INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Zhihao Zhou,Soomro Sarmad,Chao Huang,Guoshu Deng,Zhenkun Sun,Lunbo Duan
Ni-based catalysts supported on ordered mesoporous Al 2 O 3 with 2-D hexagonal and 3-D cubic pore structures are synthesized via evaporation-induced self-assembly for catalyzing dry CH 4 reforming to produce syngas . The Ni–Al 2 O 3 catalysts with 3-D pore structure exhibit higher activity in terms of CH 4 and CO 2 conversions than those with 2-D pore symmetry, due to the better mass transfer of the 3-D interconnected pore structure for the accessibility of Ni 0 active sites. And a higher Ni content slightly promotes catalytic activity , owing to more exposed active sites. However, a higher Ni content causes more severe carbon deposition during long-term reaction. During the long-term stability tests, the catalysts with 2.5 wt% Ni maintain the highest stability regardless of the pore structure, and the catalyst with 3-D pore structure is more advantageous to both activity and stability. Meanwhile, the catalyst with 2.5 wt% Ni and 3-D pore structure shows the lowest carbon deposition.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2023
·
IF 8.7
Qunwei Guo,Jiaqi Geng,Jiawen Pan,Bo Chi,Chunyan Xiong,Jian Pu
Liquid fuels like diesel, biodiesel , and alcohols can be utilized for onboard hydrogen production in auxiliary power systems by steam reforming , in which hydrogen productivity and carbon deposition are key issues. A-site deficient La 1-x Cr 0.95 Ru 0.05 O 3 catalysts are prepared using the Glycine-nitrate method and characterized by multiple techniques. The catalyst with 20 % A-site deficiency exhibits about 95 % fuel conversion and stable performance over a 100 h continuous test at 750 °C and a steam/carbon ratio of 3.0 using n-hexadecane. However, the catalyst with a 10 % deficiency shows fluctuating fuel conversion with higher ethylene and ethane contents. Catalyst performance is mainly determined by active oxygen. The activation of steam on oxygen vacancies and Cr ions with variable valences could produce surface-free oxygen and freely migrating lattice oxygen respectively, which can react with CH x intermediates to form CO and H 2 .
研究领域:
能源材料化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED ENERGY
·
2017
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IF 7.182
Xinghua Zhang,Wenwu Tang,Qi Zhang,Tiejun Wang,Longlong Ma
Ni-based catalysts supported on γ-Al 2 O 3 and SiO 2 were prepared by impregnation. Catalyst characterization was performed using XRD, NH 3 -TPD, H 2 -TPR and chemisorption. Effects of supports on catalytic performance were tested using the hydrodeoxygenation (HDO) of phenolic compounds as a model reaction. Experiment result shows that single phenolic compounds can be converted via HDO reaction over Ni/SiO 2 and Ni/γ-Al 2 O 3 catalysts at 300 °C. The hydrocarbon yields are in the range of 60–90%. The effect of supports on the reaction mechanism was also explored. It is found that hydrogenation of the aromatic ring preferentially occurs over Ni/SiO 2 catalyst while the cleavage of C AR O bond preferentially occurs over Ni/γ-Al 2 O 3 catalyst in the HDO of phenol. Compared to Ni/γ-Al 2 O 3 catalyst, Ni/SiO 2 catalyst exhibits better repeatability and higher catalytic activity for hydrocarbon yield when mixed phenolic compounds were used as feedstock in the HDO reaction, and the carbon deposited on the surface of Ni/SiO 2 catalyst is lower.
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
ChemistrySelect
·
2022
·Vol. 7
·期 43
·e202202460
·
IF 2.307
Guohao Xu,Jiale Zhu,Xuedong Zhu
Graphical Compared with the microporous system of MoO 3 /ZSM-5 synthesized by the the physically-blended method, the micro-mesoporous system of ZSM-5@MoO 3 with a core-shell reaction pathway of Mo-acid sites tandem could accelerate the rate of the mass-transfer, promoting aromatization reaction. A novel core-shell ZSM-5@MoO 3 catalyst was successfully synthesized by the hydrothermal coating strategy, and its physicochemical properties and catalytic properties in methane aromatization were investigated using a physically-blended ZSM-5/MoO 3 catalyst as a comparison. Multitechniques including XRD, SEM, TEM, EDS, N 2 adsorption, ICP, IR and IG were employed to investigate the characteristics of methane aromatization reaction and the deactivation of carbon deposits. At the reaction temperature of 700 °C and a space velocity of 2400 mL g −1 h −1 , methane conversion and aromatics selectivity of the core-shell ZSM-5@MoO 3 catalyst were 11.3 % and 88.1 %, respectively, which were higher than those of the physically-blended ZSM-5/MoO 3 catalyst by 3.1 % and 14.8 %, respectively. The special reaction pathway of core (ZSM-5, acid sites)-shell (MoO 3 , Mo sites) and the relatively close proximity between MoO 3 and ZSM-5 were mainly responsible for the excellent properties in the methane aromatization reaction. At the same time, the formation of the micro-mesoporous property accelerated the mass-transfer rate and inhibited the formation of carbonaceous deposition, greatly improving the stability of methane aromatization. Thanks to its core-shell structure, ZSM-5@MoO 3 catalyst showed the excellent properties in methane aromatization.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Sun Jikai,Tu Rui,Xu Yuchun,Yang Hongyan,Yu Tie,Zhai Dong,Ci Xiuqin,Deng Weiqiao
The process of CH 4 cracking into H 2 and carbon has gained wide attention for hydrogen production. However, traditional catalysis methods suffer rapid deactivation due to severe carbon deposition. In this study, we discover that effective CH 4 cracking can be achieved at 450 °C over a Re/Ni single-atom alloy via ball milling. To explore single-atom alloy catalysis, we construct a library of 10,950 transition metal single-atom alloy surfaces and screen candidates based on C–H dissociation energy barriers predicted by a machine learning model. Experimental validation identifies Ir/Ni and Re/Ni as top performers. Notably, the non-noble metal Re/Ni achieves a hydrogen yield of 10.7 gH 2 gcat –1 h –1 with 99.9% selectivity and 7.75% CH 4 conversion at 450 °C, 1 atm. Here, we show the mechanical energy boosts CH 4 conversion clearly and sustained CH 4 cracking over 240 h is achieved, significantly surpassing other approaches in the literature.
研究领域:
催化化学
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材料科学
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能源科学
✓ 已验证
DOI
PubMed
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2025
·
IF 3.5
Yang Jie,Fang Hailong,Jiang Huanjin,Wang Wenhao,Chen Jixiang
MgO–Al 2 O 3 -supported metallic Ni and bimetallic Ni–Zn catalysts (referred as Ni/MgAl and Ni x Zn/MgAl with the Ni/Zn atomic ratio of x , respectively) were prepared by the coprecipitation method, and their performance for methane dry reforming (DRM) was tested on an atmospheric quartz fixed-bed. The XRD, magnetic measurement, H 2 -TPR, TEM/EDS and XPS results demonstrate that metallic Ni and Ni–Zn alloy form in Ni/MgAl and Ni x Zn/MgAl, respectively. With reducing the Ni/Zn atomic ratio, the amount of surface Ni sites decreases, while the CO 2 adsorption capacity and strength increase due to the presence of Zn. Ni x Zn/MgAl gives higher activity than Ni/MgAl for DRM, mainly due to the suppression of carbon deposition and graphitization on Ni–Zn alloy and the enhanced adsorption of CO 2 . Under the condition of 800 °C, CH 4 /CO 2 molar ratio of 1 and weight hourly space velocity of 20,000 mL g cat −1 h −1 , Ni/MgAl gives the CH 4 and CO 2 conversions of 76% and 80%, respectively. With decreasing Ni/Zn atomic ratio from 7 to 2, the CH 4 and CO 2 conversions on Ni x Zn/MgAl first increase and then decrease, and Ni 5 Zn/MgAl has the highest activity with the CH 4 and CO 2 conversions of 81% and 87%, respectively. During the time on stream of 100 h at 800 °C, Ni 5 Zn/MgAl exhibits better stability than Ni/MgAl, mainly ascribed to its less amount of filamentous graphite carbon. In all, the formation of Ni–Zn alloy enhances the catalyst activity and remarkably suppresses the graphitization of carbonaceous deposit.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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IF 20.2
Quanqi Zhang,Zhonghua Jiang,Yimin Zhang,Xinyu Xu,Ye Yang,Yucai Qin,Lijuan Song,Yi Mei,Yun Zu
Carbon deposition, an inevitable product operated at high temperatures, is a headache-inducing obstacle to enhance catalyst stability for methane dry reforming (MDR). Herein, we have ingeniously designed sintering-resistant Ni@S-1 nanosheet zeolites to purposefully induce common linear and non-linear deactivation of catalysts during MDR reaction for deciphering carbon footprint. Multiple evidences unveiled that "transient carbon", composed of multi-phenyl-rings via rapidly rearrangement of CH x * fragments, was a crucial vane for catalyst deactivation. Accordingly, we proposed a dynamic equilibrium theory for the generation and elimination of "transient carbon". Achieving this balance was dependent of the matching degree between Ni 0 nanoparticles and NiO x (OH) y , which both separately originated from the evolutions of 1:1 and 2:1 Ni phyllosilicates controlled by nanosheet thickness. Delightfully, synthetic Ni@S-1–60nm catalyst with an optimal ratio of Ni 0 /NiO x (OH) y contributed higher MDR activity and durability. These findings derived a new MDR reaction pathway and afforded value-filled information for developing high carbon-resistant MDR catalysts.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
NANO
·
2016
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IF 0.951
Jingge Liu,Ang Cao,Jing Si,Lihong Zhang,Qinglan Hao,Yuan Liu
Sintering of the active metallic nanoparticles and carbon deposition are the key problems faced for CO methanation catalysts. For overcoming those problems, bimetallic nanocatalyst is a promising route. In this work, a series of Al 2 O 3 supported Ni-Co alloy catalysts were prepared by reducing NiCoAl layered double hydrotalcite (LDHs), and characterized with X-ray diffraction (XRD), temperature programmed reduction TPR, N 2 adsorption-desorption, transmission electron microscopy (TEM) and temperature programed oxidation (TPO) techniques. The resultant catalysts were mesoporous with nanoparticles of Ni-Co alloy ranging from 7.9 nm to 9.2 nm which were highly dispersed in alumina matrix. The sample Ni 7 Co 3 -Al 2 O 3 catalysts showed very good catalytic performance during the stability test at 500/600 ∘ C for 300 h, meanwhile exhibited excellent anti-sintering ability and anti-carbon deposition ability, owing to the formation of Ni-Co alloy and the feature of LDHs. This strategy for improving anti-sintering and anti-carbon deposition should be extendable for catalysts of other reactions.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 59
·34069-34077
·
IF 2.936
Minhua Zhang,Xuechao Tan,Tong Zhang,Zheng Han,Haoxi Jiang
A deactivation study on the ethanol/acetaldehyde conversion to 1,3-butadiene over a ZnO promoted ZrO2–SiO2 catalyst prepared by a sol–gel method was performed. The samples were characterized by N2 adsorption–desorption isotherms, scanning electron microscopy (SEM), NH3 temperature programmed desorption (NH3-TPD), X-ray powder diffraction characterization (XRD), thermogravimetric analyses (TGA), Fourier transform infrared resonance (FT-IR), 13C magic-angle spinning nuclear magnetic resonance (13C NMR) and X-ray photoelectron spectroscopy (XPS). The pore structure characteristics and surface acidity of Zn0.5–Zr–Si catalysts were largely decreased with time-on-stream and no crystal structure was formed in the used catalyst, indicating that the deactivation was caused by carbon deposition. Two main types of carbon deposition were formed, namely low-temperature carbon deposition with the oxidation temperature of around 400 °C and high-temperature carbon deposition with the oxidation temperature of 526 °C. The carbon species were mainly composed of graphitized carbon, amorphous carbon, carbon in C–O bonds and carbonyls. The deactivated catalyst could be regenerated by a simple oxidation process in air. Adding a certain amount of water into the feed had a positive effect on reducing the carbon deposition.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED ENERGY
·
2021
·
IF 9.746
Bangxin Li,John T.S. Irvine,Jiupai Ni,Chengsheng Ni
A solid oxide fuel cell utilizing bio-fuels such as methanol and ethanol could provide a carbon–neutral electricity generation and facilitate its applications in transport or stationary power unit. Herein, Ce 4+ doping in SrFe 0.95 Ni 0.05 O 3 imparts FeNi 3 exsolution and CeO 2 precipitation in a reducing condition, contributing to the fuel reforming, C-C bond cleavage and coke consumption in the anode chamber. The ferrite perovskites are stable in ethanol/steam at 800 °C, whereas they are unstable in ethanol vapor with the high C fugacity inducing the formation of Fe 0 and carbides. However, the Ce 0.2 Sr 0.8 Fe 0.95 Ni 0.05 O 3 anode maintains mostly the perovskite and is free from coke after the 300 h’ operation under C 2 H 5 OH fuel at 0.5 V or 0.7 V because of the dynamic balance between the carbon deposition and consumption since an operation for 10 h shows a clear carbon deposition. A maximum power density of 0.58 W cm −2 and a polarization resistance of 0.21 Ω cm 2 at 800 °C can be obtained for the symmetrical solid oxide fuel cell with identical Ce 0.2 Sr 0.8 Fe 0.95 Ni 0.05 O 3 cathode and anode under an ethanol fuel. The results demonstrate that the reversible and stable SrFeO 3 with Ce/Ni co-doping has a bright prospect for alcohol fuel oxidation.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
Fundamental Research
·
2022
·
IF 0
Tianxing Yang,Rui Ma,Jiale Li,Yanan Liu,Junting Feng,Yufei He,Dianqing Li
Propane dehydrogenation (PDH) is an efficient technology for the direct production of propylene. Nevertheless, current PDH catalysts mainly rely on precious Pt or toxic Cr and especially undergo severe coke deposition. Herein, we report a Ru catalyst decorated by boron species (Ru-3B/Al 2 O 3 ), which exhibits high catalytic performance for PDH. HAADF-STEM, EELS, and CO-FTIR characterization are used to identify the surface structure of the Ru active component, which shows that the high-energy unsaturated coordination sites, including corners, edges and step atoms for Ru-3B/Al 2 O 3, are appropriately modified by BO x species. The encapsulation of high-energy active sites prone to C C cracking and deep dehydrogenation leads to higher propylene selectivity (> 95%) and strong carbon resistance ( k d 0.0007 min) over Ru-3B/Al 2 O 3 . The XPS and H 2 -TPR results show that the migration of B species is driven by the reduction of B 2 O 3 to B 2 O 2 and that the coating degree of Ru particles is controlled by the chemical valance of Ru species.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Bin Li,Xiaoqing Yuan,Lvyin Li,Baitao Li,Xiujun Wang,Keiichi Tomishige
Addition of rare earth oxide, especially lanthanide oxide, was regarded as a promising strategy to improve the carbon resistance for Nickel-based catalysts in dry reforming of methane (DRM). In this work, Nickel-based catalysts containing lanthanide oxides (NiLa/SiO 2 , NiCe/SiO 2 , NiSm/SiO 2 , and NiGd/SiO 2 ) were prepared and employed to catalyze DRM. Lanthanide oxide affected the formation of Ni nanoparticles in different size. In NiLa/SiO 2 and NiCe/SiO 2 , Ni nanoparticles maintained relatively small size (4 nm), while in NiSm/SiO 2 and NiGd/SiO 2 , nickel particles were in large size (8 nm). NiLa/SiO 2 and NiCe/SiO 2 exhibited better stability than the other two catalysts, with CH 4 conversion decreasing from 64.6 to 57.6% and 61.6 to 60.3%, respectively in 10 h on stream. The kinetic study confirmed that adding lanthanide oxide significantly affected the activation energy of CH 4 dissociation and CO 2 dissociation. Compared to monometallic Ni/SiO 2 , the presence of Sm and Gd suppressed CO 2 dissociation, and introduction of Ce and La effectively promoted CO 2 dissociation. These characters contributed to the higher carbon resistance and good stability for NiLa/SiO 2 and NiCe/SiO 2 catalysts in DRM reaction.
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）