NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 23
·11318-11324
·
IF 3.3
Jiazheng Zhu,Chengjie Duan,Sen Ye,Qizhong Zhang,Kun Li,Guangke He,Xiang Liu,Zhiguo Zhang
Exploring synthetic methods and catalysts that are easy to handle, highly active, and low-cost for producing industrially important chemicals is a long-term goal in both science and industry. Herein, we present a general and facile Ni-catalyzed reductive amination of aldehydes/ketones methodology using hydrazine as both nitrogen and hydrogen sources, instead of the traditionally used hydrogen gas and ammonia. The mesostructured alumina-supported Ni catalyst with a relatively high ratio of Ni0 and small-sized Ni nanoparticles plays a critical role in this transformation, resulting in 55 aldehydes/ketones successfully converting to their corresponding primary amines with 61–99% yields. This work outlines a low-cost yet robust catalytic methodology for the facile and general synthesis of primary amines for practical laboratory and industrial application.
研究领域:
有机化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·
IF 4.229
Long-Fei Xie,Pei-Gao Duan,Jia-Li Jiao,Yu-Ping Xu
A series of Ni catalysts with different zeolites were prepared by wet impregnation method and used to catalyze supercritical water gasification (SCWG) of microalgae for production of hydrogen-rich fuel gas under conditions of 430 °C, 60 min, ρ H₂O = 0.162 g/cm 3 , 2 g/g Ni/zeolites. Compared with noncatalytic SCWG, the presence of Ni/zeolite could increase the hydrogen gasification efficiency and carbon gasification efficiency by promoting water–gas shift and steam reforming reactions which are mainly affected by the amount of strong acid sites and Ni, respectively. The highest carbon gasification efficiency (CGE) and hydrogen gasification efficiency (HGE) of 23.61% and 23.55% were achieved with Ni/HY (Na 2 O, 0.8%). The gaseous produced mainly consisted of H 2 and CO 2 . The H 2 content in the gaseous products varied from 27.15 to 40.51% depending on the Ni/zeolites and increased with increasing the SiO 2 /Al 2 O 3 molar ratio of HZSM-5, which is 2.3–3.6 times higher than that of produced without catalyst. The H 2 yield varied between 2.57 and 3.61 mmol/g depending on the Ni/zeolites and increased from 2.19 to 5.61 mmol/g with increasing the SiO 2 /Al 2 O 3 molar ratio from 50:1 to 170:1, which is 3.6–7.8 times higher than that of produced without catalyst. Coke formation, surface area loss, and sintering of Ni could decrease the activity of the Ni/zeolites.
研究领域:
能源生物学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2021
·Vol. 23
·期 18
·7065-7073
·
IF 10.182
Liang Jiang,Guangyue Xu,Yao Fu
The conversion of levulinic acid (LA) to γ-valerolactone (GVL) is one of the most important reactions from biomass-derived platform chemicals to value-added chemicals. In this work, nitrogen-doped carbon was introduced into a Ni/Al2O3 catalyst and was employed for the hydrogenation of LA to GVL with a full conversion and equivalent yield under mild conditions, at as low as ambient hydrogen pressure and 130 °C for 6 h. The doping of nitrogen introduced NiNx species and the imperfection of modified nitrogen-doped carbon were beneficial for the selective hydrogenation of carbonyl groups. This catalyst showed excellent activity and selectivity in various solvents and could be recycled for at least 6 runs with little deactivation. In addition to LA, various substrates with both carbonyl and carboxyl groups could also be selectively hydrogenated to the corresponding lactones. This study offers both theoretical foundation and practical instructions for the high-efficiency conversion of LA to GVL over non-noble metal catalysts under mild conditions, especially ambient H2 pressure.
研究领域:
催化化学
·
生物质能转化
✓ 已验证
DOI
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
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Yu Qiu,Enkang Fu,Feng Gong,Rui Xiao
Ammonia is a prospective fuel for hydrogen storage and production, but its application is limited by the high cost of the catalysts (Ru, etc. ) to decompose NH 3 . Decomposing ammonia using non-precious Ni as catalysts can therefore improve its prospects to produce hydrogen. This work proposes several Ni/MgAl 2 O 4 with the support properties tuned and investigates the support effect on the catalytic performance. Ni/MgAl 2 O 4 -LDH shows high NH 3 conversion (∼88.7%) and H 2 production rate (∼1782.6 mmol g −1 h −1 ) at 30,000 L. kg −1 h −1 and 600 °C, which is 1.68 times as large as that of Ni/MgAl 2 O 4 -MM. The performance remains stable over 30 h. The characterizations manifest that the high specific surface area of Ni/MgAl 2 O 4 -LDH can introduce highly dispersed Ni on the surface. Kinetics analysis implies promoted NH 3 decomposition reaction and alleviated H 2 poisoning for Ni/MgAl 2 O 4 -LDH. A roughly linear relationship is obtained by fitting the curves of dispersed Ni on the surface vs the reaction orders regarding H 2 and NH 3 . This indicates that enhanced NH 3 decomposition performance can be ascribed to the strengthened NH 3 decomposition reaction and weakened H 2 poisoning by the highly dispersed Ni on the MgAl 2 O 4 -LDH surface. This work provides an opportunity to develop highly active and cost-effective catalysts to produce hydrogen via NH 3 decomposition.
研究领域:
化学工程
·
能源科学
✓ 已验证
DOI
高影响因子
FUEL
·
2021
·
IF 6.609
Jinlei Chen,Dechao Wang,Fenqiang Luo,Xinyu Yang,Xingyong Li,Shuirong Li,Yueyuan Ye,Duo Wang,Zhifeng Zheng
Production of valuable chemicals and fuels from waste animal fat and vegetable oils can serve as alternatives to fossil energy. In this study, the selective production of alkanes and higher fatty alcohol via hydrodeoxygenation (HDO) of palmitic acid over red mud-supported nickel catalysts (Ni/RM) was reported. Meanwhile, the study has investigated the effect of Ni loading, reaction temperature, hydrogen pressure on the HDO of palmitic acid, analyzed the reusability of Ni/RM and explored the possible reaction mechanism. The results show that palmitic acid is completely converted over 7%Ni/RM. The selectivity of fatty alcohol and alkanes are 92.54% (260 °C) and 100% (300 °C), respectively. Ni/RM has shown the highest catalytic performance as compared to commercial Ni/SiO 2 and Ni/γ-Al 2 O 3 catalysts. The 7%Ni/RM also demonstrates stable catalytic performance after multiple times of reuse. Moreover, hexadecanol plays an important role in hydrodeoxygenation, decarbonylation, and decarboxylation routes.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
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
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
·
2024
·
IF 3.8
Chengjie Duan,Kun Li,Wenbo Ye,Weitao Mao,Guangke He,Xiang Liu
Graphical Exploring the impact of structural variations in organic acids on catalyst properties unveils crucial insights for enhancing arene hydrogenative activity. The Ni catalyst, supported by hydroxyapatite and aided by a hydroxy-dicarboxylic acid (tartaric acid) with an optimal ratio, resulted in relatively smaller Ni nanoparticles, a higher Ni 0 proportion, and increased acidic sites, showcasing exceptional hydrogenation performance. Developing non-noble metal catalysts that can efficiently and selectively hydrogenate arenes remains a significant challenge. In this study, we developed efficient Ni catalysts for the arene hydrogenation based on an organic acid-regulated impregnation strategy. These easily accessible Ni catalysts demonstrated exceptional efficiency, selectivity, reusability, and good substrate compatibility. The influence of carbon chain lengths and side-chain hydroxyl or amino groups on dicarboxylic acids used in the catalyst preparation was comprehensively investigated. Characterizations and kinetic studies demonstrated the influence of organic acids on the size of Ni nanoparticles, the proportion of metallic nickel, and the strength of surface acidity. These factors influenced the activation of arene and hydrogen, thereby affecting the hydrogenative activity. Notably, hydroxyapatite-supported Ni catalyst, assisted by tartaric acid (Ni-TA/HAP) with an appropriate tartaric acid-to-nickel ratio, resulted in relatively smaller Ni nanoparticles, an increased proportion of Ni 0 , and more acidic sites, thereby exhibiting the best hydrogenation performance.
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
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
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Xiaonan Xu,Nana Luo,Wan-Hui Wang,Ming Bao,Jiasheng Wang
Fatty acid hydrogenation is an important method for the production of fatty alcohols. The combination of Ni and Mo has been reported to be an effective and low-cost catalyst. However, the effect of Mo doping has yet to be fully understood. Here Ni-MoOx/TiO2 catalysts were prepared via simple impregnation. and the enhancement effects of Mo doping were comprehensively revealed. First, MoOx can attract electrons from Ni, reduce the electron density of Ni to improve the intrinsic activity of Ni, and form a Niδ+-(MoOx)δ− heterojunction to induce H2 heterolytic cleavage to active hydrogen ions. Second, the reduction of MoOx generates oxygen vacancies, which can absorb C═O of the fatty acid and facilitate the reaction progression. Third, a Ni1–xMox solid solution can be formed, which can increase the hydrogen adsorption quantity and accelerate the reaction rate. Finally, the bond strength of Mo–O is found to be the most optimum that can absorb the fatty acids while releasing the alcohols so as to recover the oxygen vacancies and avoid overhydrogenation. Therefore, high activity and selectivity for the hydrogenation of carboxylic acid substrates to alcohols can be obtained. Under significantly milder conditions (155 °C, 3 MPa H2) the catalyst provided a 98% yield of lauryl alcohol from lauric acid hydrogenation with a low activation energy of 40.1 kJ/mol. This work could provide an insightful understanding about the effects of Mo doping to Ni on catalyzing hydrogenation reactions.
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
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Qing Zhang,Boyun Gao,Fan Sun,Huijiang Huang,Yan Xu,Feng Gao,Yan Wang,Yujun Zhao
This study reports a stable catalyst for NH 3 decomposition to hydrogen. The precursor of SiO 2 @NP was prepared by hydrothermal method, and the hydrothermal treatment of spherical SiO 2 results in etching of SiO 2 and the formation of nickel phyllosilicate, which greatly increase specific surface area of the catalyst. Ru is loaded onto the SiO 2 @NP by incipient wetness impregnation, forming the catalyst 1Ru/SiO 2 @NP. At a gas hourly space velocity (GHSV) of 30,000 mL NH3 (g × h) −1 and 650 °C, the conversion of ammonia over 1Ru/SiO 2 @NP reaches 98%. Furthermore, the catalyst maintains excellent stability during a period of 210 h at 600 °C. To investigate the origination of activity and stability, various characterizations have been used. In its reduced form, Ni and Ru stay metallic, and Ru–Ni interactions are realized. Both high specific surface area and Ru–Ni interactions allow the generation of small metallic particles that are resistant to sintering during reaction process, thus improving the activity and stability of the catalyst. This study provides new insights and references for the preparation of efficient and stable catalysts for NH 3 decomposition.
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
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Feiqiang Guo,Xingmin Zhao,Kuangye Peng,Shuang Liang,Xiaopeng Jia,Lin Qian
Steel slag (SS) contains high amounts of metal oxides and could be applied as the catalyst or support material for the reforming of biomass derived tar. In this research, steel slag supported nickel catalysts were prepared by impregnation of a small amount of nickel (0–10 wt%) and calcination at 900 °C, and then tested for the catalytic reforming of biomass primary tar from pine sawdust pyrolysis . The steel slag after calcination was mainly composed of Fe 2 O 3 and MgFe 2 O 4 , and granular NiO particles was formed and highly dispersed on the surface of nickel loaded steel slag which lead to a porous structure of the catalysts. The steel slag showed good activity on converting biomass primary tar into syngas , and its performance can be further enhanced by the loading of nickel. The yield of H 2 increased significantly with the increase of nickel loading amount, while excessive nickel loading resulted in the decrease in CO and CH 4 yields and significant increase in CO 2 yield. The presence of steam contributed to enhancing the tar steam reforming as well as reactions between steam and produced gases, while decrease the contact probability between the reactants and the active sites of catalysts, leading to a little decrease in tar conversion efficiency but significant increase in syngas yield. The iron and nickel oxides were reduced by the syngas (CO and H 2 ) from the biomass pyrolysis, and stable and porous structure was formed on the surface of the nickel loaded catalysts during tar reforming.
研究领域:
能源科学
·
催化化学
✓ 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）