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A Study on the Characterization of Hydrodesulfurization Catalysts by Magnetic Properties of Co toward the Development of Highly Active Catalysts

Co磁性表征加氢脱硫催化剂的研究及高活性催化剂的开发

基本信息

批准号：
16360404
负责人：
OKAMOTO Yasuaki
金额：
$ 8.64万
依托单位：
Shimane University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (B)
财政年份：
2004
资助国家：
日本
起止时间：
2004 至 2006
项目状态：
已结题

项目摘要

The salient findings in this research project are as follows:1. The Co sulfide species in the Co-Mo-S phase show an antiferromagnetic behavior. The magnetic susceptibility of the Co atoms was simulated by a theoretical equation assuming the formation of Co dimmer clusters with Co-S-Co bonding, in conformity with the NO adsorption, which shows the maximum NO adsorption capacity is NO/Co = 1/1 molar ratio. The proposed Co-Mo-S structure was supported by our recent XAFS analysis of CVD-Co/MoS_2 catalysts.2. The addition of boron to Co-Mo/Al_2O_3 was studied to improve the hydrodesulfurization activity. It was found that the addition of boron increases the TOF by 1.6 times, indicating the ace reactions, accordingly resulting in weaker interactions between Mo oxides and Al_2O_3 surface. The dispersion of MoS_2 was decreased by the addition of boron because of ence in the dispersion of MoS2 particles.3. The intrinsic activity of the Co-Mo-S structure was increased by sulfiding at a high temperatur-Mo-S structure showed a much less activity because of strong Mo-O-Al bonding. However, the addition of boron decreased the sulfidation temperature for the formation of Type II. The thermal stability of the Co-Mo-S phase was decreased by the addition of boron.4. Highly dispersed Co sulfide clusters were successfully prepared in zeolite pores using Co(CO)_3NO as a precursor. The structure depended on the type of the host zeolite. It was found that Co sulfide clusters react with zeolite protons to form Co2+ cations liberating H_2S. The hydrodesulfurization activity of the Co_sulfide clusters depended on the structure and residual OH groups.5. It is proposed that highly active hydrotreating catalysts are prepared by synthesizing highly dispersed Co-Mo-S Type II by modifying the interactions between MoS_2 particles and support surface. Simultaneous use of boron and chelating agents will be very effective for the developments of highly active ultra-deep hydrodesulfurization catalysts.

本研究的主要发现如下：1. Co-Mo-S相中的硫化钴物种表现出反铁磁行为。通过理论方程模拟了Co原子的磁化率，结果表明，Co/Co = 1/1摩尔比时对NO的最大吸附量为NO/Co = 1/1。我们最近对CVD-Co/MoS_2催化剂的XAFS分析支持了所提出的Co-Mo-S结构.研究了硼对Co-Mo/Al_2O_3加氢脱硫活性的影响。结果表明，硼的加入使飞行时间增加了1.6倍，表明发生了ace反应，从而减弱了Mo氧化物与Al_2O_3表面的相互作用。硼的加入降低了MoS_2的分散性，这是因为硼的加入影响了MoS_2的分散性.高温硫化可提高Co-Mo-S结构的本征活性，而Mo-S结构由于Mo-O-Al键的存在，活性大大降低。然而，硼的加入降低了形成II型的硫化温度。硼的加入降低了Co-Mo-S相的热稳定性.以Co（CO）3 NO为前驱体，在沸石孔中成功地制备了高分散的硫化钴团簇。其结构取决于主体沸石的类型。发现Co硫化物团簇与分子筛质子反应生成Co ~（2+）离子，释放出H_2S。硫化钴簇合物的加氢脱硫活性取决于簇合物的结构和残余羟基.提出了通过改性MoS_2颗粒与载体表面的相互作用，合成高分散Co-Mo-S Ⅱ型催化剂，制备高活性加氢精制催化剂的设想。硼和螯合剂的同时使用将是开发高活性超深度加氢脱硫催化剂的有效途径。

项目成果

期刊论文数量（38）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Effect of Boron Addition on the Intrinsic Activity of Al_2O_3-supported Co-W and Co-Mo Sulfide Catalysts for the Hydrodesulfurization of Thiophene

添加硼对Al_2O_3负载Co-W和Co-Mo硫化物催化剂噻吩加氢脱硫本征活性的影响

DOI：
发表时间：
2006
期刊：
Bull. Chem. Soc. Jpn. 79
影响因子：
0
作者：
Usman;Takeshi Kubota;Ichiro Hiromitsu;Yasuaki Okamoto;Usman;Usman
通讯作者：
Usman

Thermal Stability of the Co-Mo-S Sturucture as Studied bu a CVD Technique using Co(CO)_3NO

使用 Co(CO)_3NO 的 CVD 技术研究 Co-Mo-S 结构的热稳定性

DOI：
发表时间：
2006
期刊：
Ind. Eng. Chem. Res. 45
影响因子：
0
作者：
Usman;Takeshi Kubota;Ichiro Hiromitsu;Yasuaki Okamoto;Usman;Usman;Usman
通讯作者：
Usman

The Structure of the Active Sites of Co-Mo Hydrodesulfurization Catalysts as Studied by Magnetic Susceptibility Measurement and NO Adsorption

磁化率测量和NO吸附研究Co-Mo加氢脱硫催化剂活性位点结构

DOI：
发表时间：
2005
期刊：
J. Phys. Chem. B 109
影响因子：
0
作者：
Takeshi Kadono;Takeshi Kubota;Ichiro Hiromitsu;Yasuaki Okamoto;Usman;Usman;Takeshi Kadono;Yasuaki Okamoto
通讯作者：
Yasuaki Okamoto

Effect of Boron Addition on a MoO_3/Al_2O_3 Catalyst : Physicochemical Characterisation

添加硼对 MoO_3/Al_2O_3 催化剂的影响：物理化学表征

DOI：
发表时间：
2005
期刊：
Appl. Catal. A, General 286
影响因子：
0
作者：
Takeshi Kadono;Takeshi Kubota;Ichiro Hiromitsu;Yasuaki Okamoto;Usman;Usman;Takeshi Kadono;Yasuaki Okamoto;Takeshi Kubota;Usman
通讯作者：
Usman

Characterization of highly dispersed cobalt sulfide catalysts by X-ray absorption fine structure and magnetic properties