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Energy Technology · 2020 ·Vol. 8 ·期 9 ·2000205 · IF 3.404

Highly Dispersed Ni–Fe Alloy Catalysts on MgAl2O4 Derived from Hydrotalcite for Direct Ethanol Synthesis from Syngas

Qiang Liu,Jiaming Wang,Kang An,Siran Zhang,Guilong Liu,Yuan Liu

In view of the dual active sites mechanism of direct ethanol synthesis and the excellent catalytic performance of bimetallic catalysts, a series of Ni–Fe alloy catalysts with different Ni/Fe molar ratios derived from layered double hydroxides (LDHs) precursors are synthesized. During the calcination and reduction process of LDHs precursors, the Ni–Fe alloy is obtained, and attributed to all the elements being evenly dispersed at the atomic level in the LDHs precursors; meanwhile, a strong interaction between Ni–Fe alloy and MgAl 2 O 4 support exists. As a result, Ni–Fe alloy nanoparticles are highly dispersed on the MgAl 2 O 4 surface. The high CO adsorption ability on the Ni–Fe alloy and synergism catalysis between Ni and Fe result in excellent catalytic activity and high selectivity to ethanol on the bimetallic Ni–Fe alloy. In addition, the strong antisintering ability and stable alloy structure bring about a good catalytic stability. This research proposes a new catalytic system for direct ethanol synthesis from syngas.

研究领域: 化学工程 · 催化材料科学
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Catalysis Science & Technology · 2019 ·Vol. 9 ·期 13 ·3454-3468 · IF 5.726

Nanoparticles of Rh confined and tailored by LaFeO3–La2O3 on SiO2 for direct ethanol synthesis from syngas

Huixian Zhong,Jiaming Wang,Kang An,Kegong Fang,Yuan Liu

A catalyst with a novel composition for direct ethanol synthesis from syngas was prepared and investigated in this work, which is Rh nanoparticles (NPs) highly dispersed on La2O3 modified LaFeO3, and the Rh NPs/La2O3–LaFeO3 was loaded on SiO2 with high surface area. The catalyst was prepared by using LaFe1−xRhxO3 in the perovskite phase as the precursor, which was transformed to Rh/La2O3–LaFeO3/SiO2 after reduction. The results showed that, compared to Rh–La2O3/SiO2, the activity and selectivity to ethanol were improved markedly, which was ascribed to the well-matched catalyzing process by the active sites of Rh0, Rh+ (or Rhδ+) and the oxygen vacancies on the surface of LaFeO3; of those, Rh0 dissociatively adsorbed CO and the latter two associatively adsorbed CO. Moreover, the interaction of La2O3 and LaFeO3 donated electrons to rhodium, which effectively adjusted the ratio of CO adsorbed associatively and dissociatively, and thus improved the selectivity to ethanol and lowered the selectivity to methanol. The catalyst also exhibited excellent resistance to the sintering of Rh NPs and to carbon deposition, which was attributed to the confinement of Rh NPs by La2O3 and LaFeO3, the eliminating effect of La2O3 and LaFeO3 and the very high dispersion of Rh NPs.

研究领域: 催化化学 · 材料科学
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY · 2020 · IF 5.278

Production of hydrogen-rich syngas and multiwalled carbon nanotubes by biogas decomposition over zirconia supported iron catalysts

Manoj Pudukudy,Zahira Yaakob,Khaleeda Mhd Syahri,Qingming Jia,Shaoyun Shan

A set of Fe/ZrO 2 catalysts were successfully synthesized by a facile urea-assisted solid-state combustion method, and their catalytic test was evaluated for the thermal decomposition of undiluted-biogas into hydrogen-rich syngas and multiwalled carbon nanotubes (MWCNTs). The as-prepared catalysts were characterized by X-Ray diffraction (XRD), Scanning and Transmission electron microscopy (SEM and TEM), Nitrogen-physisorption, X-ray photoelectron spectroscopy and Temperature programmed reduction analyses. The iron was found in the form of hematite and metallic-iron in the fresh and reduced catalysts respectively. A suitable metal-support interaction due to the fine surface dispersion of iron species on ZrO 2 was observed in the catalysts. The N 2 -physisorption analysis indicated the reduced surface area of the catalysts after iron loading. However, it does not influence the catalytic efficiency since the metal amount and metal-support interaction was determined to play the main role. The Fe/ZrO 2 catalysts exhibited improved catalytic efficiency. With increasing the amount of iron and increasing the reaction temperature, the CH 4 and CO 2 conversions were increased significantly. A highest CH 4 and CO 2 conversions of 92% and 89% respectively, with an H 2 /CO ratio of ∼2.25 were obtained for the 50%Fe/ZrO 2 catalyst at 900   °C. The enhanced catalytic performance could be attributed to the fine-surface dispersion of iron-nanocrystals on ZrO 2 . Moreover, the MWCNTs were characterized by XRD, SEM, TEM and Raman analyses for their structural properties.

研究领域: 催化化学 · 材料科学 · 能源工程
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Theoretical and experimental insights into CO2 formation on Co2C catalysts in syngas conversion to Value-Added chemicals

Minhua Zhang,Haipeng Yu,Yuzhe Sun,Yingzhe Yu,Yifei Chen,Lingtao Wang

Cobalt carbide (Co 2 C) has been discovered as the promising active phase for Fischer–Tropsch to olefins (FTO) process and higher alcohols synthesis (HAS) from syngas, in the form of nanoprisms and nanospheres, respectively. However, CO 2 formation is inevitable on Co 2 C catalysts, especially in FTO process. So far, the mechanism of CO 2 formation on Co 2 C surfaces is less understood. This work provides fundamental insights into CO 2 formation on Co 2 C nanospheres and nanoprisms through computational and experimental study. DFT calculations demonstrate that: Co 2 C (1   0   1) and (0   2   0) surfaces exposed on Co 2 C nanoprisms are basically not active for water gas shift (WGS) reactions but the introduction of Na greatly promotes CO 2 formation. CO 2 is less favored on Co 2 C(1   1   1) surface which is dominant on Co 2 C nanospheres, however, the reverse WGS activities can be promoted with Na addition. The experimental results confirmed removing Na from Co 2 C can efficiently suppress WGS activity, thus reducing CO 2 selectivity while the selectivity of light olefins retained. Though previous studies focused on Na addition to promote the yield of light olefins, our work indicates that Na also promotes undesired CO2 formation. Our results suggest that Na is crucial for active phase formation but not necessarily beneficial during the CO hydrogenation reactions.

研究领域: 化学工程 · 催化科学
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FUEL · 2022 · IF 8.035

Insight into the direct conversion of syngas toward aromatics over the Cu promoter Fe-zeolite tandem catalyst

Chengyan Wen,Ke Jin,Luying Lu,Qian Jiang,Jingcheng Wu,Xiuzheng Zhuang,Xinghua Zhang,Lungang Chen,Chenguang Wang,Longlong Ma

Direct conversion of syngas into aromatics (STA) on the tandem catalyst containing Fischer-Tropsch (F-T) synthesis catalysts and acid zeolites, especially Fe-based catalysts and ZSM-5, has been attracting significant attention due to the higher cost efficiency. Even though promoters have frequently been added into the Fe-based part to improve the performance of STA reaction, its motivating mechanism is still unclear in the tandem catalyst system. Herein, the influence of the Cu promoter was evaluated for the catalytic activity of Fe-based/zeolite tandem catalysts in the STA process. Moreover, the working mechanism of the Cu promoter had been systematically investigated by adding different copper amounts and deliberately designed experiments. It was demonstrated that the addition of copper could improve aromatic selectivity because the Cu promoter could facilitate CO to participate in the conversion of olefins into aromatics over the tandem catalyst. In addition, the Cu promoter doped into the Fe-based catalyst drastically suppressed methane formation and enhanced the stability of the catalyst in the STA reaction. These findings provide insights into the effect of the Cu promoter on producing aromatics from syngas over the Fe-based/zeolite tandem catalyst system.

CAS / MDL: 10025-77-1
研究领域: 催化 · 化学工程 · 材料科学
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FUEL PROCESSING TECHNOLOGY · 2022 · IF 8.129

Effect of ZnO morphology on the performance of CuZnAl slurry catalysts for the ethanol synthesis from syngas

Jing Liu,Yinzhao Jia,Sen Wang,Jinchuan Fan,Wei Huang

The impact of nanomaterial morphology on the structures of catalysts has drawn intense interest. Based on previous work, we discovered that ZnO plays an essential role in the ethanol production . In this research, we discussed the impact of ZnO with different morphology (rod-like, granular-like and flower-like) on the performance of CuZnAl slurry catalysts for the ethanol production. The catalytic performance was evaluated at H 2 /CO = 2, 250 °C and 4.0 MPa, and the catalyst structures were tested by XPS, in situ DRIFT and so on. The results show that CuZnAl catalysts prepared with rod-like and granular-like ZnO show the better selectivity of methanol and DME, which is assigned to the highly dispersion of Cu species and more quantity of acidic sites, respectively. CuZnAl catalyst prepared with flower-like ZnO possesses the higher total alcohol selectivity (45.0%) and the highest ethanol proportions in total alcohol (50.0%). Flower-like ZnO that exposed more polar (002) facets results in more surface defect structures (oxygen vacancy, Zn (2-δ) ) and high ratio of Cu 0 /Cu + in this catalyst, all of which are related to the formation of ethanol.

CAS / MDL: 1314-13-2
研究领域: 催化化学 · 纳米材料科学
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Efficient visible-light-driven CO2 reduction into tunable syngas by cobalt phthalocyanine modified flower-like ZnIn2S4 nanosheets

Shuming Li,Hongbang Rui,Tengfei Bao,Yuanyuan Qi,Heng Rao,Ping She,Jun-sheng Qin

Photocatalytic carbon dioxide (CO 2 ) reduction into syngas (the mixture of CO and H 2 ) has been considered as an attractive method to solve the greenhouse effect and energy shortage. Polychalcogenides semiconductors such as ZnIn 2 S 4 (ZIS) have been widely utilized in photocatalysis but are still hampered by limited photo-induced charge separation and poor product selectivity. Molecular catalysts for CO 2 reduction possess superior selectivity for specific reduction products but suffer from low stability and recycling difficulty. Herein, we modified a molecular phthalocyanine (Pc) on flower-like ZIS nanosheets. This hybrid exhibited enhanced photocatalytic CO 2 reduction and exhibited a tunable ratio of CO/H 2 in syngas (0.01–4.65) under visible light irradiation. The enhanced photocatalytic activity of ZIS-Pc hybrids can be attributed to dimension-matched ultrathin heterojunction, which facilitated charge separation, broad light utilization, and recycling stability. The unique design holds great potential for other highly efficient photocatalytic reactions.

研究领域: 化学 · 材料科学 · 环境科学
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FUEL PROCESSING TECHNOLOGY · 2023 · IF 7.5

Enhanced conversion of syngas to high-quality gasoline hydrocarbons over ZnZrOx coupled SAPO-11 nanosheets bifunctional catalyst

Saisai Liu,Jing Liu,Guanyi Chen,Jingang Yao,Beibei Yan,Weiming Yi,Zhanjun Cheng,Chunyan Tian,Huijie Zao

Syngas is a key precursor for synthesizing gasoline (C 5 -C 11 ) hydrocarbons, offering an efficient route for utilizing non-petroleum carbon sources. However, the conventional Fischer-Tropsch synthesis (FTS) process faces a constraint with a maximum 45% selectivity for C 5 -C 11 , attributed to the Anderson-Schultz-Flory (ASF) distribution. Herein, bifunctional catalysts comprising ZnZrO x with different Zr/Zn ratios along with SAPO-11 zeolite sieves featuring varied morphologies like nanosheets (SA-A), petals (SA-B), and spheres (SA-C) have been effectively formulated and employed for the syngas-to-gasoline hydrocarbons (STG) reaction. Notably, the selectivity toward C 5 -C 11 far exceeded the ASF limits. Under identical reaction parameters, the Zn 1 Zr 4 O x /SA-A catalyst demonstrated notable enhancements of 6.6% and 26.2% in CO conversion, along with 4.6% and 7.6% increases in C 5 -C 11 selectivity, as compared to that of Zn 1 Zr 4 O x /SA-B and Zn 1 Zr 4 O x /SA-C catalysts, respectively. Furthermore, under the ideal conditions (380 °C, 4.5 MPa and gas hourly space velocity (GHSV) of 2400 mL min −1  g −1 ), Zn 1 Zr 4 O x /SA-A exhibited an exceptional C 5 -C 11 selectivity of 69.8% (CO 2 -free) alongside a single-pass CO conversion of 30.4%. Impressively, isoparaffin constituted 39.2% of the total composition , with the iso/n-paraffin ratio reaching 11.8. Even after 100 h, the catalyst maintained its remarkable catalytic activity , with the CO conversion and C 5 -C 11 selectivity maintaining levels of 27.5% and 66.85%, respectively.

研究领域: 化学工程 · 催化科学
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Catalysts · 2025 ·Vol. 15 ·期 11 ·1032 · IF 4

Modified Metal-Doped Fe-Al Catalysts for H2-Rich Syngas Production from Microwave-Assisted Gasification of HDPE Plastic

Jingmo Zhou,Chaoyue Liu,Wenke Zhao,Faizan Ahmad,Yaning Zhang

This study pioneers the application of metal-doped Fe-Al as multifunctional redox catalysts for tunable syngas production from plastics via a microwave-assisted process (CLG). We rationally designed a series of redox catalysts (Ni, Ca, Ce, Sr, Co) to unlock efficient H2-rich syngas production from (high-density polyethylene) HDPE. A class of metal-doping (Ni, Ca, Ce, Sr, and Co) Fe-Al redox catalysts was engineered, with Ni-doped Fe-Al (Ni-Fe-Al) exhibiting the excellent H2-rich syngas production (75.32 mmol/gHDPE syngas, 47.09 mmol/gHDPE H2). This is attributed to the improved redox activity, which facilitates efficient lattice oxygen transfer and catalytic reforming reactions, alongside improved microwave absorption and a porous structure that promotes reactant access. This strategic material design, coupled with process parameter optimization (800 W, redox catalyst/plastic = 2.0), developed a highly efficient HDPE-to-syngas conversion system. The process produced a high-quality syngas (90.03% H2+ CO, H2/CO ratio = 2.27) with a rapid heating rate (233.0 °C/min) and minimal energy input (3.52 kWh/molgas). This work provides not just an effective upcycling route for plastics, but a fundamental blueprint for designing advanced redox catalysts to unlock the full potential of microwave-CLG.

研究领域: 催化化学 · 能源工程 · 环境科学 · 材料科学 · 化学工程
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ENERGY · 2021 · IF 7.147

Investigation on hydrogen-rich syngas production from catalytic co-pyrolysis of polyvinyl chloride (PVC) and waste paper blends

Chao Wang,Zhiqiang Jiang,Qingbin Song,Mingzheng Liao,Jiahong Weng,Rui Gao,Ming Zhao,Ying Chen,Guanyi Chen

Urgent need for waste disposal and renewable energy have opened up promising pathways for renewable and sustainable fuel production to substitute traditional fossil fuels. In this study, catalytic co-pyrolysis of waste paper (WP) and polyvinyl chloride (PVC) as typical municipal solid wastes was experimentally investigated towards hydrogen-rich syngas production . Results indicated the maximum H 2 yield (429 μmol·g cat −1 ·min −1 ) was obtained with 60% PVC weight ratio under 900 °C which was higher than single component pyrolysis . Higher hydrogen yield (681.76 μmol·g cat −1 ·min −1 ) appeared over Fe/CeO 2 –CaO under the optimal conditions compared to that of Ru/ZSM-5-CaO (445.54 μmol·g cat −1 ·min −1 ). From the calculated non-isothermal kinetic parameters , both catalysts could reduce activation energies. Proper porous structure and CaO content in the catalyst could enhance hydrogen production via carbon species fixation.

研究领域: 能源科学 · 环境工程
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FUEL PROCESSING TECHNOLOGY · 2023 · IF 7.5

Catalytic pyrolysis of waste cooking oil for hydrogen-rich syngas production over bimetallic Fe-Ru/ZSM-5 catalyst

Liujie Xu,Yi Li,Mingzheng Liao,Qingbin Song,Chao Wang,Jiahong Weng,Ming Zhao,Ningbo Gao

Waste cooking oil (WCO) energy development offers an effective method for producing renewable fuels , enabling simultaneous resource recovery and pollution reduction. This study aims to develop a novel bimetallic Fe(Ni)-Ru/ZSM-5 catalyst toward H 2 -rich syngas production from WCO. The results show that Fe-Ru/ZSM-5 produced a higher maximum H 2 yield (84.05 μmol·g cat. −1 ·s −1 ) than did Ni-Ru/ZSM-5 (41.76 μmol·g cat. −1 ·s −1 ) when fed at a 50 L/min rate at an optimal temperature of 700 °C. Fe-Ru/ZSM-5 presented a more prolific microporous distribution, whose structure contributes to the diffusion of the short-chain hydrocarbon intermediate reactants to enhance hydrogen production . Fe(III) can help to improve the conversion ratio of benzene and the anti‑carbon deposition capability of the catalyst. The dealumination and oxidation decreases the stability of the catalyst and may lead to inactivation. Furthermore, this study discusses the mechanism of bimetallic-loaded catalysts combining noble metals with transition metals in WCO pyrolysis . The results point to effective new approaches to increase H 2 production through the catalytic pyrolysis of WCO.

研究领域: 化学工程 · 环境科学 · 能源技术 · 催化
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2020 · IF 4.939

Chemical looping steam reforming of bio-oil for hydrogen-rich syngas production: Effect of doping on LaNi0.8Fe0.2O3 perovskite

Chenlong Liu,Dong Chen,Jangam Ashok,Plaifa Hongmanorom,Wenju Wang,Tianle Li,Zhigang Wang,Sibudjing Kawi

Chemical looping steam reforming of bio-oil is novel conversion technology utilizing waste energy, which is an advantage to reduce cost and improve environmental. However, complex reaction process between oxygen carrier and bio-oil constrain its development. In this study, perovskite based La 0.8 M 0.2 Ni 0.8 Fe 0.2 O 3 (M = Ca, Ce and Zr) were investigated as an oxygen carrier for chemical looping steam reforming of bio-oil model reaction. The perovskites were prepared via sol-gel method and the effect of doping for reforming of acetic acid as bio-oil model compound is also investigated. Among all the perovskite tested, Ce doped La 0.8 Ce 0.2 Ni 0.8 Fe 0.2 O 3 oxygen carrier gave superior and stable catalytic performance for 1440 min at 600 °C and steam/carbon mole ratio (S/C = 2). The fresh and spent oxygen carriers were characterized using XRD , H 2 -TPR, CO 2 -TPD, TG-DTG, Dielectric constant , Raman, XPS and XANES . Doping with base metal generally, improved coke resistance ability of the perovskite. CO 2 -TPD and XPS analysis reveal that the highest carbon resistance for La 0.8 Ce 0.2 Ni 0.8 Fe 0.2 O 3 perovskite is due to enhanced stronger surface basicity and oxygen adsorption. From DFT simulation and Dielectric constant results, the better activity for La 0.8 Ce 0.2 Ni 0.8 Fe 0.2 O 3 is attributed to its adsorption ability of reactants, oxygen and electron transfer from sub-surface to surface of the perovskite.

研究领域: 能源科学 · 催化化学 · 材料科学
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