ACS Sustainable Chemistry & Engineering
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2025
·
IF 7.3
Gaofeng Chen,Zhiwei Wang,Na Guo,Lei Liu,Huina Zhu,Qun Wang,Tingzhou Lei
Alcohols, being a substantial category of hydrogen storage liquid fuels, exhibit promising development potential. Alcohol-based hydrogen storage liquid fuels can be efficiently produced from biomass-derived syngas (CO and H2). Considerable efforts have been made in the conversion of syngas to alcohols through a higher alcohol synthesis (HAS) reaction. However, inevitably, there will be significant generation of H2O and C1 byproducts (CO2 and CH4). In this study, a hydrophobic CoCuSNT@C60 catalyst modified with fullerene (C60, an all-carbon cage molecule) was designed to hinder the formation of H2O and C1 byproducts. The hydrophobic C60 shortened the retention of H2O on the active site interface, restraining the water–gas shift reaction. This leads to a significant decrease in CO2 generation, accompanied by an increase in the CO conversion and selectivity toward alcohols. The hydrophobic CoCuSNT@C60 catalyst was characterized by X-ray diffraction, Fourier transform infrared spectra, N2 adsorption–desorption isotherms, X-ray photoelectron spectroscopy, scanning electron microscopy, and transmission electron microscopy. Compared to the unmodified CoCuSNT, the C60-modified hydrophobic CoCuSNT@C60 catalyst possesses higher CO hydrogenation activity and high alcohol selectivity, along with an impressive stability of up to 350 h to meet industrial applications.
研究领域:
能源化学
·
催化化学
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DOI
高影响因子
CARBOHYDRATE POLYMERS
·
2026
·
IF 13.2
Jinpeng Zhai,Chao Liu,Lijuan Sun,Beichen Xue,Yongxin Wu,Rui Xiao
Biomass-derived carbohydrates, as abundant and renewable feedstocks, hold great promise for producing porous carbon materials (PCMs) applicable in CO 2 capture and syngas purification. This study presents a novel strategy for synthesizing N, O-dual doped carbon (NOC) materials through co-pyrolysis using 5-hydroxymethylfurfural (5-HMF) and chitosan (CTS) as precursors, wherein 5-HMF acts as a structural modulator. Combining experimental characterization with density functional theory (DFT) calculations, this work systematically investigated the synergistic mechanism between functional group evolution and carbon framework construction during co-pyrolysis, and elucidated the influence of N, O doping configurations on CO 2 adsorption selectivity. The results indicate that the incorporation of 5-HMF promotes a three-step reaction pathway introducing N, O-containing functional groups such as imine group (C=N) and carbonyl (C=O). The NOC prepared at 800 °C exhibited a CO 2 /H 2 selectivity of 43.4 and a CO 2 /(CO + H 2 ) multicomponent selectivity of 24.4 in a continuous flow (CO 2 /CO/H 2 , 25 °C, 1 bar). Theoretical calculations further revealed that the synergistic coupling of pyridinic N and carbonyl groups on the carbon surface significantly enhances surface polarity and Lewis basicity, thereby strengthening the selective adsorption of polar CO 2 molecules via Lewis acid-base interactions and electrostatic induction.
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DOI
PubMed
高影响因子
RARE METALS
·
2025
·
IF 11
Li Qiu-Hao,Zhou Qi,Wang Yun-Long,Chen Rui-Jie,Chen Chong
Nuclear energy provides a competitive path for reduction of CO 2 with water, whereas the high-efficiency utilization of radiolytically produced active species for oriented transformation remains challenging. Herein, we report the assembling of yttrium-decorated bimetallic MOFs via one-step hydrothermal strategy, which can act as a sensitized nanoreactor for syngas production under γ-ray irradiation. The flower-shaped CuNi-MOF matrix with tunable metal centers exposed plentiful cooperative active sites for CO 2 binding, and its nanopetals enabled the well dispersion of Y 2 O 3 nanoparticles on the surfaces. The introduction of high- Z element Y enhanced the secondary electron scattering and promoted the water radiolysis to produce more hydrated electrons (e aq − ), thus accelerating the initial CO 2 activation to CO 2 •− . Moreover, the in situ formed coupling interlayer provided a fast charge transfer channel between Y 2 O 3 and the MOF framework, which facilitated the interfacial electron migration for intermediate generation and subsequent CO 2 conversion. By regulating the contents of Cu and Y 2 O 3 within the nanocomposites, the affinity toward CO 2 and the product compositions could be modulated. As a result, the optimal 7CN-2Y catalyst achieved a high syngas evolution rate of 311.07 μmol g −1 with a H 2 /CO ratio of 2.7:1 at an absorbed dose of 4 kGy. The present study offered a feasible route for the efficient transformation of CO 2 into valuable chemicals and the design of viable catalysts for ionizing radiation. Graphical abstract
研究领域:
核能化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Guang Yang,Qiang Hu,Haiping Yang,Yang Yang,Wei Cheng,Jiageng Xia,Hanping Chen
Catalytic reforming technology holds significant potential for treating biomass gasification tar. However, the design of catalysts that offer high activity, low carbon deposition, and long-term stability remains a challenge. In this study, Ni@SiO 2 yolk-shell catalysts were synthesized and evaluated for their activity and stability in toluene steam reforming. The Ni@SiO 2 -10 catalyst demonstrated excellent stability and activity, maintaining a 100 % toluene conversion rate over a 120-h test period with virtually no carbon deposition after reforming. In contrast, Ni/SiO 2 and Ni/Al 2 O 3 catalysts, synthesized by incipient wetness impregnation, showed significant sintering and carbon deposition after use. Under identical support conditions, Ni@SiO 2 reduced the initial reaction temperature for toluene steam reforming from 462 °C to 418 °C. Increasing the Ni loading significantly enhanced the number of active sites, decreased the size of the SiO 2 microspheres, and thinned the SiO 2 shell layer, thereby elevating the toluene conversion from 72 % to 100 %. Both temperature and the GHSV (gas hourly space velocity) had a significant impact on catalytic performance, with conversion rates stabilizing at 700 °C and an GHSV = 24500 h −1 . The yolk-shell structure of Ni@SiO 2 promoted high Ni dispersion, reducing aggregation and carbon deposition, which were key to its high activity and stability. These findings are crucial for the development of catalysts for biomass tar reforming.
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DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 64
·39026-39032
·
IF 3.119
Ying Zhao,Dongyue Su,Wentao Dong,Xiaoyang Xu,Xiangjing Zhang,Yongqi Hu
The investigation of highly efficient catalysts for the electrochemical reduction of carbon dioxide (ER-CO2) is the most critical challenge to commercialize conversion and utilization of CO2. Herein we propose a new and very promising catalyst, high crystallinity Sn crystals on Ni foam (Sn@f-Ni), for the electroreduction reaction of CO2 in potassium bicarbonate aqueous solution. The catalyst is fabricated in situ on a pretreated Ni foam substrate through a galvanostatic electrodeposition strategy. SEM and XRD demonstrate that high crystallinity Sn crystals, with an average size of 2–3 μm, evenly dispersed on the Ni foam support can be reproducibly obtained. Electrochemical measurements demonstrate that the Sn@f-Ni electrode at the deposition current of 15 mA exhibits superior performance in promoting the ER-CO2. Tafel measurements show that except for electrodes with a deposition current of 5 mA, the Tafel slopes of the other four electrodes are all above 100 mV dec−1, which is consistent with a rate-determining initial electron transfer to CO2 to form a surface adsorbed intermediate, a mechanism that is commonly invoked for metal electrodes. A stable composition of syngas can be obtained by electrolysis at −1.7 V potential (vs. Ag/AgCl), indicating that the Sn surface with high crystallinity conforms to the Heyrovsky–Volmer mechanism at a potential of −1.7 V. The ratio of CO and H2 generation was about 1 : 2, meaning it could be used as syngas for preparing some valuable fuels. This work provided an efficient method to convert the surplus CO2 to valuable syngas.
研究领域:
材料科学
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电化学
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环境科学
✓ 已验证
DOI
高影响因子
ENERGY
·
2022
·
IF 8.857
Haifeng Jiang,Haipeng Liu,Jiaxin Dong,Jiaxing Song,Sunhua Deng,Jie Chen,Yu Zhang,Wenpeng Hong
Using cellulose to produce high-quality oxygenated fuels or chemicals is becoming an important way to replace chemical synthesis technology. In this work, the Ce–Co–Na ternary composite metal catalyst is synthesized and used for catalytic cracking of cellulose to prepare the ketone-rich bio-oil production. To construct an environment-friendly process, CO 2 is used as a pyrolysis reaction atmosphere to improve the enrichment of ketones. Strong synergistic effects among metal components effectively promote the thermal-cracking of cellulose to produce primary products (anhydrosugars), and further convert to oxygenates due to the excellent oxygen transferability of the catalyst. The introduction of CO 2 enhances the selectivity of ketones in the liquid product, especially 2,3-dimethyl-2-cyclopenten-1-one. The highest content of ketones in the liquid is 22.73%, which is about four times higher than that of the blank sample. In addition, the generation of CO in the syngas is promoted. This study provides an alternative way for the pyrolysis of biomass to prepare ketone platform compounds and syngas production .
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DOI
高影响因子
ChemCatChem
·
2023
·Vol. 15
·期 22
·e202300967
·
IF 4.5
Ting Li,Yuhao Tian,Xiaoli Yan,Weijie Cai
Graphical CO 2 Reforming : Transition metal-based SiO 2 -Ni@CeO 2 catalyst with typical core@shell structure exhibited the better activity/stability in CO 2 reforming with ethanol reaction compared to SiO 2 -Cu@CeO 2 sample. It is of great significance to design the high-performance catalysts with good anti-sintering and coke-resistance properties which can efficiently convert undesirable greenhouse gas CO 2 with bio-ethanol into high value-added syngas. To be addressed this issue, a series of SiO 2 -M@CeO 2 (M: Cu, Ni) catalysts with typical core@shell structure were prepared via a strong electrostatic adsorption technique. Interestingly, Ni-based catalyst exhibited the higher activity towards ethanol dry reforming at the relatively low temperature. Meanwhile, SiO 2 -Ni@CeO 2 catalyst presented good stability after a 50 h tests while a serious deactivation occurred for SiO 2 -Cu@CeO 2 within 20 h reaction due to heavy carbon deposition and reactor blockage. Herein, the higher catalytic performance of SiO 2 -Ni@CeO 2 catalyst compared to SiO 2 -Cu@CeO 2 sample was attributed to the combination effect of its mesoporous structure, higher Ni dispersion as well as stronger Ni-Ce interaction as depicted by BET, TEM, XPS, H 2 -TPR and XRD findings. This work might provide meaningful information to other reforming processes involving coke formation and active metal sintering problems.
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
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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DOI
高影响因子
Catalysts
·
2019
·Vol. 9
·期 7
·606
·
IF 3.444
Chuanmin Ding,Junwen Wang,Yufeng Li,Qian Ma,Lichao Ma,Jing Guo,Zili Ma,Ping Liu,Kan Zhang
The supporting modes of active metal over mesoporous materials play an important role in catalytic performance. The location of Ni nanoparticles inside or outside the mesoporous channel of MCM-41 has a significant influence on the reactivity in partial oxidation of methane to syngas reaction. The characterization data using different techniques (Transmission Electron Microscope (TEM), X-Ray Diffraction (XRD), N2adsorption-desorption, H2Temperature-Programmed Reduction (H2-TPR), and Inductively Coupled Plasma (ICP)) indicated that nickel was located outside the mesoporous channels for the impregnation method (Ni/MCM-41), while nickel was encapsulated within MCM-41 via the one-step hydrothermal crystallization method (Ni-MCM-41). The nickel atoms were mainly dispersed predominantly inside the skeleton of zeolite. When the load amount of Ni increased, both of Ni species inside the skeleton or pore channel of zeolite increased, and the ordered structure of MCM-41 was destroyed gradually. Contributed by the strong interaction with MCM-41, the Ni particles of Ni-MCM-41 were highly dispersed with smaller particle size compared with supported Ni/MCM-41 catalyst. The Ni-MCM-41 displayed higher catalytic performance than Ni/MCM-41, especially 10% Ni-MCM-41 due to high dispersity of Ni. The confinement effect of MCM-41 zeolite also afforded high resistance of sintering and coking for 10% Ni-MCM-41 catalyst. Especially, 10% Ni-MCM-41 catalyst showed outstanding catalytic stability.Keywords:partial oxidation of methane;sintering and coking resistance;Ni location;confinement effect;MCM-41 zeolite
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DOI
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2017
·Vol. 33
·期 9
·1865-1874
·
IF 0.767
NING Hong-Yan,YANG Qi-Lei,YANG Xiao,LI Ying-Xia,SONG Zhao-Yu,LU Yi-Ren,ZHANG Li-Hong,LIU Yuan
Rh-Mn-based catalysts are promising for ethanol synthesis from syngas. In this work, a carbon fiber (CF)-supported Rh-Mn catalyst, with highly dispersed Rh and close contact Rh-Mn species, has been prepared by a new in situ polymerization route using citric acid and ethylene
glycol interaction. The structure and physicochemical properties of both the calcined and reduced samples have been characterized by TPR, XRD, TEM, EDS, CO-TPD, H2 chemisorption, and XPS techniques and the catalytic performance for ethanol synthesis from syngas has been evaluated.
The results show that the new method is beneficial in forming close contact Rh-Mn species than that obtained with the conventional impregnation method. This can enhance the dispersion and sintering resistance of Rh and effectively improve the activity of CO hydrogenation and the selectivity
to ethanol in ethanol synthesis from syngas.
研究领域:
化学工程
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材料科学
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催化化学
✓ 已验证
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2020
·
IF 6.551
Mi Yan,Hongcai Su,Zhihao Zhou,Dwi Hantoko,Jianyong Liu,Jingyi Wang,Runpei Wang,Ekkachai Kanchanatip
The effluent of food waste (FWE) is generated during food waste treatment process. It contains high organic matter content and is difficult to be efficiently treated. In this study, the sample was collected from a 200 t/d food waste treatment center in Hangzhou, China. Subcritical and supercritical water gasification were employed to decompose and convert FWE into energy. The effects of reaction temperature (300–500 °C), residence time (20–70 min) and activated carbon loading (0.5–3.5 wt%) on syngas production and the remaining pollutants in liquid residue were investigated. It was found that higher reaction temperature and longer residence time favored gasification and pollutant decomposition, resulting in higher H 2 production and gasification efficiencies. It is noteworthy that the NH 3 -N was difficult to be converted and removed under current experimental conditions. The addition of activated carbon was found to increase the gasification efficiency. The highest total gas yield, H 2 yield, carbon conversion efficiency, gasification efficiency, total organic carbon removal efficiency and chemical oxygen demand removal efficiency were obtained from gasification at 500 °C for 70 min with 3.5 wt% activated carbon.
研究领域:
环境科学
·
能源工程
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Jingjing Zhang,Yang Feng,Lixia Ling,Caiping Ma,Jungang Wang,Riguang Zhang,Maohong Fan,Bo Hou,Debao Li,Baojun Wang
The direct conversion of syngas to ethanol faces challenges due to catalyst inefficiencies and low ethanol yield. Bulk alloys with an appropriate atomic ratio can exhibit excellent catalytic performance. In this work, a series of Rh x Ni y (111) with different Rh/Ni ratios was rationally designed, and the ethanol preparation from syngas was explored based on density functional theory (DFT) calculation and microkinetic analysis. The results show that Rh 1 Ni 1 (111) was screened out to show optimum catalytic performance for ethanol production. This was attributed to a moderate quantity of charge transfer from Ni to Rh atoms, and a medium distance from the d -band center to the Fermi level. Further, to verify the catalytic performance of the catalysts at a Rh: Ni ratio of 1: 1, 1Rh1Ni/γ-Al 2 O 3 catalyst was prepared and its catalytic performance for ethanol preparation from syngas was investigated by comparing it with that of Rh/γ-Al 2 O 3 and Ni/γ-Al 2 O 3 . The catalytic performance of 1Rh1Ni/γ-Al 2 O 3 has been further confirmed to be preferred over Rh/γ-Al 2 O 3 and Ni/γ-Al 2 O 3 , achieving a 23.0 % CO conversion rate with 31.2 % ethanol selectivity.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 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）