FUEL
·
2022
·
IF 8.035
Zixuan Ma,Fenghai Cao,Yuhao Yang,Liyan Wang,Tao Zhang,Minghui Tan,Guohui Yang,Yisheng Tan
Bifunctional catalysts composed of ZnCrO x oxide and ZSM-5 were widely used in syngas-to-aromatics (STA). The CO conversion on bifunctional catalysts was generally higher than that on oxide catalysts attributed to the pulling effect of zeolite, but the key factor for the improvement of CO conversion was still short of systematical explanation. In this work, the degree of nonstoichiometric spinel of ZnCrO x (ZxC) oxides was finely tuned through modulating the ratio of Zn/Cr, which could significantly influence the catalytic behaviors of ZnCrO x /ZSM-5 catalysts for the CO hydrogenation to aromatics. The increase of nonstoichiometric spinel corresponded to the increase of oxygen vacancies and the enhancement of Zn-Cr synergistic effect, which promoted the activation of H 2 and CO, leading to a dramatic increase of CO conversion. The work revealed that the action of ZnO and oxygen vacancies was the key factor for CO pulling in ZnCrO x oxide and ZSM-5 catalyzed STA reaction.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2019
·
IF 7.467
Yajing Wang,Yane Zheng,Yuhao Wang,Hua Wang,Xing Zhu,Yonggang Wei,Yaming Wang,Lihong Jiang,Zhiyuan Yang,Kongzhai Li
Chemical looping reforming of methane (CLRM) technology is a new approach for syngas and pure hydrogen generation . During the whole reaction, methane is first partially oxidized to syngas by the lattice oxygen of the oxygen carrier, and then the lattice oxygen of the reduced oxygen carrier is recovered by thermal water splitting, with pure hydrogen produced. LaMnO 3 is used as an oxygen carrier for the CLRM. It obtains a high resistance to carbon deposition , while a lower CH 4 conversion due to the unstable structure. Fe ion substitution in LaMnO 3 can be used to improve its reactivity and thermal stability. La 1-x MnFe x O 3 /LaMn 1-x Fe x O 3 (x = 0.05, 0.1, 0.15, 0.2) oxygen carriers own higher reactivity and better resistance to carbon deposition, producing high purity syngas and hydrogen. La 0.85 MnFe 0.15 O 3 sample exhibits the highest CO selectivity (~99%), syngas productivity (3.78 mmol g −1 ) and H 2 productivity (1.76 mmol g −1 ) due to the higher oxygen vacancy concentration, and its H 2 /CO molar ratio is maintained at the ideal ratio of 2.0 (1.93–2.07) during the whole process. Notably, no carbon deposition is generated over LaMnO 3 , La 0.85 MnFe 0.15 O 3 and LaMn 0.9 Fe 0.1 O 3 oxygen carriers even after 20 redox cycles, and La 0.85 MnFe 0.15 O 3 exhibits superior resistance to carbon deposition due to the better structural and thermal stability.
研究领域:
材料科学
·
能源工程
·
化学工程
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2020
·
IF 12.35
Xiaoli Yang,Ruifeng Wang,Jia Yang,Weixin Qian,Yaru Zhang,Xuning Li,Yanqiang Huang,Tao Zhang,De Chen
Direct conversion of syngas into aromatics with tandem catalysts containing Fe-based Fischer–Tropsch synthesis (FTS) catalysts and zeolites has been attracting significant attention because of the great cost-efficiency. However, the interaction role between two active species and reaction paths are still unclear. We report here that a high yield of aromatics was achieved by serial reactions directly from syngas on a Na-Fe-ZrO2/ZSM-5 tandem catalyst. Results point out significant impacts of zeolite in the catalytic system on performance including activity and selectivity. The role of the zeolite on reaction pathways about both CO conversion and aromatic formation has been systematically investigated by steady-state isotopic transient kinetic analysis and designed experiments. The presence of zeolite in the catalytic system promotes the CO hydrogenation rate by means of improving the iron carburization degree, possibly because of the enhanced CO adsorption and the formation of surface intermediates. It also enhances selectivity to aromatics by coupling CO to participate in the olefin transformation on ZSM-5. In addition, the formation rate of aromatics is proportional to the number of Lewis acidic sites, suggesting the dehydroaromatization route as the main mechanism of olefin aromatization. These findings provide some insights into the effect of ZSM-5 on reaction paths over the FTS catalyst–zeolite tandem catalyst system.
研究领域:
化学工程
·
催化化学
✓ 已验证
DOI
高影响因子
Energies
·
2020
·Vol. 13
·期 14
·3668
·
IF 2.702
Xiaobo Wang,Anqi Liu,Zengli Zhao,Haibin Li
Raw syngas conditioning using molten salts was carried out in a fixed-bed reactor. The effects of the reaction conditions, including temperature, gas velocity, bubble diameter, molten salt static liquid heights, and inlet gas composition, on the composition of the syngas product and the properties of the spent molten salts were investigated. The molten salt absorbed CO2in all of the experiments (at temperatures from 350 °C to 500 °C) and decreased its concentration down to 1%. The H2/CO increased from 0.94 to a maximum of 11.0, which may meet most of the synthetic process’ requirements. The temperature, gas velocity, and molten salt static liquid heights had significant effects on the H2and CO concentrations in the gas product. Molten salt raw syngas conditioning can be a suitable follow-up procedure for gasification and pyrolysis.
研究领域:
能源工程
·
化学工程
·
可再生能源
·
气化技术
✓ 已验证
DOI
高影响因子
AICHE JOURNAL
·
2026
·
IF 4.4
Yan Sun,Shangwei Ma,Yiou Wang,Bruno Chaudret,Tejraj Aminabhavi,Helei Liu
Integrated carbon capture and utilization can reduce the energy penalty of CO 2 valorization, but is often limited by slow transport between capture and catalytic sites. Here, we report a proximity-engineered dual-functional material for direct conversion of captured CO 2 into syngas via isothermal calcium-looping dry reforming of methane at 650°C. Embedding trace Ni into a CaO framework and introducing CeO 2 creates abundant Ni–Ce–Ca interfacial sites with shortened carbonate diffusion pathways, enhanced oxygen mobility, and improved resistance to sintering and coking. The optimized material achieves a CO 2 capture capacity of 12.6 mmol g −1 and a syngas yield of 58 mmol g −1 , representing up to a 2.9-fold improvement over conventional materials. Operando spectroscopy and density functional theory reveal that captured carbonates are directly converted through a lower-energy COOH-mediated interfacial pathway, demonstrating an effective strategy to overcome transport limitations in integrated CO 2 capture and conversion.
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xiaohui Sun,Linglong Wang,Yongxiao Tuo,Bangyan Zhang,Tao Gan,Jiansong Miao,Chunming Xu
Renewable-driven electrochemical reduction of CO 2 (CO 2 RR) to syngas is an attractive approach to achieve carbon neutrality. However, high current density at specific H 2 /CO molar ratios is challenging. Herein, a sulfur, nitrogen co-doped carbon supported Ni an Co dual-atom-system is designed as electrocatalyst to produce syngas from CO 2 RR. By regulating the molar ratio of Co and Ni in the dual atom system, H 2 /CO molar ratios of 1 and 2 that are typically suitable for a downstream Fischer-Tropsch synthesis process can be controlled in a wide current density range from 50 to 250 mA/cm 2 . This is attributed to the fact that single Ni sites are highly active for CO 2 RR to CO, while single Co sites are highly active for H 2 production. Moreover, experiments combined with theory confirm the presence of a sulfur-bridged Co and Ni moiety in the dual-atom system, and electrons are transferred from the Co and neighboring Ni sites to the bridged S atom. These electron deficient Co and Ni sites efficaciously balanced the adsorption strength of COOH* and H*, further facilitating syngas production without scarifying total current densities. This study provides a useful case for the fabrication of dual-atom catalysts with industrial relevant syngas production via CO 2 RR.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jinpeng Zhai,Zhenjiang Wang,Jia Ouyang,Beichen Xue,Chao Liu,Rui Xiao
Sewage sludge (SS), as a common solid waste with large production and rich organic nitrogen, has the potential to synthesize N-doped carbon (N-C) for CO 2 adsorption. In this paper, A novel synthesis method of N-C CO 2 adsorbent from SS by structural regulation of glucose (Glc) and further activating with K 2 CO 3 was proposed. Besides, the influence mechanism of N-doping form and content on CO 2 absorption capacity of N-C was studied by density functional theory calculations (DFT). Results showed that Glc had the effect of promoting the formation of internal mesoporous structure and adjusting pyrrole-N (N-5) structure into quaternary-N (N-Q) structure. The N-C prepared with feedstock mixing sludge, Glc and K 2 CO 3 powder (mass ratio of SS/Glc/K 2 CO 3 = 3:1:4) at 800 °C showed the highest CO 2 adsorption capacity (3.00 mmol/g at 25 °C and 1 bar) and superior CO 2 selectivity for CO 2 /CO/CH 4 under continuous flow. Theoretical calculations identified a nitrogen-doping threshold effect, where elevated nitrogen content strengthened pyridine-N (N-6) induction effects to enhance localized polarity for CO 2 adsorption. Conversely, lower doping levels amplify conjugation effects via N-5 prevalence, significantly improving adsorption capacity. This dual mechanism demonstrates that N-6 configurations optimize local polarity at high doping ratios, while N-5 architectures maximize electron delocalization efficiency at reduced nitrogen concentrations.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Tingwei Wang,Hanpeng Liu,Sam Toan,Zhao Sun,Zhiqiang Sun
Deoxygenation-based biomass gasification provides a feasible solution for the effective utilization of biomass and value-added syngas production. However, the behavior of bio-oil formation during the pyrolysis stage and the characteristics of tar abatement at the gasification stage with applied deoxidizer still require exploration. Thus, this study investigates the effects of different deoxidizer/biomass (D/B) mass ratios, pyrolysis-gasification temperatures, and water-injection velocities on the composition and yield of bio-oil and tar-elimination law. The techniques of 2D HSQC nuclear magnetic resonance, attenuated total reflectance, gel permeation chromatography, and gas chromatography-mass spectrometer are used to investigate the formation behavior and evolution law of the bio-oil produced. The results indicate that the addition of the deoxidizer not only improves the quality and yield of syngas but promotes the deoxygenation of oxygen-containing bio-oil by donating electrons. Specifically, the phenolic compounds decreased by 12.4% under D/B = 0.3 as compared with D/B = 0. The results also confirm the promoting effect of tar elimination via reforming and cracking by Fe and CaO, respectively: Tar production during the gasification stage decreased by 54% under D/B = 0.3, as compared with non-deoxygenation. This study demonstrates the superiority of iron-calcium-based deoxidizer in bio-oil deoxygenation and tar elimination, which will promote the development of deoxygenation-based bio-oil and syngas poly-generation.
研究领域:
能源与燃料
·
环境科学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Junya Wang,Chenxi Ma,Shikun Wen,Ping Ning,Yu Zhang,Yi Liu
This study synthesized a composite material of ZIF-67 and black titanium (BT) with high CO 2 reduction capability via a mechanochemical method. Through in-depth analysis of the morphology, structure, optical properties, and electrochemical behavior of the ZIF-67-BT composite photocatalyst, it was confirmed that the composite successfully formed an S-scheme heterojunction structure. This configuration can effectively separate photogenerated charge carriers, resulting in superior CO 2 reduction performance. The findings indicate that the composite material has optimal catalytic performance when the ZIF-67 doping content reaches 30 wt% (30 %ZIF-BT). Within 5 h, 30 %ZIF-BT exhibited excellent photocatalytic activity, with CO and H 2 yields reaching 2486.4 μmol·g −1 and 3495.0 μmol·g −1 , which were 44.0 and 29.4 times greater than the yields of BT, and 2.4 and 1.4 times than ZIF-67. The syngas (comprising CO and H 2 ) generated by ZIF-BT, with an adjustable CO to H 2 ratio ranging from 1:1.40 to 1:2.47, is regarded as a significantly beneficial and crucial intermediate for further conversion into valuable hydrocarbon fuels via Fischer-Tropsch synthesis. This research offers a feasible method to construct S-scheme heterojunction in ZIF-BT composite materials.
研究领域:
材料科学
·
环境科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Xinjun He,Mengqiao Gao,Fukun Li,Zhiyang Tang,Jie Qu,Jinxing Long,Qiang Zeng,Xuehui Li
Catalytic hydrogenolysis of lignin has attracted steady attentions in regard of producing high-value aromatic chemicals from the renewable resource and achieving the “carbon neutrality” goal. However, current techniques for lignin hydrogenolysis are highly challengeable due to the necessity of pure H2 and relatively low yields in monomers. In this work, a novel and efficient approach has been proposed for the conversion of lignin to monophenols under readily available and cost-effective syngas. The results demonstrated that CO has the dramatic promotion on the bagasse lignin hydrogenolysis over commercialized Pd/C at 230 °C for 4 h, the yield of monophenols reaches 357.2 mg/g at 3.0 MPa syngas (CO/H2=2/1), which is approximately 1.7 times of that under pure H2. As evidenced by quantitative 31P NMR analysis, the promoting effects of CO on lignin depolymerization are positively correlated with the content of side-chain hydroxyl groups in lignin. Further investigations on lignin model conversion reveal that CO suppresses the dehydroxylation at Cα-OH, with concomitant enhancement of Cβ-O bond cleavage (increasing from 10% in H₂ to 64% in syngas). This inhibitory effect on side-chain hydroxyls elimination directly correlates with the 1.7-fold increase of monophenol yields observed during catalytic depolymerization. Therefore, this work provides a new insight in lignin depolymerization using industrial catalyst of Pd/C and the cost-effective syngas.
研究领域:
化学工程
·
可再生能源
·
催化
·
生物质转化
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2025
·
IF 6.2
Wenzhe Zhang,Shanshan Dai,Yong Liu,Jie Li,Guozhang Chang,Cuiping Wang,Jian Zhang
The utilization of industrially generated lignin is an important aspect of achieving worldwide carbon neutrality. In this study, Ni/CaO, Ce/CaO and (Ni-Ce)/CaO catalysts were prepared using an impregnation method to improve the production of H 2 -enriched syngas from lignin steam gasification. Results show that the Ni/CaO and Ce/CaO exhibited different effects when applied to steam gasification, the former improved the conversion of solid lignin whereas the latter promoted decomposition of the resulting volatiles. The (Ni-Ce)/CaO catalyst provided a remarkable synergistic effect on production of H 2 -enriched syngas. The mass-based yield of gaseous products and the volume-based proportion of H 2 in these products were respectively 70.8% and 61.1% in the presence of the (Ni-Ce)/CaO catalyst with a Ni-to-Ce molar ratio of 1:0.9. The H 2 yields obtained from this material were found to gradually decrease from 763 to 681 mL/(g lignin) during five repeated uses. This gradual deactivation of the (Ni-Ce)/CaO catalyst was ascribed to both carbon deposition and the formation of CaSO 4 by reactions between sulfur in the lignin ash and the CaO component.
研究领域:
能源工程
·
催化
·
生物质利用
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
KINETICS AND CATALYSIS
·
2024
·Vol. 65
·期 3
·251-260
·
IF 1.3
Yang Zhi,Luo Mingsheng,Liu Qinglong,Li Chenmeng,Wang Yatao,Li Hongjuan,Yao Lifei
Abstract The direct production of higher alcohols from syngas in a single step remains a great challenge. In this work, a series of K and Ni promoted Mo 2 C/Al 2 O 3 catalysts were prepared by impregnation method to enhance the selectivity of Mo 2 C-based catalysts for the one-step conversion of syngas to higher alcohols. The catalysts were continuously tested under the following conditions: 300°C, 3.0 MPa, velocity—11.50 \({\text{Lg}}_{{{\text{Mo}}}}^{{ - 1}}\) h –1 , H 2 /CO ratio of 2. The catalysts promoted with K and Ni demonstrated the highest total alcohol selectivity of 67.7%. Moreover, the selectivity for total C 2+ alcohols reached as high as 56%, with 37% being ethanol. X-ray diffraction (XRD), hydrogen temperature-programmed reduction (H 2 -TPR) and X-ray photoelectron spectroscopy (XPS) characterization data reveal that K can promote the crystallinity of β-Mo 2 C, lower the catalyst reduction temperature and increase the proportion of high-valent Mo on the catalyst surface. In addition, adding Ni as a promoter to the KMo 2 C/Al 2 O 3 catalyst can generate a synergistic effect to further enhance the catalytic activity and the selectivity of higher alcohols.
研究领域:
化学工程
·
催化
·
材料科学
✓ 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）