JOURNAL OF CATALYSIS
·
2016
·
IF 7.354
Junjie Su,Zhengpai Zhang,Donglong Fu,Da Liu,Xin-Chao Xu,Bianfang Shi,Xu Wang,Rui Si,Zheng Jiang,Jing Xu,Yi-Fan Han
A comparative study of higher alcohols synthesis directly from syngas has been performed over monometallic Co and bimetallic CoCu/SiO 2 catalysts. Particularly, the role of Cu on the origin of active sites and reaction mechanism were investigated thoroughly using multiple techniques such as ex situ X-rays diffraction (XRD), X-ray absorption spectroscopy (XAS) and Raman spectroscopy. Reduction process of CoCu/SiO 2 catalysts was also determined using in situ XRD and in situ Raman spectroscopy while the surface structure of reduced catalysts was detected by CO-DRIFTS. CoCu bimetallic particles covered by Cu atoms are responsible for alcohols synthesis. The intrinsic kinetics was performed over both catalysts under realistic reaction conditions. By comparing the kinetic parameters, including apparent activation energies and reaction orders, the promotional effects of Cu have been identified as: (1) weakening the CO/HCO dissociation and reducing the formation of CH x species; (2) controlling surface Co ensemble size and inhibiting CH x insertion.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
Carbon Capture Science & Technology
·
2024
·
IF 10.4
Yangna Luo,Xianglin Chen,Xiang Liu,Yafei Guo,Yuxuan Gao,Guoyang Zhao,Chuanwen Zhao
Electrochemical CO 2 reduction to synthetic fuels and commodity chemicals using renewable energy offers a promising approach to mitigate CO 2 emissions and alleviate energy crisis. Copper-based catalysts show potential for electrochemical CO 2 reduction applications, while they face the key challenges of high potential, sluggish kinetics, and poor selectivity. In this work, Cu-Zn, Cu-Co, Cu-Cd, and Cu-In bimetallic catalysts are synthesized via the electrodeposition method for electrochemical CO 2 reduction to syngas with adjustable CO/H 2 ratios. The bimetallic catalysts are characterized using various techniques to reveal their crystalline structures, morphologies, and elemental compositions. The structure-property-activity relationships of these catalysts are investigated to identify optimal candidates for electrochemical CO 2 reduction applications. The findings reveal that the bare Cu mesh catalyst exhibits poor CO 2 reduction activity, and the products are dominated by hydrogen evolution reaction (HER). The bimetallic catalysts exhibit improved CO 2 reduction performance, with the Cu-Zn and Cu-Cd catalysts showing excellent activity, and the CO/H 2 ratio in syngas can be tuned over a wide range by adjusting the applied potential. The Cu-Zn and Cu-Cd catalysts demonstrate outstanding performance with Faradic efficiencies of ∼90 % and ∼80 % towards syngas production with CO/H 2 ratios of ∼2.0 and ∼1.5 at −0.81 and −1.01 V vs. RHE, respectively, making the produced syngas suitable for various industrial applications. Stability tests over 450 min show that the Cu-Zn and Cu-Cd catalysts maintain stable catalytic activity, syngas selectivity and CO/H 2 ratio, making them robust candidates for syngas production. The results will provide valuable insights into the design of robust catalysts for electrochemical CO 2 reduction, offering a promising path toward sustainable syngas production.
研究领域:
材料科学
·
电化学
·
能源转换
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Zhicheng Xie,Bin Shao,Chonghui Jin,Conghe Song,Jun Hu
Direct hydrogenation of carbonates (DHC) technology represents a breakthrough alternative to conventional syngas production processes that rely on fossil fuels. Nevertheless, it is constrained by a low carbonate conversion efficiency and suboptimal hydrogen utilization. Here, a novel strategy of chemical-looping-enhanced hydrogenation of carbonates (HC-CL) is proposed for the coproduction of metal oxides and syngas, which divides the DHC process into two half-looping processes involving H2-reduction and decarbonation-oxidation. An excellent redox catalyst of spinel Ce5/MgFe2O4 is developed to drive the HC-CL, which can transform into the rock salt structure of Ce5/MgxFeyO–Fe0 to provide abundant Fe metal sites and oxygen vacancies (Ov) after H2-reduction, and regenerate itself through efficiently splitting CO2 from carbonates into CO during the decarbonation-oxidation. Reduction-regeneration mechanism of Fe species ensures the redox reversibility of Ce5/MgFe2O4, achieving a high CO2-splitting efficiency of 70% over 10 HC-CL cycles. The techno-economic analysis based on the process simulation further illustrates that the HC-CL process can save 2 GJ/tcarbonate of energy consumption, 0.5 tCO2/tcarbonate of CO2 emissions, and 55 $/tcarbonate of costs than the DHC process coupled with H2 separation and recycling utilization. Therefore, the HC-CL process turns out to be a promising novel technology for syngas production.
研究领域:
化学工程
·
能源技术
·
催化
·
可持续能源
·
材料科学
✓ 已验证
DOI
高影响因子
NATURE
·
2026
·Vol. 652
·期 8108
·89-95
·
IF 56.1
Han Yu,Yu Jiafeng,Wei Jian,Fang Chuanyan,Han Jianxiang,Sun Yannan,Chen Huaican,Yin Wen,Tan Li,Wang Ning,Ge Qingjie,Sun Jian
Light olefins—ethylene, propylene and butylene (C 2 = –C 4 = )—are essential building blocks in the chemicals industry and are traditionally produced by thermal or catalytic cracking of hydrocarbon feedstocks. Directly converting syngas (CO and H 2 ) into light olefins under mild conditions is attractive but challenging 1 , 2 , 3 , 4 . Prismatic cobalt carbide (Co 2 C) and associated hydrophobic modifications have shown potential for selective light-olefin synthesis under mild conditions 5 , 6 . Here we show another hydrophilic-promotion strategy in which a set of hydroxy promoters, exemplified by hydroxyapatite (Ca 5 (PO 4 ) 3 (OH), HAP), fumed silica (SiO 2 (F)) and amorphous boehmite (AlO(OH), AB), is physically mixed with a Co 2 MnO 4 precursor, inducing synergistic cobalt–manganese (Co–Mn) oxides and Co 2 C for syngas conversion. The induced anorthic Co–Mn oxides may serve as active phase for adsorbed-hydrogen-assisted CO dissociation to CH x /CH x O intermediates, whereas induced Co 2 C or the Co 2 C–oxide interface may mediate C–C coupling of these intermediates to form light olefins. This design achieved 70–82% CO conversion with light-olefins selectivity of more than 60% at 250–260 °C, 0.1 MPa with H 2 /CO ratios of 1–2, giving light-olefins carbon utilization efficiency up to 13%, among the highest reported for syngas to light olefins. This simple hydrophilic strategy for facilitating CO activation may provide useful insights for improving industrial Fischer–Tropsch processes.
✓ 已验证
DOI
PubMed
高影响因子
Nature Communications
·
2026
·
IF 18.1
Li Yihui,Zhao Ziang,Jiang Miao,Wang Guoqing,Li Zheng,Lu Wei,Cui Wenhao,Liu Rong,Lin Ronghe,Meng Yu,Lyu Yuan,Yan Li,Zhu Hejun,Ding Yunjie
The selective conversion of syngas to C 4+ long-chain alcohols holds significant industrial and scientific interest, but challenges in product selectivity and process efficiency remain. Here, we report a precisely catalytic strategy for C 4+ alcohol synthesis with a selectivity of 80% at 17% CO conversion. The reaction channel involves: (i) the development Cs 2 O-Co 2 C-Co catalysts, capable of catalyzing CO hydrogenation to long-chain oxygenates/olefins; and (ii) complete conversion to C 4+ alcohols is subsequently achieved on the single-Rh-site and Cu-ZrO 2 interfaces by integrated cooperative catalysis. A comprehensive catalyst design and compatibility assessment of each catalytic module ensures optimal combinations, meanwhile effectively eliminates costly separation steps, and reduces CO 2 selectivity down to 1%. The developed process achieves ultra-high carbon-efficiency (>95%) and improves oxygen-efficiency, effectively overcoming the key limitations of current syngas conversion technologies and thus representing a competitive and sustainable solution for producing high-value long-chain alcohols with a minimal carbon footprint.
✓ 已验证
DOI
PubMed
高影响因子
Results in Engineering
·
2025
·
IF 7.9
Yuan Zhou,Shaojie Zheng,Hao Lei,Liu Liu,Zhenting Xie,Yanxiao He,Nianbing Zhong,Shuai Xiao,Xuefeng He
The electrochemical CO 2 reduction reaction (eCO 2 RR) provides a sustainable route for producing high value-added syngas through renewable electricity. Nevertheless, the low solubility of CO 2 and the competing hydrogen evolution reaction in eCO 2 RR systems often restrict product selectivity and conversion efficiency. In this study, we propose a microenvironment engineering strategy by incorporating hydrophobic SiO 2 aerogel into Ag nanoparticle (NP) catalysts to enhance reaction kinetics. Experimental results demonstrate that the Ag NPs/20 wt.% SiO 2 -300 electrode delivers a peak CO Faradaic efficiency (FE CO ) of 85.7% at −1.5 V vs. Ag/AgCl in an H-cell, marking a 71.0% improvement compared to the bare Ag NP electrode (50.1%). In-situ Fourier-transform infrared spectroscopy verifies a *COOH-mediated reaction pathway, where the modified catalyst surface promotes intermediate enrichment due to enhanced mass transport. Furthermore, the membrane electrode assembly reactor equipped with the Ag NPs/20 wt.% SiO 2 -300 cathode maintains high FE CO (79.2% to 88.7%) across a broad current range (25 to 150 mA cm −2 ). The CO/H 2 ratio can be precisely adjusted by varying the applied current density, allowing tailored syngas production. This study highlights the pivotal role of hydrophobic microenvironments in modulating product selectivity and presents a scalable method for designing gas diffusion electrodes suitable for industrial eCO 2 RR applications.
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Jinhua Xiong,Xinyu Bi,Song He,Changsheng Cao
Herein, CdS nanorods (CdS-NR) was synthesized through a simple and facile solvothermal method. XRD pattern and TEM/HRTEM images indicated that hexagonal CdS nanorods with a diameter of 10 nm were successfully prepared. When used as electrocatalyst for CO 2 reduction reaction (CO 2 RR), CdS-NR afforded an excellent electrocatalytic performance in aqueous electrolyte. In comparison with commercial CdS nanoparticles (CdS-NP), CdS-NR could trigger the electroreduction of CO 2 to CO with a higher faradic efficiency and current densities. The enhanced electrochemical performance of CdS-NR than that of CdS-NP were ascribed to its enhanced adsorption of CO 2 , charge transfer ability and more exposed active sites. More importantly, it was noticed that H 2 generated along with CO, and the generated gas products with controllable ratios exhibited impressive potentials to directly using as syngas.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Green Energy & Environment
·
2026
·
IF 16.7
Zhiyang Tang,Xianyuan Wu,Jie Qu,Xinjun He,Fukun Li,Jinxing Long,Qiang Zeng,Haixia Su,Hongyan He,Xuehui Li
Selective hydrogenolysis of cellulose into C 6 -ketones offers a promising route for the production of high-value carbonyl compounds. However, conventional metal-catalyzed hydrogenolysis methods typically rely on externally added acids and require high-purity H 2 . Herein, we report an alternative syngas-promoted hydrogenolysis method that eliminates these dual dependencies while enabling the selective transformation of cellulose into value-added C 6 -ketones. Under optimal conditions, using a commercial Pd/C catalyst at 230 °C and 3.0 MPa total pressure (H 2 /CO = 1.5/1.5 MPa) for 2 h, the yield of C 6 -ketones reached 37.8 C-mol%, representing a 6.8-fold enhancement compared to that obtained under pure H 2 . Mechanistic studies demonstrated a dual promotional effect of CO in directing cellulose to C 6 -ketones. First, competitive adsorption of CO on Pd active sites suppresses excessive hydrogenation and undesired hydrogenolysis of cellulose-derived intermediates. Second, CO participates in the water–gas shift (WGS) reaction (CO + H 2 O ⇌ CO 2 + H 2 ), generating carbonic acid (H 2 CO 3 ) in-situ via CO 2 + H 2 O ⇌ H 2 CO 3 , which provides a controllable acidic environment that promotes key intermediate transformations associated with C 6 -ketone precursor formation.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Rongrong Cui,Qi Shen,Chenyan Guo,Bo Tang,Nianjun Yang,Guohua Zhao
Syngas has been synthesized via (photo) electrochemical CO 2 reduction. Its amount and yield efficiency are determined the utilizable CO 2 . Here we show syngas electrosynthesis using self-supplied CO 2 , namely in situ generated CO 2 from photoelectrocatalytic pollutant oxidation. In a single-chamber based two-electrode system, CO 2 is produced continuously during photoelectrocatalytic phenol oxidization on the anode of TiO 2 nanotubes decorated with Pd nanoparticles. Such in-situ generated CO 2 is then reduced into CO at a Pd-Cu cathode. With a phenol oxidation efficiency of 87% and a faradaic efficiency of 75%, the syngas yield is as high as 339.3 μmol. The ratio of carbon-to-hydrogen in syngas is variable from 0 to 1:10 under different current densities. The reactions for syngas generation are investigated using in-situ electrochemical infrared technique and confirmed to be C 6 H 5 OH→CO 2 →CO 2 *→COOH*→CO*+H + →CO+H 2 . This study thus provides an approach to degrade pollutants and simultaneously utilize produced CO 2 for the production of value-added chemicals like syngas.
研究领域:
环境科学
·
电化学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Shujin Shen,Cheng Han,Bing Wang,Yiang Du,Yingde Wang
Electroreduction of aqueous CO 2 is a sustainable approach to produce tunable syngas, which demands the rational design of dual-active-sites catalysts for individual CO 2 reduction reaction (CRR) and hydrogen evolution reaction (HER). Here, the self-supporting nickel@nitrogen-doped carbon nanotubes grown on carbon nanofiber (Ni@NCNTs-CNF) is developed with Ni single atoms (SAs) and nanoparticles (NPs) functioning as CRR and HER sites respectively. Benefiting from the hierarchical nanostructures for effective electron transport and mass diffusion, as well as the high accessibility of dual-active sites, Ni@NCNTs-CNF catalysts can mediate aqueous CO 2 into CO/H 2 (2:1) with a 100 % Faraday efficiency and a high current density (25 mA cm −2 ) at low working potential (-0.8 V). By manipulating the Ni SAs/Ni NPs ratio, the CO/H 2 proportion is easily modulated in a wide range from 1:4 to 5:1, independence of the working potential (-0.6 to -0.8 V). Our findings provide fresh insights into the design of dual-active-sites catalysts.
研究领域:
材料科学
·
电化学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2017
·
IF 5.651
Yu Hong,Wanru Chen,Xiang Luo,Chengheng Pang,Edward Lester,Tao Wu
In this study, three different marine biomasses, i.e., microalgae-spirulina, chlorella and macroalgae-porphyra, were pyrolyzed in a laboratory-scale multimode-microwave cavity at 400, 550 and 700 °C. Ovalbumin and cellulose were also chosen as model compounds to simulate algae. The influence of heating rate on pyrolysis and the βi curves of different samples under different temperatures were studied in detail. The porphyra was found to be the most reactive and produced the largest gaseous fraction (87.1 wt%) amongst the three algae, which comprised of 73.3 vol% of syngas. It was found that nitrogenated compounds in bio-oil were derived from protein in algae while carbohydrate led to the formation of PAHs. For the production of bio-oil, protein-rich microalgae is favorable compared with porphyra due to their lower amount of PAHs, while porphyra is more suitable for the production of H 2 + CO rich gas product, which is comparable with that of conventional gasification processes.
研究领域:
能源生物学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2022
·
IF 6.437
Hao Qi,Qirong Yang,Zhaoying Li,Chenyu Yang,Xinru Ma,Haoxi Ben
The mechanism of gas-phase products from pyrolysis of polysaccharides from Enteromorpha prolifera (PE) is researched. The sulfated polysaccharides are the most important polysaccharides in Enteromorpha prolifera . The molecular dynamics (MD) method is used to simulate the pyrolysis process of sulfated polysaccharides of Enteromorpha prolifera . Combined with the results of the pyrolysis simulations and density functional theory (DFT), rhamnose , glucuronic acid , glucose, and xylose are used as model compounds to estimate and calculate the reaction paths of hydrogen and carbon monoxide . In addition, fixed-bed pyrolysis experiments are performed with the above four monomers . The pyrolysis simulation results show that the pyrolysis process of sulfated polysaccharides is approximately divided into three stages: low-temperature, medium-temperature, and high-temperature stages. Gas-phase products are mainly produced in the high-temperature stage, and the main components of syngas are hydrogen, methane, and carbon monoxide. The simulation and experimental results show that pyrolysis of xylose is the most likely to generate hydrogen, followed by glucose, rhamnose, and glucuronic acid. The process of producing carbon monoxide from monomers goes through reactions such as dehydration, isomerization , C-C bond breakage, and decarbonylation . Moreover, the results of fixed-bed experiments indicate that when the four monomers are pyrolyzed individually, the highest proportions of hydrogen, carbon monoxide, and methane in the gas-phase products are obtained from the pyrolysis of xylose, glucuronic acid, and rhamnose. When the four monomers are mixed and then pyrolyzed, the proportion of hydrogen and carbon monoxide in the obtained gas-phase products decreases, and the proportion of carbon dioxide increases.
研究领域:
生物化学
·
能源科学
✓ 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）