Methanation of syngas over coral reef-like Ni/Al_2O_3 catalysts

Coral reef-like Ni/Al2O3 catalysts were prepared by co-precipitation of nickel acetate and aluminium nitrate with sodium carbonate aqueous solution in the medium of ethylene glycolye.Methanation of syngas was carried out over coral reef-like Ni/Al2O3 catalysts in a continuous flow type fixed-bed reactor.The structure and properties of the fresh and used catalysts were studied by SEM,N2 adsorption-desorption,XRD,H2-TPR,O2-TPO,TG and ICP-AES techniques.The results showed that the coral reef-like Ni/Al2O3 catalysts exhibited better activity than the conventional Ni/Al2O3-H2O catalysts.The activities of coral reef-like catalysts were in the order of Ni/Al2O3-673Ni/Al2O3-573Ni/Al2O3- 473Ni/Al2O3-773.Ni/Al2O3-673-EG catalyst showed not only good activity and improved stability but also superior resistance to carbon deposition,sintering,and Ni loss.Under the reaction conditions of CO/H2（molar ratio）=1：3,593 K,atmospheric pressure and a GHSV of 2500 h-1,CH4 selectivity was 84.7%,and the CO conversion reached 98.2%.

Effect of Alumina Particle Size on Ni/Al2O3 Catalysts for p-Nitrophenol Hydrogenation

The catalytic hydrogenation of p-nitrophenol to p-aminophenol was investigated over Ni/Al2O3 catalyst on alumina support with different particle size. It is found that support particle size has significant influences on physiochemical properties and catalytic activity of the resulting Ni/Al2O3 catalyst, but little influence on the selec-tivity. At a comparable amount of Ni loading, the catalytic activity of Ni/Al2O3 prepared with alumina support of smaller particle size is lower. The reduction behavior of the catalyst is a key factor in determining the catalytic activity of Ni/Al2O3 catalyst. The supported nickel catalyst 10.3Ni/Al2O3-3 improves the life span of the membrane by reducing fouling on the membrane surface compared to nano-sized nickel.

Effects of Cerium Oxide on Ni/Al_2O_3 Catalysts for Decomposition of CH_4 and C_2H_4

Characteristics of carbon deposition of CH 4 and C 2H 4 decomposition over supported Ni and Ni Ce catalysts were studied by using a pulse reaction as well as BET, TPR, XPS and hydrogen chemisorption techniques. It is found that there is a metal semiconductor interaction (MScI) in the Ni Ce catalyst, and the effect of MScI on the carbon deposition of CH 4 decomposition is opposite to that of C 2H 4. A novel model of carbon deposition of CH 4 or C 2H 4 decomposition was proposed.

Carbon dioxide reforming of methane on monolithic Ni/Al_2O_3-based catalysts

Nickel-alumina catalysts supported on cordierite monoliths of honeycomb structure surpass essentially the conventional granulated ones with respect to the output in carbon dioxide reforming of methane. Adjusting the surface acid-base properties of catalysts by introduction of alkali metal （Na, K） oxides inhibits the carbonization and as a result, improves the operational stability of these catalysts. An effect of promotion of nickel-alumina based composite doped by lanthanum oxide is found. This effect, caused by an additional route for the CO2 activation on Ni-La2O3/Al2O3/cordierite catalyst, is displayed in increase of methane conversion under conditions of an oxidant excess.

Selective Hydrogenation of Butyne-1,4-diol to Butane-1,4-diol over Ni/Al_2O_3-SiO_2 Catalysts

Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by a series of characterization techniques including BET, XRD, SEM, EDX-mapping, TEM, H_2-TPR, XPS, NH_3-TPD and Py-FTIR. Compared to Ni/Al_2O_3 catalyst, the SiO_2-doped samples exhibited better B_3D conversion. SiO_2 could help to form a strong interaction between NiO with the support, which inhibited Ni agglomeration at high temperature, improved the Ni dispersion, and enhanced the hydrogenation activity. B_1D selectivity was mainly influenced by the quantity of Lewis acid sites in addition to the Ni dispersion. The catalyst with a silica loading of 6.4% demonstrated an excellent selectivity of 75.18%(by 13% higher than the contrastive Ni/Al_2O_3 catalyst), which was attributed to the larger amount of Lewis acid sites and the moderate interaction between NiO with the support, which could facilitate the nickel dispersion on a preferable surface area of 176.3 m^2/g of support.

Oxidative desulfurization of dibenzothiophene over Fe promoted Co–Mo/Al_2O_3 and Ni–Mo/Al_2O_3 catalysts using hydrogen peroxide and formic acid as oxidants

This work reports the enhancing effect of a highly cost effective and efficient metal, Fe, incorporation to Co or Ni based Mo/Al2O3 catalysts in the oxidative desulfurization （ODS） of dibenzothiophene （DBT） using H2O2 and formic acid as oxidants. The influence of operating parameters i.e. reaction time, catalyst dose, reaction temperature and oxidant amount on oxidation process was investigated. Results revealed that 99% DBT conversion was achieved at 60℃ and 150 min reaction time over Fe-Ni-Mo/Al2O3. Fe tremendously enhanced the ODS activity of Co or Ni based Mo/Al2O3 catalysts following the activity order：Fe-Ni-Mo/Al2O3 〉 Fe-Co-Mo/Al2O3 〉 Ni-Mo/Al2O3 〉 Co-Mo/Al2O3, while H2O2 exhibited higher oxidation activity than formic acid over all catalyst systems. Insight about the surface morphology and textural properties of fresh and spent catalysts were achieved using scanning electron microscopy （SEM）, X-ray diffraction （XRD）, energy dispersive X-ray （EDX） analysis, Atomic Absorption Spectroscopy （AAS） and BET surface area analysis, which helped in the interpretation of experimental data. The present study can be deemed as an effective approach on industrial level for ODS of fuel oils crediting to its high efficiency, low process/catalyst cost, safety and mild operating condition.

Sn修饰的Ni/Al_2O_3对降解N,N-二甲基甲酰胺制氢反应的催化性能

利用浸渍法制备了一系列不同含量Sn修饰的Ni/Al2O3催化剂(Ni-Sn/Al2O3),并考察了催化剂对降解N,N-二甲基甲酰胺(DMF)制氢反应的催化性能。结果表明,利用Sn修饰Ni/Al2O3催化剂提高了其降解DMF制氢活性,当Sn/Ni摩尔比为0.1时,H2的产率从Ni/Al2O3催化剂上的43.4μmol/min提高到69.8μmol/min。但当Sn含量进一步增加时,DMF转化率和H2产率都明显下降。催化剂的N2物理吸附、X射线衍射(XRD)和H2程序升温还原(H2-TPR)表征结果表明,Ni-Sn/Al2O3催化剂中形成了Ni3Sn2的合金,且Ni-Sn/Al2O3与Sn-Raney Ni催化剂具有相近的晶体结构,但Ni-Sn/Al2O3比Sn-Raney Ni具有更高的比表面积及降解DMF制氢的活性。

泡沫Ni/Sn复合钎料超声波钎焊Al_2O_3陶瓷接头组织及力学性能研究

采用泡沫Ni增强Sn基复合钎料片,通过超声波辅助钎焊工艺对Al_2O_3陶瓷进行了低温连接,研究了不同钎焊时间对Al_2O_3接头显微结构及抗剪强度的影响。结果表明,钎焊时间从4 s延长至12 s时,Ni骨架从多边形向条状转变,钎缝宽度从90μm减小到30μm,Sn金属逐渐填充到泡沫Ni的空隙中,钎缝中的缺陷逐渐减少至消失。在泡沫Ni骨架表面形成了Ni_3Sn_4金属间化合物层,其厚度随钎焊时间的延长而增大,同时接头的抗剪强度呈现先提高后降低的趋势。钎焊时间为8 s时,接头获得了最佳的抗剪强度值38.6 MPa。

The nature of the deactivation of hydrothermally stable Ni/SiO2–Al2O3 catalyst in long-time aqueous phase hydrogenation of crude 1,4-butanediol

The deactivation of Ni/SiO2-Al2 O3 catalyst in hydrogenation of crude 1,4-butanediol was investigated.During the operation time of 2140 h,the catalyst showed slow activity decay.Characterization results,for four spent catalysts used at different time,indicated that the main reason of the catalyst deactivation was the deposition of carbonaceous species that covered the active Ni and blocked mesopores of the catalyst.The TPO and SEM measurements revealed that the carbonaceous species included both oligomeric and polymeric species with high C/H ratio and showed sheet.Such carbonaceous species might be eliminated through either direct H2 reduction or the combined oxidation-reduction methodologies.

Ni/Al_2O_3上甲烷二氧化碳氧气转化制备合成气的研究

在固定床流动反应装置上，从活性组分的负载量、载体的焙烧温度、反应温度、空速等几个方面考察了Ｎｉ／Ａｌ２Ｏ３催化剂对ＣＨ４ＣＯ２Ｏ２转化制备合成气的催化活性，发现采用１１００℃焙烧的γＡｌ２Ｏ３载体制备的镍负载量为９．１７ｗ％的Ｎｉ／Ａｌ２Ｏ３催化剂，在原料气配比为ＣＨ４∶ＣＯ２∶Ｏ２＝１∶１∶０．５时，低温高空速有利于甲烷部分氧化反应的进行，而高温低空速却有利于甲烷二氧化碳重整反应的进行。通过对催化剂的寿命考察可知，Ｎｉ／Ａｌ２Ｏ３催化剂对ＣＨ４ＣＯ２Ｏ２转化制备合成气具有较好的选择性和稳定性。

MgO添加量对CO甲烷化Ni-Al2O3催化剂结构和性能的影响

采用溶液燃烧法制备CO甲烷化Ni基催化剂,考察助剂MgO添加量对催化剂结构和性能的影响,并探讨MgO添加量-催化剂结构-CO甲烷化性能的构效关系。结果表明,MgO添加质量分数6%的催化剂具有适当的还原温度,其CO转化率、CH 4选择性和收率分别高达99%、97%和94.5%。催化剂寿命实验表明,在24 h反应时间内,6%MgO添加量的催化剂上CO转化率和CH 4选择性分别高达96%和94%以上,表现出较高的活性、选择性和稳定性。

Ni/Al_2O_3催化2-甲基呋喃加氢制2-甲基四氢呋喃性能的研究

采用浸渍法制备了不同NiO含量的Ni/Al_2O_3催化剂,并进行了2-甲基呋喃加氢制2-甲基四氢呋喃性能的考察。结果表明,在制备的NiO负载量为10%、20%、25%、30%和40%的Ni/Al_2O_3催化剂中,随着NiO负载量增加,加氢反应的选择性与2-甲基呋喃的转化率均呈现出先增加后减小的趋势。其原因是由于适当增加NiO负载量有利于催化剂表面活性中心的形成,有利于加氢反应的进行;但是过度负载的NiO容易堵塞Al_2O_3载体中的介孔通道,降低反应的转化率与选择性。在釜式反应器中进行反应,对加氢反应条件进行了优化,发现在反应压力为3 MPa、反应温度150℃、机械搅拌速率为1000 r/min时,Ni/Al_2O_3催化2-甲基呋喃加氢制2-甲基四氢呋喃具有较高的选择性。当NiO负载量为25%时,2-甲基四氢呋喃的选择性最高为97.1%,2-甲基呋喃的转化率达到99.4%。

Effects of MgO promoter on properties of Ni/Al_(2)O_(3) catalysts for partial oxidation of methane to syngas

The effects of MgO promoter on the physico-chemical properties and catalytic performance of Ni/Al_(2)O_(3) catalysts for the partial oxidation of methane to syngas were studied by means of BET,XRD,H2-TPR,TEM and perfor-mance evaluation.It was found that the MgO promoter bene-fited from the uniformity of nickel species in the catalysts,inhibited the formation of NiAl2O4 spinel and improved the interaction between nickel species and support.These results were related to the formation of NiO–MgO solid solution and MgAl_(2)O_(4) spinel.Moreover,for the catalysts with a proper amount of MgO promoter,the nickel dispersiveness was enhanced,therefore making their catalytic performance in methane partial oxidation improved.However,the excessive MgO promoter exerted a negative effect on the catalytic performance.Meanwhile,the basicity of MgO promoted the reversed water–gas shift reaction,which led to an increase in CO selectivity and a decrease in H2 selectivity.The suitable content of MgO promoter in Ni/Al_(2)O_(3) catalyst was∼7 wt-%.

铕对Pt-Sn/γ-Al_2O_3重整催化剂性能的影响

研究了添加RE2O3(RE=Eu)的Pt-Sn/γ-Al2O3重整催化剂的反应性能.研究结果表明添加稀土后,催化剂的液收增加,芳产增加,积炭降低.采用氢氧滴定(TPT)、程序升温还原(TPR)、吡啶红外光谱(IRS)、程序升温氧化(TPO)等对催化剂进行了物化表征.结果表明,催化剂中添加RE2O3之后,催化剂中Pt的两种活性中心不变,但改变了两种活性中心的相对比率,低温活性中心降低,高温活性中心增加;稀土与Pt和Sn之间发生相互作用,产生了电子效应,使得它们的还原峰温向低温移动;载体的酸量减少,酸性减弱.