ENERGY
·
2021
·
IF 7.147
Xiuquan Li,Zhongqing Yang,Li Zhang,Ziqiang He,Ruiming Fang,Ziqi Wang,Yunfei Yan,Jingyu Ran
The catalytic reaction of C 2 H 6 with CO 2 provides an opportunity to use shale gas and the greenhouse gas as source materials to produce ethylene through oxidative dehydrogenation or produce syngas through dry reforming . In this work, the reaction characteristics of ethane with CO 2 on Fe/Co/Ni/Cu monometallic catalysts and Pd-doped bimetallic catalysts were studied through activity test, kinetic analysis , catalyst characterization and DFT calculation. It is found that Pd–Fe 6 /CeO 2 has a high and stable C 2 H 4 selectivity of 80.4%, which is suitable for oxidative dehydrogenation reaction, while Ni 6 /CeO 2 has a large ethane/CO 2 conversion and a high CO selectivity of 96.5%, which is suitable for dry reforming reaction. For Fe-based catalyst, the doping of Pd form double active component structure. It only reduces the energy barrier of ethylene formation and CO 2 direct activation to provide O∗, but also increases the energy barrier of ethylene deep dehydrogenation, thus increasing the conversion of reactants and selectivity of C 2 H 4 . For Ni-based catalysts, the doping of Pd forms the alloy structure, which reduces the energy barrier of O∗-assisted dehydrogenation reaction and increases the conversion of reactants, but increases the energy barrier of C–C bond cleavage and CO 2 activation reaction, which reduces the selectivity of reforming to syngas.
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
ACS Omega
·
2022
·
IF 4.132
Xiaofeng Li,Xiaohui Liu,Jiamao Hao,Lijun Li,Yanfang Gao,Yousong Gu,Zhenzhu Cao,Jinrong Liu
A strong metal–support interaction (SMSI) type catalyst has been synthesized and applied to a molten hydroxide direct carbon fuel cell (MHDCFC) to enhance the reaction activity of the anode carbon fuel through the interaction between the metal Ni and the support CeO2. Two catalysts have been prepared by a direct precipitation method (denoted NiO@CeO2) and a hydrothermal method (denoted NiO-CeO2), which are reduced by H2 to obtain Ni@CeO2 and Ni-CeO2, respectively. X-ray photoelectron spectroscopy (XPS), Raman, and temperature-programmed hydrogen reduction (H2-TPR) analysis results show that there are obvious oxygen vacancies and a Ni-O-Ce interface structure in NiO-CeO2 and Ni-CeO2, which is induced by the interaction between Ni and CeO2. The calculation results of current density and power density show that the performance of the MHDCFC is significantly improved in the presence of Ni-CeO2. The function fitting curves of the logarithm of the reaction rate constant (ln k) and the reciprocal of the temperature (1/T) show that the slope of the curve is decreased significantly after the addition of Ni-CeO2. In combination with density functional theory (DFT), the anode carbon reaction path is simulated in the MHDCFC, and the calculation results show that the reaction energy for the anodic carbon to generate carbon dioxide is decreased by 1.03 eV in the presence of Ni-CeO2.
研究领域:
材料科学
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能源技术
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产品关联
DOI
PubMed
高影响因子
Catalysts
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2022
·Vol. 12
·期 5
·460
·
IF 4.501
Yifan Zheng,Lijun Lu,Wei Chen,Anmin Zheng,Aiwen Lei,Abhishek Dutta Chowdhury
Global warming and rising waste content collectively accelerate the development of renewable-derived ‘low-carbon’ chemical technologies. Among all abundant renewables, marine-/food-waste-derived chitin, the only nitrogen-containing sustainable biomass, contains the uniqueN-acetylglucosamine units, which could be synthetically manipulated to a plethora of organonitrogen chemicals. Herein, we report the efficient one-step catalytic valorization of chitin toN-acylethanolamine over cost-effective Ni/CeO2-based materials, which interestingly demonstrate shape-based reactivity based on CeO2supports. In general, all three catalysts (Ni on cubic-, rod-, and polyhedral-shaped CeO2supports) were active for this reaction, but they differed in their catalytic efficiency and time-monitored reaction profiles. Herein, Ni on cubic-shaped CeO2delivered relatively better and stable catalytic performance, along with its rod-shaped counterpart, while the polyhedral CeO2-based material also delivered decent performance. Such interesting catalytic behavior has been corroborated by their physicochemical properties, as revealed by their characterization studies. Herein, to establish an appropriate structure-property-reactivity relationship, multimodal characterization techniques and control mechanistic experiments have been performed. This work demonstrates a concept to reduce the consumption of primary carbon resources and increase the utilization of secondary waste materials to facilitate a smooth transition from a linear economy (cf. cradle-to-grave model) to a circular economy (cf. cradle-to-cradle model).Keywords:chitin;waste valorization;heterogeneous catalysis;ceria;functionalization of C–C bonds
研究领域:
生物化学
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环境科学
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催化化学
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产品关联
DOI
高影响因子
Catalysts
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2025
·Vol. 15
·期 9
·812
·
IF 4
Xinru Gao,Han Meng,Changan Wang,Jinzhang Tao,Hongyi Gao
The development of highly efficient catalysts for the hydrogenation of dicyclopentadiene (DCPD) remains a critical challenge. In this study, we designed a series of bimetallic Ce–Ni metal–organic framework (MOF)-derived nanocatalysts by precisely tuning the Ce/Ni ratio and calcination temperatures. The optimized catalyst, Ni–CeO2(7:3)@C–400 °C, featuring highly dispersed carbon-coated Ni nanoparticles, achieved complete hydrogenation of DCPD to tetrahydrodicyclopentadiene (THDCPD) with 100% conversion and nearly 100% selectivity within 2 h under 100 °C and 2 MPa. The porous carbon framework significantly facilitated the diffusion and accessibility of DCPD molecules, combined with Ce species reconstructing the electronic structure of Ni active centers through electronic interactions, synergistically enhancing the hydrogenation efficiency. Furthermore, the catalyst demonstrated good structural stability. This work not only provides a robust strategy for the rational design of bimetallic MOF-derived catalysts but also highlights their potential for practical applications in industrial hydrogenation processes.
研究领域:
催化化学
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材料科学
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加氢化学
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纳米材料
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金属有机框架（MOFs）
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产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
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2025
·
IF 6.2
Xiaohua Li,Zhufeng Liu,Shanshan Shao,Yongbo Yu,Weicheng Wang,Tianrui Sun,Shiliang Wu
Steam reforming of bio-oil is a promising technology for the industrial-scale conversion of biomass into hydrogen energy, in which the catalyst plays the crucial role. This study proposes a Ni-Ca-Al-Ce-O catalyst, prepared by CaO loading onto Ni/CeO 2 ·Al 2 O 3 , and tested in the two-stage adsorption-enhanced reforming of biomass pyrolysis oil for hydrogen production. The effects of carrier type and Ni loading on the physicochemical properties of the Ca modified Ni-based reforming catalyst and its reforming performance were investigated, and its reusability was tested finally. The results revealed that more Ni metal active sites are available on CeO 2 ·Al 2 O 3 compared to biochar as carrier. However, side reactions such as ketonization were significantly promoted due to the metal oxides in red mud (RM), resulting in a large amount of methane as a by-product over the Ni/RM catalyst. When Ca additive introduced on the well selected Ni/CeO 2 ·Al 2 O 3 , the selectivity of hydrogen in the reforming gas was enhanced. Meanwhile, more spinel NiAl 2 O 4 was formed due to the interaction between NiO and Al 2 O 3 , which enhanced the stability and activity of the Ni-Ca-Al-Ce-O catalyst. With a Ca/Al ratio of 1:1, Ni was more uniformly dispersed, and the yield and selectivity of hydrogen reached 73.35 % and 76.90 %. In the reusability tests, the yield of hydrogen remained above 60 % after six runs, which was superior to that of similar reforming catalysts, suggesting that the proposed Ni-Ca-Al-Ce-O catalyst is reliable in terms of reusability.
研究领域:
能源化学
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催化材料
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产品关联
DOI
高影响因子
JOURNAL OF RARE EARTHS
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2022
·
IF 4.632
Tingting Bao,Hui zhou,Yi Zhang,Chenxu Guo,Wenming Guo,Hang Qin,Pengzhao Gao,Hanning Xiao,Weixiong Liu
Ni/CeO 2 catalysts ( n CeO2 : n Ni = 0, 1, 4, 7, 10) supported on SiC porous ceramics for ethanol steam reforming (ESR) were investigated with respect to hydrogen production performance and growth of carbon deposition. The oxygen released from CeO 2 enables the oxidation of CH x species to serve as carbon precursors, thus providing Ni/CeO 2 catalysts with stronger resistance to carbon deposition compared with Ni catalysts. The Ni/CeO 2 catalysts prepared by inverse microemulsion and impregnation methods exhibit regular semicircular spherical shape on SiC porous ceramics. Under 500 °C for 25 h of ESR reaction, the ethanol conversion rate over Ni/CeO 2 catalysts ( n CeO2 : n Ni = 7) is sustained up to 100% and H 2 selectivity is essentially kept at 74%. The by-product selectivity declines stepwise with increasing content of CeO 2 , which is attributed to the adsorption and oxidation of CO and of CH x species as CH 4 precursor from CeO 2 . The scanning electron microscopy (SEM) and transform electron microscopy (TEM) results reveal that further loading of CeO 2 on the surface of Ni catalysts can alleviate both migration and sintering of Ni particles. Furthermore, carbon deposition on Ni/CeO 2 catalysts preferentially outgrow filamentous rather than amorphous carbon , with a tendency for the latter to be more deactivated.
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
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Songlei Mo,Jia Kou,Jianrong Zeng,Kepeng Song,Yayun Zhang,Shangming He,Yongfeng Hu,Yong Guo,Xiaohui Liu,Xi Chen,Yanqin Wang
Upcycling polyethylene terephthalate (PET) wastes into high value-added oxygenated chemicals is desirable, yet it remains challenging. Herein, we develop a novel strategy to convert PET into 1,4-cyclohexanedimethanol (CHDM) via two steps, the conversion of PET to dimethyl 1,4-cyclohexanedicarboxylate (DMCD) over Ni-based catalysts, followed by the hydrogenolysis of DMCD to CHDM over a CuMgAl catalyst. The key step is the production of DMCD from PET in one-pot reaction and an unprecedent yield of 86.5% DMCD yield is achieved over Pd-modified Ni/CeO 2 catalyst, which to the best of our knowledge is the highest yield reported to date. Comprehensive characterizations demonstrate that the addition of Pd enhances hydrogen dissociation, but weakens the adsorption activation ability for C–O bond in esters, thus DMCD selectivity is improved. Over CuMgAl catalyst, DMCD is directly converted into CHDM with 83.8% yield. Furthermore, the techno-economic analysis proves the economic feasibility of converting PET into CHDM via our proposed strategy. The study provides a promising and effective approach to upcycle PET wastes into high value-added products.
研究领域:
化学工程
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催化
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废物管理
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可持续化学
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产品关联
DOI
高影响因子
SURFACE & COATINGS TECHNOLOGY
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2017
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IF 2.589
Xiaowei Zhou,Chun Ouyang
This paper presented an effective approach for electroplating of coatings on the activated surface of pure Ti substrate using pulsed electro deposition. Regarding the ceramic-like TiO 2 barrier layer on its surface of Ti substrate to inhibit surface activity, a novel activating solution that composed of HF, HCl, Ce(NO 3 ) 2 , TiCl 3 , and bal. DMF dissolvent was applied for surface modifications of Ti substrate in order to increase interfacial bonding strength of surface Ni coatings. Besides a comparative study of Ni nanocrystalline coatings without and with CeO 2 addition was carried out for disclosing the role of the Ce-rich phase on managing microstructure and high-temperature oxidation resistance during oxidation at 800 or 1000 °C. Results indicated that Ce-rich precipitations, where dispersed along grain boundaries (GBs), were favorable for completing the spalling oxide-layers on Ni-CeO 2 nanocomposite coatings during oxidation at 800 °C. Furthermore, an analytical modeling was validated for better understanding of Ce-rich precipitations along GBs defects for monitoring oxidation mechanisms. Furthermore, this finding would be therefore leading to the guidelines for Ce-rich precipitations on the strengthening of Ni-based superalloys.
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DOI
高影响因子
JOURNAL OF CATALYSIS
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2020
·
IF 7.888
Jiehua Bao,Yuming Zhou,Yiwei Zhang,Yanyun Wang,Shuang Liang,Zhiwu Guo,Chang Guo,Yi Xue,Tao Zhuang,Yingjie Hu
In this study, we synthesized a series of Ni-based catalysts with different CeO 2 contents (0, 1, 2, 5 and 10 wt%) anchoring on the Al-Mg oxide spheres (AMO) with three-dimensional hollow flower-like structure. The triethoxyoctylsilane (TEOOS) and polyvinylpyrrolidone (PVP) were selected as effective modified reagents to introduce hydrophobic functionality on the surface of AMO and Ni-CeO 2 nanoparticles, respectively, for controllable anchoring Ni-CeO 2 nanoparticles on AMO by hydrophobic interaction driving mechanism. The effects of CeO 2 content on the texture, dispersion of Ni species, the reducibility of Ni 2+ , surface electronic states and acidity were investigated in detail. The Ni-5CeO 2 /AMO was found to achieve the highest 2,2′-bipyridine selectivity of 90.6% and maximum turnover number (TON) of 8611, specifically. Moreover, the Ni-5CeO 2 /AMO exhibits superior stability, maintaining 89% of 2,2′-bipyridine yield after 6 runs, due to the mitigated nickel leaching and promotion of the desorption of 2,2′-bipyridine. Furthermore, with the help of DFT calculations, a possible reaction mechanism was discussed and illustrated.
研究领域:
催化化学
·
材料科学
·
表面化学
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2026
·
IF 13.6
Li-Nan Huang,Han Zhao,Lei Jiang,Jiahao Geng,Zhiqiang Li,Yuelun Li,Kongzhai Li
The activation of CH4 and CO2 as well as the formation of carbon deposit are crucial for dry reforming of methane (DRM), and mechanistic insights into the relationship between reactant activation and carbon evolution during the DRM process are expected to provide guidance for the design of high-performance catalysts. Herein, by utilizing carefully defined Ni/CeO2 model catalysts with different CeO2 crystal planes, we elucidate at the atomic scale the roles of crystal plane in determining the reactant activation and carbon deposit formation in DRM by a joint experimental–theoretical method. The crystal planes of CeO2 determine the active sites and activation ability for CH4 and CO2 by influencing Ni–CeO2 interactions and oxygen vacancy (OV) concentrations. Both the metal and interface active sites of Ni/CeO2(111) and Ni/CeO2(110) can activate CH4 and exhibit good DRM activity. In contrast, only the metal site on Ni/CeO2(100) can activate CH4, leading to a reduced DRM activity. The relatively balanced CH4 and CO2 activation pathways for Ni/CeO2(110) and Ni/CeO2(100) catalysts ensured the stability of the catalysts, whereas Ni/CeO2(111) was rapidly deactivated due to carbon deposits. This study provides insights into the roles of metal–support interactions and OV sites on catalysts for CH4 dissociation activity, CO2 activation, and carbon deposit elimination in the DRM process, which can provide valuable guidance for the design of efficient catalysts with high activity and stability in DRM.
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产品关联
DOI
高影响因子
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