JOURNAL OF CATALYSIS
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2016
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IF 7.354
Xuelin Zou,Zebao Rui,Shiqi Song,Hongbing Ji
Poor durability and low Pd utilization efficiency are the main drawbacks of supported Pd catalysts for low-temperature methane combustion. Here, we present a facile way to stabilize the performance of Pd/Al 2 O 3 by introducing a spinel NiAl 2 O 4 interface as a promoter at no cost to the activity. The NiAl 2 O 4 interface is formed by impregnation of alumina supports in the nickel-containing solution, followed by high-temperature calcination. A series of 0.4 wt.% Pd/ x NiO/γ-Al 2 O 3 with NiO loading varying among 0.0, 0.5, 1.0, and 9.0 wt.% is investigated. The formation of a NiAl 2 O 4 interface promotes the distribution and crystallization of PdO, suppresses PdO particles aggregation and surface OH − species accumulation during the reaction, and finally leads to the excellent performance of Pd/0.5NiO/γ-Al 2 O 3 . Pd/0.5NiO/γ-Al 2 O 3 demonstrates higher Pd utilization efficiency than the state-of-the-art Pd-based catalysts and better stability than Pd/Al 2 O 3 . Such a spinel interface promotion strategy may bring new insight into the design of highly efficient Pd-based catalysts and their potential technological applications.
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
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xing Zhang,Jingfeng Wu,Tian Li,Chengzhi Zhang,Lingjun Zhu,Shurong Wang
Hydrodeoxygenation (HDO) of lignin-derived bio-oil offers a promising route for the production of advanced biofuels. However, the conventional HDO of lignin-derived bio-oil faces serious problems, such as low hydrocarbon yield and easy deactivation of catalysts. Herein, a novel reaction system consisting of a highly stable bifunctional catalyst (i.e., Ni−WO x /NiAl 2 O 4 ) and a dodecane solvent was developed for the HDO of lignin-derived phenolics. The Ni 0 species, derived from NiWO 4 precursors on the NiAl 2 O 4 , were of small crystallite size and high dispersion, together with the strong oxophilicity of W, thereby exhibiting high activity. The use of a highly stable NiAl 2 O 4 spinel support and the replacement of common solid acid with more stable WO x for the cleavage of C O bond accounted for excellent stability. The optimized 10Ni−15WO x /NiAl 2 O 4 exhibited a high guaiacol conversion of 97.8% with a high cycloalkane yield of 83.8% under the optimum conditions (250 °C, 5 MPa H 2 , and 4 h). Cycloalkanes with a high yield over 90% were also obtained by the HDO of other complex lignin-derived compounds. More importantly, the catalyst always retained its initial activity for the HDO of guaiacol in five runs, with negligible coke formation. Subsequently, the HDO behavior of the bio-oil obtained from walnut shell pyrolysis was also studied. The relative content of cycloalkanes in the products reached 44.3% after the reaction. This study highlights the prospect of a highly stable catalyst consisting of hydrogenation metal and oxophilic promoter, and dodecane solvent to enable efficient production of cycloalkanes from the HDO of lignin-derived phenolics.
研究领域:
能源化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2019
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IF 12.221
Didi Li,Yi Li,Xiaohui Liu,Yong Guo,Chih-Wen Pao,Jeng-Lung Chen,Yongfeng Hu,Yanqin Wang
The production of hydrogen from the aqueous-phase reforming (APR) of oxygenated hydrocarbons is promising. Herein, the performances of Pt loaded on NiAl2O4 spinel and γ-Al2O3 were investigated in the APR of methanol. The conversion of methanol and the yield of hydrogen over Pt/NiAl2O4 reached 99.9% and 95.7%, respectively. In comparison with Pt/γ-Al2O3 catalyst (26.5% and 23.3%, respectively), these values were enhanced by 4-fold. More importantly, Pt/NiAl2O4 had high stability with only 10% loss of its initial conversion after 600 h on stream. In situ diffuse reflectance infrared Fourier transform spectra (DRIFTS) of the APR of methanol revealed that the reaction underwent the dehydrogenation of methanol and the sequential water–gas shift (WGS) reaction. These two reactions were then investigated independently, in which Pt/NiAl2O4 showed more efficient performance than Pt/γ-Al2O3. Intensive characterization methods revealed that the chemical state of Pt played a pivotal role in the dehydrogenation of methanol to generate the adsorbed CO intermediate. For Pt/NiAl2O4 catalyst, the reduction of PtOx to metallic state Pt was easier because of the presence of the oxygen vacancy, leading to the higher catalytic performance in the dehydrogenation of methanol. Further studies with in situ DRIFTS-MS of WGS demonstrated a redox mechanism over Pt/NiAl2O4 catalyst, which was different from the associative route that occurred over Pt/γ-Al2O3 and made the WGS reaction faster. The addition of Ni (NiAl2O4 spinel) creates oxygen vacancies, giving WGS which underwent a redox route. This work presents the deep understanding into the pathway and mechanism in the APR of methanol and is expected to have important implications for the future development of APR catalysts.
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
JOURNAL OF THE ENERGY INSTITUTE
·
2024
·
IF 5.6
Chenlong Liu,Yijun Zhang,Yiman Xiao,Ruyue Zhang,Siddig Abuelgasim,Chenghua Xu,Atif Abdalazeez
Bio-oil by-products are inevitable with biomass gasification. It is considered a potential resource for hydrogen production via steam reforming. This study investigated acetic acid as a bio-model compound using a NiAl 2 O 4 catalyst. The effect of reaction conditions on hydrogen-rich production has also been discussed, including reaction time (1 h, 3 h, 5 h and 7 h), steam/carbon ratio (S/C = 1–4) and the blend of NiAl 2 O 4 and CaO (1:0, 3:1, 1:1, 1:3 and 0:1). The fresh and spent samples were characterized by XRD, XPS, SEM, BET, etc. The result showed that the CaO addition has several advantages: 1) it increases hydrogen gas purification; 2) it prevents Ni separation from NiAl 2 O 4 ; 3) it decreases the sintering of NiAl 2 O 4 . However, Ca 5 Al 6 O 14 formation decreases the activity of hydrogen production. In reaction conditions, steam is an essential factor for hydrogen gas production. The S/C ratio = 3 shows the optimum result for hydrogen gas production. Although the higher S/C ratio = 4 can maintain the adsorption activity of CaO, it causes Ni separation from NiAl 2 O 4 . The blend of NiAl 2 O 4 and CaO is another essential factor for hydrogen gas production. Adding CaO has increased hydrogen gas production significantly. However, a little CaO in a blend ratio 3:1 does not maintain the stability of the NiAl 2 O 4 structure. In the end, the optimum conditions are S/C ratio = 3 and blend = 1:1 at 650 °C, which produces hydrogen gas yield (2.1 mol/mol) and H 2 /CO (5.83).
研究领域:
能源科学
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催化化学
✓ 已验证
DOI
高影响因子
ACS Omega
·
2025
·
IF 4.3
Tao Tian,Ze-Min Zhao,Yu Zhang,Jieying Jing,Wen-Ying Li
Hydrogenation saturation of phenanthrene (a typical component of coal tar) could not only improve the combustion performance of fuel oil, but also obtain the raw material for preparing high-energy-density fuel. Nickel-based catalysts have been considered promising catalysts for the hydrogenation saturation of phenanthrene due to their appealing capacity to activate phenanthrene molecules. However, the Ni derivation precursor greatly affects its hydrogenation activity. In this work, the NiAl2O4 catalyst was obtained by the sol–gel method. Under the experimental conditions of temperature 300 °C, pressure 5 MPa, and WHSV 0.52 h–1, the phenanthrene conversion over NiAl2O4 catalysts can be up to 99.7 and 93.9% for perhydrophenanthrene yield, while those of the traditional Ni/Al2O3 catalysts are just up to 96.8 and 77.3%, respectively. Moreover, the TOF of phenanthrene hydrogenation of the NiAl2O4 catalyst (3.01 × 10–3 s–1) surpasses that of the traditional Ni/Al2O3 catalyst (2.46 × 10–3 s–1), which indicates that Ni derived from NiAl2O4 has stronger phenanthrene hydrogenation activity. According to relevant characterizations, the superior hydrogenation performance of the NiAl2O4 catalyst derives from the stronger H2 adsorption and dissociation ability and the formation of an electron-deficient structure of active metal Ni, which contributes to the improved adsorption and activation of the polycyclic aromatic hydrocarbons.
研究领域:
催化化学
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能源化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zheng Li,Jiehao Xie,Zipin Peng,Zhuo Ma,Yihui Li,Xingkun Chen,Yuan Tan,Wenshao Yang,Yunjie Ding
4-Chlorophenol (4-CP) is a pervasive environmental pollutant commonly found in wastewater and groundwater, posing great risks to both human health and the ecosystem. Catalytic hydrodechlorination (HDC) of 4-CP by utilizing hydrogen (H 2 ) as a reductant has emerged to be an efficient and sustainable way to treat pollutant water. This study focuses on the development of an efficient and stable Pd-based catalyst for the catalytic HDC of 4-CP. By incorporating an appropriate amount of Ni into Al 2 O 3 support, a NiAl 2 O 4 (NA) spinel was synthesized, enhancing the interaction between Pd and the support, leading to precise control over Pd species and oxygen vacancies. The tailored properties of the Pd/NA-1 catalyst result from meticulous adjustment of the Pd 2+ /Pd 0 ratio and oxygen vacancies, which promotes electron transfer from Pd to Ni within the NiAl 2 O 4 spinel. In comparison to the Pd/Al 2 O 3 catalyst, the Pd/NA-1 catalyst exhibits exceptional stability, with continuous operation for over 120 h without deactivation. Comprehensive characterization analyses indicate that the Pd/NA-1 catalyst effectively prevented the aggregation of Pd nanoparticles, maintaining the Pd 2+ /Pd 0 ratio at 1, which is crucial for its superior stability. This work provides valuable insights into the development of Pd-based catalysts for HDC reactions, highlighting the potential use of Pd/NA-1 catalysts in treating hazardous pollutants like 4-CP in waste systems.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2025
·
IF 8.1
Zixuan Sheng,Khomidov Fakhriddin Gafurovih,Kadyrova Zulayho Raimovna,Bingying Gao,Linqiang Mao
The widespread use of NiO/Al 2 O 3 catalysts in the petrochemical industry generates hazardous spent materials due to the formation of refractory nickel-aluminum spinel (NiAl 2 O 4 ), which complicates metal recovery and exacerbates resource inefficiency. Traditional direct acid and alkali leaching cannot recover Ni and Al due to excellent stable structure of NiAl 2 O 4 . Here, we propose a simple soda roasting-water leaching strategy to disrupt the spinel lattice and recover Ni and Al with high efficiency. By roasting spent catalysts with Na 2 CO 3 at 1000 °C, Na + ions substituted Al 3+ in the octahedral sites, which destroyed the spinel framework and converted Al 2 O 3 /NiAl 2 O 4 into water-soluble NaAlO 2 . Over 98.31 % of Al was selectively leached at 90 °C, followed by pH-controlled precipitation and calcination at 600 °C to regenerate γ-Al 2 O 3 with the purity of 98.21 %. Residual NiO was recovered via 2 M H 2 SO 4 leaching, with Fe impurities removed through pH-selective precipitation. The kinetic analysis revealed a chemically controlled leaching mechanism ( E a = 47.61 kJ/mol). Final Ni(OH) 2 through calcination at 400 °C yielded reusable NiO. This approach achieved >98 % metal recovery, minimized waste, and aligned with circular economy principles by transforming hazardous spent catalysts into high-purity industrial feedstocks.
研究领域:
冶金学
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环境工程
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化学工程
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材料科学
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产业生态学
·
废弃物管理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yuying Zhao,Jiahui Zhan,Rui Hu,Gang Luo,Jiajun Fan,James H. Clark,Shicheng Zhang
Extensive use of grey hydrogen in traditional hydrodeoxygenation (HDO) severely reduces the sustainable development of lignin valorization processes. Conversely, the catalytic transfer hydrogenation (CTH) mediated by green hydrogen is an alternative strategy that promotes the sustainability of in-situ hydrogenation of lignin. In this work, a bifunctional catalyst (Ru/NiAl 2 O 4 ) was developed to assist the proposed green hydrogen-driven cosolvent system composed of isopropanol and water for the CTH of guaiacol. Results indicate that 95% conversion of guaiacol and 80% cyclohexanol selectivity can be achieved at 200 ℃ within 3 h with a high water/isopropanol ratio (6/4), significantly increasing the greenness and sustainability. Furthermore, the recycling experiments verify the stability of the catalyst’s active sites. Analysis of the mechanism suggests that the high efficiency of such system can be attributed to the activation of metal and acid dual functional sites of Ru/NiAl 2 O 4 catalyst on aromatic rings and C-O bonds. The acceleration of the in-situ hydrogen supply is due to hydrogen exchange between water and isopropanol. The participation of water in the reaction is also demonstrated by the presence of deuterium in the product after the reaction in D 2 O. This work provided the insights into the development of a strategy for the production of cyclohexanol from lignin derivatives by an in-situ CTH system.
研究领域:
化学工程
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Zhoufeng Bian,Wenqi Zhong,Yang Yu,Zhigang Wang,Bo Jiang,Sibudjing Kawi
Catalysts of Ni supported on home-made mesoporous alumina (Ni/M-Al 2 O 3 ) were prepared via facile incipient impregnation method and calcined under different temperature (500–800 °C). Compared with catalysts of Ni supported on commercial alumina, they showed much higher conversion and lower carbon deposition in methane dry reforming (DRM). Among the catalysts, Ni/M-Al 2 O 3 -700 exhibited the highest DRM activity, with 77.6% CH 4 conversion and 85.4% CO 2 conversion at 700 °C. TPR revealed that almost all the Ni was in the form of NiAl 2 O 4 spinel after calcination at 700 °C. Due to the strong metal-support interaction of NiAl 2 O 4 structure, the Ni crystal size of Ni/M-Al 2 O 3 -700 after reduction was around 5 nm. TGA and TEM results showed its carbon deposition after 20 h DRM test was only 3.8% and mainly in the form of amorphous carbon . This work indicates that the formation of NiAl 2 O 4 spinel is beneficial to activity and stability towards DRM reaction and controlling calcination temperature is crucial.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Biomass Conversion and Biorefinery
·
2022
·
IF 4.05
Wang Jiacheng,Li Xingyong,Wu Yankun,Duan Jinyi,Zhuang Nihong,Wang Dechao,Zhang Zhaoxia,Ye Yueyuan,Li Shuirong,Zheng Zhifeng
The wide-scale application in the bio-fuel area of fatty acid methyl esters (FAME) has been limited because of its high oxygen content, awful low temperature flowability, and low heating value. In this work, the hydrodeoxygenation (HDO) of methyl palmitate as fatty acid methyl ester model compounds for long-chain alkane via Nb 2 O 5 modified NiAl 2 O 4 catalysts was investigated. The effect of Nb/Ni atomic ratio (0.05:0.30), reaction temperature (260–340 ℃), time (2–10 h), and H 2 pressure (1–5 MPa) on the production of long-chain alkane is exhaustively researched. The results show that the products are mainly pentadecane with a few other alkane hydrocarbons and nickel metal was the main active site. Besides, the added promoter Nb promoted the dispersion of active metal Nickel, increased the acidity, and thus substantially enhanced the HDO activity of methyl palmitate. In response to the best conditions (0.3 g catalyst, 3 g methyl palmitate), the methyl palmitate conversion and pentadecane selectivity over Nb 2 O 5 -NiAl 2 O 4 with 0.20 Nb/Ni atomic ratio reached 91.14% and 80.07%, respectively. However, the methyl palmitate conversion and pentadecane selectivity over pure NiAl 2 O 4 catalyst were only 62.53% and 74.67%, respectively. Therefore, Nb 2 O 5 -NiAl 2 O 4 catalysts exhibit remarkable catalytic ability for HDO of methyl palmitate to alkanes. The low cost, easy preparation, high catalytic performance, and recycling stability of Nb 2 O 5 -NiAl 2 O 4 catalyst demonstrate that catalyst Nb 2 O 5 -NiAl 2 O 4 is a promising effective and efficient catalyst for producing long-chain alkane from methyl palmitate. Graphical abstract
研究领域:
催化化学
·
可再生燃料化学
✓ 已验证
产品关联
DOI
高影响因子
OZONE-SCIENCE & ENGINEERING
·
2023
·
IF 2.7
Tingfeng Xue,Jing Zhang,Jingcheng Wei,Bingyan Zhu,Jianwei Song,Shuang Xu,Liwei Pan
In this study, a novel NiAl2O4/NiO@γ-Al2O3 catalyst was prepared by the impregnation-calcination method and used for the catalytic ozonation of tartrazine wastewater. The NiAl2O4/NiO@γ-Al2O3 catalyst were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, and nitrogen adsorption-desorption experiments. It was found that NiAl2O4/NiO@γ-Al2O3 significantly improved the removal of chemical oxygen demand of the dye wastewater from 40% for the direct ozone oxidation to 65%, and the ozone concentration depletion for catalytic ozonation was 120% of that for ozone alone. The catalytic activity of the catalyst did not significantly decrease after reuse for six cycles and leaching concentration of metal ions less than 1%. However, the toxicity of the dye wastewater was greatly reduced after the catalytic ozonation. The pyridine Fourier transform infrared spectroscopy showed the catalytic ozonation reaction was related with Lewis acid sites. The presence of hydroxyl radicals, superoxide anion radicals, and singlet oxygen was verified by an electron paramagnetic resonance, and the quenching experiments confirmed that the removal of organic pollutants from the tartrazine wastewater mainly relied on hydroxyl radicals and singlet oxygen. Therefore, the NiAl2O4/NiO@γ-Al2O3 could be an effective catalyst for the rapid catalytic ozonation of dye wastewater.
研究领域:
环境工程
·
催化化学
·
水处理
·
高级氧化技术
·
材料科学
✓ 已验证
DOI
高影响因子
ACS ES&T Engineering
·
2022
·
IF 0
Xiangyu Ma,Hui Xu,Zhang Liu,Yanfei Liu,Chen Wang,Meiqing Shen,Chun Du,Bin Shan
Catalytic oxidation is a valuable residual methane removal method, and Pd-based catalysts are the most robust and widely applied system. Yet, they suffer from poor stability in practical applications due to sintering and water poisoning. In this work, we prepared a high-performance PdNi/Al2O3 catalyst with PdO-NiO and PdO-NiAl2O4 dual interfaces. PdNi/Al2O3 showed excellent hydrothermal stability after aging at 750 °C, 10% H2O for 72 h, with the T50 remaining below 315 °C. In addition, compared to bare Pd/Al2O3, PdNi/Al2O3 exhibited a better low-temperature activity with a T50 of 287 °C, rivaling state-of-the-art Pd-based catalysts. Combining structural characterizations and DFT calculations, it was shown that dual interfaces promoted the activation of methane C–H bonds and suppressed the adsorption of surface water/hydroxyl groups and agglomeration of PdO particles. This study has provided new perceptions for exploring the influence of interfacial interactions and offered a route to synthesize high-stability palladium catalysts.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
危险品化学品经营许可证（带存储）