 . In situ experiments and theoretical calculations reveal that the excellent CO selectivity observed in Co 3 O 4 /BiOBr heterojunction can be ascribed to a lower energy for *CO species compared with that of hydrogenation to *HCOOH and *CHO intermediates. Conversely, the presence of *HCOOH and *CHO intermediates with lower energy levels compared with *CO species achieved superior CH 4 selectivity in CoOOH/BiOBr heterojunction. This precise design strategy insights into the meticulous customization of Co species in semiconductor-based heterostructures at the molecular level, and enlightens the selective regulation of desired products for catalysis applications.
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Molecular Catalysis
·
2024
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IF 3.9
Yinan Ren,Wei Li
Solar-driven CO 2 reduction into hydrocarbon fuels has a great potential for mitigating the issues of greenhouse effect and fossil energy crisis we are currently facing. It is a great challenge for visible-light-driven photocatalytic CO 2 reduction into CH 4 with high selectivity and conversion efficiency. Herein, we report a synthesis of N/K-doped TiO 2 nanospheres with Ag nanoparticles decoration (N/K-TiO 2 -Ag) by a solvothermal method and study its photocatalytic CO 2 reduction performance. It is found that the N/K-TiO 2 -Ag composite exhibits superior photocatalytic CO 2 reduction into CH 4 yield and selectivity than K-TiO 2 and N/K-TiO 2 . Indeed, the N/K-TiO 2 -Ag-0.5 sample shows the highest CH 4 yield with rate of 113.84 μmol g −1 h −1 and selectivity of CH 4 (93.71%) under light irradiation. The enhancement might be attributed to the synergy of N/K doping and silver loading. In particular, the N/K doping and the Ag cocatalysts introducing triggered improvement of solar energy utilization and charge separation as well as Ag-induced SPR effect and the K + -induced redistribution of photogenerated charge carriers cooperatively promotes photocatalytic CO 2 conversion into CH 4 . It is expected this work would offer a guide for rational design of K/TiO 2 -based photocatalyst for selectively converting CO 2 into fuels.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2025
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IF 14.3
Wenjiao Chang,Honghuo Wang,Tingting Wu,Shuting Zhang,Yifan Li,Junying Wang,Yongqiang Yang,Lei Wang
Photocatalytic CO 2 reduction reaction is regarded as a potential strategy to convert greenhouse gases into valuable chemicals. However, achieving photocatalysts with high efficiency and target product selectivity under visible light still faces great challenges. Herein, sub-2 nm RuO 2 @TiO 2 (RTO) nanorods with lattice matching interface are rationally designed and prepared via a hydrothermal reaction step-by-step. Due to the strong interaction of the lattice-matched interface with the Ru-O-Ti bond, new energy levels have emerged at the interface, leading to effective visible light absorbance. Moreover, the photo-generated electrons could be transferred to the RuO 2 efficiently via the lattice-matched interface. As a result, the RTO photocatalyst exhibits superior CO 2 -to-CH 4 conversion performance of 15.6 µmol g −1 with a selectivity of 87.9% under visible light irradiation. Density functional theory (DFT) calculation reveals that the energy barrier of CO* to CO is significantly higher than that of *CHO, resulting in the preferential production of CH 4 . This work provides an effective strategy for designing photocatalyst with promoted visible light absorption and improved product selectivity.
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THERMOCHIMICA ACTA
·
2024
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IF 3.1
Guolan Dou,Liying Zhang,Deming Wang,Xiaoxing Zhong,Botao Qin
The study examined the oxidative pyrolysis of raw and residual coals extracted with tetrahydrofuran, as well as the CO/CO 2 /H 2 /CH 4 emissions at high temperatures (200∼900 °C). Tetrahydrofuran was found to extract aromatic and aliphatic hydrocarbons from lower metamorphic coal, as well as hydroxyl, increasing the specific surface area of char formed by oxidative pyrolysis of residual coal. The CO 2 /CO ratio was temperature dependent, and the increase period was fit by a polynomial and a linear function, with critical temperature of around 570 °C. The greater CO 2 /CO ratio of raw coal suggested that oxidative pyrolysis produced more CO 2 . The kinetic analysis showed that the change in activation energy is inconsistent with the gas production, and the gases were found to be proportionate to the specific surface area of the coal chars, implying that the char structure has a significant influence on gaseous product emissions and the coal oxidative pyrolysis at high temperatures is a diffusion-controlled heterogeneous reaction. The findings of this study could be useful for determining the status of coal fire.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Yuntao Qi,Bin Zhang,Dengrong Xue,Hui Zhang,Xiaoning Liu,Zhi Liu,Shichao Zhao,Zhuo Li,Fanchun Meng,Yong Qin
The catalytic conversion of CO2 to CO through hydrogenation has emerged as a promising strategy for CO2 utilization, given that CO serves as a valuable C1 platform compound for synthesizing liquid fuels and chemicals. However, the predominant formation of CH4 via deep hydrogenation over Ru-based catalysts poses challenges in achieving selective CO production. High reaction temperatures often lead to catalyst deactivation and changes in selectivity due to dynamic metal evolution or agglomeration, even with a classic strong metal–support interaction. Herein, we have developed a FeOx/Ru/Rutile multilayer epitaxial structure by depositing a FeOx layer onto the epitaxially grown RuO2 nanolayers on the surface of rutile nanoparticles. This multilayer epitaxial structure transformed into a structure in which Ru nanoparticles were decorated with FeOx layers with ultrastable strong metal-support interaction (SMSI). Subsequently, the FeOx decoration on Ru nanoparticles effectively shifted the dominant product from CH4 to 95% CO during CO2 hydrogenation. Remarkably, this catalyst exhibits exceptional stability and can be operated stably at 550 °C for a long time without apparent deactivation. Compared with the dynamic changes observed in supported Ru nanoparticles, the interaction between Ru and FeOx maintains their electronic states at different reaction temperatures. Furthermore, this Ru–FeOx interaction inhibits H2 activation capability, CO adsorption, and subsequent hydrogenation of CO. The transformation strategy employed here, which utilizes initial multilayer epitaxial structures, can be applied to construct SMSI to enhance metal catalysts’ catalytic performance.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Qingping Xin,Yucheng Pan,Chao Zhang,Lei Zhang,Chensheng Dong,Ligang Lin,Lizhi Zhao,Hui Ye,Yuzhong Zhang
The CH 4 /N 2 high-efficiency membrane separation technology is capable of effectively enriching CH 4 from natural gas, and holds great potential for application in the fields of biogas purification and natural gas pipeline leak detection. However, preparing high-performance separation membranes is challenging due to the similarity between CH 4 and N 2 molecules. To enhance the CH 4 /N 2 separation performance, block polyetheramide copolymer (Pebax)/EVA blended membranes were fabricated in this study. Additionally, a novel gas leakage detection tube was prepared. The EVA14 (14 wt% VA) membrane exhibits an optimal transport-facilitated channel among a series of pure EVA membranes, resulting in a CH 4 permeability of 21.41 Barrer and CH 4 /N 2 selectivity reaches 1.80 under mixed-gas feed conditions at 35 °C. The CH 4 permeability of Pebax/EVA (30 wt%) reaches 120.5 Barrer by physical blending, and the CH 4 permeability is increased by 191 % in comparison with pure EVA14 membrane. The Pebax/EVA (10 wt%) membrane exhibits the optimum CH 4 /N 2 selectivity, and compared with pure EVA membrane increased by 35.5 %. EVA and Pebax polymers are blended for the first time for CH 4 /N 2 separation, and the blending of block polyetheramide copolymer intensifies the membrane's separation performance comprehensively. The natural gas leak detection tube was fabricated with a membrane, offering a new and efficient CH 4 /N 2 separation strategy.
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ACS Sustainable Chemistry & Engineering
·
2024
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IF 7.1
Xupeng Zhang,Kaiqian Li,Longxin Guo,Zhiping Xu,Shuduan Deng,Ying Liu,Gang Zhu
To effectively mitigate the global warming problem caused by excessive CO2 emissions, the implementation of direct air capture (DAC) technology has emerged as one of the most promising strategies for capturing CO2 from the atmosphere. The key to DAC technology hinges on the development of high-performance solid sorbent materials that demonstrate high CO2 adsorption capacity and gas separation selectivity, particularly under low CO2 partial pressure conditions. Herein, we have successfully developed a class of MOF@carboxylated wood sponge (MOF@CWS) hybrid sorbents, capable of efficient CO2 capture from low-concentration (less than 10,000 ppm) CO2 sources, achieved by embedding the porous MOF into carboxylated wood sponges (CWS) substrate via an in situ growth route. Within the MOF@CWS series, the CO2 uptake capacity of Mg-MOF-74@CWS is 3.61 and 2.65 mmol/g at 1 bar, 273 and 298 K, respectively, significantly higher than those of CWS and HKUST-1@CWS. Moreover, this material exhibited outstanding DAC performance, with the CO2 sorption capacity at 273 K up to 0.56 mmol/g from ambient air (ca. 400 ppm of CO2), surpassing most other solid sorbents. The obtained Mg-MOF-74@CWS also demonstrated exceptional CO2/CH4 separation performance, primarily due to the unique pore structure and augmented interaction between the CO2 molecules and the hybrid sorbents. The results of this study indicate that Mg-MOF-74@CWS has potential as an efficient solid sorbent for the DAC of CO2.
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危险品化学品经营许可证（带存储）