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
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
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
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催化
·
生物质利用
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化学工程
·
环境科学
✓ 已验证
产品关联
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
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可再生能源
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催化
·
生物质转化
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2018
·
IF 11.384
Tian-yuan Chen,Junjie Su,Zhengpai Zhang,Chenxi Cao,Xu Wang,Rui Si,Xianglin Liu,Bianfang Shi,Jing Xu,Yi-Fan Han
CeO2 nanorods supported Co–CoOx catalysts showed high selectivity for higher alcohol synthesis (HAS) from syngas. The selectivity has found to increase with lowering the Co loadings, and the value over Co1/CeO2 (19.86%) is twice higher than that over Co5/CeO2 (8.67%). The active sites at the interfaces between Co0 and CoOx, or to say, Co–CoOx pairs, have evidenced to be responsible for HAS. The strong metal–support interactions between Co and CeO2 retard the reduction of CoOx and stabilize the intermediates such as CO–Coδ+. Likely, CO favors dissociating on the metallic Co surface to form CHx species, while CO is associatively activated on Coδ+ sites. Moreover, the structure evolution of the Co–CoOx interface was revealed during calcination, reduction, and reaction using in situ X-ray diffraction (XRD), in situ Raman spectroscopy, X-ray absorption spectroscopy (XAS), and in situ diffuse reflectance infrared fourier transform spectroscopy (CO-DRIFTS). The structure–performance relationship of HAS over Co/CeO2 was proposed.
研究领域:
催化化学
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材料科学
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化学工程
·
无机化学
✓ 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
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Fen Wang,Wei-Zhen Li,Jing-Dong Lin,Zhi-Qiang Chen,Yong Wang
Catalyst durability is one of the major problems hindering the commercialization of partial oxidation of methane (POM) for syngas production. We report that a Pt/MgAl 2 O 4 -HS catalyst with the MgAl 2 O 4 -HS support being synthesized via hydrolysis solvothermal (HS) method demonstrates high stability for POM during a 500 h life testing at 900 °C without detectable coke formation, while a Pt/MgAl 2 O 4 -CP counterpart in which MgAl 2 O 4 was prepared by an optimized co-precipitation (CP) method exhibits continuous deactivation accompanied by coking. Using a suite of characterizations incluidng BET, H 2 chemisorption, XRD, STEM, TEM, TG/DTA and TPD of NH 3 and CO 2 , we reveal that the high catalytic durability of the Pt/MgAl 2 O 4 -HS is due to the spinel surface of MgAl 2 O 4 -HS that can efficiently stabilize Pt against sintering. The Pt/MgAl 2 O 4 -CP, however, has defect Al 2 O 3 or MgO-like species on the MgAl 2 O 4 -CP surface, inhibiting its capability to stabilize Pt. We confirm that the POM reaction undergoes a combustion-reforming pathway by monitoring the temperatures and gaseous product compositions along the catalyst bed. These results provide guidance for rational design of a longevity catalyst for POM process.
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
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Jiaming Wang,Guilong Liu,Huixian Zhong,Pengfei Song,Kang An,Ziyang Zhang,Ang Cao,Yuan Liu
In this work, Co δ+ -Co 2 C decorated-Co-Ni alloy nanoparticles (NPs) loaded on Mg-Al-O complex oxides were fabricated via an in-situ reduction and topochemical carbonization strategy by using hydrotalcite as the precursor. The Co δ+ -Co 2 C decorated-Co-Ni alloys were obtained via the following process: (I) after reduction, Co-Ni alloy was obtained and Co could donate electrons to Ni in the Co-Ni alloy NPs; (II) in syngas atmosphere, some of cobalt atoms on the surface of Co-Ni NPs reacted with CO and were converted to Co 2 C. Resultantly, in the reaction process, Co-Ni alloy NPs were transformed into Ni-Co alloy@Co-Co 2 C, a core-shell structure with Ni-Co alloy core and Co-Co 2 C shell. When used as the catalysts for direct ethanol synthesis (DES) from syngas, the bimetallic Co-Ni alloy@Co-Co 2 C catalyst performed excellent selectivity to ethanol, owing to the regulation of dissociatively and associatively adsorbed CO by Co δ+ -Co 2 C active sites formed on the surface of Co-Ni alloy NPs. Moreover, the mutual dilution between Co and Ni in the Co-Ni alloy NPs inhibited the generation of heavy hydrocarbons, further improving the selectivity to alcohols. The total alcohol selectivity of 43.0% and ethanol occupied 45.2 wt% could be reached over the optimal catalyst.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Yang Liu,Haimiao Yu,Jiecheng Liu,Dezhen Chen
In this study, innovative Ni-based catalysts supported by five typical slag carriers (magnesium slag (MS), steel slag (SS), blast furnace slag (BFS), pyrite cinder (PyC) and calcium silicate slag (CSS)) were prepared by wet impregnation. With the prepared catalysts and Ni/γ-Al 2 O 3 catalyst, catalytic reforming of pyrolysis volatiles from pine sawdust for syngas production and tar removal was investigated. The catalysts were characterized by BET, XRD , SEM, TEM and Raman. The catalytic performances of the six catalysts were decreasing in the following order: Ni/MS > Ni/γ-Al 2 O 3 > Ni/SS > Ni/BFS > Ni/CSS > Ni/PyC. Ni/MS catalyst exhibited excellent catalytic reactivity as well as thermal stability in terms of tar conversion (95.19%), gas yield (1.46 Nm 3 /kg) and CO 2 capture ability (CO 2 yield of 0.5%). Both amorphous carbon and graphite-type carbon were formed on the catalysts after catalytic reforming and the D/G ratio (the relative intensity ratio of the D-band to the G-band) was positively correlated to the catalytic activity .
研究领域:
催化
·
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Huixian Zhong,Jiaming Wang,Shaoxia Guo,Kegong Fang,Yuan Liu
In this work, Rh–Co/La2O3–SiO2 showed excellent selectivity to ethanol for direct ethanol synthesis from syngas. The best catalyst exhibited 42.8% selectivity to ethanol with CO conversion of 12.3% and in 145 h’ running maintained stable at 553 K, 3 MPa and GHSV of 3900 mL (gcat h)−1. The investigate results indicated that the interaction of cobalt denoting electron to rhodium adjusted the amounts of carbon monoxide adsorbed associatively and dissociatively, and maybe created a new active site pair of Rh0/Coδ+ for generating ethanol. Moreover, the mutually doping effect could dilute Co and Rh atoms in Rh–Co nanoparticles (NPs), which effectively suppressed the formation of C2+H and C3+OH, and thus led to the high ethanol selectivity and good anticoking property assisting with the carbon eliminating effect of La2O3. Owing to the high dispersion of Rh–Co NPs, the catalyst showed good activity and high resistance to sintering.
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
危险品化学品经营许可证（带存储）