Frontiers of Environmental Science & Engineering
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2022
·Vol. 17
·期 3
·1-12
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IF 6.048
Gao Yuchen,Jiang Jianguo,Meng Yuan,Ju Tongyao,Han Siyu
Biogas is a renewable biomass energy source mainly composed of CH 4 and CO 2 . Dry reforming is a promising technology for the high-value utilization of biogas. Some impurity gases in biogas can not be completely removed after pretreatment, which may affect the performance of dry reforming. In this study, the influence of typical impurities H 2 S and NH 3 on dry reforming was studied using Ni/MgO catalyst. The results showed that low concentration of H 2 S in biogas could cause serious deactivation of catalyst. Characterization results including EDS, XPS and TOF-SIMS confirmed the adsorption of sulfur on the catalyst surface, which was the cause of catalyst poisoning. We used air calcination method to regenerate the sulfur-poisoned catalysts and found that the regeneration temperature higher than 500 °C could help catalyst recover the original activity. NH 3 in the concentration range of 50–10000 ppm showed a slight inhibitory effect on biogas dry reforming. The decline rate of biogas conversion efficiency increased with the increase of NH 3 concentration. This was related to the reduction of oxygen activity on catalyst surface caused by NH 3 . The synergetic effect of H 2 S and NH 3 in biogas was investigated. The results showed that biogas conversion decreased faster under the coexistence of H 2 S and NH 3 than under the effect of H 2 S alone, so as the surface oxygen activity of catalyst. Air calcination regeneration could also recover the activity of the deactivated catalyst under the synergetic effect of H 2 S and NH 3 .
研究领域:
能源化学
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催化化学
✓ 已验证
DOI
高影响因子
Catalysts
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2022
·Vol. 12
·期 6
·606
·
IF 4.501
Yadong Wang,Qing Hu,Ximing Wang,Yanpeng Huang,Yuanhao Wang,Fenghuan Wang
Methane reforming with carbon dioxide (DRM) is one promising way to achieve carbon neutrality and convert methane to syngas for high-value chemical production. Catalyst development with better performance is the key to its potential large-scale industrial application due to its deactivation caused by carbon deposition and metal sintering. Hence, a Ni/CeO2catalyst (Ni/CeO2-M) with higher CO2conversion and better stability is prepared, supported on CeO2precipitated via a novel microimpinging stream reactor. A series of ex-situ or in-situ characterizations, such as CO titration measurements, two-step transient surface reaction (two-step TSR), CO2and CH4temperature-programmed surface reaction (CO2-TPSR and CH4-TPSR), X-ray absorption fine structure (XAFS), and in-situ Raman spectroscopy study, were used to investigate its structure and mechanism. In contrast to Ni supported on commercial CeO2(Ni/CeO2-C), the Ni/CeO2-M catalyst with stronger lattice oxygen mobility and higher oxygen storage capacity enhances its CO2activation ability and carbon deposition. The Ni particle size of the Ni/CeO2-M catalyst decreased, and a higher oxidation state was obtained due to the strong metal–support interaction. Besides the reaction performance improvement of the Ni/CeO2-M catalyst, the novel microimpinging stream reactor could achieve catalyst continuous production with a high preparation efficiency. This work provides a novel method for the high-performance catalyst preparation for DRM reaction and its mechanism study gives a deep insight into high-performance catalyst development via bottom-up study.Keywords:dry reforming of methane;oxygen vacancy;Ni/CeO2catalyst
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
Yinghui Sun,Guojie Zhang,Haizhu Cheng,Jun Liu,Guoqiang Li
The mechanism and kinetic features of dry reforming with methane (DRM) over Ca promoted 1Co–1Ce/AC-N catalyst was investigated. The mechanistic pathway studies have conducted by FTIR and XPS analysis, structure-activity correlations demonstrated the CH 4 and CO 2 could adsorb on catalyst active sites and generate intermediate CH x , OH and CH x O, continue to generate CO and H 2 and then desorbed from active sites. Moreover, CH 4 could also oxidized by Ce 4+ and CO 2 reduced by Ce 3+ , the same content of Ce 4+ and Ce 3+ on promoted catalyst greatly improved the reaction rate. The kinetic of dry reforming with methane was examined for temperature between 650 and 850 at 800 °C. The research was carried out by changing the CH 4 /CO 2 ratios between 0.3 and 3.0. The obtained experiment data were fitted by three typical kinetic models (Power Law, Eley-Rideal and Langmuir-Hinshelwood), the fitting results demonstrated that the best prediction of reforming rates can provided by Langmuir-Hinshelwood model for the reaction temperatures between 650 and 800 °C. Moreover, activation energies of methane and carbon dioxide consumption were −117 and −47 kJ/mol, indicating that much higher energy barrier is needed for methane activation compared to carbon dioxide.
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
Materials Today Sustainability
·
2022
·
IF 7.244
R. Zeng,G. Jin,D. He,L. Zhang,D. Chen,Y. Zhang,L. Zhu,Y. Mei,W. Wu,Y. Luo
Utilizing propane and CO 2 as coreactants to produce syngas (CO/H 2 ) via dry reforming shows several advantages over direct propane dehydrogenation and traditional methane dry reforming . It is of great importance to establish high-efficiency catalytic systems that can break C–C bonds and activate CO 2 simultaneously. Herein, acidic H 2 O 2 was applied to etch LaCoO 3 . Surprisingly, highly dispersed Co 3 O 4 at the edges of support along with high oxygen vacancies were obtained from acidic H 2 O 2 treatment. Furthermore, the treated LaCoO 3 catalyst facilitated the generated intermediates of formate to convert into the desired products. The results showed that acidic H 2 O 2 treated LaCoO 3 catalyst can reach 18% for propane conversion and 35% for CO 2 conversion at 550 °C, showing high catalytic activity . Consequently, the present work provides some ideas for the synthesis of efficient LaCoO 3 catalysts for dry reforming of propane.
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
Chemical Science
·
2018
·Vol. 9
·期 14
·3426-3437
·
IF 9.063
Xinyu Li,Zhi-Jian Zhao,Liang Zeng,Jiubing Zhao,Hao Tian,Sai Chen,Kang Li,Sier Sang,Jinlong Gong
La2O3 exhibits good performance for various catalytic applications, such as oxidative coupling of methane (OCM) and dry reforming of methane (DRM), during which coke formation may lead to the deactivation of catalysts. Typically, the reaction between CO2 adsorbed on La2O3 and coke is the rate-determining step of the coke elimination process. This paper describes the influence of Ce addition on the CO2 adsorption and activation over La2O3. Combined with in situ and ex situ characterization and density functional theory (DFT) calculation, we show that Ce addition promotes the formation of bidentate carbonate on La2O3via tuning CO2 adsorption energy. In addition, Ce addition adjusts the ratio of bidentate/monodentate carbonate, and affects the ratio of hexagonal/monoclinic La2O2CO3 on the binary oxides. DRM is used as a probe reaction to examine the coke elimination performance of Ce–La binary oxide. It is found that when the Ce/La ratio reaches the optimal value (0.15), Ce–La binary oxide has the highest CO2 adsorption energy and predominantly promotes the formation of bidentate carbonate, and hence possesses the highest basicity above 700 °C and finally exhibits the best coke elimination performance.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
PubMed
高影响因子
ChemCatChem
·
2023
·Vol. 15
·期 8
·e202300136
·
IF 4.5
Ruifan Tan,Ping Wang,Luyao Guo,Zupeng Chen,Ronghe Lin,Xiaoling Mou,Yunjie Ding
Graphical The shape of zirconia hosts can tune the nature of active nickel species and the number of lattice oxygen species, which strongly influences the reaction and coking rates in the dry reforming of methane. The shape of the carriers has a profound impact on the catalytic performance of metal-supported catalysts. Herein, ZrO 2 of different shapes (nanorods-like, spherical or irregular nanoparticles, demoted as RZ, SPZ, and IPZ, respectively) are adopted to disperse Ni species to assess the shape effects on the catalytic performance in dry reforming of methane. To this end, the fresh and spent catalysts are thoroughly characterized by multiple techniques including N 2 sorption, powder X-ray diffraction, temperature-programmed reduction with H 2 , thermogravimetric analyses, transmission electron microscopy, Raman and X-ray photoelectron spectroscopies. It is revealed that the reducibility of NiO species follows the orders of Ni/RZ
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
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2020
·
IF 4.982
Bin Li,Xiaoqing Yuan,Baitao Li,Xiujun Wang
The hierarchical supports have motivated intensive research interests of chemists in the catalytic field because of the rational combination of mass transport property and large surface area. In this work, hydroxyapatite (HAP) supported nickel catalysts were prepared and employed to promote the dry reforming of methane (DRM). The proportion of mesopore/macropore in HAP was adjusted by the heating temperature (20, 50, 80, 120 °C) during the preparation process. The pore structure played an important role in regulating the physiochemical properties and thus affecting the catalytic performance in DRM. With increasing the proportion of mesopore on HAP, Ni preferentially dispersed on mesopore channel to form small-size particles. All catalysts possessed weak interaction between Ni nanoparticles and HAP; however, the interaction enhanced gradually with decreasing the Ni particles diameter. High proportion of macropore led to large-size Ni nanoparticle, while high proportion of small-size mesopore at 2–5 nm resulted in the complete blockage of these pore structures. These two boundary situations led to relatively weak interaction between nickel particles and the support, low metal dispersion and hence low activity as well as rapid deactivation in the DRM evaluation. Ni nanoparticles on HAP-80 and HAP-120 supports possessed relatively higher dispersion, which imparted these two catalysts with the function of strong anti-sintering ability and carbon resistance, thereby exhibiting better catalytic activity and stability in DRM evaluation. The deactivation of all catalysts during the reforming reaction was mainly ascribed to the sintering as well as encapsulation of Ni nanoparticles by graphitic carbon .
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Yong Bai,Xinran Qiu,Qian Zhang,Songbai Qiu,Yanlin Qin,Tiejun Wang
Recently, the ecofriendly techniques for production of nanohybrids using natural biomass have aroused great attention. This study reported a green and facile synthesis of highly dispersed supported metal catalysts using sesbania powder (SP) extracted from the natural sesbania plant. Well-dispersed Ni/SiO2 catalysts were effectively fabricated by an SP-assisted sol–gel method. The influencing factors including the additive amounts of SP, metal loadings, and metal types on the physicochemical properties of supported catalysts were primarily investigated. The testing results revealed that the additive SP significantly facilitated the uniform distribution of metal species during heat treatment, leading to the existence of ultrasmall nanoparticles (<4 nm) and high dispersion of supported metal. The as-prepared Ni/SiO2 catalysts were applied to the dry reforming of methane and demonstrated excellent catalytic performance due to the prevention of the agglomeration of Ni species and fabrication of Ni embedded in the silica framework through the introduction of SP.
研究领域:
催化化学
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环境科学
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材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Su Li,Jinkai Qiu,Zijun Bian,Bin Shao,Zhicheng Liu,Cheng Lian,Honglai Liu,Jun Hu
The dry reforming of carbonate with methane (CaDRM) can be one of the breakthrough technologies to address the challenge of mitigating inevitable CO 2 emissions into value-added chemicals but remains great challenges for efficient catalysts design. In this study, we break the trade-off between the catalytic activity and the carbon deposit by tailoring the d-band center of Ni through Fe doping, which matches the energy level of CH 4 * dehydrogenation but is far away from that of the over cleavage of CH* . In this light, the porous spherical Fe x Ni/Al 2 O 3 catalysts with Ni 3 Fe alloy nanoaggregates are obtained through a one-step spray drying method. The optimized Fe 0.6 Ni/Al 2 O 3 catalyst shows an excellent catalytic activity with a superior CO selectivity of 91.75 % at a complete CaCO 3 conversion at 700°C, and successfully prevents the carbon deposit to maintain its excellent stability. Moreover, the extremely low activation energy of 45.2 kJ/mol and the good porosity of Fe x Ni/Al 2 O 3 ensure its fast dynamics. Therefore, this tailoring d-band center approach through the formation of alloy catalysts supplied a novel strategy for effectively cracking hydrogen species while avoiding over cleavage of CH x * in the thermal catalysis, which promoted the CaDRM technology to be a promising solution for carbon neutrality in industrial sectors in near future.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
·
IF 7.2
Jiming Wang,Min Ji,Jiaqi Lv,Min Wang
Photo-thermo-chemical dry reforming of methane (PTC-DRM) produces syngas has been a promising strategy to utilize abundant solar energy and alleviate greenhouse effect. Herein, we report an efficient PTC-DRM process on Ni-based catalyst with Zn doping and investigate the effect of Zn on the catalytic performance of catalysts. Zn promoted the generation of active sites on the surface of Ni-Al 2 O 3 , suppressed the accumulation of coke during the reaction process and enhanced the photocatalytic activity of the catalyst. Ni-ZnO-Al 2 O 3 catalyst exhibited highest thermal catalytic performance and the conversion of CH 4 and CO 2 are 50.2% and 58.1% at 650 ℃, respectively. All catalysts exhibited higher reaction rates of CH 4 and CO 2 and higher hydrogen selectivity under light conditions. Light also significantly enhanced the carbon deposition resistance and stability of the catalyst. And possible reaction mechanism of the Ni-ZnO-Al 2 O 3 was proposed during PTC-DRM process.
研究领域:
化学工程
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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
CANADIAN JOURNAL OF CHEMICAL ENGINEERING
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2025
·
IF 1.9
Sarmad Soomro,Zhenkun Sun,Dennis Y. Lu,Zhihao Zhou,Lin Li,Lunbo Duan
Catalyst deactivation due to carbon deposition and sintering poses a significant challenge to the efficient dry reforming of CH 4 and CO 2 into syngas, particularly at high Ni loadings. To tackle this difficulty, ordered mesoporous silicas with varied pore symmetries were employed as supports in this study to synthesize the Ni-based catalysts using hydrothermal treatment. The 10% Ni/MCM-41 catalyst exhibited the highest conversion rates for CO 2 (81%) and CH 4 (77%), with favourable H 2 /CO (0.92) ratios indicating efficient syngas production Higher Ni concentrations increase active sites and catalytic performance, they also increase carbon deposition, reducing catalyst durability. At lower Ni loadings (4% Ni), catalysts with a 3D pore structure showed improved activity and stability, effectively reducing carbon deposition. This study demonstrates that optimized mesopore symmetries and Ni loadings can enhance catalyst efficiency and durability for syngas production.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2019
·
IF 4.914
Jingqing Tian,Haocheng Li,Xin Zeng,Zichun Wang,Jun Huang,Chen Zhao
ABSTRACT Development of dry reforming of methane and carbon dioxide is an effective route to convert in-dustrial waste gases such as coke-oven gas and coal-to-oil gas into platform syngas. However, this process encounters severe problems of metal particle sintering and coke formation at high tem-peratures. In this work, we developed a new synthetic method for preparing confined Ni/MCM-41 catalysts, which impede the sintering of metal nanoparticles (NPs) and coke deposition at high temperatures, enabling them to be successfully applied to methane dry reforming . The method results in high activity and stability of the catalyst at 700 °C for 200 h. The Ni precursor is immersed in ethanol and impregnated into MCM-41 by the peculiar capillary action of hexagonal straight mesopores . By this method, 10 wt% Ni NPs (d = 2 nm) is equably confined to the mesoporous channels with strong metal-support interactions, as confirmed by HRTEM, TEM mapping, H2-TPR, and XRD measurements. Such a confined structure has a significant effect on the inhibition of metal NP agglomeration and carbon deposition during methane dry reforming, as evidenced by TEM, Raman, TGA, and TPO measurements of used Ni/MCM-41 catalysts. In contrast, unconfined Ni/MCM-41 catalysts, with Ni NPs located on the pore exteriors, are rapidly deactivated after 12 h due to the blocked contact between the active metal centers and the gas feedstock. Additionally, a fast increase in the Ni NP size and the formation of substantial carbon nanotubes on the unconfined catalyst surface are seen. This work offers a facile approach for the synthesis of anti-sintering, car-bon-resistant confined Ni catalysts that can operate at high temperatures
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
危险品化学品经营许可证（带存储）