ACS Catalysis
·
2023
·
IF 12.9
Xingzhen Qi,Tiejun Lin,Yunlei An,Xinxing Wang,Dong Lv,Zhiyong Tang,Liangshu Zhong
Constructing highly efficient dual active sites for preferential formation of higher oxygenates via direct syngas conversion remains a grand challenge. Herein, we reported that the regulation of oxygen vacancy density of metal–oxide support could effectively promote the production of oxygenates. Compared with an inert SiO2-supported Co-based catalyst, the rutile TiO2-supported catalyst with abundant oxygen vacancies exhibited up to 44.7% CO conversion with the selectivity and space–time yield (STY) of the oxygenate increased to 43.4 wt % and 50 mg gcat.–1 h–1, respectively. Further studies established a nearly linear relationship between the density of the oxygen vacancy and the atomic ratio of Co2+/Co0 or the STY of oxygenated products. Characterization confirmed that the oxygen vacancies not only promote CO adsorption, dissociation, and subsequently the carburization of cobalt species to form Co2C but also create a C-rich and H-poor local microchemical environment that benefits CO associative adsorption and C═O bond insertion to form oxygenates. The synergistic effect of oxygen vacancies and the Co0/Co2C interface site contributed to the observed enhanced performance for direct syngas conversion to higher oxygenates.
研究领域:
催化化学
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材料科学
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能源化学
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产品关联
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2024
·Vol. 18
·期 10
·1-10
·
IF 4.3
Zhao Qiao,Wang Hongyu,Liang Haoting,Han Xiaoxue,Wei Chongyang,Wang Shiwei,Wang Yue,Huang Shouying,Ma Xinbin
Lower olefins, produced from syngas through Fischer-Tropsch synthesis, has been gaining worldwide attention as a non-petroleum route. However, the process demonstrates limited selectivity for target products. Herein, a hybrid catalyst system utilizing Fe-based catalyst and SAPO-34 was shown to enhance the selectivity toward lower olefins. A comprehensive study was conducted to examine the impact of various operating conditions on catalytic performance, such as space velocity, pressure, and temperature, as well as catalyst combinations, including loading pattern, and mass ratio of metal and zeolite. The findings indicated that the addition of SAPO-34 was beneficial for enhancing catalytic activity. Furthermore, compared with AlPO-34 zeolite, the strong-acid site on SAPO-34 was identified to crack the long-chain hydrocarbons, thus contributing to the lower olefin formation. Nevertheless, an excess of strong-acid sites was found to detrimentally impact the selectivity of lower olefins, attributed to the increased aromatization and polymerization of lower olefins. The detailed analysis of a hybrid catalyst in Fischer-Tropsch synthesis provides a practical strategy for improving lower olefins selectivity, and has broader implications for the application of hybrid catalyst in diverse catalytic systems.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
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2025
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IF 6.2
Weiqi Chen,Tingting Xu,Runtian Yu,Zhimei Shu,Jiayi Xiao,Dong Liu
Flame synthesis of oxygen carriers (OCs) with specific functions remains challenging. In this study, the brownmillerite Ca 2 Fe 2 O 5 OCs properties are precisely regulated by adjusting the type of ester solvent, oxygen concentration, and carrier gas flow rate during diffusion flame synthesis. The utilization of flame-synthesized OCs in the chemical looping reforming coupled with water splitting (CLRWS) to produce syngas and hydrogen has been elucidated. At a high oxygen concentration (60 % O 2 ), OCs synthesized using propyl propionate solvent aerosol flame, yielding 33 nm polycrystalline particles, exhibit exceptional performance with an 82.6 % fuel conversion rate, 3.09 Nm 3 /L syngas yield, and 11.16 mmol/g OC hydrogen yield at 850 °C, surpassing classical methods. The high reduction capacity and lattice oxygen activity can be attributed to the multiple exposed crystal faces and active sites. This study aimed at regulating and producing OCs with excellent activity for biomass utilization and catalysis.
研究领域:
材料科学
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能源化学
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催化化学
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化学工程
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纳米材料
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可再生能源
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多相催化
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产品关联
DOI
高影响因子
ACS Applied Energy Materials
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2020
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IF 4.473
Yuanxing Wang,Cailing Niu,Yachuan Zhu,Da He,Weixin Huang
Producing syngas from electrochemical reduction of CO2 by renewable energy offers an opportunity to reduce CO2 emissions and provide chemicals and fuels. Herein, we report the careful manipulation of the reduction treatment to synthesize copper nanowire arrays (Cu NAs). By thermal oxidation, copper oxide nanowires were grown on a Cu mesh. Then, thermal reduction and electrochemical reduction were used to reduce copper oxide to Cu with the morphologic features largely preserved. The derived Cu NAs are cost-effective electrocatalysts capable of reducing CO2 and H2O for tunable syngas production. It is demonstrated that syngas, the mixture of H2 and CO, could be attained with a wide range of compositions (from 1:2 to 3:1) from CO2 reduction and H2O reduction on these Cu NAs in aqueous solutions. In addition, Cu NAs show a high current density, 4 mA/cm2, at a low potential, −0.5 V, with a high syngas faradaic efficiency of over 70%. This approach explores a new method that sheds light on tuning the syngas composition from the electrochemical CO2 reduction by Cu-based catalysts.
研究领域:
电化学
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材料科学
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可再生能源
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催化
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
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2018
·Vol. 11
·期 3
·1112-1122
·
IF 4.674
Chang Liu,Xue-Ying Cui,Yong-Hong Song,Min-Li Zhu,Zhao-Tie Liu,Zhong-Wen Liu
Graphical Cutting edge : The bulk MoS 2 with varied crystallite sizes was investigated for the catalytic hydrogenation of CO, and a hexagonal-prism-shaped model was developed to describe the nature of different active sites on the MoS 2 crystallite. The CO conversion decreased in the order of rim sites > edge sites ≫ basal sites, and the highest activity over the bulk MoS 2 with smallest particles was ascribed to the highest exposure of the rim sites. Molybdenum disulfides are attractive sulfur-tolerant catalysts suitable for the direct conversion of sulfur-containing syngas, which avoids the expensive step of the deep desulfurization. However, the catalytic activity of MoS 2 -based catalysts is relatively low. To improve the activity, previous works have focused on modifying MoS 2 with various promoters and supports, but the structural aspects are largely overlooked. In this work, we investigated the active nature of the MoS 2 -based catalysts for the catalytic hydrogenation of carbon monoxide. Thus, the bulk MoS 2 with varied crystallite sizes was synthesized by the hydrothermal and the thermal decomposition methods. The catalysts before and after catalytic tests were characterized by in-situ X-ray diffraction, X-ray photoelectron spectroscopy, and transmission electron microscope techniques. The CO hydrogenation under low-temperature methanation conditions (The syngas with a H 2 /CO=2 and 40.0 ppm H 2 S, T=360 °C, and P=2 MPa) was applied to evaluate MoS 2 as a catalyst for converting syngas. The catalytic results indicate that the MoS 2 with smaller crystallite sizes exhibited a higher CO conversion. By correlating the structural propriety with the catalytic activity, a hexagonal-prim-shaped model was developed to describe different sites on the MoS 2 crystallite. Based on this model, the activity of different active sites on the bulk MoS 2 for CO hydrogenation decreased in the order of rim sites > edge sites ≫ basal sites. The highest catalytic activity over the bulk MoS 2 with smallest particles was attributed to the highest exposure of the rim sites.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
Reaction Chemistry & Engineering
·
2022
·Vol. 7
·期 6
·1447-1460
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IF 5.2
Jianchao Liu,Hong Xu,Jinxiang Dong,Ligong Zhou,Xuekuan Li,Hui Ge
The synthesis of alkylbenzenes produced from syngas and benzene over a ZnCrOx/beta bifunctional catalyst has been studied. Our characterization results showed that in the mixed catalyst the beta-zeolite crystallites were dispersed on the surface of the ZnCr oxides. The close contact facilitated the methanol intermediate formed on ZnCrOx to diffuse to the acidic sites of the beta-zeolite crystallites, reacting with benzene to produce alkylbenzenes. The competitive side reactions, which lead to by-products such as CO2 and hydrocarbons, were suppressed. The medium strong acidity and mesopores of the beta-zeolite crystallites contributed to the high activity and selectivity. The optimized ZnCrOx/beta-11 = 1 : 3 (w/w) afforded 40.72% benzene and 62.40% CO conversion with high alkylbenzene selectivity during the initial stage of the reaction, which then underwent quick deactivation, and maintained a benzene conversion of ∼27%. Coke formation on the beta-zeolite crystallites was proposed to be the main cause of deactivation.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Yanpeng Chen,Xing Zhu,Kongzhai Li,Yonggang Wei,Yane Zheng,Hua Wang
Syngas generation via thermochemical H2O–CO2 splitting relies heavily on a high-temperature decomposition of metal oxides into a reduced state. Meanwhile, typical chemical looping partial oxidation of methane to syngas suffers from the carbon deposition and the low selectivity toward syngas. To overcome these drawbacks, the partial oxidation of methane and H2O–CO2 splitting are coupled to consist of an alternative chemical looping redox scheme for the generation of Fischer–Tropsch (F–T)-ready syngas. The usability of lattice oxygen in a redox catalyst is facilitated, and its redox property is also thermodynamically optimized by using H2O and CO2 as soft oxidants, guaranteeing an effective generation of syngas from both redox steps. The carbon tolerance is greatly enhanced due to H2O or CO2 gasification in the reoxidization step. Experimental studies confirm the redox scheme by using CeO2–LaFeO3 redox catalyst, demonstrating generation of syngas with an H2/CO molar ratio around 2.0 in both methane partial oxidation and H2O–CO2 splitting steps over 30 repeated cycles at 850 °C. A syngas selectivity of 95% in methane partial oxidation and nearly 100% conversion of CO2 to CO can be achieved. Synergistic effect and competing reaction between H2O and CO2 splittings over the reduced redox catalyst are the key factors for the control of syngas composition and the intensification of CO2 splitting. The proposed approach can potentially be applied for production of F–T-ready syngas with an increased yield without the need for gas separation when compared to the state-of-the-art thermochemical splitting or methane chemical looping partial oxidation processes.
研究领域:
能源科学
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化学工程
✓ 已验证
DOI
高影响因子
Processes
·
2024
·Vol. 12
·期 11
·2505
·
IF 2.8
Bo Zhang,Lei Wu,Fei Li,Wuwan Xiong,Peiyu Yao,Yang Zhang,Xiang Li
The production of waste textiles has increased rapidly in the past two decades along with the rapid development of the economy, the majority of which has been either landfilled or incinerated, resulting in energy loss and environmental pollution. Microwave pyrolysis, which can transform heterogeneous and complex waste feedstocks into value-added products, is considered one of the most competitive technologies for processing waste textiles. However, achieving selective product formation during the microwave pyrolysis of waste textiles remains a significant challenge. Herein, sodium acetate, potassium acetate, and nickel acetate were introduced into waste textiles through an impregnation method as raw materials to improve the pyrolysis efficiency. The optimized process parameters indicated that nickel acetate had the most favorable promotional effect of the three acetates. Notably, the waste textiles containing 1.0% Ni exhibited the highest gas production rate, with the hydrogen-containing combustible gas reaching 81.1% and 61.0%, respectively. Using X-ray diffraction (XRD), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), and Raman spectroscopy to characterize the waste textiles before and after pyrolysis, it was found that nickel acetate was converted into metallic nickel (Ni0) during microwave pyrolysis. This active site significantly enhanced the pyrolysis process, and as the gas yield increased, the disorder of the resulting pyrolytic carbon also rose. The proposed Ni0-enhanced microwave pyrolysis mediated by nickel acetate offers a novel method for the efficient disposal and simultaneous resource recovery of waste textiles.
研究领域:
环境科学
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能源工程
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产品关联
DOI
高影响因子
ChemistrySelect
·
2026
·Vol. 11
·期 21
·e06267
·
IF 2.3
Wuqiang Si,Lin Xia,Chao Lu,Zhong Cheng,Shunli Kou,Xuangan Liu,Chuang Xing,Peng Lu,Shuyao Chen,Yanhong Wang
Co-based composite catalysts with assorted zeolite have been extensively utilized to improve gasoline octane numbers by isomerization enhancement in Fischer-Tropsch synthesis products. Nevertheless, their catalytic potential remains constrained due to insufficient secondary isomerization activity. Herein, we propose a three-stage catalyst system, denoted as (Co/SiO 2 + 0.5Pt/SiO 2 ) + ZSM-5 + Beta, designed to synergistically promote multi-branched alkane formation. Elaborate experimental results confirm the formation of straight-chain hydrocarbons on Co/SiO 2 , while the 0.5Pt/SiO 2 component elevates intermediate olefin concentrations from 11.0% to 12.5%. The subsequent zeolite cascade enables precision isomerization: ZSM-5 (10-membered ring channels) preferentially generates mono-branched alkanes, whereas Beta zeolite (12-membered ring channels) drives secondary branching through advanced isomerization. This catalyst configuration achieves a significant increase in multi-branched alkane selectivity within isomerized products. The demonstrated cascade mechanism establishes a framework for direct syngas-to-branched hydrocarbon conversion, suggesting generalizable principles for cascade catalyst design in selective hydrocarbon upgrading. Graphical
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DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Guihua Yan,Paulina Pršlja,Gaofeng Chen,Jiahui Kang,Yongde Liu,Miguel A. Caro,Xi Chen,Xianhai Zeng,Bo Peng
Syngas conversion into higher alcohols represents a promising avenue for transforming coal or biomass into liquid fuels. However, the commercialization of this process has been hindered by the high cost, low activity, and inadequate C2+OH selectivity of the catalysts. Herein, we have developed Cu/Co carbon wood catalysts, offering a cost-effective and stable alternative with superior selectivity for catalytic conversion. The formation of Cu/Co nanoparticles was found, influenced by water-1,2-propylene glycol ratios in the solution, resulting in bidisperse nanoparticles. The Cu/Co-CW-W1P1 catalyst (the ratio between water and 1,2-propanediol is 0.5:0.5) exhibited a remarkable CO conversion rate of 74.8% and a selectivity of 58.7% for C2+OH, primarily comprising linear primary alcohols. This catalyst demonstrated enduring stability and selectivity under industrial conditions, maintaining its efficacy for up to 350 h of operation. We also employed density functional theory (DFT) to analyze selectivity, particularly focusing on the binding strength of CO, a crucial intermediate for subsequent reactions leading to the formation of alcohols. DFT identified the pathway of CHx and CO coupling, ultimately yielding C2H5OH. This computational understanding, coupled with the high performance of the Cu/Co-carbon wood catalyst, paves the way to develop catalytically selective materials tailored for higher alcohol production from a nature-based source.
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
Journal of the American Chemical Society
·
2025
·
IF 15.6
Su Li,Zili Ma,Xinyu Zhong,Bo Wu,Jingxuan Guo,Bin Chai,Jianfei Ji,Chengyuan Liu,Jungang Wang,Qiang Wang,Jun Bao,Kegong Fang,Yuhan Sun
The direct conversion of syngas to higher oxygenates presents a fundamental challenge in simultaneously achieving high CO conversion, superior oxygenate selectivity, and minimal undesired C1 byproducts. Here, we develop a series of multifunctional CuxPd1/SiO2|CoMn catalysts with granule stacking architecture, which overcome the challenge by precisely controlling the spatial arrangement of active sites and the intermediate transport pathway. Systematic optimization reveals a distinct volcano-shaped relationship on Pd loadings, with the Cu28Pd1/SiO2|CoMn composite emerging as the optimal candidate. Such a catalyst achieves an exceptional oxygenates molar selectivity of 44.4% (C2+OH/ROH = 95.4%) while maintaining low C1 products (6.4% CO2 and 5.7% CH4) at considerable 27.3% CO conversion. Mechanistic studies reveal that the breakthrough stems from precise control of spatial intimacy of functional components, optimized mass balance between CHxO* and CHx*, and isolated Pd atom-mediated hydrogen spillover effects. Based on spectroscopic evidence with theoretical calculations, we propose a synergistic catalytic system wherein PdCu single-atom alloys facilitate H2 activation and CHxO* formation through hydrogen spillover, while Co0-Co2C interfaces produce abundant CHx* species. The synergistic interaction enables the migration of CHxO* intermediates from single-atom alloy sites to Co0-Co2C interfaces, where they undergo further insertion into CHx* species, ultimately leading to hydrogenation and formation of higher oxygenates.
研究领域:
催化化学
·
材料化学
·
化学工程
·
能量转换
·
表面科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2021
·Vol. 17
·期 19
·2100082
·
IF 13.281
Jiatong Wei,Yanping Chen,Yanfu Ma,Xin Shi,Xiaoli Zhang,Chunjing Shi,Ming Hu,Jian Liu
Fischer-Tropsch synthesis (FTS) is an effective route to produce olefins, gasoline, diesel, and oxygenates from syngas (CO + H 2 ). However, it still remains a challenge for regulating the product distribution of FTS. Here, a series of Co/C sub-microreactors with precise designed nanoarchitectures are synthesized for selective syngas conversion. Through a combination of surface protection-assisted etching and following carbonization process, Co/C sub-microreactors with solid cube, double-shelled hollow box, and hollow box architectures, namely, Co/C-Cube, Co/C-DBox, Co/C-Box can be obtained. In FTS, comparing with solid Co/C-Cube, double-shelled hollow structured Co/C-DBox is inclined to grow long-chain hydrocarbon products, whereas hollow structured Co/C-Box avails the formation of short-chain hydrocarbon chemicals. Therefore, shape selective catalysis and controlled product distribution of FTS are realized by tuning the architectures of Co/C sub-microreactors. It is expected to fundamentally unravel the heterogeneous catalytic process via upfront designing and precisely regulating the architectures of micro/nanoreactors.
研究领域:
化学工程
·
材料科学
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催化科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）