APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Yangyang Zhou,Chen Chen,Qiling Li,Yanbo Liu,Ting Wei,Youzhen Liu,Zebing Zeng,Darren Bradshaw,Bing Zhang,Jia Huo
Hydrogenation of unsaturated biomass in a control manner is highly desirable but challenging, especially under mild conditions. We here report selective hydrogenation of α,β-unsaturated aldehydes (UALs), featuring a precise control of all potential products by adjustment of the role of ammonia borane (AB) in transfer and/or catalytic hydrogenation. The hydrogenation can be readily operated in neat water without using any external H 2 -source, because AB as the H 2 -source is favorable in aqueous solution. Impressively, unsaturated alcohols are prepared in 100% conversion by the room-temperature transfer hydrogenation of UALs with AB, while saturated aldehydes are obtained in 100% conversion and > 90% selectivity with high activity ( i.e ., turnover frequency = 0.98 s −1 for cinnamaldehyde), by the catalytic hydrogenation with H 2 released from AB and Pd immobilized on two-dimensional metal organic layer. On the other hand, UALs can be completely converted into the saturated alcohols through a combination of transfer and catalytic hydrogenation in one pot. This strategy can be extended to more than 8 types of UALs, and provides a facile way to fine-control the selective hydrogenation of unsaturated compounds with competing bonds.
研究领域:
化学
·
生物质能
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2019
·
IF 5.128
Xue-Ke Li,Zhi-Min Zong,Yi-Feng Chen,Zheng Yang,Guang-Hui Liu,Fang-Jing Liu,Xian-Yong Wei,Bao-Jun Wang,Feng-Yun Ma,Jing-Mei Liu
A highly active difunctional Ni-Mg 2 Si/γ-Al 2 O 3 was prepared by thermally decomposing nickel tetracarbonyl onto γ-Al 2 O 3 impregnated with Mg 2 Si. The non-catalytic hydroconversion (NCHC) and catalytic hydroconversion (CHC) of the extract ( E ) and extraction residue (ER) from Yinggemajianfeng lignite were investigated over Ni-Mg 2 Si/γ-Al 2 O 3 at 240 °C in n -hexane. Benzyloxybenzene and oxybis(methylene)dibenzene were used as lignite-related model compounds to speculate the possible mechanisms for the catalytic hydrocracking and hydrogenation over Ni-Mg 2 Si/γ-Al 2 O 3 . As a result, more organic matter in ER was converted to soluble portion (SP) by the CHC than by the NCHC. The main SP from the CHC are chain alkanes and cyclanes, while that from the NCHC is rich in arenes and oxygen-containing organic compounds. The results indicate that Ni-Mg 2 Si/γ-Al 2 O 3 effectively catalyze the hydrocracking of >C alk –O– linkages and the hydrogenation of aromatic rings in E and ER.
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
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Qinglei Wu,Chenyang Shen,Kaihang Sun,Menghui Liu,Chang-jun Liu
Tuning the hydrogenation activity of Pd is an effective method to achieve selective hydrogenation of acetylene. The previous study shows that Pd has a strong interaction with In 2 O 3 , causing a significant change in the electronic structure of the palladium catalyst. Herein, Pd/In 2 O 3 @SiO 2 was prepared by a deposition-precipitation method for selective hydrogenation of acetylene. After the reduction by flowing hydrogen, Pd-In intermetallic compounds can be formed. The concentration of the formed intermetallic compounds is closely associated with the reduction temperature. The Pd-In intermetallic compounds suppress the hydrogen activation ability of Pd and significantly weaken the adsorption of ethylene. Especially, a weak adsorption of di-σ-bonded ethylene is observed, which facilitates the desorption of ethylene and promotes the ethylene selectivity in the semi-hydrogenation of acetylene. The experimental study confirms that there exists an optimum reduction temperature (250 °C) for the formation of the Pd-In intermetallic compounds, with which ∼ 80 % ethylene selectivity and 100 % acetylene conversion have been achieved at 140 °C.
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
Applied Catalysis O: Open
·
2024
·
IF 0
Kaiyang Xu,Lingfeng Weng,Lizhi Wu,Li Tan,Yu Tang
Cyclohexanone is a key raw material for manufacturing nylon and other chemicals. The sustainable conversion of biomass-derived phenol to cyclohexanone meets the requirements of sustainable development goal but still be challenging. Herein, a catalyst containing isolated Pd cations in zeolite, namely Pd 1 /ZSM-5, is investigated for the partial hydrogenation of phenol to cyclohexanone. Under 140 °C and 1.5 MPa of initial hydrogen pressure, the conversion of phenol reaches 95.6% with the selectivity to cyclohexanone of 99.9%. Besides, the turnover rate (TOR) of partial hydrogenation of phenol reaches 382.7 h −1 . The mild adsorption affinity of cyclohexanone on catalytic sites leads to the high selectivity. Moreover, as unveiled by surface reactivity of phenol monitored by in-situ infrared spectrum, the oxygen atom of phenol hydroxyl group is adsorbed on the Brönsted acid site of Pd 1 /ZSM-5 as the key reaction step. The reaction intermediate involves the partial hydrogenation of benzene ring of phenol.
研究领域:
催化化学
·
绿色化学
·
可持续发展
·
生物质转化
✓ 已验证
DOI
JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Bolong Jiang,Tianhan Zhu,Hua Song,Feng Li
The Fe-doped Ni 2 P/Fe-SBA-15 was prepared by the temperature programmed reduction method at a relative low temperature of 673 K. The effect of Fe on the catalytic performance for benzofuran (BF) hydrodeoxygenation (HDO) and dibenzothiophene (DBT) hydrodesulfurization (HDS) were investigated. The catalysts were characterized by means of X-ray diffraction (XRD), N 2 adsorption-desorption, inductively coupled plasma mass spectrometry (ICP-MS), X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption of ammonia (NH 3 -TPD), and transmission electron microscope (TEM) and CO uptakes. The results indicate the incorporation of Fe into SBA-15 contributes to the exposure of smaller Ni 2 P particles (5.6 nm) with an uniform dispersion, along with enhancement of weak and medium acid strengths . Compared with Ni 2 P/SBA-15, the Fe-doped Ni 2 P/Fe-SBA-15 exhibited a much higher BF conversion of 91.7% with an improved total deoxygenated product yield of 83.3%. The excellent HDO performance of Ni 2 P/Fe-SBA-15 can be ascribed to the exposure of highly-dispersed smaller Ni 2 P particles. Meanwhile, the improved dehydration of 2-EtPh to EB and the high deoxygenated product selectivity can be attributed to the enhanced acidity. As compared to the Ni 2 P/SBA-15, the Fe-doped Ni 2 P/Fe-SBA-15 showed a higher DBT HDS activity of 96.3% with the BP formation at a great proportion of 90.3%, indicating that DBT was mainly transformed through the desulfurization pathway during HDS.
研究领域:
催化化学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2018
·
IF 4.667
Guanhua Xing,Siyang Liu,Qingxin Guan,Wei Li
This paper focused on the isomerization and cracking of n -alkanes to synthesize bio-jet fuel. A series of SAPO-11 supports with different Si/Al molar ratio (0.2, 0.4, 0.6) were prepared, characterized, and evaluated by the hydroisomerization on hydrodeoxygenation product of castor oil. As a result, a Ni-Mo/SAPO-11(0.4) catalyst with hollow tubular structure and moderate acidic strength exhibited optimum conversion (97.2%) and jet fuel selectivity (81.6%) in the reaction. Subsequently, Ni-Mo/SAPO-11(0.4) was selected to carry out further experiments on studying the hydroisomerization and hydrocracking of long chain n -alkanes. The results show that increasing temperature may promote hydroisomerization and hydrocracking. Temperature is more favorable for the reaction with the length of the carbon chain decreasing, no matter conversion, hydrocracking degree or isomerization tendency. The product selectivity of different n -alkanes is associated with the carbon number. In reaction to n -C 18 , Ni-Mo/SAPO(0.4) surpassed the other two catalysts in the conversion and i/n ratio at 623 K which is the optimum temperature.
研究领域:
催化化学
·
能源科学
✓ 已验证
DOI
高影响因子
Chemical Science
·
2013
·Vol. 5
·期 3
·1082-1090
·
IF 8.314
Gang Lu,Peng Zhang,Dongqing Sun,Lei Wang,Kebin Zhou,Zhi-Xiang Wang,Guo-Cong Guo
Clean gold surface is inactive toward H2, however, computations, aided by experiments, reveal that gold surface could serve as a Lewis acid coupling with Lewis bases (e.g. imine and nitrile) to construct effective frustrated Lewis pairs (FLPs) to activate H2 and subsequently to achieve hydrogenation of small imines and nitriles. The Lewis base-coupled Au FLPs avoid tight adsorption of Lewis bases to gold surface via repulsion between nitrogen lone pair and the filled d-band electrons of the gold surface. This is different from the normal FLPs that use sterically demanding groups or a molecular scaffold to prevent formation of stable Lewis acid–base complexes. The enhanced reactivity of the gold surface toward H2 is due to the synergetic catalytic effects of Lewis acid (Au surface) and the coupled Lewis base (imine or nitrile), which is supported by projected density of states (PDOS) analyses. Among Cu, Ag and Au surfaces, Au surface exhibits such reactivity most significantly, because Au is much more electronegative than Cu and Ag. The study enriches the FLP chemistry by adding a new type (heterogeneous) of FLPs and reveals a new reaction mode for gold surface.
研究领域:
催化化学
·
表面科学
·
理论计算化学
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
·
2015
·Vol. 7
·期 16
·2485-2492
·
IF 4.556
Guangyue Xu,Jianhua Guo,Ying Zhang,Yao Fu,Jinzhu Chen,Longlong Ma,Qingxiang Guo
Graphical Phosphate aids palladium: A highly reactive, selective, compatible, stable and low-cost catalytic system for selective hydrogenation of phenol to cyclohexanone is described, which consists of well-dispersed Pd nanoparticles anchored to the hydroxylapatite surface that supports the specificity through its basic sites. The production of pure cyclohexanone under mild conditions over catalysts with high reactivity, selectivity, compatibility, stability, and low cost is still a great challenge. Here we report a hydroxyapatite-bound palladium catalyst (Pd–HAP) to demonstrate its excellent performance on phenol hydrogenation to cyclohexanone. Based on catalyst characterization, the Pd nanoclusters (≈0.9 nm) are highly dispersed and bound to phosphate in HAP. Only basic active sites on HAP surface are detected. At 25 °C and ambient H 2 pressure in water, phenol can be 100 % converted into cyclohexanone with 100 % selectivity. This system shows a universal applicability to temperature, pH, solvent, low H 2 purity, and pressure. The catalyst reveals high stability to be recycled without deactivation or morphology change; and Pd nano-clusters barely aggregate even at 400 °C. During the reaction, HAP adsorbs phenol, and Pd nanoclusters activate and spillover H 2 . The mechanism is also investigated, proposed, and verified.
研究领域:
催化化学
·
材料科学
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 9
·1-11
·
IF 2.4
Du Yuhao,Hu Dawei,Wang Zhen,Hu Anpeng,Han Wei,Pu Ning
The hydrotreating of residual oil is crucial for producing cleaner fuels, as catalyst deactivation due to metal deposits, particularly nickel (Ni) and vanadium (V), remains a significant challenge. Contrary to the conventional view that metal deposits invariably poison catalysts, our recent studies have observed an unexpected enhancement in the activity of commercial NiMo/Al 2 O 3 catalysts during industrial operation. This study systematically investigates the mechanism behind this counter-intuitive phenomenon, with a particular focus on the effects induced by nickel. X-ray photoelectron spectroscopy (XPS) analysis revealed that low-concentration of Ni deposits preferentially formed highly active NiMoS phases during the reaction process, thereby minimized the formation of NiS x , a typical poisoning species. This increases the number of reactive sulfur sites, boosting the hydrodesulfurization (HDS) activity for 4,6-dimethyldibenzothiophene (4,6-DMDBT), with the conversion rate rising from 17.1 to 73.3%. Similar promoting trends were also observed in conventional NiMo/Al 2 O 3 catalysts upon Ni deposition, demonstrating the generality of this effect. Our findings not only provide new insights into the dual role of Ni deposits in catalyst performance but also offer a promising strategy designing industrial metal-poisoning-resistant catalysts with significantly enhanced operational lifespan as well as catalytic performance.
研究领域:
催化化学
·
化学工程
·
材料科学
·
石油炼制
·
表面科学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Qinglei Wu,Chenyang Shen,Chang-jun Liu
Suppressing the excessive hydrogenation capacity of palladium has great significance for selective hydrogenation of acetylene. Herein, an amino acid (histidine or His in abbreviation) modified Pd/SiO 2 catalyst (Pd-His/SiO 2 ) for selective hydrogenation of acetylene was prepared by incipient wetness impregnation, followed by hydrogen reduction at 240 °C. The intense interaction between Pd and histidine greatly affects the structure and properties of Pd-His/SiO 2 . The Pd nanoparticles are highly dispersed on the support with an average diameter of 1.0 nm and positively charged. The use of histidine weakens the adsorption of acetylene and ethylene on the metal. Especially, the adsorption of di-σ-bonded ethylene is significantly impaired on the catalyst, which is beneficial to improve the ethylene selectivity. The conversion of acetylene is up to 100.0 % at 160 °C on Pd-His/SiO 2 while the ethylene selectivity reaches 81.5 %. A 50-hour test at 160 °C confirms the good stability of Pd-His/SiO 2 .
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
Scientific Reports
·
2017
·Vol. 7
·期 1
·1-11
·
IF 4.259
Lu Xinhuan,He Jie,Jing Run,Tao Peipei,Nie Renfeng,Zhou Dan,Xia Qinghua
Biocarbon supported Ni catalysts have been prepared by facile impregnation of Ni species by microwave-heating and used for selective hydrogenation of nitrobenzene to cyclohexylamine. These catalysts were characterized by X-ray diffraction, Raman spectra, N2 sorption measurement, X-ray photoelectron spectroscopy, temperature programmed reduction of H2 and H2 temperature-programmed desorption. The morphology and particle size of catalysts were imaged by scanning electron microscope and transmission electron microscope. For the hydrogenation of nitrobenzene to cyclohexylamine, 10%Ni/CSC-II(b) exhibits the best catalytic activity to achieve 100 mol% conversion of nitrobenzene and 96.7% selectivity of cyclohexylamine under reaction conditions of 2.0 MPa H2 and 200 °C, ascribed to high dispersion of Ni species and formation of nanosized Ni particles on the support aided by microwave-heating. Thus-prepared Ni/CSC catalyst is greatly activated, in which the addition of precious metal like Rh is totally avoided.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Hongmei Yang,Menglu Xu,Lili Zhang,Weiwei Fang,E. Liu,Huaxin Zhang
A benzotrizole-based hyper-crosslinked polymer (HCP) was employed to load cobalt and prepare a novel metal-containing nitrogen-doped carbon catalyst for the selective hydrogenation of quinoline . The high porosity, large surface area and nitrogen-containing monomer of HCP made a positive contribution to metal loading. Owing to the excellent thermostability of HCP, the original porous texture of HCP was partially reserved during pyrolysis , which resulted in highly dispersive Co species in the N-doped carbon material. The remaining mesopores in Co@CN catalyst during thermal decomposition provided available diffusion channels for substrates, which facilitated their full contact with catalytic active sites and their effective conversion. The prepared Co@CN catalyst achieved a conversion rate of 100% and a selectivity of 100% in the hydrogenation of quinoline into 1, 2, 3, 4-tetra-hydroquinoline in water at 100 °C under 3 MPa H 2 . The as-synthesized catalyst had good reuse performance, exhibiting >95% conversion rate and >99% selectivity even after 12 cycles. Moreover, the catalyst could also be applied to the selective hydrogenation of a serial of quinoline derivatives. The study provided a useful strategy for constructing metal-doped carbon materials which might be applicable for other metals and other reactions.
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）